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arXiv 2211.04593cond-mat.mtrl-sciphysics.optics
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时域和频光谱中声子共振的光谱窄化

Spectral narrowing of a phonon resonance in time-domain sum-frequency spectroscopy

Riko Kiessling, Martin Wolf, Alexander Paarmann

AI总结:

本研究利用自由电子激光器的可调谐皮秒红外脉冲,通过红外-可见振动和频生成光谱学,在频域和时域探测了4H-SiC的非线性光学响应,发现通过在红外和可见上转换脉冲间引入时间延迟可实现声子SFG共振的光谱窄化。

摘要:

和频生成(SFG)光谱学为研究非中心对称介质和界面提供了一种多功能方法。在此,利用来自自由电子激光器的可调谐皮秒红外(IR)脉冲,通过红外-可见振动SFG光谱学,在频域和时域上探测了4H-SiC(碳化硅的一种常见多型体)的非线性光学响应。在SFG光谱中,我们在纵向光学声子频率附近观察到一个尖锐的共振,这源于IR介电常数处于近零状态所引起的线性光学效应。在时域中,SFG强度的建立与感应相干IR极化的自由感应衰减有关。当接近声子共振频率时,与非共振IR激发相比,观察到了更慢的极化退相。因此,通过在IR和可见上转换脉冲之间引入时间延迟,我们能够展示声子SFG共振的光谱窄化,模型计算证实了这一点。

英文摘要:

Sum-frequency generation (SFG) spectroscopy provides a versatile method for the investigation of non-centrosymmetric media and interfaces. Here, using tunable picosecond infrared (IR) pulses from a free-electron laser, the nonlinear optical response of 4H-SiC, a common polytype of silicon carbide, has been probed in the frequency- and time-domain by infrared-visible vibrational SFG spectroscopy. In the SFG spectra we observe a sharp resonance near the longitudinal optical phonon frequency, arising from linear optical effects due the epsilon-near-zero regime of the IR permittivity. In the time domain, the build-up of the SFG intensity is linked to the free-induction decay of the induced coherent IR polarization. When approaching the frequency of the phonon resonance, a slower polarization dephasing is observed as compared to off-resonant IR excitation. Thus, by introducing a temporal delay between the IR and the visible up-conversion pulse we are able to demonstrate spectral narrowing of the phonon SFG resonance, as corroborated by model calculations.

机构、总结、中文摘要均由AI分析而来,可能存在错误,请以论文正文为准。

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