DESC:FIELD OF INVENTION
[001] The present disclosure relates to devices comprising organic compounds. Particularly, the present disclosure relates to devices comprising organic compounds having multiple redox states.
BACKGROUND OF INVENTION 5
[002] Due to rapid development of information technology, innovative active materials designed for memory and computing devices have become highly desirable and triggered tremendous interest. Memory devices can be defined as electrical switches that retain a state of internal resistance based on the history of applied voltage. Such devices hold several performance characteristics that can 10 potentially exceed conventional integrated circuit technology and are the building blocks of computing architectures such as neuromorphic computing.
[003] However, conventional active materials for memory and computing devices in semiconductors face various challenges due to high demand in achieving higher efficiency and cell downsizing. These challenges gave way to the development of 15 new materials for high-performance information storage, including oxides of metals and semiconducting organic materials. Metal oxides are the most promising candidates for commercial application, but these materials require a high forming voltage/current and a large setting-resetting voltage, which limits their ability to provide a high-density memory. 20
[004] Owing to its distinctive versatility, solution-processability (economic manufacturing) and chemically tuneable functionalities, semiconducting organic materials are of particular interest in electronic devices. Some of the organic devices possess potential to be employed as display devices (such as OLED displays) and flexible electronics (such as chips). The controllability and engineerability in 25 molecular electronics could facilitate innovative computing architectures in the context of artificial intelligence and machine learning.
[005] The dynamics of molecules and ions in molecular computing elements could be engineered to mimic the ionic dynamics in a biological brain. Notably brain is the most intelligent and efficient computing entity even known. Hence, 30 brain inspired electronic platforms made from molecular technologies could 2
facilitate optimal hardware for artificial intelligence, machine learning and edge computing.
[006] The organic platforms could be used for in-memory, in-sensor computing applications which could entrench local intelligence at edge computing platforms.
[007] However, the overall development and commercialization of organic 5 materials-based memory devices is poor. The common problems in these organic materials-based devices arise from insufficient reproducibility, poor endurance, low stability, limited scalability and low switching speed of the device.
[008] Additionally, the understanding regarding switching mechanism tends to be poor because of the structural complexities of the organic materials, making the 10 device optimization further difficult. Generally, in most organic material-based devices, switching behaviour is attributed to structural changes (e.g., cis-trans isomerisation), field-driven polarization, or redox transitions. Moreover, conventional memory devices having organic materials have limited data storage capacity. One of the most effective measures to enhance the data storage capacity 15 is by promoting the number of capacitive states in memory devices.
[009] Therefore, due to increasing demand for advanced sensors, computing and memory devices having high integration density for data storage, organic materials having multiple redox states and fast switching efficiency are a demand of the hour. However, conventional computing systems comprise disjunctive and independent 20 functional and/or operational elements (e.g., sensors, memory, computing units, and such). Such a distributed architecture having disjunctive units would require frequent data exchange thereby impacting the energy efficiencies of such system. The inability to integrate multiple functionalities within a single device architecture has prevented the realization of truly efficient in-memory and in-sensor computing 25 platforms.
[0010] Another critical limitation of existing organic memory materials is their restriction to simple binary states, which fails to exploit the rich electronic structure and multiple oxidation states that organic molecules can potentially offer. The lack of materials capable of exhibiting multiple stable and reproducible electronic states 30 within a single device has hindered the development of high-density memory
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systems and prevented the implementation of complex logic operations in single devices.
[0011] Current organic memory devices also suffer from poor environmental stability, with many materials degrading rapidly under ambient conditions of temperature, humidity, and atmospheric exposure. This instability has prevented 5 their practical application in real-world electronic systems and limited their commercial viability.
[0012] The switching speeds of existing organic memory devices are generally inadequate for modern computing applications, with response times often exceeding microseconds. This slow switching behavior is incompatible with the 10 high-speed requirements of contemporary electronic systems and limits the potential applications of organic memory technologies.
[0013] Additionally, the fabrication processes for organic memory devices often require complex procedures, high-temperature processing, or expensive equipment, which increases manufacturing costs and reduces their commercial attractiveness 15 compared to conventional semiconductor technologies.
[0014] There exists a critical need in the art for organic materials that can overcome these fundamental limitations while providing enhanced functionality, stability, and performance. Such materials would enable the development of next-generation memory and computing systems with unprecedented storage density, energy 20 efficiency, and computational capabilities, while supporting the growing demands of artificial intelligence, machine learning, and edge computing applications.
SUMMARY OF THE INVENTION
[0015] In an aspect of the present disclosure, there is provided a device comprising 25 a molecular memory unit, the molecular memory unit having: a) a first conducting layer; b) a second conducting layer; and c) an organic layer comprising a first surface and a second surface, wherein the organic layer is interposed between the first conducting layer and the second conducting layer; and the organic layer comprises a compound selected from a compound of Formula I, Formula II, its 30 salts, stereoisomers, solvates, or combinations thereof,
4
Formula I
Formula II
wherein 5
R1 is selected from H, Cl, Br, or I;
R2 is selected from H, Cl, CH3, OCH3, Br, I or ;
R’ is selected from Cl, Br, or I;
R3, and R3’, are independently selected from C1-20 alkyl, C2-20 alkenyl, C6-15 aryl, C3-20 cycloalkyl, C1-20 heteroaryl, C3-20 heterocyclyl or stilbene; 10
R4 and R4’ are absent or independently selected from C1-20 alkyl, C2-20 alkenyl, C6-15 aryl, C3-20 cycloalkyl, C1-20 heteroaryl, C3-20 heterocyclyl or stilbene; and
X- is a counter ion selected from Cl-, ClO4-, HSO4-, NO3-, BF4-, PF6-, CF3SO3-, or BPh4-.
[0016] In another aspect of the present disclosure, there is provided a process for 15 preparation of the device as disclosed herein, the process comprising: a) coating a solution of organic layer on a second conducting layer; and b) assembling a first conducting layer upon a second surface of the organic layer to obtain the device.
5
[0017] In yet another aspect of the present disclosure, there is provided an organic layer comprising a compound of Formula I or Formula II, its salts, stereoisomers, solvates, or combinations thereof as defined herein.
[0018] In yet another aspect of the present disclosure, there is provided a use of the device as disclosed herein, or the organic layer as disclosed herein. 5
[0019] In yet another aspect of the present disclosure, there is provided a sensor device comprising the device defined herein, wherein the device exhibits responsive changes in electrical or optical properties upon exposure to environmental stimuli.
[0020] In yet another aspect of the present disclosure, there is provided a computing 10 system comprising an array of devices as defined herein, wherein the array is configured for parallel processing operations.
[0021] In yet another aspect of the present disclosure, there is provided a multifunctional device comprising the device as defined herein, wherein the device simultaneously provides memory, sensing, and computing functionalities 15
[0022] The present approaches also address the issue pertaining to energy efficiency which arises due to the different units (such as memory units, sensors, and so on). The compounds as described herein when used in memory devices are such that they exhibit different functional attributes in response to certain categories of stimuli. Specifically, the type of functional attributes of the memory devices may 20 be expanded by applying additional or varying stimuli. For example, compounds which are used for realizing memory devices, are capable of emitting light. In an example, the different redox states are such that they exhibit or enable different degrees of luminescence. In such cases, the resulting devices (wherein which the compounds are integrated into a circuit onto a memristor crossbar) the emitted light 25 may be used as a probe to determine the information that may be stored in the memory device. In another embodiment, compounds in memory devices have been observed to exhibit selective responses to changes in pH as well. Therefore, an assembly formed by a combination of such memory devices may be used as a sensing element (in addition to a computing element), without needing any 30 additional functional elements. 6
[0023] It may be noted that the above examples depicting light or changes in pH as stimuli to effect change in functional attributes of the memory devices is only indicative. The same should not be construed as a limitation. Other stimuli, such as applied voltage, may also be used without deviating from the scope of the present subject matter. Such other examples too would fall within the scope of the present 5 subject matter.
[0024] These and other features, aspects, and advantages of the present subject matter will be better understood with reference to the following description. This summary is provided to introduce a selection of concepts in a simplified form. This summary is not intended to identify key features or essential features of the 10 disclosed subject matter, nor is it intended to be used to limit the scope of the disclosed subject matter.
BRIEF DESCRIPTION OF THE DRAWINGS
[0025] The following drawings form a part of the present specification and are 15 included to further illustrate aspects of the present disclosure. The disclosure may be better understood by reference to the drawings in combination with the detailed description of the specific embodiments presented herein.
[0026] Figure 1 depicts the schematic representation of the device (100), in accordance with an embodiment of the present disclosure. 20
[0027] Figure 2 depicts the cyclic voltammetry response of compounds (A) 1 and (B) 11, in accordance with an embodiment of the present disclosure.
[0028] Figure 3 depicts the contact- atomic force microscopy (c-AFM) current vs voltage (I-V) plot for compound 11, in accordance with an embodiment of the present disclosure. 25
[0029] Figure 4 depicts the photoluminescence spectra for the compounds (A) 1 and (B) 11, in accordance with an embodiment of the present disclosure.
[0030] Figure 5 depicts the photo absorption and emission spectra for the (A) compound 1 in response to light irradiation in acetonitrile solution, or (B) spectral change of compound 11 upon change of pH in the range of 2 to 8, in accordance 30 with an embodiment of the present disclosure.
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DETAILED DESCRIPTION OF THE INVENTION
[0031] Those skilled in the art will be aware that the present disclosure is subject to variations and modifications other than those specifically described. It is to be understood that the present disclosure includes all such variations and modifications. The disclosure also includes all such steps, features, compositions, 5 and compounds referred to or indicated in this specification, individually or collectively, and any and all combinations of any or more of such steps or features.
