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Femtosecond fluorescence spectroscopy by upconversion with tilted gate pulses
Lijuan Zhao1, J Luis Pérez Lustres, Vadim Farztdinov
1Department of Chemistry, Humboldt University, Berlin, Germany.
Physical Chemistry Chemical Physics : PCCP
|October 1, 2009
Summary
This study presents a new spectrometer for observing time-resolved emission bands with 80 fs resolution. Nuclear coherence in the excited state significantly influences fluorescence properties.
Area of Science:
- Spectroscopy
- Physical Chemistry
- Femtochemistry
Background:
- Time-resolved spectroscopy is crucial for understanding ultrafast molecular dynamics.
- Previous methods faced limitations in resolution and background noise.
Purpose of the Study:
- To develop a high-resolution spectrometer for time-resolved emission measurements.
- To investigate the role of nuclear coherence in excited-state fluorescence.
Main Methods:
- Simultaneous sum-frequency mixing with femtosecond near-infrared gate pulses.
- Utilizing tilted gate pulses in a noncollinear geometry for enhanced time resolution.
- Optimization of spectrometer components for routine applications.
Main Results:
- Achieved 80 fs time resolution with background-free upconverted spectra.
- Demonstrated the spectrometer's capability using Coumarin 153 fluorescence.
- Observed nuclear coherence modulating fluorescence band width and asymmetry.
Conclusions:
- The developed spectrometer enables routine, high-resolution time-resolved emission studies.
- Nuclear coherence plays a significant role in excited-state dynamics, impacting spectral features.
- This technique offers new insights into fundamental photophysical processes.
