Unveiling Negative Differential Resistance and Superionic Conductivity: Water Anchored on Layered Materials.

Autor: Manamel LT; eNDR Lab, School of Physics, IISER Thiruvananthapuram, Vithura, Trivandrum 695551, Kerala, India., Singh A; Department of Physics, Indian Institute of Technology Delhi, Hauz Khas, New Delhi 110016, India., Saha P; eNDR Lab, School of Physics, IISER Thiruvananthapuram, Vithura, Trivandrum 695551, Kerala, India., Sathyanarayana S; eNDR Lab, School of Physics, IISER Thiruvananthapuram, Vithura, Trivandrum 695551, Kerala, India., Bhattacharya S; Department of Physics, Indian Institute of Technology Delhi, Hauz Khas, New Delhi 110016, India., Das BC; eNDR Lab, School of Physics, IISER Thiruvananthapuram, Vithura, Trivandrum 695551, Kerala, India.
Jazyk: angličtina
Zdroj: The journal of physical chemistry letters [J Phys Chem Lett] 2024 Aug 15; Vol. 15 (32), pp. 8167-8176. Date of Electronic Publication: 2024 Aug 02.
DOI: 10.1021/acs.jpclett.4c01319
Abstrakt: Unravelling the perplexing nature of negative differential resistance (NDR) in 2D transition metal dichalcogenide (2D TMD) devices, especially regarding intrinsic properties, is hindered by experiments conducted in ambient environments. A thorough investigation is essential for unveiling the actual mechanism. In this study, we provide compelling evidence of the NDR effect with a remarkably high peak-to-valley current ratio and proton-diffused superionic conductivity in quantum-confined water molecules anchored to a thin film of 2D TMDs. Our investigation underscores the crucial role of ambient moisture for this robust NDR effect independent of underlying materials used. The bonding of water molecules to the existing sulfur defect sites on 2D TMD nanoflakes facilitates the formation of bridges between two planar metal electrodes, thus enabling superionic in-plane protonic conduction. During electrolysis of chemisorbed water, protons are liberated at the anode and migrate toward the cathode during bias voltage sweeping. Nevertheless, proton diffusion encounters increasing impedance beyond a certain applied bias, thereby restricting current flow even with higher biasing voltages, which is attributed to the interfacial Schottky energy barrier influenced by the Fermi level pinning effect. Our DFT simulations corroborate this mechanism, revealing minimal intermolecular interaction of H + ions compared to OH - ions at distinct atomic sites on 2D TMD nanoflakes.
Databáze: MEDLINE