Definitions
[0032] For convenience, before further description of the present disclosure, certain terms employed in the specification, and examples are delineated here. 10 These definitions should be read in the light of the remainder of the disclosure and understood as by a person of skill in the art. The terms used herein have the meanings recognized and known to those of skill in the art, however, for convenience and completeness, particular terms and their meanings are set forth below. 15
[0033] The articles “a”, “an” and “the” are used to refer to one or to more than one (i.e., to at least one) of the grammatical object of the article.
[0034] The terms “comprise” and “comprising” are used in the inclusive, open sense, meaning that additional elements may be included. It is not intended to be construed as “consists of only”. Throughout this specification, unless the context 20 requires otherwise, the word “comprise”, and variations such as “comprises” and “comprising”, will be understood to imply the inclusion of a stated element or step or group of elements, or steps but not the exclusion of any other element or step or group of element or steps.
[0035] The term “including” is used to mean “including but not limited to”. 25 “Including” and “including but not limited to” are used interchangeably.
[0036] In the structural formulae given herein and throughout the present disclosure, the following terms have been indicated meaning, unless specifically stated otherwise.
[0037] As used herein, the term "device" refers to any apparatus, structure, or 30 system comprising at least two electrodes with an intermediate functional material, 8
wherein the intermediate material comprises one or more organic compounds capable of undergoing reversible physical or chemical changes (including, but not limited to, redox transitions, conformational rearrangements, or ionic redistributions) in response to an external stimulus such as an applied voltage. Such changes can impart or modify one or more operational characteristics of the device, 5 including but not limited to electrical switching, information storage, signal processing, or sensing functionality. The device may function as a memory unit, switching element, sensor, computing element, or any combination thereof, and includes all associated structural components such as substrates, electrodes, interconnects, and protective layers that enable the operation of the polycyclic 10 redox-active organic materials for electronic and optical switching applications. The device encompasses single units, arrays of multiple units, and integrated systems incorporating the disclosed organic materials for applications including but not limited to data storage, in-memory computing, neuromorphic computing, sensing, and multifunctional electronic systems. 15
[0038] The term “molecular memory unit” refers to a unit in a memory device wherein individual molecules are used to store data. Each individual molecules in a memory unit contains a bit of data, leading to massive data capacity for the memory device. The molecular component can be described as a molecular switch, and may perform by charge storage, photochromism, or capacitance change 20 mechanisms.
[0039] The term “conducting layer” refers to an electrically conducting layer which is attached to a voltage adjusting or measuring device to facilitate flow of electrons in a device. In an aspect of the present disclosure, there is provided a device comprising a molecular memory unit having a first conducting layer, and a second 25 conducting layer independently selected from indium tin oxide (ITO), fluorine doped tin oxide (FTO), chromium, titanium, platinum, gold, tungsten, nickel, or graphite.
[0040] The term “organic layer” refers to a layer comprising an organic compound. In an aspect of the present disclosure, the organic layer comprises a compound 30
9
selected from compound of Formula I, Formula II, its salts, stereoisomers, solvates, or combinations thereof.
[0041] The term “substrate” refers to the layer or film which acts as a template upon which other components are arranged in order. In an aspect of the present disclosure, the substrate is selected from yttria stabilized zirconia (YSZ), silicon, 5 silicon oxide, silicon nitride, or sapphire.
[0042] The term “memory effect” refers to the phenomenon by which an individual molecule in a memory unit contains a bit of data via mechanisms such as charge storage, photochromism, or capacitance change. In an aspect of the present disclosure, the organic layer exhibits memory effect via ionic and 10 intermolecular rearrangements.
[0043] The term "root mean square roughness" as used herein refers to a statistical measure of the surface topography of the organic layer, defined as the square root of the arithmetic mean of the squares of the deviations in surface height relative to the mean surface plane. 15
[0044] The term "switching time" as used herein refers to the duration required for the device to transition from one conductance state to another in response to an applied electrical stimulus.
[0045] The term "geometric isomerism" as used herein refers to different spatial arrangements of atoms or groups around double bonds or ring structures that result 20 in distinct molecular conformations with potentially different electronic and optical properties.
[0046] The term "counter ion" as used herein refers to an anion that balances the positive charge of the organic cation in ionic organic compounds, including but not limited to halides, oxyanions, and complex anions. 25
[0047] The term "multiple accessible redox states" as used herein refers to two or more distinct oxidation-reduction states of the organic compound that can be reversibly accessed within the operating voltage range of the device, each state being sufficiently stable to serve as a distinct memory state.
[0048] The term "ionic and intermolecular rearrangements" as used herein refers to 30 changes in the spatial arrangement of ions and molecules within the organic layer,
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including conformational changes, charge redistribution, and molecular reorientation that contribute to the memory effect and switching behavior.
[0049] The term "memory effect" as used herein refers to the ability of the organic layer to retain a particular conductance state or electronic configuration after removal of the applied stimulus, thereby storing information through stable 5 molecular arrangements.
[0050] The term "switching events" as used herein refers to discrete changes in electrical conductance or resistance of the organic layer in response to applied voltage, wherein each event corresponds to a transition between different redox states or molecular configurations. 10
[0051] The term "redox states" as used herein refers to distinct oxidation states of a molecule characterized by different numbers of electrons, wherein each state exhibits unique electronic properties, conductance characteristics, and stability under applied electrical fields.
[0052] The term “solvate”, as used herein, refers to a crystal form of a substance 15 which contains solvent. Hydrate is a solvate form of a substance wherein the solvent is water.
[0053] Salts and solvates having counter-ions or associated solvents are within the scope of the present disclosure, for example, for use as intermediates in the preparation of other compounds of Formula I, and their salts. Thus, one 20 embodiment of the disclosure embraces a compound of Formula I, and salts thereof. Compounds according to Formula I contain a basic functional group and are therefore capable of forming acid addition salts by treatment with a suitable salt of the respective anion. Suitable acids include inorganic acids and organic acids. Representative acid addition salts include, without limitation, chloride, nitrate, 25 tetrafluoroborate, trifluoromethanesulfonate, hexafluorophosphate, and tetraphenylborate.
[0054] The term “stereoisomers” refers to two or more isomers of a compound that have the same molecular formula and sequence of bonded atoms but differ in the three-dimensional orientations of their atoms in space. The compounds described 30 herein may contain one or more chiral centers and/or double bonds and therefore, 11
may exist as stereoisomers, such as enantiomers and diastereomers (“E” or “Z” isomer or a mixture of ‘E’ and ‘Z’ isomers). Accordingly, the chemical structures depicted herein encompass all possible enantiomers and stereoisomers of the illustrated or identified compounds including the stereoisomerically pure form (e.g., geometrically pure, enantiomerically pure or diastereomerically pure) and 5 enantiomeric and stereoisomeric mixtures. Further, the mixture of enantiomeric and other stereoisomeric forms can be resolved into their pure component by the methods known in the art, such as chiral-phase gas chromatography, chiral-phase high performance liquid chromatography, crystallization, using chiral derivatizing agents, etc. Also, pure enantiomers and diastereomers can be obtained from 10 intermediates or metabolites and reagents that are in the form of pure enantiomers and diastereoisomers by known asymmetric synthetic methods.
[0055] The term “alkyl” refers to a saturated hydrocarbon chain having the specified number of carbon atoms. For example, which are not limited, C1-20 alkyl refers to an alkyl group having from 1–20 carbon atoms. Alkyl groups may be 15 straight or branched chained groups which may be optionally substituted. Representative branched alkyl groups have one, two, or three branches. Preferred alkyl groups include, without limitation, methyl, ethyl, n-propyl, and isopropyl, butyl, isobutyl and t-butyl. One or more hydrogens of the alkyl groups may be optionally replaced with deuterium. Similarly, the other atom(s) may be replaced 20 by their respective isotopic forms as well.
[0056] The term “alkenyl” refers to an unsaturated hydrocarbon chain having a specific number of carbon atoms and at least one double bond between carbon atoms. For example, which are not limited, C2-20 alkenyl refers to an alkenyl group having from 2–20 carbon atoms. Alkenyl groups may be straight or branched chain 25 groups which may be optionally substituted. Representative branched alkenyl groups have one, two, or three branches. Preferred alkenyl groups include, without limitation, ethenyl, n-propenyl, and isopropenyl.
[0057] The term “aryl” refers to aromatic systems having 6 to 15 carbon atoms, which may be optionally substituted by one or more substituents. The aryl may be 30 monocyclic, bicyclic or polycyclic and may be fused, bridged or spirocyclic rings.
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The aryl groups may be optionally substituted. Preferred aryl groups include, but not limited to phenyl, naphthyl and the like.
[0058] The term “heteroaryl” refers to an aryl ring system as defined above having a heteroatom in the ring. The heteroaryl ring system may be attached to the main structure at any heteroatom or carbon atom resulting in the creation of a stable 5 structure. The term “C1-20 heteroaryl” refers to an aromatic ring with one or more hetero atoms selected from N, O or S with carbon ranging between 1 to 20.
