Charge disproportionate molecular redox for discrete memristive and memcapacitive switching

Goswami, Shyamaprosad; Rath, Santi Prasad; Thompson, Damien; Hedström, Svante; Annamalai, Meenakshi; Pramanick, Rajib; Ilić, B.; Sarkar, Soumya; Hooda, Sonu; Nijhuis, Christian A.; Martin, Jens; Williams, R. Stanley; Goswami, Sreebrata; Venkatesan, T.

doi:10.1038/s41565-020-0653-1

Nat. Nanotechnol.

2020

DOI: 10.1038/s41565-020-0653-1

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Charge disproportionate molecular redox for discrete memristive and memcapacitive switching

Shyamaprosad Goswami

Santi Prasad Rath

Damien Thompson

et al.

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Cited by 83 publications

(82 citation statements)

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“…[43,44] Figure 1b,c shows the current-voltage I(V) data measured on systems A and B respectively. Consistent with previous reports, [47,48] while system-A shows a binary memristive characteristic (Figure 1b), system-B yields a ternary memristor ( Figure 1c). The traces in black represent an average curve while the background cloud (purple for system-A and green for system-B) consists of all data points obtained by measuring the I(V)s at 100 different points (for both systems), showing the reproducibility and consistency of our measurement.…”

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confidence: 92%

“…Note that the I(V)s presented in Figure 1b,c are qualitatively similar to those reported in refs. [47,48]. However, in usual memristive geometry with flat electrodes the spin cast interface is known to offer a large charge injection barrier.…”

mentioning

confidence: 99%

“…Since the molecular film is nonvolatile (see refs. [47,48]), once written, the corresponding state is maintained during reading. For reading the surface conductance in both the ON-and OFF-states, the film surface was scanned with a tip voltage of 150 mV (V RB ) for both states (which can neither turn the film ON nor OFF), as shown with the red circles in Figure 2b.…”

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confidence: 99%

“…Refs. [47,48] established that the memristive switching in both systems A and B are caused by molecular redox. In those reports, bulk spectroscopic techniques (such as UV-vis and micro-Raman spectroscopy) were used to determine the molecular changes during the switching events.…”

mentioning

confidence: 99%

“…We compared our nano-Raman data to the micro-Raman data (schematically shown in the right panel of Figure 3a) adopted from refs. [47,48] (micro-Raman resolution ≈1 µm [52] ). As shown in Figure 3b,c, the spectral changes observed in our TERS data between different conductance states are essentially identical to those observed in micro-Raman for both systems A and B.…”

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confidence: 99%

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Nanometer‐Scale Uniform Conductance Switching in Molecular Memristors

et al. 2020

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energy-efficient, high-density data storage, and computing are the subject of intense research. [1-3] Memristors are promising building blocks for the next generation of electronics because they enable emerging highly efficient computing platforms such as in-memory and neuromorphic computing. [4,5] Of all genres of memristors, nonvolatile oxide materials are believed to be the most successful candidates in terms of their commercial potential. All the oxide memristors in use today are primarily based on filamentary mechanisms, which are inherently nonuniform [6-8] and thus exhibit performance variability and compromised device-yield. [9] In fact, the issue of nonuniformity and stochasticity is not only specific to oxides but is common in other genres of memristors like phase change memories, [10] nitrides, [11] or those working on metal-ion migration. [12-14] One of the problematic features inherent to any filamentary mechanism is electroforming, which is the first-time switching process involving dissolution, injection, and orientation of the active conducting atoms/ions into the dielectric layer. [7,15-17] The forming process usually requires much higher voltage and current than the reading/writing processes, resulting in One common challenge highlighted in almost every review article on organic resistive memory is the lack of areal switching uniformity. This, in fact, is a puzzle because a molecular switching mechanism should ideally be isotropic and produce homogeneous current switching free from electroforming. Such a demonstration, however, remains elusive to date. The reports attempting to characterize a nanoscopic picture of switching in molecular films show random current spikes, just opposite to the expectation. Here, this longstanding conundrum is resolved by demonstrating 100% spatially homogeneous current switching (driven by molecular redox) in memristors based on Ru-complexes of azo-aromatic ligands. Through a concurrent nanoscopic spatial mapping using conductive atomic force microscopy and in operando tip-enhanced Raman spectroscopy (both with resolution <7 nm), it is shown that molecular switching in the films is uniform from hundreds of micrometers down to the nanoscale and that conductance value exactly correlates with spectroscopically determined molecular redox states. This provides a deterministic molecular route to obtain spatially homogeneous, forming-free switching that can conceivably overcome the chronic problems of robustness, consistency, reproducibility, and scalability in organic memristors.

