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首页> 外文期刊>The Journal of Chemical Physics >AN ANALYTICAL DERIVATION OF MC-SCF VIBRATIONAL WAVE FUNCTIONS FOR THE QUANTUM DYNAMICAL SIMULATION OF MULTIPLE PROTON TRANSFER REACTIONS - INITIAL APPLICATION TO PROTONATED WATER CHAINS
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AN ANALYTICAL DERIVATION OF MC-SCF VIBRATIONAL WAVE FUNCTIONS FOR THE QUANTUM DYNAMICAL SIMULATION OF MULTIPLE PROTON TRANSFER REACTIONS - INITIAL APPLICATION TO PROTONATED WATER CHAINS

机译：多质子转移反应的量子动力学模拟的MC-SCF振动波函数的解析推导-质子化水链的初步应用

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This paper presents an analytical derivation of a multiconfigurational self-consistent-held (MC-SCF) solution of the time-independent Schrodinger equation for nuclear motion (i.e. vibrational modes). This variational MC-SCF method is designed for the mixed quantum/classical molecular dynamics simulation of multiple proton transfer reactions, where the transferring protons are treated quantum mechanically while the remaining degrees of freedom are treated classically. This paper presents a proof that the Hellmann-Feynman forces on the classical degrees of freedom are identical to the exact forces (i.e. the Pulay corrections vanish) when this MC-SCF method is used with an appropriate choice of basis functions. This new MC-SCF method is applied to multiple proton transfer in a protonated chain of three hydrogen-bonded water molecules. The ground state and the first three excited state energies and the ground state forces agree well with full configuration interaction calculations. Sample trajectories are obtained using adiabatic molecular dynamics methods, and nonadiabatic effects are found to be insignificant for these sample trajectories. The accuracy of the excited states will enable this MC-SCF method to be used in conjunction with nonadiabatic molecular dynamics methods. This application differs from previous work in that it is a real-time quantum dynamical nonequilibrium simulation of multiple proton transfer in a chain of water molecules. (C) 1997 American Institute of Physics. [References: 79]
机译：本文介绍了针对核运动（即振动模式）的与时间无关的Schrodinger方程的多配置自洽保持（MC-SCF）解的解析推导。此变体MC-SCF方法设计用于多重质子转移反应的混合量子/经典分子动力学模拟，其中转移质子经过量子力学处理，而其余自由度则经过经典处理。本文提供了一个证明，当使用此MC-SCF方法并选择适当的基函数时，经典自由度上的Hellmann-Feynman力与精确力相同（即Pulay校正消失）。这种新的MC-SCF方法应用于三个氢键水分子质子化链中的多次质子转移。基态和前三个激发态能量以及基态力与完整构型相互作用计算非常吻合。使用绝热分子动力学方法获得了样品轨迹，并且发现非绝热效应对于这些样品轨迹而言无关紧要。激发态的准确性将使该MC-SCF方法与非绝热分子动力学方法结合使用。此应用程序与以前的工作有所不同，它是对水分子链中多个质子转移的实时量子动力学非平衡模拟。 （C）1997美国物理研究所。 [参考：79]

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