title: Equilibrium excited state and emission spectra of molecular aggregates from the hierarchical equations of motion approach.
abstract: The hierarchical equations of motion (HEOM) method was applied to calculate the emission spectra of molecular aggregates using the Frenkel exciton model. HEOM equations for the one-exciton excited state were first propagated until equilibration. The reduced density operator and auxiliary density operators (ADOs) were used to characterize the coupled system-bath equilibrium. The dipole-dipole correlation functions were then calculated to obtain the emission spectra of model dimers, and the B850 band of light-harvesting complex II (LH2) in purple bacteria. The effect of static disorder on equilibrium excited state and the emission spectra of LH2 was also explicitly considered. Several approximation schemes, including the high temperature approximation (HTA) of the HEOM, a modified version of the HTA, the stochastic Liouville equation approach, the perturbative time-local and time-nonlocal generalized quantum master equations, were assessed in the calculation of the equilibrium excited state and emission spectra.
authors: Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Zhongguancun, Beijing 100190, China.
authors: Yuanyuan
authors: Y
authors: Jing
authors: Liping
authors: L
authors: Chen
authors: Shuming
authors: S
authors: Bai
authors: Qiang
authors: Q
authors: Shi
mesh_terms: D001426:Bacterial Proteins / Q000737:chemistry*; D045342:Light-Harvesting Protein Complexes / Q000737:chemistry*; D009038:Motion; D011789:Quantum Theory; D013696:Temperature
chemical_list: D001426:Bacterial Proteins; D045342:Light-Harvesting Protein Complexes