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John A McGuire

Publications and source records attributed to John A McGuire.

2 recordsLinked to original sources

Ultrafast vibrational dynamics at water interfaces.

Time-resolved sum-frequency vibrational spectroscopy permits the study of hitherto neglected ultrafast vibrational dynamics of neat water interfaces. Measurements on interfacial bonded OH stretch modes revealed relaxation behavior on sub-picosecond time scales in close resemblance to that of bulk water. Vibrational excitation is followed by spectral diffusion, vibrational relaxation, and thermalization in the hydrogen-bonding network. Dephasing of the excitation occurs in </=100 femtoseconds. Population relaxation of the dangling OH stretch was found to have a time constant of 1.3 picoseconds, the same as that for excitation transfer between hydrogen-bonded and unbonded OH stretches of water molecules surrounded by acetone.

Journal Article↗

Electron dynamics of silicon surface states: second-harmonic hole burning on Si(111)-(7 x 7).

We report the first all-optical study of homogeneous linewidths of surface excitations by the spectral-hole-burning technique with surface-specific second-harmonic generation as a probe. Measurement of transient spectral holes induced by a 100 fs pump pulse in excitations of the surface dangling-bond states of Si(111)-(7 x 7) led to a pump-fluence-dependent homogeneous linewidth as broad as approximately 100 meV or a dephasing time as short as 15 fs. The hole-burning spectra also revealed a strong coupling between the localized dangling-bond states and the associated surface phonon mode at 570 cm(-1). Carrier-carrier scattering was responsible for the linear dependence of the dephasing rate on pump fluence, and the carrier screening effect appeared to be weak.

Journal Article↗