Non-adiabatic direct quantum dynamics using force fields: Toward solvation

被引:6
|
作者
Cigrang, L. L. E. [1 ]
Green, J. A. [2 ]
Gomez, S. [3 ]
Cerezo, J. [4 ,5 ]
Improta, R. [6 ]
Prampolini, G. [7 ]
Santoro, F. [7 ]
Worth, G. A. [1 ]
机构
[1] UCL, Dept Chem, 20 Gordon St, London WC1H 0AJ, England
[2] Goethe Univ, Inst Phys Theoret Chem, Max von Laue Str 7, D-60438 Frankfurt, Germany
[3] Univ Salamanca, Dept Quim Fis, Salamanca 37008, Spain
[4] Univ Autonoma Madrid, Dept Quim, Madrid 28049, Spain
[5] Univ Autonoma Madrid, Inst Adv Res Chem Sci IAdChem, Madrid 28049, Spain
[6] Ist Biostrutture & Bioimmagini CNR, Via De Amicis 95, I-80145 Naples, Italy
[7] Area Ric CNR, Ist Chim Composti Organometall ICCOM CNR, Via Moruzzi 1, I-56124 Pisa, Italy
来源
JOURNAL OF CHEMICAL PHYSICS | 2024年 / 160卷 / 17期
基金
英国工程与自然科学研究理事会;
关键词
POTENTIAL-ENERGY SURFACES; MOLECULAR-DYNAMICS; GAUSSIAN WAVEPACKETS; PHOTOCHEMISTRY; ALGORITHM; PHOTOPHYSICS; SIMULATIONS; THYMINE; SYSTEMS; STATES;
D O I
10.1063/5.0204911
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Quantum dynamics simulations are becoming a powerful tool for understanding photo-excited molecules. Their poor scaling, however, means that it is hard to study molecules with more than a few atoms accurately, and a major challenge at the moment is the inclusion of the molecular environment. Here, we present a proof of principle for a way to break the two bottlenecks preventing large but accurate simulations. First, the problem of providing the potential energy surfaces for a general system is addressed by parameterizing a standard force field to reproduce the potential surfaces of the molecule's excited-states, including the all-important vibronic coupling. While not shown here, this would trivially enable the use of an explicit solvent. Second, to help the scaling of the nuclear dynamics propagation, a hierarchy of approximations is introduced to the variational multi-configurational Gaussian method that retains the variational quantum wavepacket description of the key quantum degrees of freedom and uses classical trajectories for the remaining in a quantum mechanics/molecular mechanics like approach. The method is referred to as force field quantum dynamics (FF-QD), and a two-state pi pi*/n pi* model of uracil, excited to its lowest bright pi pi* state, is used as a test case.
引用
收藏
页数:14
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