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We apply the Merrifield variational method to the Holstein molecular crystalmodel in D dimensions to compute non-adiabatic polaron band energies andFranck-Condon factors at general crystal momenta. We analyze these observableproperties to extract characteristic features related to polaron self-trappingand potential experimental signatures. These results are combined with othersobtained by the Global-Local variational method in 1D to construct a polaronphase diagram encompassing all degrees of adiabaticity and all electron-phononcoupling strengths. The polaron phase diagram so constructed includes disjointregimes occupied by "small" polarons, "large" polarons, and a newly-definedclass of "compact" polarons, all mutually separated by an intermediate regimeoccupied by transitional structures

Franck−Condon Factors as Spectral Probes of Polaron Structure