[0059] The term “heterocyclyl” refers to a heterocyclic ring system that may be optionally substituted by one or more substituents. The heterocyclyl ring system may be attached to the main structure at any heteroatom or carbon atom resulting 10 in the creation of a stable structure. Furthermore, the term “C3-20 heterocyclyl” refers to a stable 3 to 20 membered ring system, which consists of carbon atoms and heteroatoms selected from nitrogen, phosphorus, oxygen and sulphur. For purposes of this disclosure, the heterocyclic ring system may be monocyclic, bicyclic or tricyclic ring systems, fused, bridged or spirocyclic rings, and the 15 nitrogen, phosphorus, oxygen or sulphur atoms in the heterocyclic ring system, may be optionally oxidized to various oxidation states. The heterocyclic rings further include heteroaryl rings which are aromatic heterocyclic rings. In addition, the nitrogen atom may be optionally quaternized; and the ring system, may be partially or fully saturated. The term “heterocyclyl” refers to monocyclic or polycyclic ring, 20 polycyclic ring system refers to a ring system containing 2 or more rings, preferably bicyclic or tricyclic rings, in which rings can be fused, bridged or spirocyclic rings or any combinations thereof. A fused ring as used herein means that the two rings are linked to each other through two adjacent ring atoms common to both rings. The fused ring can contain 1-4 hetero atoms independently selected from N, O, or S. 25 The rings can be either fused by nitrogen, -CH- or -C- group.
[0060] The term “cycloalkyl” refers to a cyclic carbon moiety comprising saturated bonds between the carbons. The cycloalkyl compounds includes a non-aromatic carbocyclic ring system, polycyclic ring compounds, and bicyclic (spiro, fused, bridged, non-fused) ring compounds. The term C3-20 cycloalkyl comprises 3 to 20 30
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carbon atoms. Preferred cycloalkyl groups include, without limitation, cyclopentyl, cycloheptenyl, cyclobutene, or cyclononane.
[0061] Unless otherwise substituted, the valency of an atom such as carbon, nitrogen, in the compounds of the present disclosure is understood to satisfy by the presence of hydrogen atoms. 5
[0062] The compounds described herein can also be prepared in any solid or liquid physical form, for example the compound can be in a crystalline form, in amorphous form and have any particle size. Furthermore, the compound particles may be micronized or nanonized, or may be agglomerated, particulate granules, powders, oils, oily suspensions, or any other form of solid or liquid physical forms. 10
[0063] Ratios, concentrations, amounts, and other numerical data may be presented herein in a range format. It is to be understood that such range format is used merely for convenience and brevity and should be interpreted flexibly to include not only the numerical values explicitly recited as the limits of the range, but also to include all the individual numerical values or sub-ranges encompassed within that range as 15 if each numerical value and sub-range is explicitly recited.
[0064] Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this disclosure belongs. Although any methods and materials similar or equivalent to those described herein can be used in the practice or testing of the 20 disclosure, the preferred methods, and materials are now described.
[0065] As discussed in the background, there is a need in the art to develop a molecular memory unit having multiple redox states and capacitive states. However, existing organic materials used for memory devices face stability issues and exhibit low response to voltages and other inputs such as light irradiation and 25 pH variation. Further, the conventional organic materials used also face challenges in aspects of switching time. The switching mechanisms in these materials remain poorly understood due to structural complexities, making systematic optimization nearly impossible and resulting in devices with unpredictable performance characteristics. Furthermore, current computing architectures require separate and 30 independent functional units for sensing, memory, and processing operations, 14
necessitating frequent data exchange that dramatically reduces overall system efficiency and prevents the realization of truly integrated in-memory and in-sensor computing platforms essential for artificial intelligence and edge computing applications. Therefore, there exists a need to develop organic materials having multiple redox states and high switching efficiency which contribute towards the 5 memory units in which it is incorporated.
[0066] The present disclosure overcomes these fundamental limitations through the development of polycyclic redox-active organic materials that exhibit multiple accessible redox states, enabling unprecedented switching capabilities and multifunctional device architectures. The compounds of Formula I and Formula II 10 demonstrate up to 16 distinct switching events within a single voltage sweep cycle at low operating voltages of ±1.5V, representing a dramatic improvement over binary switching systems and providing ultrahigh-density memory capacity with switching current ratios exceeding 10². The organic layer achieves memory effects through precisely controlled ionic and intermolecular rearrangements that stabilize 15 molecular states, resulting in exceptional endurance exceeding 108 switching cycles and maintaining operational stability for months under ambient conditions, thereby solving the reliability and durability problems that have plagued prior organic memory devices. The disclosure’s switching times ranging from 1 nanosecond to 1×106 nanoseconds represent orders of magnitude improvement over existing 20 organic materials, while the solution-processable fabrication using spin coating at controlled speeds of 2000-4000 rpm enables cost-effective manufacturing with precise thickness control of 5-50 nm. Most significantly, the compounds of Formula I and Formula II integrate multiple functionalities within a single device architecture by exhibiting responsive changes to voltage, light irradiation with 25 wavelengths of 200-1000 nm, and pH variations in the range of 2-8, thereby eliminating the need for separate sensing, memory, and computing units and dramatically improving energy efficiency by reducing data exchange requirements. This multifunctional approach enables the realization of true in-memory and in-sensor computing platforms suitable for neuromorphic architectures, artificial 30 intelligence applications, and edge computing systems, while supporting both 15
digital and analog storage modes through the multiple stable redox states of the organic materials. As discussed previously, the present approaches also address the issue pertaining to energy efficiency which arises due to the different units (such as memory units, sensors, and so on). The compounds as described herein when used in memory devices are such that they exhibit different functional attributes in 5 response to certain categories of stimuli. Specifically, the type of functional attributes of the memory devices may be expanded by applying additional or varying stimuli. For example, compounds which are used for realizing memory devices, are capable of emitting light. In an example, the different redox states are such that they exhibit or enable different degrees of luminescence. In such cases, 10 the resulting devices (wherein which the compounds are integrated into a circuit onto a memristor crossbar) the emitted light may be used as a probe to determine the information that may be stored in the memory device. In another embodiment, compounds in memory devices have been observed to exhibit selective responses to changes in pH as well. Therefore, an assembly formed by a combination of such 15 memory devices may be used as a sensing element (in addition to a computing element), without needing any additional functional elements.
[0067] Accordingly, the present disclosure provides a device comprising: a first conducting layer; a second conducting layer; and an organic layer comprising a first surface and a second surface, wherein the organic layer is interposed between the 20 first electrode and the second electrode; and the organic layer comprises a compound of Formula I, Formula II, their salts, stereoisomers, solvates, or combinations thereof,
Formula I 25
16
Formula II
wherein R1 is selected from H, Cl, Br, or I;
R2 is selected from H, Cl, CH3, OCH3, Br, I or ;
R’ is selected from Cl, Br, or I; 5
R3, and R3’, are independently selected from C1-20 alkyl, C2-20 alkenyl, C6-15 aryl, C3-20 cycloalkyl, C1-20 heteroaryl, C3-20 heterocyclyl or stilbene; R4 and R4’ are absent or independently selected from C1-20 alkyl, C2-20 alkenyl, C6-15 aryl, C3-20 cycloalkyl, C1-20 heteroaryl, C3-20 heterocyclyl or stilbene; and X- is a counter ion selected from Cl-, ClO4-, HSO4-, NO3-, BF4-, PF6-, CF3SO3-, or BPh4-. 10
[0068] In an embodiment of the present disclosure, there is provided a device as disclosed herein, wherein the compound of Formula I is selected from the compound of Formula Ia or Formula Ib,
Formula Ia 15
17
Formula Ib
wherein, R1 is selected from H, or Cl; R2 is selected from H, or CH3; R3 is selected from H, CH3, OMe, Cl, or Br; R’ is selected from Cl, Br, or I; and X- is a counter ion selected from Cl-, ClO4-, HSO4-, NO3-, BF4-, PF6-, CF3SO3-, or BPh4-. 5
[0069] In an embodiment of the present disclosure, there is provided a device as disclosed herein, wherein the compound of Formula II is selected from a compound of Formula IIa or Formula IIb,
Formula IIa Formula IIb 10
wherein, R3, R3’, R4 and R4’ are independently selected from C1-20 alkyl, C2-20 alkenyl, C6-15 aryl, C3-20 cycloalkyl, C1-20 heteroaryl, C3-20 heterocyclyl or stilbene; and X- is a counter ion selected from Cl, NO3, BF4, PF6, CF3SO3, or BPh4.
[0070] In an embodiment of the present disclosure, there is provided a device as disclosed herein, wherein the first conducting layer and the second conducting layer 15 are independently selected from indium tin oxide (ITO), fluorine doped tin oxide (FTO), chromium, titanium, platinum, gold, tungsten, nickel, or graphite. In another embodiment of the present disclosure, the first conducting layer and the second conducting layer are independently indium tin oxide (ITO).
[0071] In an embodiment of the present disclosure, there is provided a device as 20 disclosed herein, wherein the first surface of the organic layer is in contact with the 18
second conducting layer. In another embodiment, the second surface of the organic layer is in contact with the first conducting layer.
[0072] In an embodiment of the present disclosure, there is provided a device as disclosed herein, wherein the organic layer has a thickness in a range of 10 to 100nm; and the first conducting layer and the second conducting layer 5 independently have a thickness in a range of 10 to 100 nm. In another embodiment of the present disclosure, the organic layer has a thickness in a range of 10 to 50 nm. In one another embodiment of the present disclosure, the organic layer has a thickness in a range of 5 to 50 nm. In yet another embodiment of the present disclosure, the organic layer has a thickness in a range of 5 to 9 nm. In another 10 embodiment of the present disclosure, the organic layer has a thickness in a range of 5 to 100 nm.
[0073] In an embodiment of the present disclosure, there is provided a device as disclosed herein, wherein the organic layer has a root mean square roughness in a range of 0.1 to 4 nm. In another embodiment of the present disclosure, the organic 15 layer has a root mean square roughness in a range of 0.2 to 4 nm.
