Optical line shapes of molecular aggregates: Hierarchical equations of motion method

被引：122

作者：

Chen, Liping ^{[1
]}

Zheng, Renhui ^{[1
]}

Shi, Qiang ^{[1
]}

Yan, YiJing ^{[2
]}

机构：

[1] Chinese Acad Sci, Beijing Natl Lab Mol Sci, State Key Lab Struct Chem Unstable & Stable Speci, Inst Chem, Beijing 100190, Peoples R China

[2] Hong Kong Univ Sci & Technol, Dept Chem, Kowloon, Hong Kong, Peoples R China

来源：

JOURNAL OF CHEMICAL PHYSICS | 2009年 / 131卷 / 09期

关键词：

biexcitons; Liouville equation; macromolecules; master equation; molecular clusters; perturbation theory; quantum chemistry; spectral line breadth; QUANTUM MASTER EQUATION; ELECTRON-TRANSFER; ENERGY-TRANSFER; PROTEIN COMPLEX; DYNAMICS; SYSTEM; SPECTROSCOPY; RELAXATION; OSCILLATOR; COHERENT;

D O I：

10.1063/1.3213013

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The absorption line shapes of model molecular aggregates are investigated using the recently developed Liouville space hierarchical equations of motion (HEOM) method. The exact results are further exploited for the assessment of several approximation schemes, including the high temperature approximation of HEOM, the stochastic Liouville equation approach, and the perturbative time-local and time-nonlocal quantum master equations (QMEs). The calculations on dimers, larger ring-shaped aggregates, and a model of the B850 ring in the LH2 of purple bacteria show that while the other approximate methods can give reasonable absorption line shapes over a wide range of parameter regimes, the second-order time-nonlocal QME is generally inaccurate and may give spurious peaks in the absorption spectra.

引用

页数：11

共 80 条

[1] Optical line shapes of dynamically disordered ring aggregates [J].