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
相关论文
共 50 条
  • [31] Non-adiabatic quantum wavepacket dynamics simulation based on electronic structure calculations using the variational quantum eigensolver
    Hirai, Hirotoshi
    Koh, Sho
    CHEMICAL PHYSICS, 2022, 556
  • [32] A modular molecular dynamics quantum dynamics program for non-adiabatic proton transfers in solution
    Billeter, SR
    van Gunsteren, WF
    COMPUTER PHYSICS COMMUNICATIONS, 1997, 107 (1-3) : 61 - 91
  • [33] Non-adiabatic QM/MM: A hybrid approach to doing non-adiabatic excited state dynamics
    Tracy, Dustin
    Bjorgaard, Josiah
    Tretiak, Sergei
    Roitberg, Adrian
    ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY, 2017, 253
  • [34] Direct simulation of non-adiabatic dynamics in large-scale enzymatic systems
    Kretchmer, Joshua
    Miller, Thomas
    ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY, 2017, 254
  • [35] Non-adiabatic quantum dynamics of the electronic quenching OH(A2σ+) + Kr
    Gamallo, Pablo
    Zanchet, Alexandre
    Aoiz, F. Javier
    Petrongolo, Carlo
    PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2020, 22 (30) : 17091 - 17105
  • [36] Non-adiabatic chemistry at the conical intersection seam studied with "on the fly" quantum dynamics
    Robb, Michael A.
    Lasorne, Benjamin
    Mendive-Tapia, David
    Bearpark, Michael J.
    Allan, Charlotte S. M.
    Worth, Graham
    ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY, 2012, 244
  • [37] Quantum non-adiabatic dynamics through conical intersections: Spectroscopy to reactive scattering
    Mahapatra, S
    INTERNATIONAL REVIEWS IN PHYSICAL CHEMISTRY, 2004, 23 (04) : 483 - 512
  • [38] Non-adiabatic quantum molecular dynamics: ionization of many-electron systems
    Uhlmann, Mathias
    Kunert, Thomas
    Schmidt, Ruediger
    JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS, 2006, 39 (14) : 2989 - 3008
  • [39] Non-adiabatic couplings in Liouville description of mixed quantum-classical dynamics
    Ando, K
    CHEMICAL PHYSICS LETTERS, 2002, 360 (3-4) : 240 - 242
  • [40] Partial linearized density matrix dynamics for dissipative, non-adiabatic quantum evolution
    Coker, David F.
    Huo, Pengfei
    ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY, 2012, 243