[0074] In an embodiment of the present disclosure, there is provided a device as disclosed herein, wherein the device comprises a substrate (104).
[0075] In an embodiment of the present disclosure, there is provided a device as disclosed herein, wherein the substrate preferably is in contact with the second 20 conducting layer.
[0076] In an embodiment of the present disclosure, there is provided a device as disclosed herein, wherein the substrate is selected from yttria stabilized zirconia (YSZ), silicon, silicon oxide, hafnium oxide, silicon nitride, or sapphire. In another embodiment of the present disclosure, the substrate is yttria stabilized zirconia 25 (YSZ).
[0077] In an embodiment of the present disclosure, there is provided a device as disclosed herein, wherein the device comprises a substrate (104) selected from yttria stabilized zirconia (YSZ), silicon, silicon oxide, silicon nitride, or sapphire.
[0078] In an embodiment of the present disclosure, there is provided a device as 30 disclosed herein, wherein the device further comprises metal nanoparticles selected 19
from gold, silver, tungsten, or chromium. In another embodiment of the present disclosure, the metal nanoparticles are gold.
[0079] In an embodiment of the present disclosure, there is provided a device as disclosed herein, wherein the metal nanoparticle having a diameter in the range of 10 to 200 nm. 5
[0080] In an embodiment of the present disclosure, there is provided a device as disclosed herein, wherein the organic layer, the first conducting layer and the second conducting layer are arranged in series.
[0081] In an embodiment of the present disclosure, there is provided a device as disclosed herein, wherein the organic layer exhibits memory effect via ionic and 10 intermolecular rearrangements.
[0082] In an embodiment of the present disclosure, there is provided a device as disclosed herein, wherein the organic layer exhibits at least two redox states. In another embodiment of the present disclosure, the organic layer exhibits two to six redox states. 15
[0083] In an embodiment of the present disclosure, there is provided a device as disclosed herein, wherein the device exhibits up to 16 distinct switching events within a voltage range of ±1.5V.
[0084] In an embodiment of the present disclosure, there is provided a device as disclosed herein, wherein the device exhibits a switching time in a range of 1 to 1 20 × 106 ns.
[0085] In an embodiment of the present disclosure, there is provided a device as disclosed herein, wherein the device exhibits response to a voltage in a range of -5 to 5V; or a light irradiation having wavelength in a range of 200 to 1000 nm; or a pH in a range of 2 to 8. In another embodiment of the present disclosure, there is 25 provided a device as disclosed herein, wherein the device exhibits response to the light irradiation having wavelength in a range of 500 to 800 nm.
[0086] In an embodiment of the present disclosure, there is provided a process for preparation of the device as disclosed herein, the process comprising: coating a solution of organic layer on a second conducting layer; and assembling a first 30 conducting layer upon second surface of the organic layer to obtain the device.
20
[0087] In an embodiment of the present disclosure, there is provided a process as disclosed herein, wherein the solution of organic layer comprises a solvent and at least one compound of Formula I or Formula II as disclosed herein.
[0088] In an embodiment of the present disclosure, there is provided a process as disclosed herein, wherein the solvent is selected from acetonitrile (CH3CN), 5 dimethyl formamide (DMF), dichloromethane (CH2Cl2), dichloroethane (ClCH2CH2Cl), chloroform (CH3Cl), methanol (CH3OH), ethanol (C2H5OH), or combinations thereof. In another embodiment of the present disclosure, the solvent is CH3CN, dimethyl formamide (DMF), or combinations thereof.
[0089] In an embodiment of the present disclosure, there is provided a process as 10 disclosed herein, wherein the coating is carried out by spin coating, jet printing, sol-gel coating, slot die coating, or combinations thereof. In another embodiment of the present disclosure, the coating is carried out by spin coating and drying.
[0090] In an embodiment of the present disclosure, there is provided a process as disclosed herein, wherein the coating is carried out by spin coating at a speed in a 15 range of 1000 to 12000 rpm, for a period in a range of 20 to 120 seconds. In another embodiment of the present disclosure, wherein the coating is carried out by spin coating at a speed in a range of 2000 to 4000 rpm, for a period in a range of 60 to 120 seconds.
[0091] In an embodiment of the present disclosure, there is provided a process as 20 disclosed herein, wherein the first conducting layer is deposited over the second surface of the organic layer by vacuum vapor deposition method, cluster ion beam method, pulsed laser deposition (PLD) method, chemical vapor deposition (CVD) method, plasma polymerization method, molecular beam epitaxy (MBE) method, or sputtering method. In another embodiment of the present disclosure, the first 25 conducting layer is deposited over the second surface of the organic layer by pulsed laser deposition (PLD) method.
[0092] In an alternate embodiment of the present disclosure, there is provided a process for preparing the device as described herein, the process comprising: a) providing a substrate with a first conducting layer; b) depositing a solution 30 comprising the polycyclic redox-active organic compound onto the first conducting
21
layer to form the organic layer; and c) depositing a second conducting layer over the organic layer. In another embodiment of the present disclosure, there is provided a process for preparing the device as described herein, wherein the depositing of the organic layer is performed by spin coating, printing, evaporation, or solution casting. In yet another embodiment of the present disclosure In an alternate 5 embodiment of the present disclosure, there is provided a process for preparing the device as described herein, wherein spin coating is performed at speeds of 1000 to 12000 rpm for 20 to 120 seconds. In a further embodiment of the present disclosure, there is provided a process for preparing the device as described herein, wherein the solution comprises a solvent selected from acetonitrile, dimethyl formamide, 10 dichloromethane, alcohols, or combinations thereof.
[0093] In an embodiment of the present disclosure, there is provided an organic layer comprising a compound of Formula I or Formula II as defined herein.
[0094] In an embodiment of the present disclosure, there is provided an organic layer comprising a compound selected from a compound of Formula Ia, Formula 15 Ib, Formula IIa, or Formula IIb.
[0095] In an embodiment of the present disclosure, there is provided an organic layer as described herein wherein the organic layer exhibits multiple accessible redox states and memory effects via ionic and intermolecular rearrangements.
[0096] In an embodiment of the present disclosure, there is provided a use of the 20 device as disclosed herein, or the organic layer as disclosed herein.
[0097] In an embodiment of the present disclosure, there is provided a use of the device as disclosed herein, or the organic layer as disclosed herein, in electrical, sensory and computing appliances.
[0098] In an embodiment of the present disclosure, there is provided a sensor 25 device comprising the device as disclosed herein, wherein the device exhibits responsive changes in electrical or optical properties upon exposure to environmental stimuli.
[0099] In an embodiment of the present disclosure, there is provided a sensor device as described herein, wherein the environmental stimuli comprise light 30 irradiation, pH changes, temperature variations, or chemical exposure.
22
[00100] In an embodiment of the present disclosure, there is provided a computing system comprising an array of devices as described herein, wherein the array is configured for parallel processing operations.
[00101] In an embodiment of the present disclosure, there is provided a computing system as described herein, wherein the system is configured for 5 artificial intelligence or machine learning applications.
[00102] In an embodiment of the present disclosure, there is provided a multifunctional device comprising the device as described herein, wherein the device simultaneously provides memory, sensing, and computing functionalities
[00103] The present approaches also address the issue pertaining to energy 10 efficiency which arises due to the different units (such as memory units, sensors, and so on). The compounds as described herein when used in memory devices are such that they exhibit different functional attributes in response to certain categories of stimuli. Specifically, the type of functional attributes of the memory devices may be expanded by applying additional or varying stimuli. For example, compounds 15 which are used for realizing memory devices, are capable of emitting light. In an example, the different redox states are such that they exhibit or enable different degrees of luminescence. In such cases, the resulting devices (wherein which the compounds are integrated into a circuit onto a memristor crossbar) the emitted light may be used as a probe to determine the information that may be stored in the 20 memory device. In another embodiment, compounds in memory devices have been observed to exhibit selective responses to changes in pH as well. Therefore, an assembly formed by a combination of such memory devices may be used as a sensing element (in addition to a computing element), without needing any additional functional elements. 25
[00104] It may be noted that the above examples depicting light or changes in pH as stimuli to effect change in functional attributes of the memory devices is only indicative. The same should not be construed as a limitation. Other stimuli, such as applied voltage, may also be used without deviating from the scope of the present subject matter. Such other examples too would fall within the scope of the 30 present subject matter. 23
[00105] Although the subject matter has been described in considerable detail with reference to certain examples and implementations thereof, other implementations are possible.
EXAMPLES 5
[00106] The disclosure will now be illustrated with the following examples, which are intended to illustrate the working of disclosure and not intended to take restrictively to imply any limitations on the scope of the present disclosure. Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood to one of ordinary skill in the art to which this 10 disclosure belongs. Although methods and materials similar or equivalent to those described herein can be used in the practice of the disclosed methods and devices, the exemplary methods, devices and materials are described herein. It is to be understood that this disclosure is not limited to particular methods, and experimental conditions described, as such methods and conditions may apply. 15
[00107] The forthcoming examples explain how the present disclosure provides the device comprising the compounds of Formula I or II.
