In this work we construct a novel dissipaton-equation-of-motion （DEOM） theory in quadratic bath coupling environment, based on an extended algebraic statistical quasi-particle approach. To validate the new ingredient of the underlying dissipaton algebra, we derive an extended Zusman equation via a totally different approach. We prove that the new theory, if it starts with the identical setup, constitutes the dynamical resolutions to the extended Zusman equation. Thus, we verify the generalized （non-Gaussian） Wick＇s theorem with dissipatons-pair added. This new algebraic ingredient enables the dissipaton approach being naturally extended to nonlinear coupling environments. Moreover, it is noticed that, unlike the linear bath coupling case, the influence of a non-Gaussian environment cannot be completely characterized with the linear response theory. The new theory has to take this fact into account. The developed DEOM theory manifests the dynamical interplay between dissipatons and nonlinear bath coupling descriptors that will be specified. Numerical demonstrations will be given with the optical line shapes in quadratic coupling environment.
A two-dimensional generalized Langevin equation is proposed to describe the protein conformational change, compatible to the electron transfer process governed by atomic packing density model. We assume a fractional Gaussian noise and a white noise through bond and through space coordinates respectively, and introduce the coupling effect coming from both fluctuations and equilibrium variances. The general expressions for autocorrelation functions of distance fluctuation and fluorescence lifetime variation are derived, based on which the exact conformational change dynamics can be evaluated with the aid of numerical Laplace inversion technique. We explicitly elaborate the short time and long time approximations. The relationship between the two-diraensional description and the one-dimensional theory is also discussed.
To advance hierarchical equations of motion as a standard theory for quantum dissipative dynamics, we put forward a mixed Heisenberg-SchrSdinger scheme with block-matrix implementation on efficient evaluation of nonlinear optical response function. The new approach is also integrated with optimized hierarchical theory and numerical filtering algorithm. Different configurations of coherent two-dimensional spectroscopy of model excitonic dimer systems are investigated, with focusing on the effects of intermolecular transfer coupling and bi-exciton interaction.
