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Updated: Apr 11, 2026

Resonance Fluorescence of an InGaAs Quantum Dot in a Planar Cavity Using Orthogonal Excitation and Detection
Published on: October 13, 2017
Coherent (photon) vs incoherent (current) detection of multidimensional optical signals from single molecules in open
Bijay Kumar Agarwalla1, Upendra Harbola2, Weijie Hua1
1Department of Chemistry, University of California, Irvine, California 92697, USA.
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.
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