EXAMPLE 1
Preparation of Compound of the present disclosure
[00108] Various compounds of Formula I/Ia were synthesized using known 20 synthetic methods. The synthesized compounds and their substituents are provided in the Table 1 below:
Formula Ia
Table 1 25
Compound
R1
R2
R3
Counter ion X-
24
1
H
H
H
Cl-
2
H
H
H
ClO4-
3
H
H
H
NO3-
4
H
H
H
HSO4-
5
H
CH3
H
Cl-
6
H
H
CH3
Cl-
7
H
H
OCH3
Cl-
8
Cl
H
H
Cl-
9
H
H
Cl
Cl-
10
H
H
Br
Cl-
[00109] Two representative compounds 5 and 7 were characterized using ¹H NMR spectroscopy. For example, compound 5 exhibited characteristic NMR signals in CD3CN at d 9.87 (d, J = 6.5 Hz, 1H), 9.20 (d, J = 8.27 Hz, 1H), 8.99 (dd, J1 = 7.5 Hz, J2 = 7.5 Hz, 1H), 8.82 (s, 1H), 8.71 (d, J = 8.8 Hz, 1H), 8.51 (dd, J1 = 6.5 Hz, J2 5 = 6.7 Hz, 1H), 8.30 (d, J = 8.8 Hz, 1H), and 2.75 (s, 3H) ppm.
Similarly, compound 7 showed NMR signals at d 9.91 (d, J = 6.65 Hz, 1H), 9.07 (d, J = 8.1 Hz, 1H), 8.94-8.85 (m, 2H), 8.45 (dd, J1 = 5.7 Hz, J2 = 6.6 Hz, 1H), 8.14 (s, 1H), 7.88 (d, J = 9.2 Hz, 1H), and 4.21 (s, 3H) ppm.
Additionally, the following compounds were synthesized using known synthetic 10 methods for the compound of Formula Ib.
Compound
NMR Spectra
Compound 11
1H NMR (CD3CN, 300 MHz): d 9.31 (d, J = 7.4 Hz, 1H), 8.59-8.53 (m, 2H), 8.36 (d, J = 9.5 Hz, 1H), 8.26 (s, 1H), 8.15 (d, J = 9.2 Hz, 1H), 8.03 (dt, J1 = 2 Hz, J2 = 7 Hz, 1H), 7.60-7.56 (m, 2H), 7.45-7.43 (m, 2H), 7.11-7.08 (m, 1H), 6.74 (d, J = 9.4 Hz, 1H), 6.23 (dt, J1 = 2 Hz, J2 = 7 Hz, 1H) ppm
25
Compound 12
1H NMR (CD3CN, 300 MHz): d 9.30 (d, J = 7.5 Hz, 1H), 8.62-8.55 (m, 2H), 8.36 (d, J = 9.5 Hz, 1H), 8.28 (s, 1H), 8.16 (d, J = 9.2 Hz, 1H), 8.07 (dt, J1 = 2 Hz, J2 = 7 Hz, 1H), 7.61-7.59 (m, 2H), 7.52-7.50 (m, 1H), 7.13-7.09 (m, 1H), 6.75 (d, J = 9.4 Hz, 1H), 6.25 (dt, J1 = 2 Hz, J2 = 7 Hz, 1H) ppm
Compound 13
1H NMR (CD3CN, 300 MHz): d 9.30 (d, J = 7.53 Hz, 1H), 8.58-8.49 (m, 2H), 8.35 (d, J = 9.53 Hz, 1H), 8.26 (s, 1H), 8.13 (d, J = 9.58 Hz, 1H), 8.02 (dd, J1 = 5.47 Hz, J2 = 6.64 Hz, 1H), 7.587.55 (m, 2H), 7.44-7.41 (m, 2H), 7.107.05 (m, 1H), 6.74 (d, J = 9.42 Hz, 1H), 6.22 (dd, J1 = 6.64, J2 = 6.67 Hz, 1H) ppm
Compound 14
1H NMR (CD3CN, 300 MHz): d 9.44 (d, J = 7.5 Hz, 1H), 8.62-8.54 (m, 2H), 8.38 (d, J = 9.5 Hz, 1H), 8.31 (s, 1H), 8.20 (d, J = 9.6 Hz, 1H), 8.08 (dd, J1 = 5.5 Hz, J2 = 6.6 Hz, 1H), 7.76-7.71 (m, 2H), 7.52-7.47 (m, 2H), 7.18-7.13 (m, 1H), 6.85 (d, J = 9.5 Hz, 1H), 6.26 (dd, J1 = 6.6, J2 = 6.7 Hz, 1H) ppm
Compound 15
1H NMR (CD3CN, 300 MHz): d 9.48 (d, J = 8.27 Hz, 1H), 8.79-8.71 (m, 2H), 8.45 (d, J = 9.65 Hz, 1H), 8.38 (s, 1H), 8.25 (d, J = 10.92 Hz, S22 1H), 8.15 (dd, J1 = 6.25 Hz, J2 = 6.85 Hz, 1H), 7.67-7.64 (m, 3H), 7.64 (d, J = 8.6 Hz,
26
1H), 7.19-7.13 (m, 1H), 6.85 (d, J = 9.35 Hz, 1H), 6.26 (dd, J1 = 6.85, J2 = 7.31 Hz, 1H) ppm
[00110] Furthermore, the compounds of Formula IIb were synthesized using known synthetic methods and the same are tabulated below.
Compounds
NMR spectra
Compound 16
1H NMR (500 MHz, DMSO): d = 9.64 (d, J = 6.4 Hz, 4H,), 9.39 (s, 2H), 8.94 (d, 4H, J = 4.2 Hz), 8.89 (d, 4H, J = 6.4 Hz), 8.16 (d, 4H, J = 5.2 Hz), 7.02 (s, 4H), 2.26 (s, 6H), 2.03 (s, 12H)
Compound 17
1H NMR (500 MHz, MeOD): d = 9.86 (d, J = 6.4 Hz, 4H), 9.55 (d, J = 6.4 Hz, 4H), 9.38 (s, 2H), 9.02 (d, J = 6.5 Hz, 4H), 8.88 (d, J = 6.4 Hz, 4H), 7.61 (d, J = 7 Hz,4H), 7.47 (m, 6H), 7.02 (s, 4H), 5.97 (s, 4H), 2.26 (s, 6H), 2.03 (s, 12H).
EXAMPLE 2 5
Preparation of device
[00111] A stock solution for each of the compounds were prepared in either acetonitrile (CH3CN) or dimethyl formamide (DMF) with a concentration between 27
10 and 50 mM. A stock solution of the representative compound 11 depending on the specific application and desired film thickness was prepared with the concentration range 10-50 mM.
[00112] Indium tin oxide (ITO) was grown on annealed yttria-stabilized zirconia (YSZ; substrate) to obtain second conducting layer having a thickness of 5 5 to 80 nm. For compound 11 based on the concentration of the solution used during spin coating, the thickness of the second conducting layer was 5-50 nm.
[00113] In an example, the stock solution of compound 11 was filtered through a 0.2 µm syringe filter and subsequently spin-coated onto the surface of the second conducting layer (ITO) at a speed of 3000 rpm, for 2 minutes to obtain an 10 organic layer having root mean square roughness in the range of 0.2 to 4 nm and thickness of 10 to 50 nm.
[00114] After deposition, the samples were stored in a vacuum chamber with a pressure of ~10-8 torr for 12 h. Subsequently, a first conducting layer of ITO was deposited by pulsed laser deposition (PLD) technique upon the second surface of 15 the organic layer. Further, gold nanoparticles with diameters of 10-200 nm and thickness of 10-60 nm were deposited on the ITO conducting layers using electron beam evaporation. Figure 1 shows the general representation of the fabricated device (100), having: a first conducting layer of indium doped tin oxide (ITO), (101); a second conducting layer (102) also comprising indium doped tin oxide 20 (ITO); an organic layer (103) comprising a first surface and a second surface (interposed between the conducting layers) and a YSZ substrate (104). The organic layer contained the polycyclic redox-active organic compounds and exhibited multiple redox states enabling electronic switching functionality 25
EXAMPLE 3
ELECTROCHEMICAL CHARACTERIZATION
Cyclic voltammetric measurements of compounds :
[00115] Cyclic voltammetric (CV) experiments were performed on compounds 1 and 11 to evaluate their redox properties. The measurements were 30 carried out in anhydrous acetonitrile using tetraethylammonium 28
hexafluorophosphate as the supporting electrolyte. All electrochemical measurements were performed using a CH electrochemical instrument (model number: CHI620E), keeping the CV-cell assembly inside a glove box maintained at an oxygen level and a moisture level each below 1 ppm.
[00116] A three-electrode cell was used for the CV measurements where the 5 working electrode was glassy carbon (area = 3.14 mm2), the reference electrode was saturated calomel electrode (SCE), the electrolyte was acetonitrile containing 0.1 M [Et4N]PF6 and the counter electrode was a Pt-wire (area = 220.69 mm2) dipped in a glass compartment having solution of 0.1 M [Et4N]PF6 in acetonitrile. The responses of the synthesized compounds are captured in Figure 2. 10
[00117] Figure 2 A presented the cyclic voltammetry responses of the synthesized compounds 1 and 11. Figure 2A displayed the CV plot of compound 1, which exhibited 2 well-resolved reduction peaks, indicating multiple accessible redox states. Figure 2B showed the CV plot of compound 11, which demonstrated 1 well-resolved reduction peak and 2 oxidation peaks. These results confirmed that 15 that the compounds 1 and 11 were promising candidates for high-density memory applications as the different redox states offered different intermolecular coupling resulting in variations in conductance and electronic switching behaviour.
[00118] It was observed from their representative cyclic voltammetry measurements that the poly cyclic redox active organic molecular materials 20 (compounds of the present disclosure) have multiple accessible antibonding orbitals. By selecting appropriate electrode work functions and applying external bias voltage, these antibonding orbitals could be populated or depopulated resulting in multiple possible electronic states of the organic layer. The compounds were ionic where the molecular charge was balanced by counter anion(s). 25
[00119] In a device comprising the organic layer of said compounds, the applied voltage between the first and second conducting layer changed the redox states of the molecules in the organic layer. While electrically controlled redox states offer switching, the ionic and intermolecular rearrangements stabilized the molecular states and provided a memory effect. The multiple redox-active centers 30
29
in the compounds facilitated multiple redox combinations and was engineered to show different extents of delocalization and memory effects.
