Speaker
Description
We have developed a fully quantum, numerically accurate wave function-based approach for the calculation of third-order spectroscopic signals of polyatomic molecules and molecular aggregates at finite temperature including statiuc disorder effects. The systems are described by multimode nonadiabatic vibronic-coupling Hamiltonians, in which diagonal terms are treated in harmonic approximation, while off-diagonal interstate couplings are assumed to be coordinate independent. The approach is based on the Thermo Field Dynamics (TFD) representation of quantum mechanics and Tensor-Train (TT) representation of the vibronic wave function, providing a very efficient numerical simulation of quantum evolution of systems with many degrees of freedom. The effect of static disorder is included using a novel approach based on auxiliary harmonic oscillators variables. The developed TFD-TT approach is applied to the calculation of time- and frequency-resolved fluorescence spectra of the Fenna−Matthews−Olson (FMO) antenna complex at room temperature taking into account finite time-frequency resolution in fluorescence detection, orientational averaging, and static disorder.
