Parallels between multiple population-period transient spectroscopy and multidimensional coherence spectroscopies

The Journal of Chemical Physics
Champak Khurmi, Mark A Berg

Abstract

We have recently shown that homogeneous and heterogeneous kinetics can be distinguished by experiments that compare the evolution of the population of a state over two time intervals [E. van Veldhoven et al., ChemPhysChem 8, 1761 (2007)]. This paper elaborates on the analogy between these multiple population-period transient spectroscopy (MUPPETS) experiments and more familiar spectroscopies based on the evolution of coherences. Using a modified inverse-Laplace transform, a standard kinetics decay is re-expressed as a "rate spectrum." A nonexponential decay creates a linewidth in this spectrum. Mechanisms for line broadening in rate spectra are compared to those for line broadening in frequency-domain spectra. Homogeneous and heterogeneous kinetics are defined precisely and are shown to be the counterparts of homogeneous and inhomogeneous line broadenings in frequency-domain spectra. Homogeneous line broadening mechanisms are further divided into equilibrium and nonequilibrium mechanisms, with equilibrium mechanisms more prevalent in frequency spectra and nonequilibrium mechanisms more prevalent in rate spectra. Spectral representations of two-dimensional MUPPETS experiments are developed that are equivalent to two-dimensional ...Continue Reading

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Citations

Apr 19, 2011·The Journal of Chemical Physics·Kalyanasis Sahu, Mark A Berg
Jan 25, 2013·The Journal of Chemical Physics·Haorui Wu, Mark A Berg
Jan 15, 2016·The Journal of Physical Chemistry Letters·Sachin Dev VermaMark Alan Berg
Jul 28, 2016·The Journal of Chemical Physics·Brian P MoleskyAndrew M Moran
Aug 9, 2016·The Journal of Chemical Physics·Mark A Berg, Jason R Darvin
Nov 17, 2016·The Journal of Chemical Physics·Brian P MoleskyAndrew M Moran
Apr 19, 2017·Proceedings of the National Academy of Sciences of the United States of America·Carey PhelpsAndrew H Marcus
May 20, 2009·Accounts of Chemical Research·Sean Garrett-Roe, Peter Hamm
Jul 26, 2011·Nano Letters·Sean J KernMark A Berg
Oct 4, 2011·The Journal of Physical Chemistry Letters·Chris T MiddletonMartin T Zanni
Aug 19, 2015·The Journal of Physical Chemistry Letters·Haorui Wu, Mark A Berg

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Methods Mentioned

BETA
NMR

Software Mentioned

MUPPETS

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