Our proposal titled “CD&E: Ab Initio Ultrafast Dynamics of Spin, Valley and Charge in Quantum Materials” has been funded by NSF/DMR-CMMT (Condensed Matter and Materials Theory) under grant number 1956015, in collaboration with Prof. Sundararaman at RPI.
Technical Summary: The goal of this research project is to predict quantitatively quantum dynamics of electrons with spin, valley, or other internal degrees of freedom, entirely from first principles. Our research team will develop a novel computational methodology and associated massively-parallel open-source software rapidly to evolve density matrices of quantum materials in a Lindbladian formulation, with ab initio treatment of electron-electron, electron-phonon, and electron-photon interactions. This will facilitate calculation of both coherent dynamics and dephasing of spin or valley polarization, along with their experimental signatures in ultrafast spectroscopy. Using this technique, they will investigate spin dynamics in systems with strong spin-orbit coupling and Rashba splitting such as lead halide perovskites and ferroelectric oxides, and valley dynamics in layered transition metal dichalcogenides. This fundamentally new predictive capability will facilitate quantitative analysis of ultrafast optical and free-electron laser measurements with linear and circular polarization, and accurate predictions of spin relaxation of quantum materials. This will be critical for the design and discovery of new material platforms for spintronics, valleytronics and quantum information.