(Invited) Electron Transport Characteristics through Ferrocene in Aqueous Solution: Density Functional Theory – Non-Equilibrium Green Function Approach

Tuesday, 11 October 2022: 14:40
Room 304 (The Hilton Atlanta)
J. I. Choi (Georgia Institute of Technology), H. S. Kim (Korea Institute of Science and Technology Information), Y. S. Shin, C. Johnson, N. Fomina, A. Darvish, C. Lang (Robert Bosch LLC), and S. S. Jang (Georgia Institute of Technology)
Charge transport properties through aqueous solutions are investigated using computational device models in which aqueous solution is sandwiched between two Pt electrodes. The device includes three characteristic material phases, such as metal electrode, electrode-solution interface, and bulk solution phases. In order to achieve a fundamental understanding of electron transport via molecule solvated in aqueous solution, we prepare a model by introducing a ferrocene molecule in the water phase between Pt electrodes, and then calculate quantum transport properties using DFT-based non-equilibrium Green function method. It turns out that water-Pt interaction affects the orientations of water molecules at the interface and redistributes the surface charge density at the electrodes. To address the water phase configurations, we perform ab-initio molecular dynamics simulations at given bias conditions established by the effective screening medium method, presenting higher water density at the Pt-water interface region and a noticeable change in electrostatic potential profile due to the presence of ferrocene molecule in water phase. A noteworthy discovery in this study is that the ferrocene solution specifically produces strong transmission distribution near the Fermi level, and high electron density of states spatially connecting both electrodes, which explains the drastic increase in current-voltage characteristics. Therefore, it is conclusive that the ferrocene takes role in enhancing electron transport through the solution.