The branching corrected surface hopping(BCSH)has been demonstrated as a robust approach to improve the performance of the traditional fewest switches surface hopping(FSSH)for nonadiabatic dynamics simulations of stand...The branching corrected surface hopping(BCSH)has been demonstrated as a robust approach to improve the performance of the traditional fewest switches surface hopping(FSSH)for nonadiabatic dynamics simulations of standard scattering problems[J.Chem.Phys.150,164101(2019)].Here,we study how reliable populations of both adiabatic and diabatic states can be interpreted from BCSH trajectories.Using exact quantum solutions and FSSH results as references,we investigate a series of one-dimensional two-level scattering models and illustrate that excellent timedependent populations can be obtained by BCSH.Especially,we show that different trajectory analysis strategies produce noticeable differences in different representations.Namely,the method based on active states performs better to get populations of adiabatic states,while the method based on wavefunctions produces more reliable results for populations of diabatic states.展开更多
Photoinduced carrier dynamic processes are without doubt the main driving force responsible for the efficient performance of semiconductor nanomaterials in applications like photoconversion and photonics.Nevertheless,...Photoinduced carrier dynamic processes are without doubt the main driving force responsible for the efficient performance of semiconductor nanomaterials in applications like photoconversion and photonics.Nevertheless,establishing theoretical insights into these processes is computationally challenging owing to the multiple factors involved in the processes,namely reaction rate,material surface area,material composition etc.Modelling of photoinduced carrier dynamic processes can be performed via nonadiabatic molecular dynamics(NA-MD)methods,which are methods specifically designed to solve the time-dependent Schrodinger equation with the inclusion of nonadiabatic couplings.Among NA-MD methods,surface hopping methods have been proven to be a mighty tool to mimic the competitive nonadiabatic processes in semiconductor nanomaterials,a worth noticing feature is its exceptional balance between accuracy and computational cost.Consequently,surface hopping is the method of choice for modelling ultrafast dynamics and more complex phenomena like charge separation in Janus transition metal dichalcogenides-based van der Waals heterojunction materials.Covering latest stateof-the-art numerical simulations along with experimental results in the field,this review aims to provide a basic understanding of the tight relation between semiconductor nanomaterials and the proper simulation of their properties via surface hopping methods.Special stress is put on emerging state-ot-the-art techniques.By highlighting the challenge imposed by new materials,we depict emerging creative approaches,including high-level electronic structure methods and NA-MD methods to model nonadiabatic systems with high complexity.展开更多
Inspired by the branching corrected surface hopping(BCSH)method[J.Xu and L.Wang,J.Chem.Phys.150,164101(2019)],we present two new decoherence time formulas for trajectory surface hopping.Both the proposed linear and ex...Inspired by the branching corrected surface hopping(BCSH)method[J.Xu and L.Wang,J.Chem.Phys.150,164101(2019)],we present two new decoherence time formulas for trajectory surface hopping.Both the proposed linear and exponential formulas characterize the decoherence time as functions of the energy difference between adiabatic states and correctly capture the decoherence effect due to wave packet reflection as predicted by BCSH.The relevant parameters are trained in a series of 200 diverse models with different initial nuclear momenta,and the exact quantum solutions are utilized as references.As demonstrated in the three standard Tully models,the two new approaches exhibit significantly higher reliability than the widely used counterpart algorithm while holding the appealing efficiency,thus promising for nonadiabatic dynamics simulations of general systems.展开更多
基金supported by the National Natural Science Foundation of China(No.21922305 and No.21873080)。
文摘The branching corrected surface hopping(BCSH)has been demonstrated as a robust approach to improve the performance of the traditional fewest switches surface hopping(FSSH)for nonadiabatic dynamics simulations of standard scattering problems[J.Chem.Phys.150,164101(2019)].Here,we study how reliable populations of both adiabatic and diabatic states can be interpreted from BCSH trajectories.Using exact quantum solutions and FSSH results as references,we investigate a series of one-dimensional two-level scattering models and illustrate that excellent timedependent populations can be obtained by BCSH.Especially,we show that different trajectory analysis strategies produce noticeable differences in different representations.Namely,the method based on active states performs better to get populations of adiabatic states,while the method based on wavefunctions produces more reliable results for populations of diabatic states.
基金supported by the National Natural Science Foundation of China(No.22073045)the Fundamental Research Funds for the Central Universities。
文摘Photoinduced carrier dynamic processes are without doubt the main driving force responsible for the efficient performance of semiconductor nanomaterials in applications like photoconversion and photonics.Nevertheless,establishing theoretical insights into these processes is computationally challenging owing to the multiple factors involved in the processes,namely reaction rate,material surface area,material composition etc.Modelling of photoinduced carrier dynamic processes can be performed via nonadiabatic molecular dynamics(NA-MD)methods,which are methods specifically designed to solve the time-dependent Schrodinger equation with the inclusion of nonadiabatic couplings.Among NA-MD methods,surface hopping methods have been proven to be a mighty tool to mimic the competitive nonadiabatic processes in semiconductor nanomaterials,a worth noticing feature is its exceptional balance between accuracy and computational cost.Consequently,surface hopping is the method of choice for modelling ultrafast dynamics and more complex phenomena like charge separation in Janus transition metal dichalcogenides-based van der Waals heterojunction materials.Covering latest stateof-the-art numerical simulations along with experimental results in the field,this review aims to provide a basic understanding of the tight relation between semiconductor nanomaterials and the proper simulation of their properties via surface hopping methods.Special stress is put on emerging state-ot-the-art techniques.By highlighting the challenge imposed by new materials,we depict emerging creative approaches,including high-level electronic structure methods and NA-MD methods to model nonadiabatic systems with high complexity.
基金supported by the National Natural Science Foundation of China(No.21922305,No.21873080,No.21703202)。
文摘Inspired by the branching corrected surface hopping(BCSH)method[J.Xu and L.Wang,J.Chem.Phys.150,164101(2019)],we present two new decoherence time formulas for trajectory surface hopping.Both the proposed linear and exponential formulas characterize the decoherence time as functions of the energy difference between adiabatic states and correctly capture the decoherence effect due to wave packet reflection as predicted by BCSH.The relevant parameters are trained in a series of 200 diverse models with different initial nuclear momenta,and the exact quantum solutions are utilized as references.As demonstrated in the three standard Tully models,the two new approaches exhibit significantly higher reliability than the widely used counterpart algorithm while holding the appealing efficiency,thus promising for nonadiabatic dynamics simulations of general systems.
