Coherent (photon) vs incoherent (current) detection of multidimensional optical signals from single molecules in open junctions.
- Author(s): Agarwalla, Bijay Kumar
- Harbola, Upendra
- Hua, Weijie
- Zhang, Yu
- Mukamel, Shaul
- et al.
Published Web Locationhttps://doi.org/10.1063/1.4919955
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.