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Loss and gain signals in broadband stimulated-Raman spectra: Theoretical analysis

Upendra Harbola, Siva Umapathy, and Shaul Mukamel
Phys. Rev. A 88, 011801(R) – Published 2 July 2013

Abstract

Stimulated optical signals obtained by subjecting the system to a narrow band and a broadband pulse show both gain and loss Raman features at the red and blue side of the narrow beam, respectively. Recently observed temperature-dependent asymmetry in these features [Mallick et al., J. Raman Spectrosc. 42, 1883 (2011); Dang et al., Phys. Rev. Lett. 107, 043001 (2011)] has been attributed to the Stokes and anti-Stokes components of the third-order susceptibility, χ(3). By treating the setup as a steady state of an open system coupled to four quantum radiation field modes, we show that Stokes and anti-Stokes processes contribute to both the loss and gain resonances. χ(3) predicts loss and gain signals with equal intensity for electronically off-resonant excitation. Some asymmetry may exist for resonant excitation. However, this is unrelated to the Stokes vs anti-Stokes processes. Any observed temperature-dependent asymmetry must thus originate from effects lying outside the χ(3) regime.

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  • Received 6 October 2012

DOI:https://doi.org/10.1103/PhysRevA.88.011801

©2013 American Physical Society

Authors & Affiliations

Upendra Harbola and Siva Umapathy

  • Inorganic and Physical Chemistry, Indian Institute of Sciences, Bangalore, Karnataka 560012, India

Shaul Mukamel

  • Department of Chemistry, University of California, Irvine, California 92697-2025, USA

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Issue

Vol. 88, Iss. 1 — July 2013

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