The photo-induced ultrafast electron dynamics in both anatase and rutile TiO_(2) are investigated by using the Boltzmann transport equation with the explicit incorporation of electron-phonon scattering rates.All struc...The photo-induced ultrafast electron dynamics in both anatase and rutile TiO_(2) are investigated by using the Boltzmann transport equation with the explicit incorporation of electron-phonon scattering rates.All structural parameters required for dynamic simulations are obtained from ab initio calculations.The results show that although the longitudinal optical modes significantly affect the electron energy relaxation dynamics in both phases due to strong Fr?hlich-type couplings,the detailed relaxation mechanisms have obvious differences.In the case of a single band,the energy relaxation time in anatase is 24.0 fs,twice longer than 11.8 fs in rutile.This discrepancy is explained by the different diffusion distributions over the electronic Bloch states and different scattering contributions from acoustic modes in the two phases.As for the multiple-band situation involving the lowest six conduction bands,the predicted overall relaxation times are about 47 fs and 57 fs in anatase and rutile,respectively,very different from the case of the single band.The slower relaxation in rutile is attributed to the existence of multiple rate-controlled steps during the dynamic process.The present findings may be helpful to control the electron dynamics for designing efficient TiO_(2)-based devices.展开更多
基金supported by the National Natural Science Foundation of China(No.22033006,No.21833006 and No.21773191)。
文摘The photo-induced ultrafast electron dynamics in both anatase and rutile TiO_(2) are investigated by using the Boltzmann transport equation with the explicit incorporation of electron-phonon scattering rates.All structural parameters required for dynamic simulations are obtained from ab initio calculations.The results show that although the longitudinal optical modes significantly affect the electron energy relaxation dynamics in both phases due to strong Fr?hlich-type couplings,the detailed relaxation mechanisms have obvious differences.In the case of a single band,the energy relaxation time in anatase is 24.0 fs,twice longer than 11.8 fs in rutile.This discrepancy is explained by the different diffusion distributions over the electronic Bloch states and different scattering contributions from acoustic modes in the two phases.As for the multiple-band situation involving the lowest six conduction bands,the predicted overall relaxation times are about 47 fs and 57 fs in anatase and rutile,respectively,very different from the case of the single band.The slower relaxation in rutile is attributed to the existence of multiple rate-controlled steps during the dynamic process.The present findings may be helpful to control the electron dynamics for designing efficient TiO_(2)-based devices.
