Time-domain measurements of S-branch N2–N2 Raman linewidths using picosecond pure rotational coherent anti-Stokes Raman spectroscopy

Time-domain measurements of S-branch N2–N2 Raman linewidths using picosecond pure rotational coherent anti-Stokes Raman spectroscopy
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使用皮秒纯旋转相干反斯托克斯拉曼光谱对 S 分支 N2–N2 拉曼线宽进行时域测量

DOI:
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发表时间:
2012
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通讯作者:
T. Settersten
T. Settersten
中科院分区:
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文献类型:
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作者:
C. Kliewer;A. Bohlin;E. Nordström;B. Patterson;P. Bengtsson;T. Settersten

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时间分辨双宽带皮秒纯旋转 CARS 已用于测量 294-1466 K 温度范围内的自展宽 S 分支 N2-N2 拉曼线宽。通过遵循 J 相关 CARS 信号衰减作为探针延迟的函数,在时域中直接检测相干性衰减。旋转拉曼 N2-N2 线宽源自这些与时间相关的衰减,并评估了测温精度。对能量校正突然 (ECS) 和修正指数间隙 (MEG) 动态标度定律进行了比较,结果用于量化纳秒旋转 CARS 测温对所用线宽模型的灵敏度。基于纯 N2 中使用的线宽模型的不确定性为 2%。讨论了这种快速确定拉曼线宽的快速方法的优点和局限性。
Time-resolved dual-broadband picosecond pure rotational CARS has been applied to measure self-broadened S-branch N2–N2 Raman linewidths in the temperature range 294–1466 K. The coherence decays were detected directly in the time domain by following the J-dependent CARS signal decay as a function of probe delay. The rotational Raman N2–N2 linewidths were derived from these time-dependent decays and evaluated for thermometric accuracy. Comparisons were made to the energy-corrected sudden (ECS) and modified exponential gap (MEG) dynamical scaling laws, and the results were used to quantify the sensitivity of nanosecond rotational CARS thermometry to the linewidth model employed. The uncertainty based on the linewidth model used in pure N2 was found to be 2 %. The merits and limitations of this rapid method for the determination of accurate Raman linewidths are discussed.