Sahu, Satyajit

Scanning tunneling microscopy (STM) is a powerful technique for investigating the nanoscale properties of functional materials. Additionally, scanning tunneling spectroscopy (STS) facilitates the determination of the local density of states (LDOS) within the material. In this study, we present an exploration of the resistive switching (RS) properties and neuromorphic computing capabilities of individual AgInS2 quantum dots, utilizing STM and STS techniques. By examining the material’s bandgap and its temperature dependence, we uncover a nonlinear variation below the Debye temperature and a linear trend at higher temperatures. Moreover, STS measurements demonstrate changes in the conducting states induced by localized pulses, further confirming the unique characteristics of the quantum dots. The experimental devices constructed by using these quantum dots effectively replicate the RS properties observed at the nanoscale. To assess the neuromorphic application of the devices, pulse transient measurements simulating the learning and forgetting processes were conducted. The gradual set and reset processes successfully mimic the information retention and erasure capabilities essential for neuromorphic computing. Notably, the resistive switching mechanism in these devices is attributed to localized ionic transport, which highlights the significant involvement of ionic species in the observed RS behavior. The outcomes of this study contribute to the fundamental understanding of RS properties in single AgInS2 quantum dots and offer valuable insights into their potential applications in neuromorphic computing.

Hydrogen (H2) is widely used in industrial processes and is one of the well-known choices for storage of renewable energy. H2 detection has become crucial for safety in manufacturing, storage, and transportation due to its strong explosivity. To overcome the issue of explosion, there is a need for highly selective and sensitive H2 sensors that can function at low temperatures. In this research, we have adequately fabricated an unreported van der Waals (vdWs) PdSe2/WS2 heterostructure, which exhibits exceptional properties as a H2 sensor. The formation of these heterostructure devices involves the direct selenization process using chemical vapor deposition (CVD) of Pd films that have been deposited on the substrate of SiO2/Si by DC sputtering, followed by drop casting of WS2 nanoparticles prepared by a hydrothermal method onto device substrates including pre-patterned electrodes. The confirmation of the heterostructure has been done through the utilization of powder X-ray diffraction (XRD), depth-dependent X-ray photoelectron spectroscopy (XPS) and field-emission scanning electron microscopy (FE-SEM) techniques. Also, the average roughness of thin films is decided by Atomic Force Microscopy (AFM). The comprehensive research shows that the PdSe2/WS2 heterostructure-based sensor produces a response that is equivalent to 67.4% towards 50 ppm H2 at 100 °C. The response could be a result of the heterostructure effect and the superior selectivity for H2 gas in contrast to other gases, including NO2, CH4, CO and CO2, suggesting tremendous potential for H2 detection. Significantly, the sensor exhibits fast response and a recovery time of 31.5 s and 136.6 s, respectively. Moreover, the explanation of the improvement in gas sensitivity was suggested by exploiting the energy band positioning of the PdSe2/WS2 heterostructure, along with a detailed study of variations in the surface potential. This study has the potential to provide a road map for the advancement of gas sensors utilizing two-dimensional (2D) vdWs heterostructures, which exhibit superior performance at low temperatures.

The tunable molecular scaffold of organic moieties in metallopolymers generates variation in their properties, but what could be the minimal change that can produce variation in the properties of these macromolecules is still untouched. This research has meticulously explored the trivial change in the molecular scaffold of the ligand capable of making a mammoth difference in the nonvolatile memory and coordination pattern in two metallopolymers. The significance of this research lies in the fact that it demonstrates how a slight change in the organic building block can significantly alter the memristive and fluorescence properties of iron(ii) metallopolymers, opening up new possibilities for their design and synthesis. Two novel positional isomeric ligands and their corresponding iron(ii)-polymers were synthesized and thoroughly characterized using NMR, XRD, ATR-IR, FESEM, AFM and other techniques. Bright orange solid and solution state fluorescence was observed both in the solid and solution states for ligand L2 (3,3′-bis((E)-(pyridin-3-ylimino)methyl)-[1,1′-biphenyl]-4,4′-diol), while ligand L1 (3,3′-bis((E)-(pyridin-2-ylimino)methyl)-[1,1′-biphenyl]-4,4′-diol) showed blue fluorescence in the solution state only. A robust memristive property for Fe(ii)-L1-poly with a high current ON/OFF ratio of 104, remarkable random access behaviour, and a long retention time greater than 35 000 seconds was observed while its counterpart was entirely silent. Both polymers showed solution-state electrochromism. These synthesised metallopolymers also showed good specific capacitance in the range of 50-60 F g−1 with a remarkable retention of 98% of the initial value even after 5000 charge-discharge cycles. The AFM and FESEM micrographs revealed the formation of long polymer nano-rods, which correlates with the NMR, ATR-IR, and XRD results. The difference in the properties of polymers generated by such a slight change in the organic building block forces different coordination patterns of these two ligands around the same central metal ion, and this is also evident in all the characterization methods.

