Spin versus boson baths in nonlinear spectroscopy
The third-order optical response function of a chromophore coupled to a bath consisting of noninteracting two-level systems (TLSs) undergoing stochastic jumps is calculated. The results can be applied to a broad class of nonlinear optical techniques in single-molecule spectroscopy and bulk measureme...
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sg-ntu-dr.10356-939552020-06-01T10:26:30Z Spin versus boson baths in nonlinear spectroscopy Zhao, Yang Chernyak, Vladimir Mukamel, Shaul School of Materials Science & Engineering DRNTU::Science::Chemistry::Physical chemistry::Solid state chemistry The third-order optical response function of a chromophore coupled to a bath consisting of noninteracting two-level systems (TLSs) undergoing stochastic jumps is calculated. The results can be applied to a broad class of nonlinear optical techniques in single-molecule spectroscopy and bulk measurements in glasses, polymers, and mixed crystals. In the limit of many TLSs weakly coupled to the chromophore, the response can be obtained using the second-order cumulant expansion and resembles that of the Brownian oscillator model. Quantum corrections to the spectral density which accounts for the Stokes shift can be included in this limit using the fluctuation−dissipation theorem. However, the temperature dependence predicted by the two models is very different. Corrections to the cumulant expansion to fourth order in coupling strength are derived. 2011-12-16T07:56:00Z 2019-12-06T18:48:26Z 2011-12-16T07:56:00Z 2019-12-06T18:48:26Z 1998 1998 Journal Article Zhao, Y., Chernyak, V., & Mukamel, S. (1998). Spin versus Boson Baths in Nonlinear Spectroscopy. Journal of Physical Chemstry A, 102 (33), 6614–6634. https://hdl.handle.net/10356/93955 http://hdl.handle.net/10220/7419 10.1021/jp981799s en Journal of physical chemstry A © 1998 American Chemical Society |
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DRNTU::Science::Chemistry::Physical chemistry::Solid state chemistry Zhao, Yang Chernyak, Vladimir Mukamel, Shaul Spin versus boson baths in nonlinear spectroscopy |
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The third-order optical response function of a chromophore coupled to a bath consisting of noninteracting two-level systems (TLSs) undergoing stochastic jumps is calculated. The results can be applied to a broad class of nonlinear optical techniques in single-molecule spectroscopy and bulk measurements in glasses, polymers, and mixed crystals. In the limit of many TLSs weakly coupled to the chromophore, the response can be obtained using the second-order cumulant expansion and resembles that of the Brownian oscillator model. Quantum corrections to the spectral density which accounts for the Stokes shift can be included in this limit using the fluctuation−dissipation theorem. However, the temperature dependence predicted by the two models is very different. Corrections to the cumulant expansion to fourth order in coupling strength are derived. |
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School of Materials Science & Engineering |
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School of Materials Science & Engineering Zhao, Yang Chernyak, Vladimir Mukamel, Shaul |
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Article |
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Zhao, Yang Chernyak, Vladimir Mukamel, Shaul |
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Zhao, Yang |
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Spin versus boson baths in nonlinear spectroscopy |
title_short |
Spin versus boson baths in nonlinear spectroscopy |
title_full |
Spin versus boson baths in nonlinear spectroscopy |
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Spin versus boson baths in nonlinear spectroscopy |
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Spin versus boson baths in nonlinear spectroscopy |
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spin versus boson baths in nonlinear spectroscopy |
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2011 |
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https://hdl.handle.net/10356/93955 http://hdl.handle.net/10220/7419 |
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1681058715125415936 |