The effect of overlapping pump and gate pulses on time- and frequency-gated spontaneous emission spectra is explored for a model of material dynamics that accounts for strong nonadiabatic and electron-vibrational coupling effects, vibrational relaxation, and optical dephasing, thus representing characteristic features of photoinduced excited-state dynamics in large molecules in the gas phase or in condensed phases. The behaviors of the sequential, coherent, and doorway-window contributions to the spontaneous emission spectrum are studied separately. The interrelation between the sequential and coherent contributions is demonstrated to be sensitive to the carrier frequencies of the pump and gate pulses and also to the optical dephasing rate, opening the possibility of an experimental determination of the latter. The coherent contribution is shown to dominate the spectrum at specific emission frequencies.The effect of overlapping pump and gate pulses on time- and frequency-gated spontaneous emission spectra is explored for a model of material dynamics that accounts for strong nonadiabatic and electron-vibrational coupling effects, vibrational relaxation, and optical dephasing, thus representing characteristic features of photoinduced excited-state dynamics in large molecules in the gas phase or in condensed phases. The behaviors of the sequential, coherent, and doorway-window contributions to the spontaneous emission spectrum are studied separately. The interrelation between the sequential and coherent contributions is demonstrated to be sensitive to the carrier frequencies of the pump and gate pulses and also to the optical dephasing rate, opening the possibility of an experimental determination of the latter. The coherent contribution is shown to dominate the spectrum at specific emission frequencies.

The Journal of Physical Chemistry AApr 1, 20058 citations

Coherent effects in laser spectroscopy

N. C. Wong

Jan 1, 19830 citations

Coherent resonant interactions with molecules and slow light in photonic band-gap fibers

Saikat Ghosh, Jay E. Sharping, Dimitre G. Ouzounov +1 more

We perform coherent three-level spectroscopy and demonstrate induced transparency in acetylene molecules in a hollow-core photonic band-gap fiber (HC-PBF) at 1.5 $\\mu$ m. The induced spectral transmission window is used to demonstrate slow-light effects, and we show that the observed broadening of the spectral features is due to collisions of the molecules with the inner walls of the fiber core. Our results illustrate that such fibers can be used to facilitate strong coherent light-matter interactions even when the optical response of the individual molecules is weak.We perform coherent three-level spectroscopy and demonstrate induced transparency in acetylene molecules in a hollow-core photonic band-gap fiber (HC-PBF) at 1.5$\\mu$m. The induced spectral transmission window is used to demonstrate slow-light effects, and we show that the observed broadening of the spectral features is due to collisions of the molecules with the inner walls of the fiber core. Our results illustrate that such fibers can be used to facilitate strong coherent light-matter interactions even when the optical response of the individual molecules is weak.

Dec 2, 20040 citations

We perform coherent three-level spectroscopy and demonstrate induced transparency in acetylene molecules in a hollow-core photonic band-gap fiber (HC-PBF) at 1.5

\\mu

m. The induced spectral transmission window is used to demonstrate slow-light effects, and we show that the observed broadening of the spectral features is due to collisions of the molecules with the inner walls of the fiber core. Our results illustrate that such fibers can be used to facilitate strong coherent light-matter interactions even when the optical response of the individual molecules is weak.