EXAMPLE 4
ELECTRICAL SWITCHING CHARACTERIZATION
[00120] Contact Atomic Force Microscopic (c-AFM) measurement were 5 performed to evaluate the electrical switching properties of the fabricated devices. A JEOL JSPM 5200/ OmegaScope, based on SmartSPM AFM set up was used for all AFM measurements. Cantilever probe of CSC17/Pt tip and CSC17/Cr-Au tip were employed with tip radius of curvature < 30 nm, tip height: 12-18 µm, tip cone angle: 40°, resonant frequency: 10-17 kHz, force constant: 0.18 N/m, length: 450 10 µm, width: 50 µm, thickness: 2 µm. The c-AFM measurements were performed in contact mode with the resultant current measured using a preamplifier capable of detecting currents up to 100 µA with a 10 fA detection sensitivity. The cantilever probe was approached to the sample with a set point of 2-10 nN.
[00121] Figure 3 demonstrated the c-AFM derived current-voltage I(V) 15 characteristics of the device comprising the compound 11 as the organic layer. The measurements revealed a total of 16 sharp switching events in the voltage range of ± 1.3 V with the switching current ratio of approximately 10² in the 10 nm thin film. The Figure 3 showed that the number of sharp switching decreased with increasing thickness from 10 nm to 50 nm. 20
[00122] The multiple switching events were attributed to compound 11 containing multiple redox centres connected by sigma bonds, which existed in multiple orientations depending on their charge state and charge delocalization, giving rise to different thermodynamic states and resulting in multiple switching events and various stabilized electronic states. 25
EXMAPLE 5
ANALYSIS OF RESPONSE OF THE COMPOUNDS TO LIGHT IRRADIATION (PHOTOLUMINESCENCE CHARACTERIZATION)
[00123] Compounds of Formula I and II of the devices of the present disclosure, were also found to be light emitters and different redox states were 30 expected to have different luminescence. When integrated into a circuit, for 30
example in a crossbar, the emitted light was used as a probe to read out the information stored in the crossbar. This provided parallel means to read, monitor, and communicate the computation. The photoluminescence properties of compounds 1 and 11 were investigated to evaluate their optical switching capabilities. UV-Visible absorption spectra and photoluminescence emission 5 spectra were recorded using standard spectroscopic techniques.
[00124] The UV-Vis spectra of the compounds 1 and 11 were analyzed to check their sensitivity towards light irradiation.
[00125] Figure 4 showed the photoluminescence spectra for the compounds 1 and 11. Figure 4A showed that the compound 1 exhibited a strong p-p* absorption 10 peak near 260 nm and a weaker n-p* band around 350 nm. When excited at 340 nm, compound 1 emitted light at 535–540 nm with a quantum yield of 0.15–0.22. The fluorescence lifetime at room temperature was 3.90 ns. The light irradiation induced electronic transitions in these compounds, indicating that optical stimuli were likely to impact their transport properties as well, thereby enabling optical 15 switching functionality.
EXAMPLE 6
ANALYSIS OF RESPONSE OF THE COMPOUNDS TO pH VARIATION (pH RESPONSIVE OPTICAL PROPERTIES)
[00126] Other than light, the pH-responsive behavior of the compounds was 20 evaluated by monitoring changes in their optical properties upon exposure to different pH conditions. Hence, an assembly of these circuit elements is useful both as a sensor network and also for computing applications. This could be useful for in-sensor as well as in-memory computing applications. UV-Visible absorption spectra were recorded for solutions of the compounds in 1:1 MeOH-H2O mixtures 25 at various pH values.
[00127] The UV-Vis spectra of the compounds 1 and 11 were analyzed to check their sensitivity towards pH variation, as shown in Figure 5 (A) and (B) respectively.
[00128] Figure 5 illustrated the pH-responsive optical properties of the 30 synthesized compounds. Figure 5A showed the photo absorption and emission 31
spectra for compound 1 in response to light irradiation in acetonitrile solution, demonstrating the compound's photoswitching capabilities. Figure 5B presented the spectral changes of compound Ib upon pH variation in the range of 2 to 8.
[00129] When H+ was added to a 1:1 MeOH-H2O solution of compound 11, the deep blue colour shifted to a light yellowish-green, as evidenced by the changes 5 in the UV-Vis spectra provided in Figure 5 (B). This color change was caused by the protonation of one of the nitrogen atoms and was completely reversible. A distinct isosbestic point was observed at 510 nm, confirming the reversible nature of the pH-induced transformation.
[00130] Therefore, the compounds of the present disclosure had the potential 10 to act as a switching device using pH variation as stimulus or as a sensor to detect a pH variation.
EXAMPLE 7
DEVICE PERFORMANCE EVALUATION
[00131] The fabricated devices were subjected to comprehensive 15 performance testing to evaluate their switching characteristics, endurance, and stability. Electrical measurements were performed using standard semiconductor parameter analyzers under controlled environmental conditions.
[00132] The devices demonstrated exceptional performance characteristics including switching times ranging from 1 nanosecond to 1×106 nanoseconds, 20 representing significant improvements over existing organic memory technologies. The devices exhibited high endurance, sustaining repeated switching cycles on the order of at least billions and in some cases trillions or more, while maintaining consistent performance. Long-term stability testing further revealed that the devices remained functional over extended periods under ambient atmospheric conditions 25 without significant degradation.
[00133] The voltage range for device operation was typically ±1.5V, though depending on the specific device interface, operational voltages could vary from 0.5V to 2.5V. The devices showed excellent reproducibility across multiple fabrication batches, with hundreds of devices tested demonstrating consistent 30 switching behavior.
32
[00134] A device according to any of the preceding claims, wherein the device is operable in multiple switching modes, including (i) digital switching characterized by sharp transitions under electrical pulses higher than switching threshold, and (ii) analog switching characterized by gradual conductance modulation under subthreshold or fast electrical pulses, wherein said switching is 5 non-volatile and thereby enables use of the device as a memory or compute element, and wherein, in alternative operational regimes employing ultrafast pulses and/or modified molecular designs such as the selection of smaller counteranions, the device exhibits volatile switching behaviour suitable for dynamic or neuromorphic computation. 10
EXAMPLE 8
MULTIFUNCTIONAL DEVICE APPLICATIONS
[00135] The fabricated devices were evaluated for multifunctional applications combining memory, sensing, and computing capabilities. The devices 15 responded to multiple stimuli including electrical voltage, light irradiation with wavelengths ranging from 200 to 1000 nm, and pH variations in the range of 2 to 8.
[00136] When integrated into crossbar array configurations, the devices enabled parallel processing operations suitable for artificial intelligence and 20 machine learning applications. The photoluminescence properties of the compounds allowed the emitted light to serve as a probe for reading stored information, providing an additional communication channel for the memory system.
[00137] The pH-responsive properties enabled the devices to function as 25 chemical sensors while simultaneously providing memory and computing capabilities, demonstrating the potential for in-sensor computing applications where local intelligence could be implemented at edge computing platforms.
EXAMPLE 9 30
33
DEVICE COMPRISING COMPOUNDS OF FORMULA II AND ITS APPLICATION
[00138] Compounds of Formula II, wherein the substituent groups R3 and R4 were varied, exhibited voltage-dependent geometric isomerism. This dynamic structural behavior resulted in the formation of multiple stable isomeric 5 configurations under different applied voltages. Each geometric isomer corresponded to a distinct electronic state, thereby significantly enriching the current-voltage (I–V) response profile of the device. The ability to access multiple electronic states through controlled voltage modulation enabled enhanced data encoding capabilities and supports multilevel memory operations. This feature 10 contributed to the ultrahigh-density data storage potential of the invention, surpassing the limitations of conventional binary systems and offering a versatile platform for advanced memory and logic applications.
EXAMPLE 10
COMPARATIVE PERFORMANCE ANALYSIS 15
[00139] The performance of the disclosed devices was compared against existing organic memory materials and inorganic alternatives. The results demonstrated significant advantages in multiple performance metrics.
[00140] In contrast to existing alternatives, the disclosed platform exhibited up to 16 distinct switching events within a single sweep cycle, compared to binary 20 switching in conventional devices. These responses were reproducible, robust, and durable, enabling ultrahigh-density in-memory computing systems where complex combinatorial logic operations, such as XOR8 or XNOR8, could be executed in a single step. The system showed promise as high-bandwidth memory suitable for on-chip integration. The I-V characteristics revealed that these circuit elements 25 could be configured for either digital or analog storage and computation, thereby supporting conventional digital operations as well as analog acceleration in applications such as dot-product engines.
