Energy-Conserving Surface Hopping for Auger Processes

• DOI: 10.1021/acs.jctc.4c00562
• Publication Date: 2024-06-21T03:44:47Z
• Authors: Shriya Gumber; Oleg V. Prezhdo
• Keywords: Surface hopping; Auger effect; Electric potential energy

Auger-type processes are ubiquitous in nanoscale materials because quantum confinement enhances Coulomb interactions, and there exist large densities of states. Modeling Auger requires the modification nonadiabatic (NA) molecular dynamics algorithms to include transitions caused by both NA couplings. The system is split into classical subsystems, e.g., electrons vibrations, as a result, energy conservation becomes nontrivial. In surface hopping, an electronic transition induced coupling accompanied velocity readjustment ensure total quantum-classical energy. A different treatment needed for driven interactions. We develop methodology that meticulously differentiates redistribution accompanying hops interaction correctly conserves at each transition. If interaction, hop redistributed within subsystem only. NA, between subsystems. Properly maintaining types crucial generate correct order events, obtain accurate times, maintain proper statistical distribution state populations, reach thermodynamic equilibrium. test method with biexciton annihilation Auger-assisted hot electron relaxation CdSe dot. sequence phonon-driven calculated time scales excellent agreement experimental results. developed approach can be coupled any surface-hopping provides practical advance study charge-carrier condensed matter systems.