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QM/MM Modeling of Vibrational Polariton Induced Energy Transfer and Chemical Dynamics

Tao E. LiSharon Hammes-Schiffer
Dec 2022
摘要
Vibrational strong coupling (VSC) provides a novel means to modify chemicalreactions and energy transfer pathways. To efficiently model chemical dynamicsunder VSC in the collective regime, herein a hybrid quantum mechanics/molecularmechanics (QM/MM) cavity molecular dynamics (CavMD) scheme is developed andapplied to an experimentally studied chemical system. This approach can achievelinear scaling with respect to the number of molecules for a dilute solutionunder VSC by assuming that each QM solute molecule is surrounded by anindependent MM solvent bath. Application of this approach to a dilute solutionof Fe(CO)$_5$ in n-dodecane under VSC demonstrates polariton dephasing to thedark modes and polariton-enhanced molecular nonlinear absorption. Thesesimulations predict that strongly exciting the lower polariton may provide anenergy transfer pathway that selectively excites the equatorial CO vibrationsrather than the axial CO vibrations. Moreover, these simulations also directlyprobe the cavity effect on the dynamics of the Fe(CO)$_5$ Berry pseudorotationreaction for comparison to recent two-dimensional infrared spectroscopyexperiments. This theoretical approach is applicable to a wide range of otherpolaritonic systems and provides a tool for exploring the use of vibrationalstrong coupling for selective infrared photochemistry.
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