Abstract
In a recent work [U. Harbola, B. K. Agrawalla, and S. Mukamel, J. Chem. Phys. 141, 074107 (2014)], we have presented a superoperator (Liouville space) diagrammatic formulation of spontaneous and stimulated optical signals from current-carrying molecular junctions. We computed the diagrams that contribute to the spontaneous light emission SLE (fluorescence and Raman) signal using a diagrammatic method which clearly distinguishes between the Raman and the fluorescence contributions. We pointed out some discrepancies with the work of Galperin, Ratner and Nitzan (GRN) [M. Galperin, M. A. Ratner and, A. Nitzan, J. Chem. Phys. 130, 144109 (2009)]. In their response [M. Galperin, M. A. Ratner and A. Nitzan, “Comment on‘ Frequency-domain stimulated and spontaneous light emission signals at molecular junctions’” [J. Chem. Phys. 141, 074107 (2014)], J. Chem. Phys. 142, 137101 (2015)] to our work, GRN have argued that there are no differences in the choice of Raman diagrams in both works. Here we reply to their points and show where the differences exist.
Highlights
Response to “Comment on ‘Frequencydomain stimulated and spontaneous light emission signals at molecular junctions’” [J
Two types of issues were raised by Galperin, Nitzan, and Ratner (GRN). (1) The correct formal diagrammatic definition of the stimulated light emission (SLE) signal in terms of molecular correlation functions and the identification of the sub-set of diagrams that contribute to the Raman signal
A nonequilibrium Green’s function approach is available in Liouville space2,3 which can account for the effects of broadening due to the lead-molecule interaction
Summary
Response to “Comment on ‘Frequencydomain stimulated and spontaneous light emission signals at molecular junctions’” [J. Upendra Harbola,1 Bijay Kumar Agarwalla,2 and Shaul Mukamel2 1Department of Inorganic and Physical Chemistry, Indian Institute of Science, Bangalore 560012, India 2Department of Chemistry, University of California, Irvine, California 92697, USA (Received 2 December 2014; accepted 16 March 2015; published online 7 April 2015) (1) The correct formal diagrammatic definition of the stimulated light emission (SLE) signal in terms of molecular correlation functions and the identification of the sub-set of diagrams that contribute to the Raman signal.
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