Frequency-domain stimulated and spontaneous light emission signals at molecular junctions.
- Author(s): Harbola, Upendra;
- Agarwalla, Bijay Kumar;
- Mukamel, Shaul
- et al.
Published Web Locationhttps://doi.org/10.1063/1.4892108
Using a diagrammatic superoperator formalism we calculate optical signals at molecular junctions where a single molecule is coupled to two metal leads which are held at different chemical potentials. The molecule starts in a nonequilibrium steady state whereby it continuously exchanges electrons with the leads with a constant electron flux. Expressions for frequency domain optical signals measured in response to continuous laser fields are derived by expanding the molecular correlation functions in terms of its many-body states. The nonunitary evolution of molecular states is described by the quantum master equation.