Wavelength-tunable ultrashort-pulse output of a photonic-crystal fiber designed to resolve ultrafast molecular dynamics

Abstract

Wavelength-tunable $100\mathrm{fs}$ pulses generated through the soliton self-frequency shift in a photonic-crystal fiber are employed to visualize femtosecond coherence and population relaxation dynamics in molecular aggregates by means of time-resolved sum-frequency generation. This technique reveals an ultrafast dephasing of coherent molecular excitations with a phase relaxation time of about $120\mathrm{fs}$ and resolves an ultrafast switching of the nonlinear-optical response of molecular aggregates.

© 2006 Optical Society of America

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