Abstract
Quantum electron-vibrational dynamics in molecular systems at finite temperature is described using an approach based on Thermo Field Dynamics theory. This formulation treats temperature effects in the Hilbert space without introducing the Liouville space. The solution of Thermo Field Dynamics equations with a novel technique for the propagation of Tensor Trains (Matrix Product States) is implemented and discussed. The methodology is applied to the study of the exciton dynamics in the Fenna-Mathews-Olsen complex using a realistic structured spectral density to model the electron-phonon interaction. The results of the simulations highlight the effect of specific vibrational modes on the exciton dynamics and energy transfer process, as well as call for careful modeling of electron-phonon couplings.
Highlights
Unraveling the role of quantum effects in the time evolution of various molecular systems and assemblies under realistic conditions at ambient temperatures is a key problem of modern physical and biological chemistry[1]
Accurate evolution of large systems has been described by the density matrix renormalization group (DMRG) methodology, and the associated time-evolution algorithms[26, 27]
Wave function propagation methods employing a basis set representation, such as the multiconfiguration time-dependent Hartree (MCTDH) method and its multilayer extension (ML-MCTDH)[28, 29], Gaussian based MCTDH and other basis set methods[30,31,32,33], are powerful tools at very low temperature[34], but become unhandy in high temperature cases, as their application requires a statistical sampling of the initial conditions and faces both theoretical and computational difficulties[35,36,37]
Summary
Received: 9 May 2017 Accepted: 18 July 2017 Published: xx xx xxxx based on Thermo Field Dynamics. In this work we discuss a novel theoretical methodology based on Thermo Field Dynamics theory[40, 41] that combines an accurate Hamiltonian description of quantum dynamics at finite temperature with the flexibility of a basis set representation[42]. We apply this methodology to the study of exciton dynamics in the Fenna-Matthews-Olsen (FMO) complex, which has nowadays become a “guinea pig” of exciton dynamics theory and quantum biology[1, 2, 43, 44]. We simulate exciton dynamics in FMO at ambient temperature modeling the electron-phonon interaction with a realistic spectral density obtained from experimental data[51]
Sign-in/Register to view highlights & summary Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a callDisclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.