New 2D layered materials WX2N4(X≐Si, Ge)1 are suitable for thermoelectric applications for a pretty good value of the figure of merit (ZT). Here, the thermoelectric properties of the 2D monolayer of WX2N4(X≐Si, Ge) using Density Functional Theory (DFT) is investigated combined with Boltzmann Transport Equation (BTE) along with spin-orbit coupling (SOC). An excellent thermoelectric (Formula presented.) of 0.91 (0.92 with SOC) is obtained at 900 K for p-type WGe2N4, and a (Formula presented.) of 0.81 (0.86 with SOC) is observed for n-type at the same temperature. Furthermore, the WGe2N4 showed a (Formula presented.) of more than 0.7 (0.79 with SOC) at room temperature for p-type. On the other hand, the WSi2N4 showed a comparatively lower (Formula presented.) at room temperature. However, the (Formula presented.) value increases significantly at higher temperatures, reaching 0.72 (0.79 with SOC) and 0.71 (0.62 with SOC) for p and n-type at 900 K, respectively. The electronic band structure is examined and discovered that WSi2N4 and WGe2N4 possess indirect bandgaps (BG) of 2.68 eV (2.57 eV with SOC) and 1.53 eV (1.46 eV with SOC), respectively, according to Heyd-Scuseria-Ernzerhof (HSE) approximation. These materials may also be useful in UV and visible range optoelectronic devices because of their strong absorption in the respective regions.

Recently, researchers have focused on developing more stable, Pb-free perovskites with improved processing efficiency and notable light harvesting ability. In this regard, Sn-based (Sn-b) perovskites have gained considerable interest in developing eco-friendly perovskite solar cells (PSCs). However, the oxidation of Sn2+ to Sn4+ deteriorates the performance of Sn-b PSCs. Nevertheless, this issue could be mitigated by doping alkaline earth (AE) metal. Herein, we have studied the significance of AE doping on CsSnX3 (X = Br, I) perovskites using density functional theory based calculations. The structural, electronic, and optical properties of CsAE y Sn1−y X3 (y = 0, 0.25; AE = Be, Mg, Ca, Sr) compounds were systematically investigated to explore potential candidate materials for photovoltaic applications. Formation energy calculations suggested that the synthesis of other AE-doped compounds is energetically favorable except for the Be-doped compounds. The band gaps of the materials were calculated to be in the range of 0.12-1.02 eV using the generalized gradient approximation. Furthermore, the AE doping considerably lowers the exciton binding energy while remarkably enhancing the optical absorption of CsSnX3, which is beneficial for solar cells. However, in the case of Be and Mg doping, an indirect band gap is predicted. Our theoretical findings demonstrate the potential of executing AE-doped perovskites as absorber material in PSCs, which could deliver better performance than pristine CsSnX3 PSCs.

All inorganic halide perovskites have received tremendous significance in the perovskite solar cells (PSCs) technology. The toxicity in PSCs due to Pb element concerns to the environment, thus replacement of Pb is a prerequisite in the development of PSCs. In this study, we have studied strain-induced structural and electronic properties of lead-free ASnBr3 (A = Cs, Rb, K) perovskites using density functional theory based first principles calculation. The band gap values of these perovskites are varied from 0 to 1.14 eV within the strain range of -4 to 4%.

