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1.
ACS Nano ; 18(22): 14457-14468, 2024 Jun 04.
Artículo en Inglés | MEDLINE | ID: mdl-38764188

RESUMEN

In artificial synaptic devices aimed at mimicking neuromorphic computing systems, electrical or optical pulses, or both, are generally used as stimuli. In this work, we introduce chiral materials for tailoring the characteristics of photonic synaptic devices to achieve handedness-dependent neuromorphic computing and in-memory logic gates. In devices based on a pair of chiral perovskites, the use of circularly polarized light (CPL) as the optical stimuli mimicked a series of electrical and opto-synaptic functionalities in order to emulate the multifunctional complex behavior of the human brain. Upon illumination in this two-terminal device, anisotropy in current has been observed due to the out-of-plane carrier transport, originating from spin-selective carrier transport. More importantly, the logic gate achieved in devices based on optoelectronic memristors turned out to be chirality-dependent; while an R-device functioned as an AND gate, the device based on the same perovskite of the opposite chirality (S-device) acted as a NOR gate toward in-memory logic operations. These findings in chiral perovskite-based artificial synapses can identify further strategies for future neuromorphic computing, vision simulation, and artificial intelligence.

2.
Nanoscale ; 15(10): 5001-5010, 2023 Mar 09.
Artículo en Inglés | MEDLINE | ID: mdl-36786743

RESUMEN

A family of rudorffites based on silver-bismuth-iodide shows a transition from a conventional positive photoconductivity (PPC) to an unusual negative photoconductivity (NPC) upon variation in the precursor stoichiometry while forming the rudorffites. The NPC has arisen in silver-rich rudorffites due to the generation of illumination-induced trap-states which prompted the recombination of charge carriers and thereby a decrease in the conductivity of the compounds. In addition to photoconductivity, sandwiched devices based on all the rudorffites exhibited resistive switching between a pristine high resistive state (HRS) and a low resistive state (LRS) under a suitable voltage pulse; the switching process, which is reversible, is associated with a memory phenomenon. The devices based on NPC-exhibiting rudorffites switched to the HRS under illumination as well. That is, the resistive state of the devices could be controlled through both electrical and optical inputs. We employed such interesting optoelectronic properties of NPC-exhibiting rudorffites to exhibit OR logic gate operation. Because the devices could function as a logic gate and store the resistive state as well, we concluded that the materials could be an ideal candidate for in-memory logic operations.

3.
J Phys Chem Lett ; 13(7): 1660-1667, 2022 Feb 24.
Artículo en Inglés | MEDLINE | ID: mdl-35147437

RESUMEN

In this Letter, we introduce scanning tunneling spectroscopy (STS) to quantify the Urbach energy (EU) in disordered semiconductors. The technique enabled us to gain precise information on the extending component of conduction and valence band-edges responsible for Urbach tailing, individually; such information has been obtained from the width of band-energy-histograms drawn from STS studies at many different points. STS, as a probing method at the microscopic scale to derive EU, is in contrast to commonly employed optical spectroscopy studies which provide information at the macroscopic scale. A comparison between Urbach energy values from optical studies and distribution of band-edges obtained from STS revealed the inherent inaccuracies involved in the optical characterization process. We have considered copper oxide (CuxO) thin films in this regard; we show that through STS and the associated density of state (DOS) spectra, we can derive accurate information on the band-edges' distribution leading to EU in different phases of the binary oxide thin films.

4.
ACS Nano ; 15(12): 20203-20213, 2021 Dec 28.
Artículo en Inglés | MEDLINE | ID: mdl-34878256

RESUMEN

We map spatially correlated electrical current on the stacking boundaries of pristine and doped hexagonal boron nitride (hBN) to distinguish from its insulating bulk via conductive atomic force microscopy (CAFM). While the pristine edges of hBN show an insulating nature, the O-doped edges reveal a current 2 orders of higher even for bulk layers where the direct transmission through tunnel barrier is implausible. Instead, the nonlinear current-voltage characteristics (I-V) at the edges of O-doped hBN can be explained by trap-assisted lowering of the tunnel barrier by adopting a Poole-Frenkel (PF) model. However, in the stacked heterostructure with multilayer graphene (MLG) on top, the buried edge of pristine hBN shows a signature of electron conduction in the scanning mode which contradicts the first-principle calculation of spatial distribution of local density of states (LDOS) data. Enhancement of friction between the Pt-tip and MLG at the step-edge of the heterostructure while scanning in the contact mode has prompted us to construct a phenomenological model where the localization of opposite surface charges on two conducting plates (MLG and Si substrate) containing a dielectric film (hBN) with negatively charged defects creates an internal electric field opposite to the external electric field due to the applied voltage bias in the CAFM setup. An equivalent circuit with a parallel resistor network based on a vertical conducting channel through the MLG/hBN edge and an in-plane surface carrier transport through MLG can successfully analyze the current maps on pristine/doped hBN and the related heterostructures. These results yield fundamental insight into the emerging field of insulatronics in which defect-induced electron transport along the edge can be manipulated in an 1D-2D synergized insulator.

5.
J Phys Condens Matter ; 33(24)2021 May 13.
Artículo en Inglés | MEDLINE | ID: mdl-33631725

RESUMEN

We present evolution of band energies in α-NiS when alloyed with a cationic doping through isovalent cadmium (Cd2+). Optical bandgap of nickel-cadmium sulfide (Ni1-xCdxS) alloys, as a deviation from the linear relationship or Vegard's law, have exhibited a reverse bandgap-bowing in the form of downward-concave dependence. Such a phenomenon, which manifests as a negative value of bowing coefficient (b), is uncommon in chalcogenide alloys. In this work, we have deliberated on the origin of reverse bandgap-bowing in nickel-cadmium alloys and identified the band responsible for the bowing phenomenon. While thin-films of the alloys were formed through successive ionic layer adsorption and reaction method, tunnel conductance and thereby density of states of the materials were derived from scanning tunneling spectroscopy. The spectroscopy provided the variation of conduction and valence band-edges (CB and VB, respectively) with respect to the cadmium-content in Ni1-xCdxS. The CB-edge of the alloys could be seen to remain mostly unaffected with increasing cadmium-content, since the band is composed of only the S 2porbitals; the VB-energy, on the other hand, which forms due to an effective coupling between the metaldand the anionporbitals, could be seen to be affected due to ap-drepulsion. Based on our experimental findings, we inferred that an antagonism between volume deformation and structural relaxation had resulted in the reverse bandgap-bowing in Ni1-xCdxS alloys.

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