Abstract
Transient spectral holes of 70-${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ width are observed in the OH stretching band (\ensuremath{\sim}3500 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$) of hydrogen-bonded poly(vinyl butyral) films at room temperature. The lifetime of the holes is measured to be ${T}_{1}$=5\ifmmode\pm\else\textpm\fi{}2 ps and interpreted as the population lifetime of the OH stretching vibration. Simultaneously inverse holes with a red shift of 210\ifmmode\pm\else\textpm\fi{}10 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ and the same lifetime ${T}_{1}$ are observed and explained by excited-state absorption. The inhomogeneous broadening of the OH absorption band presents direct evidence for site-specific frequency shifts of the hydrogen bridges. Breaking of H bonds and establishment of a new thermal equilibrium is indicated with time constant \ensuremath{\tau}=15\ifmmode\pm\else\textpm\fi{}5 ps by blue-shifted induced absorption around the monomeric-frequency position.
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