Josef J. Felver

Seedless velocimetry at 100 kHz with picosecond-laser electronic-excitation tagging

Picosecond-laser electronic-excitation tagging (PLEET), a seedless picosecond-laser-based velocimetry technique, is demonstrated in non-reactive flows at a repetition rate of 100 kHz with a 1064 nm, 100 ps burst-mode laser. The fluorescence lifetime of the PLEET signal was measured in nitrogen, and the laser heating effects were analyzed. PLEET experiments with a free jet of nitrogen show the ability to measure multi-point flow velocity fluctuations at a 100 kHz detection rate or higher. Both spectral and dynamic mode decomposition analyses of velocity on a Ma=0.8 free jet show two dominant Strouhal numbers around 0.24 and 0.48, respectively, well within the shear-layer flapping frequencies of the free jets. This technique increases the laser-tagging repetition rate for velocimetry to hundreds of kilohertz. PLEET is suitable for subsonic through supersonic laminar- and turbulent-flow velocity measurements.

Observation of structural relaxation during exciton self-trapping via excited-state resonant impulsive stimulated Raman spectroscopy

We detect the change in vibrational frequency associated with the transition from a delocalized to a localized electronic state using femtosecond vibrational wavepacket techniques. The experiments are carried out in the mixed-valence linear chain material [Pt(en)2][Pt(en)2Cl2]⋅(ClO4)4 (en = ethylenediamine, C2H8N2), a quasi-one-dimensional system with strong electron-phonon coupling. Vibrational spectroscopy of the equilibrated self-trapped exciton is carried out using a multiple pulse excitation technique: an initial pump pulse creates a population of delocalized excitons that self-trap and equilibrate, and a time-delayed second pump pulse tuned to the red-shifted absorption band of the self-trapped exciton impulsively excites vibrational wavepacket oscillations at the characteristic vibrational frequencies of the equilibrated self-trapped exciton state by the resonant impulsive stimulated Raman mechanism, acting on the excited state. The measurements yield oscillations at a frequency of 160 cm(-1) corresponding to a Raman-active mode of the equilibrated self-trapped exciton with Pt-Cl stretching character. The 160 cm(-1) frequency is shifted from the previously observed wavepacket frequency of 185 cm(-1) associated with the initially generated exciton and from the 312 cm(-1) Raman-active symmetric stretching mode of the ground electronic state. We relate the frequency shifts to the changes in charge distribution and local structure that create the potential that stabilizes the self-trapped state.

Exciton localization probed via excited-state resonant impulsive stimulated Raman spectroscopy

We probe the transition from a delocalized to a localized electronic state in a quasi-one-dimensional system by the change in vibrational frequency detected by resonant impulsive Raman excitation of the excited state in a pump-pump-probe measurement.

Ultrafast Dispersive Transport in a-SiGe:H

Carrier dynamics in a-SiGe:H are studied using femtosecond optical techniques. The response reveals dispersive transport with a time-dependent mobility that varies systematically with temperature and with the degree of disorder in the material.