A new two-state diabatic potential energy matrix(DPEM)for H3 has been constructed,based on the fun-damental invariant neural network(FI-NN)diabatization method pro-posed in our previous work[Phys.Chem.Chem.Phys.21,150...A new two-state diabatic potential energy matrix(DPEM)for H3 has been constructed,based on the fun-damental invariant neural network(FI-NN)diabatization method pro-posed in our previous work[Phys.Chem.Chem.Phys.21,15040(2019)].In that initial effort,a two-state DPEM was constructed only with a 10 eV energy threshold.The current work aims to expand the en-ergy range and improve the accura-cy of DPEM.This is achieved by the utilization of full configuration inter-action(FCI)with aug-cc-pVnZ ba-sis sets and complete basis set(CBS)extrapolation.The original dataset is augmented with additional points with higher adiabatic energies,which give rise to a total of 10985 data points.The DPEM constructed in this work now enables accurate representation of adiabatic energies up to 18 eV.Quantum dynamic calculations based on this DPEM are nearly identical to those obtained from benchmark surfaces,which makes it the most accurate DPEM for the H3 system to date,therefore facilitating detailed exploration of reaction mechanisms at higher collision energies.展开更多
基金supported by the National Natural Science Foundation of China(No.22288201)the Inno-vation Program for Quantum Science and Technology(No.2021ZD0303305)the Dalian Innovation Sup-port Program(No.2021RD05).
文摘A new two-state diabatic potential energy matrix(DPEM)for H3 has been constructed,based on the fun-damental invariant neural network(FI-NN)diabatization method pro-posed in our previous work[Phys.Chem.Chem.Phys.21,15040(2019)].In that initial effort,a two-state DPEM was constructed only with a 10 eV energy threshold.The current work aims to expand the en-ergy range and improve the accura-cy of DPEM.This is achieved by the utilization of full configuration inter-action(FCI)with aug-cc-pVnZ ba-sis sets and complete basis set(CBS)extrapolation.The original dataset is augmented with additional points with higher adiabatic energies,which give rise to a total of 10985 data points.The DPEM constructed in this work now enables accurate representation of adiabatic energies up to 18 eV.Quantum dynamic calculations based on this DPEM are nearly identical to those obtained from benchmark surfaces,which makes it the most accurate DPEM for the H3 system to date,therefore facilitating detailed exploration of reaction mechanisms at higher collision energies.
