Spontaneous transient ultrafast coherent Raman spectroscopy

Lorenz, VirginiaI explore the application of Transient Coherent Ultrafast Phonon Spectroscopy (TCUPS) to the measurement of vibrational coherence dynamics of liquid alcohols. The demonstrated technique is complementary to and, in some cases, simpler than traditional stimulated spectroscopy techniques in that it does not require more than one laser and is free of non-resonant background. I demonstrate coherence measurements of single-photon-level collective excitations: a single vibrational state at 1033 (1/cm) in; a pair of simultaneous excited vibrational states at 2834 and 2944 (1/cm) in methanol; and three simultaneous excited states at 2885, ∼2930, and 2976 (1/cm) in isopropanol. I develop a Fourier-transform-based analysis of the TCUPS data that overcomes poor signal-to-noise ratio and signal degradation due to etaloning and fluorescence. The coherence lifetimes and oscillation frequencies agree with frequency-domain line-shape measurements and femtosecond Coherent anti-Stokes Raman Scattering (CARS) measurements.University of Delaware, Department of Physics and AstronomyPh.D