[00141] The devices of the present disclosure exhibit stability superior to conventional resistive memory devices, demonstrating operational lifetimes 30 extending for months to years and accelerated lifetime evaluation shows that these 34
should be durable for any reasonable usage duration. The devices exhibit switching speeds that are several orders of magnitude faster than existing organic alternatives, thereby rendering them suitable for high-speed computing applications. In certain embodiments, the devices demonstrate endurance sufficient to withstand cycling on the order of at least 10? to 10¹² switching events without any degradation of 5 performance. In further embodiments, the architecture of the devices enables storage and processing of data at the same physical location, thereby reducing energy consumption relative to conventional computing architectures by mitigating von Neumann bottlenecks. In yet further embodiments, the devices are configurable to operate in either digital or analog switching modes, wherein the operational mode 10 is determined at least in part by chemical design parameters and by the pattern and frequency of the applied stimulus, such configurability enabling device plasticity and facilitating brain-inspired computational paradigms and provide additional operational flexibility and reductions in energy consumption. 15
ADVANTAGES OF THE PRESENT DISCLOSURE
[00142] The present disclosure offers a transformative advancement over conventional memory and computing technologies by employing polycyclic redox-active organic materials that enable up to sixteen distinct switching events within a single voltage sweep cycle, thereby facilitating ultrahigh-density data storage with 20 switching current ratios exceeding 10². Operating at low voltages of ±1.5V, the devices significantly reduce power consumption compared to metal oxide-based alternatives, making them ideal for portable and energy-efficient applications. The organic materials demonstrate superior endurance exceeding 108 switching cycles and maintain operational stability for extended periods under ambient conditions, 25 addressing longstanding reliability concerns in organic memory systems. Fast switching responses ranging from 1 nanosecond to 1×106 nanoseconds represent a substantial improvement over existing technologies. The invention supports cost-effective manufacturing through solution-processable spin coating techniques, eliminating the need for high-temperature or complex fabrication processes. 30 Uniquely, the compounds integrate sensing, memory, and computing
35
functionalities within a single device architecture, responding to voltage, light irradiation (200–1000 nm), and pH variations (range 2–8), thereby reducing system complexity and enhancing energy efficiency. The organic layer offers precise control over thickness (10–100 nm) and surface roughness (0.1–4 nm), enabling versatile device design. Multiple accessible redox states provide stable resistance 5 states via ionic and intermolecular rearrangements, supporting both digital and analog storage modes and complex logic operations. The materials exhibit light irradiation (200–1000 nm) and pH-responsive optical properties with reversible color changes, enabling novel sensing and communication capabilities. The invention is scalable for array configurations, supporting parallel processing for 10 artificial intelligence, machine learning, and neuromorphic computing applications. Devices maintain robust performance across multiple switching cycles with excellent reproducibility and ambient stability, overcoming degradation issues common in prior organic materials. Furthermore, the invention simplifies system architecture by combining multiple functionalities into a single device, enabling 15 true in-memory and in-sensor computing platforms. Broad material compatibility with conducting layers such as ITO, FTO, metals, and carbon-based materials ensures seamless integration with existing technologies. Overall, the multiple redox states and multifunctional responsiveness of the organic materials significantly enhance data density, computational efficiency, and system versatility, establishing 20 a new paradigm in low-power, scalable, and multifunctional memory and computing devices. 36
I/We Claim:
1) A device comprising:
a. a first conducting layer;
b. a second conducting layer; and 5
c. an organic layer comprising a first surface and a second surface, wherein the organic layer is interposed between the first electrode and the second electrode; and the organic layer comprises a compound of Formula I, Formula II, their salts, stereoisomers, solvates, or combinations thereof,
10
Formula I
Formula II
wherein
R1 is selected from H, Cl, Br, or I; 15
R2 is selected from H, Cl, CH3, OCH3, Br, I or ;
R’ is selected from Cl, Br, or I;
R3, and R3’, are independently selected from C1-20 alkyl, C2-20 alkenyl, C6-15 aryl, C3-20 cycloalkyl, C1-20 heteroaryl, C3-20 heterocyclyl or stilbene;
37
R4 and R4’ are absent or independently selected from C1-20 alkyl, C2-20 alkenyl, C6-15 aryl, C3-20 cycloalkyl, C1-20 heteroaryl, C3-20 heterocyclyl or stilbene; and
X- is a counter ion selected from Cl-, ClO4-, HSO4-, NO3-, BF4-, PF6-, CF3SO3-, or BPh4-.
2) The device as claimed in claim 1, wherein the compound of Formula I is 5 selected from the compound of Formula Ia or Formula Ib,
Formula Ia
Formula Ib 10
wherein, R1 is selected from H, or Cl;
R2 is selected from H, or CH3;
R3 is selected from H, CH3, OMe, Cl, or Br
R’ is selected from Cl, Br, or I; and
X- is a counter ion selected from Cl-, ClO4-, HSO4-, NO3-, BF4-, PF6-, CF3SO3-, or 15 BPh4-.
3) The device as claimed in claim 1, wherein the compound of Formula II is selected from a compound of Formula IIa or Formula IIb, 38
Formula IIa Formula IIb
wherein, R3, R3’, R4 and R4’ are independently selected from C1-20 alkyl, C2-20 alkenyl, C6-15 aryl, C3-20 cycloalkyl, C1-20 heteroaryl, C3-20 heterocyclyl or stilbene; and X- is a counter ion selected from Cl, NO3, BF4, PF6, CF3SO3, or BPh4. 5
4) The device as claimed in claim 1, wherein the first conducting layer and the second conducting layer are independently selected from indium tin oxide (ITO), fluorine doped tin oxide (FTO), chromium, titanium, titanium nitride, platinum, gold, tungsten, nickel, or graphite.
5) The device as claimed in claim 1, wherein the first surface of the organic 10 layer is in contact with the second electrode.
6) The device as claimed in claim 1, wherein the organic layer has a thickness in a range of 10 to 100nm; and the first conducting layer and the second conducting layer independently have a thickness in a range of 10 to 100 nm.
7) The device as claimed in claim 1, wherein the organic layer has a root mean 15 square roughness in a range of 0.1 to 0.4 nm.
8) The device as claimed in claim 1, wherein the device comprises a substrate.
9) The device as claimed in claim 1, wherein the substrate preferably is in contact with the second conducting layer.
10) The device as claimed in claim 1, wherein the substrate is yttria stabilized 20 zirconia (YSZ), silicon, silicon oxide, silicon nitride, hafnium oxide or sapphire.
11) The device as claimed in claim 1, wherein the device comprises a substrate (104) selected from yttria stabilized zirconia (YSZ), silicon, silicon oxide, silicon nitride, hafnium oxide or sapphire. 25
39
12) The device as claimed in claim 1, wherein the device further comprises metal nanoparticles selected from gold, silver, tungsten, titanium nitride, titanium or chromium.
13) The device as claimed in claim 1, wherein the metal nanoparticle having a diameter in the range of 10 to 200 nm. 5
14) The device as claimed in claim 1, wherein the organic layer, the first conducting layer and the second conducting layer are arranged in series.
15) The device as claimed in claim 1, wherein the organic layer exhibits memory effect via ionic and intermolecular rearrangements.
16) The device as claimed in claim 1, wherein the organic layer exhibits at least 10 two redox states.
17) The device as claimed in claim 1, wherein the organic layer exhibits multiple redox states enabling multiple electronic switching events within a single voltage sweep cycle.
18) The device as claimed in claim 1, wherein the device exhibits up to 16 15 distinct switching events within a voltage range of ±1.5V.
19) The device as claimed in claim 1, wherein application of subthreshold electrical pulses or faster pulsed inputs transitions the device from digital switching behavior characterized by sharp conductance changes to analog switching behavior characterized by gradual conductance modulation. 20
20) The device as claimed in claim 1, wherein the device exhibits a switching time in a range of in a range of 1 to 1 × 106 ns.
21) The device as claimed in claim 1, wherein the device exhibits response to a voltage in a range of -5 to 5V; or a light irradiation having wavelength in a range of 200 to 1000 nm; or a pH in a range of 2 to 8. 25
22) The device as claimed in claim 1, wherein the compound of Formula I or Formula II exhibits geometric isomerism contributing to the multiple electronic states.
23)A process for preparation of the device as claimed in claim 1, the process comprising: 30
a. coating a solution of organic layer on a second conducting layer; and 40
b. assembling a first conducting layer upon second surface of the organic layer to obtain the device.
24) The process as claimed in claim 23, wherein the solution of organic layer comprises a solvent and at least one compound of Formula I or Formula II.
25) The process as claimed in claim 24, wherein the solvent is selected from 5 acetonitrile (CH3CN), dimethyl formamide (DMF), dichloromethane (CH2Cl2), dichloroethane (ClCH2CH2Cl), chloroform (CH3Cl), methanol (CH3OH), ethanol (C2H5OH), or combinations thereof.
26) The process as claimed in claim 23, wherein the coating is carried out by spin coating, jet printing, sol-gel coating, slot die coating, or combinations 10 thereof.
27) The process as claimed in claim 23, wherein the coating is carried out by spin coating at a speed in a range of 1000 to 12000 rpm, for a period in a range of 20 to 120 seconds.
28) The process as claimed in claim 23, wherein the first conducting layer is 15 deposited over the second surface of the organic layer by vacuum vapor deposition method, cluster ion beam method, pulsed laser deposition (PLD) method, chemical vapor deposition (CVD) method, plasma polymerization method, molecular beam epitaxy (MBE) method, or sputtering method.
29)An organic layer comprising a compound of Formula I or Formula II as 20 defined in claim 1.
30) The organic layer as claimed in claim 29, wherein the compound selected from a compound of Formula Ia, Formula Ib, Formula IIa, or Formula IIb as defined in claim 2 and 3.
31) The organic layer as claimed in any one of the claims 29-30, wherein the 25 organic layer exhibits multiple accessible redox states and memory effects via ionic and intermolecular rearrangements.
32)Use of the device as claimed in claim 1, or the organic layer as claimed in claim 29, as an in-memory computing element, wherein storage and processing of data are performed within the same physical location, thereby 30 enabling computational functions including, but not limited to, vector–
41
matrix multiplication, dot-product operations, and implementation in computing accelerators.
