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

التفاصيل البيبلوغرافية
العنوان: Spectral narrowing of a phonon resonance in time-domain sum-frequency spectroscopy
المؤلفون: Kiessling, Riko, Wolf, Martin, Paarmann, Alexander
سنة النشر: 2022
المجموعة: Condensed Matter
Physics (Other)
مصطلحات موضوعية: Condensed Matter - Materials Science, Physics - Optics
الوصف: 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.
Comment: 11 pages, 7 figures
نوع الوثيقة: Working Paper
URL الوصول: http://arxiv.org/abs/2211.04593
رقم الأكسشن: edsarx.2211.04593
قاعدة البيانات: arXiv