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The theory of linear and non-linear infrared response of vibrational Holsteinpolarons in one-dimensional lattices is presented in order to identify thespectral signatures of self-trapping phenomena. Using a canonicaltransformation the optical response is computed from the small polaron point ofview which is valid in the anti-adiabatic limit. Two types of phonon baths areconsidered: optical phonons and acoustical phonons, and simple expressions arederived for the infrared response. It is shown that for the case of opticalphonons, the linear response can directly probe the polaron density of states.The model is used to interpret the experimental spectrum of crystalineactetanilide in the C=O range. For the case of acoustical phonons, it is shownthat two bound states can be observed in the two-dimensional infrared spectrumat low temperature. At high temperature, analysis of the time-dependence of thetwo-dimensional infrared spectrum indicates that bath mediated correlationsslow down spectral diffusion. The model is used to interpret the experimentallinear-spectroscopy of model alpha-helix and beta-sheet polypeptides. This workshows that the Davydov Hamiltonian cannot explain the observations in the NHstretching range.

journal of chemical physics online/the journal of chemical physics/journal of chemical physics

Linear and non-linear infrared response of one-dimensional vibrational  Holstein polarons in the anti-adiabatic limit: optical and acoustical phonon  models