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

Harbola, Upendra and Umapathy, Siva and Mukamel, Shaul (2013) Loss and gain signals in broadband stimulated-Raman spectra: Theoretical analysis. In: Physical Review A, 88 (1). 011801_1-011801_4.

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Official URL: http://dx.doi.org/ 10.1103/PhysRevA.88.011801


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, chi((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. chi((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 chi((3)) regime.

Item Type: Journal Article
Publication: Physical Review A
Publisher: American Physical Society
Additional Information: Copyright of this article belongs to American Physical Society.
Department/Centre: Division of Chemical Sciences > Inorganic & Physical Chemistry
Date Deposited: 03 Sep 2013 06:31
Last Modified: 15 Oct 2018 14:22
URI: http://eprints.iisc.ac.in/id/eprint/46960

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