Calculations of coherent two-dimensional electronic spectra using forward and backward stochastic wavefunctions

Abstract

Within the well-established optical response function formalism, a new strategy with the central idea of employing the forward-backward stochastic Schrödinger equations in a segmented way to accurately obtain the two-dimensional (2D) electronic spectrum is presented in this paper. Based on the simple excitonically coupled dimer model system, the validity and efficiency of the proposed schemes are demonstrated in detail, along with the comparison against the deterministic hierarchy equations of motion and perturbative second order time-convolutionless quantum master equations. In addition, an important insight is provided in this paper that the characteristic frequency of the overdamped environment is an extremely crucial factor to regulate the lifetimes of the oscillating signals in 2D electronic spectra and of quantum coherence features of system dynamics. It is worth noting that the proposed scheme benefiting from its stochastic nature and wavefunction framework and many other advantages of substantially reducing the numerical cost, has a great potential to systematically investigate various quantum effects observed in realistic large-scale natural and artificial photosynthetic systems.

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Cited by in corpus (5)

• Perspective: Numerically "exact" approach to open quantum dynamics: The hierarchical equations of motion (HEOM)
• Calculating non-linear response functions for multi-dimensional electronic spectroscopy using dyadic non-Markovian quantum state diffusion
• Automatic Feynman diagram generation for nonlinear optical spectroscopies
• Simulation of absorption spectra of molecular aggregates: a Hierarchy of Stochastic Pure States approach
• Open quantum dynamics theory for a complex subenvironment system with a quantum thermostat: Application to a spin heat bath