研究目的
To demonstrate the feasibility of femtosecond time-resolved impulsive stimulated Raman spectroscopy (TR-ISRS) with synchronized triple mode-locked lasers for investigating the structural changes of photoexcited molecules without using any time-delay devices.
研究成果
The study successfully demonstrates the feasibility of TR-ISRS with synchronized triple mode-locked lasers, enabling rapid data acquisition and wide dynamic range measurements. This technique is anticipated to be valuable for studying photochemical reaction dynamics, including solvent dynamics and structural changes in photoexcited molecules.
研究不足
The technique's limitations include the complexity of synchronizing three mode-locked lasers and the need for precise control of their repetition rates. Additionally, the time jitter for the t1-scan is comparable to the time interval Δt1, requiring careful correction.
1：Experimental Design and Method Selection:
The study employs synchronized triple mode-locked lasers (MLs) for TR-ISRS measurements without mechanical delay lines. The repetition rates of three MLs are precisely controlled to achieve automatic scanning of two delay times between the pulses.
2：Sample Selection and Data Sources:
The sample used is IR144 in ethanol solution, chosen for its known photophysical properties and relevance to photochemical studies.
3：List of Experimental Equipment and Materials:
The setup includes three mode-locked lasers (ML1, ML2, ML3), optical amplifiers, optical parametric amplifiers, short-pass and long-pass filters, and detectors for measuring the fifth-order signals.
4：Experimental Procedures and Operational Workflow:
The actinic pump pulse from ML1 excites the sample, followed by Raman pump and probe pulses from ML2 and ML3, respectively. The time delays between pulses are controlled by adjusting the repetition rates of the MLs.
5：Data Analysis Methods:
The time-resolved Raman spectra (TRS) are obtained by Fourier-transforming the signal with respect to the delay time between Raman pump and probe pulses. The data is analyzed to extract vibrational modes and their dynamics.
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