With a new apparatus designed and assembled by ourselves, the matrix potential of non-saturated loess was firstly measured and studied during methane hydrate formation processes. The experimental results showed that d...With a new apparatus designed and assembled by ourselves, the matrix potential of non-saturated loess was firstly measured and studied during methane hydrate formation processes. The experimental results showed that during two formation processes, the matrix potential changes of the loess all presented a good linear relationship with water conversion ratios. In addition, although it was well known that the secondary gas hydrate formation was easier than the initial, our experimental results showed that the initial hydrate formation efficiency in non-saturated loess was higher than that of the secondary.展开更多
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
We constructed a new set of diabatic poten-tial energy surfaces(PESs)for the two low-est states involved in Li+Li_(2)reaction by us-ing the fundamental-invariant neural net-work method.The Li_(3)system exhibits a coni...We constructed a new set of diabatic poten-tial energy surfaces(PESs)for the two low-est states involved in Li+Li_(2)reaction by us-ing the fundamental-invariant neural net-work method.The Li_(3)system exhibits a coni-cal intersection(CI)at the geometric D_(3)h symmetries with the energy of the CI point significantly lower than the ground-state en-ab initio ergy of the diatomic molecule.The diabaitc PESs accurately reproduce adiabatic en-ergies,derivative coupling,and energy gradient information,thereby providing a high-fideli-ty description of the CI between the two lowest electronic states.Quantum dynamical calcu-lations have revealed significant non-adiabatic effects in the Li+Li_(2)reaction.展开更多
A new diabatic potential energy matrix(PEM)of the coupled~^(1)ππ^(*)and~1πσ*states for the~1πσ*-mediated photodissociation of thiophenol was constructed using a neural network(NN)approach.The diabatization of th...A new diabatic potential energy matrix(PEM)of the coupled~^(1)ππ^(*)and~1πσ*states for the~1πσ*-mediated photodissociation of thiophenol was constructed using a neural network(NN)approach.The diabatization of the PEM was specifically achieved by our recent method[Chin.J.Chem.Phys.34,825(2021)],which was based on adiabatic energies without the associated costly derivative couplings.The equation of motion coupled cluster with single and double excitations(EOM-CCSD)method was employed to compute adiabatic energies of two excited states in this work due to its high accuracy,simplicity,and efficiency.The PEM includes three dimensionalities,namely the S-H stretch,C-S-H bend,and C-C-S-H torsional coordinates.The root mean square errors of the NN fitting for the S1 and S2 states are 0.89 and 1.33 me V,respectively,suggesting the high accuracy of the NN method as expected.The calculated lifetimes of the S1 vibronic 00 and31 states are found to be in reasonably good agreement with available theoretical and experimental results,which validates the new EOM-CCSD-based PEM fitted by the NN approach.The combination of the diabatization scheme solely based on the adiabatic energies and the use of EOM-CCSD method makes the construction of reliable diabatic PEM quite simple and efficient.展开更多
This paper points out that equations （18a） and （18b） in Ref. [7] [Gao Y J 2008 Chin. Phys. B 17 3574] only possess the solutions M = ργc. So, there does not exist the so-called soliton solution family for the Ei...This paper points out that equations （18a） and （18b） in Ref. [7] [Gao Y J 2008 Chin. Phys. B 17 3574] only possess the solutions M = ργc. So, there does not exist the so-called soliton solution family for the Einstein-Maxwell theory with multiple Abelian gauge fields shown in Ref. [7].展开更多
基金supported by the CAS Knowledge Innovation Key Project (Grant No. KZCX2-YW-330)the National Science Fund Fostering Talents in Basic Research to Glaciology and Geocryology (Grant No. J0630966)the Training Fund of State Key Laboratory of Frozen Soil Engineering of Chinese Academy of Sciences (Grant No. 52YOSF102)
文摘With a new apparatus designed and assembled by ourselves, the matrix potential of non-saturated loess was firstly measured and studied during methane hydrate formation processes. The experimental results showed that during two formation processes, the matrix potential changes of the loess all presented a good linear relationship with water conversion ratios. In addition, although it was well known that the secondary gas hydrate formation was easier than the initial, our experimental results showed that the initial hydrate formation efficiency in non-saturated loess was higher than that of the secondary.
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.
基金supported by the National Natural Science Foundation of China(Nos.22103084 and 22233003 to Jiayu Huang,and No.22288201 to Dong H.Zhang)the Innovation Program for Quantum Science and Technology(No.2021ZD0303305)to Dong H.Zhangthe Dalian Innovation Support Program(No.2021RD05)to Dong H.Zhang.
文摘We constructed a new set of diabatic poten-tial energy surfaces(PESs)for the two low-est states involved in Li+Li_(2)reaction by us-ing the fundamental-invariant neural net-work method.The Li_(3)system exhibits a coni-cal intersection(CI)at the geometric D_(3)h symmetries with the energy of the CI point significantly lower than the ground-state en-ab initio ergy of the diatomic molecule.The diabaitc PESs accurately reproduce adiabatic en-ergies,derivative coupling,and energy gradient information,thereby providing a high-fideli-ty description of the CI between the two lowest electronic states.Quantum dynamical calcu-lations have revealed significant non-adiabatic effects in the Li+Li_(2)reaction.
基金supported by the National Natural Science Foundation of China(No.22073073)the Startup Foundation of Northwest UniversityThe Double First-Class University Construction Project of Northwest University。
文摘A new diabatic potential energy matrix(PEM)of the coupled~^(1)ππ^(*)and~1πσ*states for the~1πσ*-mediated photodissociation of thiophenol was constructed using a neural network(NN)approach.The diabatization of the PEM was specifically achieved by our recent method[Chin.J.Chem.Phys.34,825(2021)],which was based on adiabatic energies without the associated costly derivative couplings.The equation of motion coupled cluster with single and double excitations(EOM-CCSD)method was employed to compute adiabatic energies of two excited states in this work due to its high accuracy,simplicity,and efficiency.The PEM includes three dimensionalities,namely the S-H stretch,C-S-H bend,and C-C-S-H torsional coordinates.The root mean square errors of the NN fitting for the S1 and S2 states are 0.89 and 1.33 me V,respectively,suggesting the high accuracy of the NN method as expected.The calculated lifetimes of the S1 vibronic 00 and31 states are found to be in reasonably good agreement with available theoretical and experimental results,which validates the new EOM-CCSD-based PEM fitted by the NN approach.The combination of the diabatization scheme solely based on the adiabatic energies and the use of EOM-CCSD method makes the construction of reliable diabatic PEM quite simple and efficient.
文摘This paper points out that equations （18a） and （18b） in Ref. [7] [Gao Y J 2008 Chin. Phys. B 17 3574] only possess the solutions M = ργc. So, there does not exist the so-called soliton solution family for the Einstein-Maxwell theory with multiple Abelian gauge fields shown in Ref. [7].
