Journal
JOURNAL OF CHEMICAL PHYSICS
Volume 117, Issue 5, Pages 2415-2424Publisher
AMER INST PHYSICS
DOI: 10.1063/1.1487376
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A femtosecond pump-probe study of the peculiar amide I band of acetanilide, a molecular crystal with hydrogen bonded chains of peptide units, is presented. The almost perfect harmonicity of the 1666 cm(-1) subpeak is related to significant delocalization of this state at low enough temperatures (93 K). The anomalous peak (1650 cm(-1)), on the other hand, is strongly anharmonic, and hence assigned to a self-trapped state. This assignment is in agreement with a more indirect previous work. With increasing temperature, thermal disorder localizes the 1666 cm(-1) band (Anderson localization) and at the same time destroys the self-trapping mechanism. Both the self-trapped state and the delocalized state decay on a 2 ps time scale into states outside the spectral window of this study. The excitation energy reappears on a much slower 35 ps time scale in the form of an increased lattice temperature. (C) 2002 American Institute of Physics.
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