PMID- 35395901
OWN - NLM
STAT- PubMed-not-MEDLINE
LR  - 20220411
IS  - 1089-7690 (Electronic)
IS  - 0021-9606 (Linking)
VI  - 156
IP  - 13
DP  - 2022 Apr 7
TI  - Generalized master equation for charge transport in a molecular junction: Exact 
      memory kernels and their high order expansion.
PG  - 134114
LID - 10.1063/5.0086663 [doi]
AB  - We derive a set of generalized master equations (GMEs) to study charge transport 
      dynamics in molecular junctions using the Nakajima-Zwanzig-Mori projection 
      operator approach. In the new GME, time derivatives of population on each quantum 
      state of the molecule, as well as the tunneling current, are calculated as the 
      convolution of time non-local memory kernels with populations on all system 
      states. The non-Markovian memory kernels are obtained by combining the 
      hierarchical equations of motion (HEOM) method and a previous derived Dyson 
      relation for the exact kernel. A perturbative expansion of these memory kernels 
      is then calculated using the extended HEOM developed in our previous work [M. Xu 
      et al., J. Chem. Phys. 146, 064102 (2017)]. By using the resonant level model and 
      the Anderson impurity model, we study properties of the exact memory kernels and 
      analyze convergence properties of their perturbative expansions with respect to 
      the system-bath coupling strength and the electron-electron repulsive energy. It 
      is found that exact memory kernels calculated from HEOM exhibit short memory 
      times and decay faster than the population and current dynamics. The high order 
      perturbation expansion of the memory kernels can give converged results in 
      certain parameter regimes. The Pade and Landau-Zener resummation schemes are also 
      found to give improved results over low order perturbation theory.
FAU - Dan, Xiaohan
AU  - Dan X
AUID- ORCID: s0000000180691101
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 and University 
      of Chinese Academy of Sciences, Beijing 100049, China.
FAU - Xu, Meng
AU  - Xu M
AUID- ORCID: s0000000224400645
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 and University 
      of Chinese Academy of Sciences, Beijing 100049, China.
FAU - Yan, Yaming
AU  - Yan Y
AUID- ORCID: s000000027622724X
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 and University 
      of Chinese Academy of Sciences, Beijing 100049, China.
FAU - Shi, Qiang
AU  - Shi Q
AUID- ORCID: s0000000290462924
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 and University 
      of Chinese Academy of Sciences, Beijing 100049, China.
LA  - eng
PT  - Journal Article
PL  - United States
TA  - J Chem Phys
JT  - The Journal of chemical physics
JID - 0375360
SB  - IM
EDAT- 2022/04/10 06:00
MHDA- 2022/04/10 06:01
CRDT- 2022/04/09 05:14
PHST- 2022/04/09 05:14 [entrez]
PHST- 2022/04/10 06:00 [pubmed]
PHST- 2022/04/10 06:01 [medline]
AID - 10.1063/5.0086663 [doi]
PST - ppublish
SO  - J Chem Phys. 2022 Apr 7;156(13):134114. doi: 10.1063/5.0086663.