skip to main content

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

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:
; ; ;  [1] ;  [2]
  1. Department of Chemistry, University of California, Irvine, California 92697 (United States)
  2. Department of Inorganic and Physical Chemistry, Indian Institute of Science, Bangalore 560012 (India)
Publication Date:
OSTI Identifier:
22415912
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 142; Journal Issue: 21; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
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