In this dissertation, my research work on excited state dynamics of small organic molecules in solutions is presented. Using femtosecond stimulated Raman spectroscopy (FSRS) as the main experimental tool, the excited state hydrogen-bonding dynamics (ESHBD) of Coumarin 102, a common laser dye molecule, in ethanol solution is examined with <150...
We use femtosecond stimulated Raman spectroscopy (FSRS) to illuminate the choreography of intermolecular excited-state proton transfer (ESPT) of photoacid pyranine (8-hydroxypyrene-1,3,6-trisulfonic acid, HPTS) in water. The multidimensional reaction coordinate responsible for photoacidity is revealed to involve sequential activation of characteristic skeletal motions during the ca. 1 ps preparation stage preceding...
Coherent phonon dynamics in condensed-phase medium are responsible for important material properties including thermal and electrical conductivities. We report a structural dynamics technique, time-resolved surface third-harmonic generation (TRSTHG) spectroscopy, to capture transient phonon propagation near the surface of polycrystalline CaF₂ and amorphous borosilicate (BK7) glass. Our approach time-resolves the background-free,...
We achieve a series of distinct broadband third-harmonic generation (THG) signals at the amorphous glass–air interface attributed to third-order and cascaded third-order nonlinear processes. A novel THG laser sideband arises
from cascaded interaction between fundamental pulses and the cascaded four-wave mixing signals. The spatially
separated THG sidebands with distinct spectral...
We report zero kinetic energy (ZEKE) photoelectron spectroscopy of benzo[a]pyrene (BaP) via resonantly enhanced multiphoton ionization (REMPI). Our analysis concentrates on the vibrational modes of the first excited state (S₁) and those of the ground cationic state (D₀). Similar to pyrene, another peri-condensed polycyclic aromatic hydrocarbon we have investigated, the...