Nonlinear spectroscopy characterizing fluctuations
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Nonlinear Spectroscopy: Characterizing Fluctuations. Andrei Tokmakoff MIT Department of Chemistry 2009. Fluctuations in lineshapes. System-Bath Interactions. System: Spectroscopically Bright States Bath: Dark States → Energy Gap Fluctuations In spectroscopy … (Condon Approx.).

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Nonlinear spectroscopy characterizing fluctuations

Nonlinear Spectroscopy:Characterizing Fluctuations

Andrei Tokmakoff

MIT Department of Chemistry

2009


Fluctuations in lineshapes
Fluctuations in lineshapes


System bath interactions
System-Bath Interactions

  • System: Spectroscopically Bright States

  • Bath: Dark States

  • → Energy Gap Fluctuations

  • In spectroscopy … (Condon Approx.)


Energy gap fluctuations
Energy Gap Fluctuations

  • Energy Gap Correlation Function

  • Dipole Correlation Function → Absorption lineshape

  • Second Cumulant approx.


A bath of arbitrary form
A bath of arbitrary form

  • Spectral Density

  • Brownian Oscillator Model


Nonlinear response for fluctuating system
Nonlinear response for fluctuating system

  • Following earlier approach:

  • Cumulant approximation:






2d lineshapes
2D Lineshapes









Correlated energy fluctuations
Correlated Energy Fluctuations

Frequency Auto- and Cross-Correlation Functions:


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