Journal
JOURNAL OF PHYSICAL CHEMISTRY A
Volume 119, Issue 44, Pages 10893-10909Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpca.5b08909
Keywords
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Funding
- Czech-Austrian Mobility by MSMT [7AMB14AT007]
- Austrian Science Fund (FWF): START project [Y 631-N27]
- OeAD [WTZ: CZ 05/2014]
- Czech Science Foundation [GA14-25752S]
- GAUK [2040214]
- Austrian Science Fund (FWF) [Y631] Funding Source: Austrian Science Fund (FWF)
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Center line slope (CLS) analysis in 2D infrared spectroscopy has been extensively used to extract frequency frequency correlation functions of vibrational transitions. We apply this concept to 2D electronic spectroscopy, where CLS is a measure of electronic gap fluctuations. The two domains, infrared and electronic, possess differences: In the infrared, the frequency fluctuations are classical, often slow and Gaussian. In contrast, electronic spectra are subject to fast spectral diffusion and affected by underdamped vibrational wavepackets in addition to Stokes shift. All these effects result in non-Gaussian peak profiles. Here, we extend CLS-analysis beyond Gaussian line shapes and test the developed methodology on a solvated molecule, zinc phthalocyanine. We find that CLS facilitates the interpretation of 2D electronic spectra by reducing their complexity to one dimension. In this way, CLS provides a highly sensitive measure of model parameters describing electronic-vibrational and electronic-solvent interaction.
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