Artificial synapses based on resistive switching have emerged as a promising avenue for brain-inspired computing. Hybrid metal halide perovskites have provided the opportunity to simplify resistive switching device architectures due to their mixed electronic-ionic conduction, yet the instabilities under operating conditions compromise their reliability. We demonstrate reliable resistive switching and synaptic behaviour in layered benzylammonium (BzA) based halide perovskites of (BzA)2PbX4 composition (X = Br, I), showing a transformation of the resistive switching from digital to analog with the change of the halide anion. While (BzA)2PbI4 devices demonstrate gradual set and reset processes with reduced power consumption, the (BzA)2PbBr4 system features a more abrupt switching behaviour. Moreover, the iodide-based system displays excellent retention and endurance, whereas bromide-based devices achieve a superior on/off ratio. The underlying mechanism is attributed to the migration of halide ions and the formation of halide vacancy conductive filaments. As a result, the corresponding devices emulate synaptic characteristics, demonstrating the potential for neuromorphic computing. Such resistive switching and synaptic behaviour highlight (BzA)2PbX4 perovskites as promising candidates for non-volatile memory and neuromorphic computing.

All inorganic CsPbX3 perovskites (X = Br and I) are excellent candidates for stable and efficient perovskite solar cells (PSCs). Among them, CsPbIBr2 demonstrated the most balanced characteristics in terms of band gap and stability. Nevertheless, the power conversion efficiency (PCE) of CsPbIBr2-based solar cells is still far from that of Hybrid PSCs, and more research is required in this aspect. Herein, DFT and SCAPS-1D frameworks are employed to explore the optimized device configurations of CsPbIBr2 PSCs. DFT is used to explore the structural and optoelectronic characteristics of CsPbIBr2, while SCAPS-1D is employed to examine various device structures of CsPbIBr2-based PSCs. The band structure demonstrated the direct band gap nature of CsPbIBr2 with a band gap of 2.12 eV. Moreover, we have used TiO2, SnO2, ZnO, WS2, IGZO, CeO2, In2S3, and CdS as ETLs, and Cu2O, CuI, MoO3, NiO, CuSCN, CuSbS2, CBTS, CFTS, and CuO as HTLs for identifying the best ETL/CsPbIBr2/HTL configurations. Among 72 device combinations, eight sets of PSCs are identified as the most efficient configurations. In addition, the influence of various parameters like the thickness of various layers, doping concentration, perovskite defect density, ETLs and interfaces, series resistances, shunt resistances, and temperature on device performance have been comprehensively studied. The results demonstrate Cu2O as the best HTL for CsPbIBr2 with each ETL, and PSC with device structure ITO/WS2/CsPbIBr2/Cu2O/C exhibited the highest PCE of 16.53%. This comprehensive investigation will provide new path for the development of highly efficient all-inorganic CsPbIBr2 solar cells.

Semiconducting 2D transition metal dichalcogenides (TMDC) became very popular in photodetection due to their high mobility and high rate of generating electron and hole pairs. Over the past decade, MoS2 and WS2 became the most popular TMDC for several applications. On the other hand, due to the complex synthesis process compared to MoS2 and WS2, SnS2 became a less popular 2D material for photodetection. We synthesized vertically aligned SnS2 flakes by a chemical vapor deposition (CVD) process with three temperature zones with controlled argon (Ar) gas flow. Pristine SnS2-based devices are not very suitable for photodetection applications because of their low photo-to-dark current ratio (Iph/Idark), high response time, and low stability. So, they need to be decorated with oppositely doped materials. We decorated pristine SnS2-based devices with rGO nanoparticles, which significantly increased the device’s performance. We found a high responsivity (R) of 1.33 A/W, detectivity (D) of 6.95 × 1011 Jones, Iph/Idark of 102, and a rise time of 0.241 ms (fall time of 1.318 ms) with the rGO decorated SnS2-based device.

Semiconducting 2D transition metal dichalcogenides (TMDC) became very popular in photodetection due to their high mobility and high rate of generating electron and hole pairs. Over the past decade, MoS2 and WS2 became the most popular TMDC for several applications. On the other hand, due to the complex synthesis process compared to MoS2 and WS2, SnS2 became a less popular 2D material for photodetection. We synthesized vertically aligned SnS2 flakes by a chemical vapor deposition (CVD) process with three temperature zones with controlled argon (Ar) gas flow. Pristine SnS2-based devices are not very suitable for photodetection applications because of their low photo-to-dark current ratio (Iph/Idark), high response time, and low stability. So, they need to be decorated with oppositely doped materials. We decorated pristine SnS2-based devices with rGO nanoparticles, which significantly increased the device’s performance. We found a high responsivity (R) of 1.33 A/W, detectivity (D) of 6.95 × 1011 Jones, Iph/Idark of 102, and a rise time of 0.241 ms (fall time of 1.318 ms) with the rGO decorated SnS2-based device.