33)Use of the device as claimed in claim 1 or 2, or the organic layer as claimed in claim 29.
34)Use of the device as claimed in claim 1, or the organic layer as claimed in 5 claim 29, in electrical, sensory and computing appliances.
35) A sensor device comprising the device as claimed in claim 1, wherein the device exhibits responsive changes in electrical or optical properties upon exposure to environmental stimuli.
36) The sensor device as claimed in claim 35, wherein the environmental stimuli 10 comprise light irradiation, pH changes, temperature variations, or chemical exposure.
37)A computing system comprising an array of devices as claimed in claim 1, wherein the array is configured for parallel processing operations.
38) The computing system as claimed in claim 37, wherein the system is 15 configured for artificial intelligence or machine learning applications.
39)A multifunctional device comprising the device as claimed in claim 1, wherein the device simultaneously provides memory, sensing, and computing functionalities.
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ABSTRACT
A DEVICE COMPRISING ORGANIC COMPOUNDS AND IMPLEMENTATIONS THEREOF
The present disclosure relates to a molecular memory device comprising a 5 molecular memory unit that includes a first conducting layer, a second conducting layer, and an organic layer interposed between the two conducting layers. The organic layer comprises a compound selected from Formula I, Formula II, their salts, stereoisomers, solvates, or combinations thereof. These compounds exhibit multiple redox states and voltage-dependent geometric isomerism, enabling 10 enhanced electronic switching behavior and multilevel data storage capabilities. The organic materials are sensitive to external stimuli such as voltage, light irradiation, and pH variations, allowing multifunctional integration of sensing, memory, and computing functionalities within a single device architecture. This present disclosure provides a scalable, energy-efficient, and cost-effective platform 15 for advanced memory and neuromorphic computing applications. 43 ,CLAIMS:I/We Claim:
1) A device comprising:
a. a first conducting layer;
b. a second conducting layer; and 5
c. an organic layer comprising a first surface and a second surface, wherein the organic layer is interposed between the first electrode and the second electrode; and the organic layer comprises a compound of Formula I, Formula II, their salts, stereoisomers, solvates, or combinations thereof,
10
Formula I
Formula II
wherein
R1 is selected from H, Cl, Br, or I; 15
R2 is selected from H, Cl, CH3, OCH3, Br, I or ;
R’ is selected from Cl, Br, or I;
R3, and R3’, are independently selected from C1-20 alkyl, C2-20 alkenyl, C6-15 aryl, C3-20 cycloalkyl, C1-20 heteroaryl, C3-20 heterocyclyl or stilbene;
37
R4 and R4’ are absent or independently selected from C1-20 alkyl, C2-20 alkenyl, C6-15 aryl, C3-20 cycloalkyl, C1-20 heteroaryl, C3-20 heterocyclyl or stilbene; and
X- is a counter ion selected from Cl-, ClO4-, HSO4-, NO3-, BF4-, PF6-, CF3SO3-, or BPh4-.
2) The device as claimed in claim 1, wherein the compound of Formula I is 5 selected from the compound of Formula Ia or Formula Ib,
Formula Ia
Formula Ib 10
wherein, R1 is selected from H, or Cl;
R2 is selected from H, or CH3;
R3 is selected from H, CH3, OMe, Cl, or Br
R’ is selected from Cl, Br, or I; and
X- is a counter ion selected from Cl-, ClO4-, HSO4-, NO3-, BF4-, PF6-, CF3SO3-, or 15 BPh4-.
3) The device as claimed in claim 1, wherein the compound of Formula II is selected from a compound of Formula IIa or Formula IIb, 38
Formula IIa Formula IIb
wherein, R3, R3’, R4 and R4’ are independently selected from C1-20 alkyl, C2-20 alkenyl, C6-15 aryl, C3-20 cycloalkyl, C1-20 heteroaryl, C3-20 heterocyclyl or stilbene; and X- is a counter ion selected from Cl, NO3, BF4, PF6, CF3SO3, or BPh4. 5
4) The device as claimed in claim 1, wherein the first conducting layer and the second conducting layer are independently selected from indium tin oxide (ITO), fluorine doped tin oxide (FTO), chromium, titanium, titanium nitride, platinum, gold, tungsten, nickel, or graphite.
5) The device as claimed in claim 1, wherein the first surface of the organic 10 layer is in contact with the second electrode.
6) The device as claimed in claim 1, wherein the organic layer has a thickness in a range of 10 to 100nm; and the first conducting layer and the second conducting layer independently have a thickness in a range of 10 to 100 nm.
7) The device as claimed in claim 1, wherein the organic layer has a root mean 15 square roughness in a range of 0.1 to 0.4 nm.
8) The device as claimed in claim 1, wherein the device comprises a substrate.
9) The device as claimed in claim 1, wherein the substrate preferably is in contact with the second conducting layer.
10) The device as claimed in claim 1, wherein the substrate is yttria stabilized 20 zirconia (YSZ), silicon, silicon oxide, silicon nitride, hafnium oxide or sapphire.
11) The device as claimed in claim 1, wherein the device comprises a substrate (104) selected from yttria stabilized zirconia (YSZ), silicon, silicon oxide, silicon nitride, hafnium oxide or sapphire. 25
39
12) The device as claimed in claim 1, wherein the device further comprises metal nanoparticles selected from gold, silver, tungsten, titanium nitride, titanium or chromium.
13) The device as claimed in claim 1, wherein the metal nanoparticle having a diameter in the range of 10 to 200 nm. 5
14) The device as claimed in claim 1, wherein the organic layer, the first conducting layer and the second conducting layer are arranged in series.
15) The device as claimed in claim 1, wherein the organic layer exhibits memory effect via ionic and intermolecular rearrangements.
16) The device as claimed in claim 1, wherein the organic layer exhibits at least 10 two redox states.
17) The device as claimed in claim 1, wherein the organic layer exhibits multiple redox states enabling multiple electronic switching events within a single voltage sweep cycle.
18) The device as claimed in claim 1, wherein the device exhibits up to 16 15 distinct switching events within a voltage range of ±1.5V.
19) The device as claimed in claim 1, wherein application of subthreshold electrical pulses or faster pulsed inputs transitions the device from digital switching behavior characterized by sharp conductance changes to analog switching behavior characterized by gradual conductance modulation. 20
20) The device as claimed in claim 1, wherein the device exhibits a switching time in a range of in a range of 1 to 1 × 106 ns.
21) The device as claimed in claim 1, wherein the device exhibits response to a voltage in a range of -5 to 5V; or a light irradiation having wavelength in a range of 200 to 1000 nm; or a pH in a range of 2 to 8. 25
22) The device as claimed in claim 1, wherein the compound of Formula I or Formula II exhibits geometric isomerism contributing to the multiple electronic states.
23)A process for preparation of the device as claimed in claim 1, the process comprising: 30
a. coating a solution of organic layer on a second conducting layer; and 40
b. assembling a first conducting layer upon second surface of the organic layer to obtain the device.
24) The process as claimed in claim 23, wherein the solution of organic layer comprises a solvent and at least one compound of Formula I or Formula II.
25) The process as claimed in claim 24, wherein the solvent is selected from 5 acetonitrile (CH3CN), dimethyl formamide (DMF), dichloromethane (CH2Cl2), dichloroethane (ClCH2CH2Cl), chloroform (CH3Cl), methanol (CH3OH), ethanol (C2H5OH), or combinations thereof.
26) The process as claimed in claim 23, wherein the coating is carried out by spin coating, jet printing, sol-gel coating, slot die coating, or combinations 10 thereof.
27) The process as claimed in claim 23, wherein the coating is carried out by spin coating at a speed in a range of 1000 to 12000 rpm, for a period in a range of 20 to 120 seconds.
28) The process as claimed in claim 23, wherein the first conducting layer is 15 deposited over the second surface of the organic layer by vacuum vapor deposition method, cluster ion beam method, pulsed laser deposition (PLD) method, chemical vapor deposition (CVD) method, plasma polymerization method, molecular beam epitaxy (MBE) method, or sputtering method.
29)An organic layer comprising a compound of Formula I or Formula II as 20 defined in claim 1.
30) The organic layer as claimed in claim 29, wherein the compound selected from a compound of Formula Ia, Formula Ib, Formula IIa, or Formula IIb as defined in claim 2 and 3.
31) The organic layer as claimed in any one of the claims 29-30, wherein the 25 organic layer exhibits multiple accessible redox states and memory effects via ionic and intermolecular rearrangements.
32)Use of the device as claimed in claim 1, or the organic layer as claimed in claim 29, as an in-memory computing element, wherein storage and processing of data are performed within the same physical location, thereby 30 enabling computational functions including, but not limited to, vector–
41
matrix multiplication, dot-product operations, and implementation in computing accelerators.
33)Use of the device as claimed in claim 1 or 2, or the organic layer as claimed in claim 29.
34)Use of the device as claimed in claim 1, or the organic layer as claimed in 5 claim 29, in electrical, sensory and computing appliances.
35) A sensor device comprising the device as claimed in claim 1, wherein the device exhibits responsive changes in electrical or optical properties upon exposure to environmental stimuli.
36) The sensor device as claimed in claim 35, wherein the environmental stimuli 10 comprise light irradiation, pH changes, temperature variations, or chemical exposure.
37)A computing system comprising an array of devices as claimed in claim 1, wherein the array is configured for parallel processing operations.
38) The computing system as claimed in claim 37, wherein the system is 15 configured for artificial intelligence or machine learning applications.
39)A multifunctional device comprising the device as claimed in claim 1, wherein the device simultaneously provides memory, sensing, and computing functionalities.
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