Oxygen-containing rare-earth metal hydride YH_xO_y,is a newly found photochromic material showing fast photoresponse.While its preparation method,optical properties and structural features have been studied extensivel...Oxygen-containing rare-earth metal hydride YH_xO_y,is a newly found photochromic material showing fast photoresponse.While its preparation method,optical properties and structural features have been studied extensively,the photochromic mechanism in YH_xO_yremains unknown Here,using excited-state molecular dynamics simulation based on the recently developed real-time time-dependent density functional theory(RT-TDDFT)method,we study the photochemical reactions in YH_xO_y.We find that under photoexcitation,dihydrogen defects are formed within 100 fs.The dihydrogen defect behaves as a shallow donor and renders the material strongly n-type doped,which could be responsible for the photochromic effect observed in YH_xO_y.We also find that oxygen concentration affects the metastability of the dihydrogen species,meaning that the energy barrier for the dihydrogen to dissociate is related to the oxygen concentration The highest barrier of 0.28 eV is found in our model with O/Y=1:8.If the oxygen concentration is too low,the dihydrogen will quickly dissociate when the excitation is turned off.If the oxygen concentration is too high,the dihydrogen dissociates even when the excitation is still on.展开更多
基金the support by the National Natural Science Foundation of China(11774365)。
文摘Oxygen-containing rare-earth metal hydride YH_xO_y,is a newly found photochromic material showing fast photoresponse.While its preparation method,optical properties and structural features have been studied extensively,the photochromic mechanism in YH_xO_yremains unknown Here,using excited-state molecular dynamics simulation based on the recently developed real-time time-dependent density functional theory(RT-TDDFT)method,we study the photochemical reactions in YH_xO_y.We find that under photoexcitation,dihydrogen defects are formed within 100 fs.The dihydrogen defect behaves as a shallow donor and renders the material strongly n-type doped,which could be responsible for the photochromic effect observed in YH_xO_y.We also find that oxygen concentration affects the metastability of the dihydrogen species,meaning that the energy barrier for the dihydrogen to dissociate is related to the oxygen concentration The highest barrier of 0.28 eV is found in our model with O/Y=1:8.If the oxygen concentration is too low,the dihydrogen will quickly dissociate when the excitation is turned off.If the oxygen concentration is too high,the dihydrogen dissociates even when the excitation is still on.
