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Journal of Chemical Physics / Volume 135 / Issue 24 / ARTICLES / Condensed Phase Dynamics, Structure, and Thermodynamics: Spectroscopy, Reactions, and Relaxation

J. Chem. Phys. 135, 244506 (2011); http://dx.doi.org/10.1063/1.3660206 (13 pages)

Numerically exact, time-dependent treatment of vibrationally coupled electron transport in single-molecule junctions

Haobin Wang1, Ivan Pshenichnyuk2, Rainer Härtle2, and Michael Thoss2

1Department of Chemistry and Biochemistry, MSC 3C, New Mexico State University, Las Cruces, New Mexico 88003, USA, and Beijing Computational Science Research Center, No. 3 He-Qing Road, Hai-Dian District, Beijing 100084, People's Republic of China
2Institut für Theoretische Physik und Interdisziplinäres Zentrum für Molekulare Materialien, Friedrich-Alexander-Universität Erlangen-Nürnberg, Staudtstr. 7/B2, D-91058, Germany

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(Received 23 March 2011; accepted 24 October 2011; published online 29 December 2011)

The multilayer multiconfiguration time-dependent Hartree (ML-MCTDH) theory within second quantization representation of the Fock space, a novel numerically exact methodology to treat many-body quantum dynamics for systems containing identical particles, is applied to study the effect of vibrational motion on electron transport in a generic model for single-molecule junctions. The results demonstrate the importance of electronic-vibrational coupling for the transport characteristics. For situations where the energy of the bridge state is located close to the Fermi energy, the simulations show the time-dependent formation of a polaron state that results in a pronounced suppression of the current corresponding to the phenomenon of phonon blockade. We show that this phenomenon cannot be explained solely by the polaron shift of the energy but requires methods that incorporate the dynamical effect of the vibrations on the transport. The accurate results obtained with the ML-MCTDH in this parameter regime are compared to results of nonequilibrium Green's function theory.

© 2011 American Institute of Physics

Article Outline

  1. INTRODUCTION
  2. MODEL AND OBSERVABLES OF INTEREST
  3. THE MULTILAYER MULTICONFIGURATION TIME-DEPENDENT HARTREE THEORY IN SECOND QUANTIZATION REPRESENTATION
    1. General formulation of the multilayer multiconfiguration time-dependent Hartree theory
    2. Treating identical particles using the second quantization representation of Fock space
  4. RESULTS AND DISCUSSION
  5. CONCLUDING REMARKS

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KEYWORDS and PACS

Keywords

Fermi level, many-body problems, molecular electronics, multilayers, phonons, polarons, SCF calculations

PACS

ARTICLE DATA

Digital Object Identifier
http://dx.doi.org/10.1063/1.3660206

PUBLICATION DATA

ISSN

0021-9606 (print)  
1089-7690 (online)

Publisher

$abstract.society.value is a Member of CrossRef American Institute of Physics

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