Selective nonlinear response preparation using femtosecond spectrally resolved four-wave-mixing
A novel method is presented to assist the assignment of vibrational coherence in the homodyne degenerate four-wave-mixing technique. The dependence of vibrational coherence dynamics on the interaction sequence of chirped pump and Stokes excitation pulses is exploited to distinguish quantum beating f...
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| Main Authors: | , , |
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| Format: | Article (Journal) |
| Language: | English |
| Published: |
09 December 2011
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| In: |
The journal of chemical physics
Year: 2011, Volume: 135, Issue: 22, Pages: 1-14 |
| ISSN: | 1089-7690 |
| DOI: | 10.1063/1.3666846 |
| Online Access: | Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1063/1.3666846 Verlag, lizenzpflichtig, Volltext: https://aip.scitation.org/doi/10.1063/1.3666846 
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| Author Notes: | Jan Philip Kraack, Marcus Motzkus, Tiago Buckup |
| Summary: | A novel method is presented to assist the assignment of vibrational coherence in the homodyne degenerate four-wave-mixing technique. The dependence of vibrational coherence dynamics on the interaction sequence of chirped pump and Stokes excitation pulses is exploited to distinguish quantum beating from polarization interference. Moreover, by combining chirped excitation and variable delays between pump and Stokes pulses, it is possible to achieve a controlled excitation of response pathways from a single electronic state and separation of population dynamics and vibrational coherence dynamics within a single response pathway. Numerical simulations are performed in the response function framework, which clearly show that such an approach applies for oscillatory contributions originated in the electronically excited state as well as in the ground state. The approach is experimentally demonstrated in three different polyatomic molecules in solution. |
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| Item Description: | Gesehen am 08.07.2022 |
| Physical Description: | Online Resource |
| ISSN: | 1089-7690 |
| DOI: | 10.1063/1.3666846 |