Coherent (photon) vs incoherent (current) detection of multidimensional optical signals from single molecules in open junctions

Agarwalla, Bijay Kumar; Hua, Weijie; Zhang, Yu; Mukamel, Shaul; Harbola, Upendra

doi:10.1063/1.4919955

Title: Coherent (photon) vs incoherent (current) detection of multidimensional optical signals from single molecules in open junctions

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Abstract

The nonlinear optical response of a current-carrying single molecule coupled to two metal leads and driven by a sequence of impulsive optical pulses with controllable phases and time delays is calculated. Coherent (stimulated, heterodyne) detection of photons and incoherent detection of the optically induced current are compared. Using a diagrammatic Liouville space superoperator formalism, the signals are recast in terms of molecular correlation functions which are then expanded in the many-body molecular states. Two dimensional signals in benzene-1,4-dithiol molecule show cross peaks involving charged states. The correlation between optical and charge current signal is also observed.

Authors:

Agarwalla, Bijay Kumar; Hua, Weijie; Zhang, Yu; Mukamel, Shaul ^[1]; Harbola, Upendra ^[2]

Department of Chemistry, University of California, Irvine, California 92697 (United States)
Department of Inorganic and Physical Chemistry, Indian Institute of Science, Bangalore 560012 (India)

Publication Date:: Sun Jun 07 00:00:00 EDT 2015

OSTI Identifier:: 22415912

Resource Type:: Journal Article

Journal Name:: Journal of Chemical Physics

Additional Journal Information:: Journal Volume: 142; Journal Issue: 21; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; BENZENE; COMPARATIVE EVALUATIONS; CORRELATION FUNCTIONS; CORRELATIONS; DETECTION; ELECTRIC CONTACTS; MANY-BODY PROBLEM; MOLECULES; NONLINEAR PROBLEMS; PHOTONS; SEMICONDUCTOR JUNCTIONS; THIOLS; TIME DELAY; TWO-DIMENSIONAL SYSTEMS

Citation Formats


                    Agarwalla, Bijay Kumar, Hua, Weijie, Zhang, Yu, Mukamel, Shaul, and Harbola, Upendra. Coherent (photon) vs incoherent (current) detection of multidimensional optical signals from single molecules in open junctions.  United States: N. p., 2015. 
        Web.  doi:10.1063/1.4919955.

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                    Agarwalla, Bijay Kumar, Hua, Weijie, Zhang, Yu, Mukamel, Shaul, & Harbola, Upendra. Coherent (photon) vs incoherent (current) detection of multidimensional optical signals from single molecules in open junctions.  United States.  https://doi.org/10.1063/1.4919955

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                    Agarwalla, Bijay Kumar, Hua, Weijie, Zhang, Yu, Mukamel, Shaul, and Harbola, Upendra. 2015.  
        "Coherent (photon) vs incoherent (current) detection of multidimensional optical signals from single molecules in open junctions".  United States.  https://doi.org/10.1063/1.4919955.

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@article{osti_22415912,

  title        = {Coherent (photon) vs incoherent (current) detection of multidimensional optical signals from single molecules in open junctions},

  author       = {Agarwalla, Bijay Kumar and Hua, Weijie and Zhang, Yu and Mukamel, Shaul and Harbola, Upendra},

  abstractNote = {The nonlinear optical response of a current-carrying single molecule coupled to two metal leads and driven by a sequence of impulsive optical pulses with controllable phases and time delays is calculated. Coherent (stimulated, heterodyne) detection of photons and incoherent detection of the optically induced current are compared. Using a diagrammatic Liouville space superoperator formalism, the signals are recast in terms of molecular correlation functions which are then expanded in the many-body molecular states. Two dimensional signals in benzene-1,4-dithiol molecule show cross peaks involving charged states. The correlation between optical and charge current signal is also observed.},

  doi          = {10.1063/1.4919955},

  url          = {https://www.osti.gov/biblio/22415912},
  journal      = {Journal of Chemical Physics},

  issn         = {0021-9606},

  number       = 21,

  volume       = 142,

  place        = {United States},

  year         = {Sun Jun 07 00:00:00 EDT 2015},

  month        = {Sun Jun 07 00:00:00 EDT 2015}

}

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