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confidence: 92%

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confidence: 99%

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confidence: 99%

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confidence: 99%

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confidence: 99%

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Nanometer‐Scale Uniform Conductance Switching in Molecular Memristors

et al. 2020

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Gold Nanoparticle in Chemoelectronics: Fundamentals, Challenges, and Future Prospects

Wang,

Liu,

Guo

et al. 2023

Adv Funct Materials

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The basic components of modern electronics are primarily fabricated by using semiconductor material in which the movement of charges can be electrically modulated. For metallic material, however, such modulation is almost impossible because of its field‐shielding characteristics, leading to insensitive response toward applied potentials. In this perspective, how to overcome this limitation of bulk metals (here, gold is taken as a particular example) is demonstrated by reducing the size to the nanoscale and functionalizing these nanogolds with charged molecules. The movement of mobile counterions within gold nanoparticle (AuNP) layers can generate charge gradients that feed back and control the motion of electrons which enables to design and fabricate several important components such as the diode, transistor, logic circuits, memristor, and various chemiresistive sensors. The assembly of AuNP electronic components and sensors gives rise to a new class of nanoparticle‐based “chemoelectronic” logic circuits that can sense, process, and ultimately report various chemical signals. The gas sensors are believed to be the most appropriate candidates for such integration as no solvent/solution is required and therefore, in the end, the combination of AuNP gas sensors and memristors is outlooked to achieve all‐gold‐nanoparticle in‐sensor computing for the development of future artificial olfactory.

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Stable Universal 1‐ and 2‐Input Single‐Molecule Logic Gates

et al. 2022

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Controllable single‐molecule logic operations will enable development of reliable ultra‐minimalistic circuit elements for high‐density computing but require stable currents from multiple orthogonal inputs in molecular junctions. Utilizing the two unique adjacent conductive molecular orbitals (MOs) of gated Au/S‐(CH2)3‐Fc‐(CH2)9‐S/Au (Fc = ferrocene) single‐electron transistors (≈2 nm), a stable single‐electron logic calculator (SELC) is presented, which allows real‐time modulation of output current as a function of orthogonal input bias (Vb) and gate (Vg) voltages. Reliable and low‐voltage (ǀVbǀ ≤ 80 mV, ǀVgǀ ≤ 2 V) operations of the SELC depend upon the unambiguous association of current resonances with energy shifts of the MOs (which show an invariable, small energy separation of ≈100 meV) in response to the changes of voltages, which is confirmed by electron‐transport calculations. Stable multi‐logic operations based on the SELC modulated current conversions between the two resonances and Coulomb blockade regimes are demonstrated via the implementation of all universal 1‐input (YES/NOT/PASS_1/PASS_0) and 2‐input (AND/XOR/OR/NAND/NOR/INT/XNOR) logic gates.

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Charge disproportionate molecular redox for discrete memristive and memcapacitive switching

Cited by 83 publications

References 63 publications

Nanometer‐Scale Uniform Conductance Switching in Molecular Memristors

Nanometer‐Scale Uniform Conductance Switching in Molecular Memristors

Gold Nanoparticle in Chemoelectronics: Fundamentals, Challenges, and Future Prospects

Stable Universal 1‐ and 2‐Input Single‐Molecule Logic Gates

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