The ring-polymer molecular dynamics(RPMD)was used to calculate the thermal rate coefficients of the multi-channel roaming reaction H+MgH→Mg+H_(2).Two reaction channels,tight and roaming,are explicitly considered.This...The ring-polymer molecular dynamics(RPMD)was used to calculate the thermal rate coefficients of the multi-channel roaming reaction H+MgH→Mg+H_(2).Two reaction channels,tight and roaming,are explicitly considered.This is a pioneering attempt of exerting RPMD method to multichannel reactions.With the help of a newly developed optimization-interpolation protocol for preparing the initial structures and adaptive protocol for choosing the force constants,we have successfully obtained the thermal rate coefficients.The results are consistent with those from other theoretical methods,such as variational transition state theory and quantum dynamics.Especially,RPMD results exhibit negative temperature dependence,which is similar to the results from variational transition state theory but different from the ones from ground state quantum dynamics calculations.展开更多
基金supported by the National Natural Science Foundation of China(No.21503130 and No.11674212,and No.21603144)supported by the Young Eastern Scholar Program of the Shanghai Municipal Education Commission(QD2016021)+1 种基金the Shanghai Key Laboratory of High Temperature Superconductors(No.14DZ2260700)supported by Shanghai Sailing Program(No.2016YF1408400).
文摘The ring-polymer molecular dynamics(RPMD)was used to calculate the thermal rate coefficients of the multi-channel roaming reaction H+MgH→Mg+H_(2).Two reaction channels,tight and roaming,are explicitly considered.This is a pioneering attempt of exerting RPMD method to multichannel reactions.With the help of a newly developed optimization-interpolation protocol for preparing the initial structures and adaptive protocol for choosing the force constants,we have successfully obtained the thermal rate coefficients.The results are consistent with those from other theoretical methods,such as variational transition state theory and quantum dynamics.Especially,RPMD results exhibit negative temperature dependence,which is similar to the results from variational transition state theory but different from the ones from ground state quantum dynamics calculations.
