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  1. The relaxation from the lowest singlet excited state of the triphenylmethane dyes, crystal violet and malachite green, is studied via two-dimensional electronic-vibrational (2DEV) spectroscopy.
  2. Cited by 13Full Text Available
  3. Given its critical role in redox chemistry, determining the structure of the aqueous excess proton and the mechanism of proton transport in water remains an intense area of experimental and theoretical research. The ultrafast dynamics of the proton’s hydration structure has made experimental study extremely challenging. Using ultrafast broadband two-dimensional infrared spectroscopy, we show that the vibrational spectrum of the aqueous proton is fully consistent with a protonated water complex broadly defined as a Zundel like H 5O 2 + motif. Analysis of the inhomogeneously broadened proton stretch two-dimensional lineshape indicates an intrinsically asymmetric, low barrier O-H +-O potential thatmore » exhibits surprisingly persistent distributions in both its asymmetry and O-O distance. Finally, this structural characterization has direct implications for the extent of delocalization of the proton’s excess charge and possible mechanisms for proton transport in water.« less
  4. Changes in the electronic structure of pigments in protein environments and of polar molecules in solution inevitably induce a re-adaption of molecular nuclear structure. Both changes of electronic and vibrational energies can be probed with visible or infrared lasers, such as two-dimensional electronic spectroscopy or vibrational spectroscopy. The extent to which the two changes are correlated remains elusive. The recent demonstration of two-dimensional electronic-vibrational (2DEV) spectroscopy potentially enables a direct measurement of this correlation experimentally. However, it has hitherto been unclear how to characterize the correlation from the spectra. In this report, we present a theoretical formalism to demonstrate themore » slope of the nodal line between the excited state absorption and ground state bleach peaks in the spectra as a characterization of the correlation between electronic and vibrational transition energies. In conclusion, we also show the dynamics of the nodal line slope is correlated to the vibrational spectral dynamics. Additionally, we demonstrate the fundamental 2DEV spectral line-shape of a monomer with newly developed response functions« less
    Cited by 11Full Text Available

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