title: Coherent (photon) vs incoherent (current) detection of multidimensional optical signals from single molecules in open junctions.
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.affiliation: Department of Chemistry, University of California, Irvine, California 92697, USA.
authors.forename: Bijay Kumar
authors.initials: BK
authors.lastname: Agarwalla
authors.affiliation: Department of Inorganic and Physical Chemistry, Indian Institute of Science, Bangalore 560012, India.
authors.forename: Upendra
authors.initials: U
authors.lastname: Harbola
authors.affiliation: Department of Chemistry, University of California, Irvine, California 92697, USA.
authors.forename: Weijie
authors.initials: W
authors.lastname: Hua
authors.affiliation: Department of Chemistry, University of California, Irvine, California 92697, USA.
authors.forename: Yu
authors.initials: Y
authors.lastname: Zhang
authors.affiliation: Department of Chemistry, University of California, Irvine, California 92697, USA.
authors.forename: Shaul
authors.initials: S
authors.lastname: Mukamel