PMID- 26277129
OWN - NLM
STAT- PubMed-not-MEDLINE
DCOM- 20151023
LR  - 20150817
IS  - 1089-7690 (Electronic)
IS  - 0021-9606 (Linking)
VI  - 143
IP  - 6
DP  - 2015 Aug 14
TI  - A time domain two-particle approximation to calculate the absorption and circular 
      dichroism line shapes of molecular aggregates.
PG  - 064109
LID - 10.1063/1.4928584 [doi]
AB  - The hierarchical equations of motion (HEOM) method has recently emerged as an 
      effective approach to simulate linear and nonlinear spectroscopic signals of 
      molecular aggregates in the intermediate coupling regime. However, its 
      application to large systems is still limited when there are a large number of 
      molecules in the molecular aggregate. In this work, we propose a time domain 
      two-particle approximation (TPA) in combination with the HEOM method to calculate 
      the absorption and circular dichroism line shapes of molecular aggregates. The 
      new method is shown to reduce the number of auxiliary density operators (ADOs) 
      significantly for large systems, and a further truncation of the two-bath-set 
      excited terms based on geometric considerations can lead to a linear increase of 
      the number of ADOs with the system size. The validity of the HEOM-TPA method is 
      first tested on one-dimensional model systems. The new method is then applied to 
      calculate the absorption and circular dichroism line shapes of the Photosystem I 
      core complex, as well as the population evolution of the Fenna-Matthews-Olson 
      complex to demonstrate its effectiveness.
FAU - Song, Kai
AU  - Song K
AD  - Beijing National Laboratory for Molecular Sciences, State Key Laboratory for 
      Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, 
      Chinese Academy of Sciences, Zhongguancun, Beijing 100190, China.
FAU - Bai, Shuming
AU  - Bai S
AD  - Beijing National Laboratory for Molecular Sciences, State Key Laboratory for 
      Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, 
      Chinese Academy of Sciences, Zhongguancun, Beijing 100190, China.
FAU - Shi, Qiang
AU  - Shi Q
AD  - Beijing National Laboratory for Molecular Sciences, State Key Laboratory for 
      Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, 
      Chinese Academy of Sciences, Zhongguancun, Beijing 100190, China.
LA  - eng
PT  - Journal Article
PL  - United States
TA  - J Chem Phys
JT  - The Journal of chemical physics
JID - 0375360
EDAT- 2015/08/19 06:00
MHDA- 2015/08/19 06:01
CRDT- 2015/08/17 06:00
PHST- 2015/08/17 06:00 [entrez]
PHST- 2015/08/19 06:00 [pubmed]
PHST- 2015/08/19 06:01 [medline]
AID - 10.1063/1.4928584 [doi]
PST - ppublish
SO  - J Chem Phys. 2015 Aug 14;143(6):064109. doi: 10.1063/1.4928584.