Using short infrared pulses and sum-frequency up-conversion, the dephasing of the transient polarization of the Si-H adsorbate-substrate vibration is followed in real time. At 120 K, dephasing due to homogeneous linewidth or inhomogeneous broadening are separated.
We present results of the first vibrational photon-echo, transient-grating, and temperature dependent transient-bleaching experiments on a-Si:H. Using these techniques, and the infrared light of a free electron laser, the vibrational population decay and phase relaxation of the Si-H stretching mode were investigated. Careful analysis of the data indicates that the vibrational energy relaxes directly into Si-H bending modes and Si phonons, with a distribution of rates determined by the amorphous host. Conversely, the pure dephasing appears to be single exponential, and can be modeled by dephasing via two-phonon interactions.
We present the first infrared photon echo study of liquid water. For the O-H stretch vibration of HDO in D2O, femtosecond four-wave mixing experiments reveal an extraordinary short pure dephasing time T2∗ on the order of 90 fs. This unusually fast time scale of dephasing is rationalized by taking into account the large anharmonicity of the hydrogen bonded O-H stretching mode.
By extending the laser-frequency-switching technique to a 100-psec time scale, we have observed for the Na D1 line the first-order free-induction decay, its inhomogeneous dephasing time T2∗, its interference with the nonlinear free-induction decay, and a 1.8-GHz interference beat of the ground-state hfs. Detailed theoretical predictions of these new coherence effects are faithfully observed.
We present a set of experiments that provide a complete mapping of coherent and incoherent vibrational relaxation times for a molecule on a metal surface, CO/Ir{111}. Included is the first detection of a midinfrared photon echo from a metallic surface, some 15 years after the analogous measurement on a semiconductor surface, which sets a precedent for the ability to manipulate and rephase polarization on a subpicosecond time scale on surfaces. For the C-O stretch in a strongly dipole-coupled CO layer we obtain a total linewidth of 5.6 cm-1, composed of a homogeneous width of 2.7 cm-1 and an inhomogeneous contribution of 3.0 cm-1. Pure dephasing is negligible at liquid nitrogen temperatures, making CO/Ir{111} an attractive model system for quantum computing.