Frequency-resolved ultrafast dynamics of phonon polariton wavepackets in the ferroelectric crystals LiNbO₃ and LiTaO₃

During this work I built a four wave mixing setup for the time-resolved femtosecond spectroscopy of Raman-active lattice modes. This setup enables to study the selective excitation of phonon polaritons. These quasi-particles arise from the coupling of electro-magnetic waves and transverse optical lattice modes, the so-called phonons. The phonon polaritons were investigated in the optically non-linear, ferroelectric crystals LiNbO₃ and LiTaO₃. The direct observation of the frequency shift of the scattered narrow bandwidth probe pulses proofs the role of the Raman interaction during the probe and excitation process of phonon polaritons. I compare this experimental method with the measurement where ultra-short laser pulses are used. The frequency shift remains obscured by the relative broad bandwidth of these laser pulses. In an experiment with narrow bandwidth probe pulses, the Stokes and anti-Stokes intensities are spectrally separated. They are assigned to the corresponding counter-propagating wavepackets of phonon polaritons. Thus, the dynamics of these wavepackets was separately studied. Based on these findings, I develop the mathematical description of the so-called homodyne detection of light for the case of light scattering from counter propagating phonon polaritons. Further, I modified the broad bandwidth of the ultra-short pump pulses using bandpass filters to generate two pump pulses with non-overlapping spectra. This enables the frequency-selective excitation of polariton modes in the sample, which allows me to observe even very weak polariton modes in LiNbO₃ or LiTaO₃ that belong to the higher branches of the dispersion relation of phonon polaritons. The experimentally determined dispersion relation of the phonon polaritons could therefore be extended and compared to theoretical models. In addition, I determined the frequency-dependent damping of phonon polaritons.

Level thesis:degree_level

thesis.doctoral

Grantor dc:publisher

Universität Potsdam

Year

2014

Author dc:creator

• Goldshteyn, Jewgenij

Contributors dc:contributor

• Bargheer, Matias

• transient grating
• time resolved spectroskopy
• non-linear optics
• phonon polariton
• impulsive stimulated Raman scattering
• transientes Gitter
• zeitaufgelöste Spektroskopie
• nichtlineare Optik
• Phonon-Polariton
• impulsive stimulierte Raman Streuung

Statement dc:rights

• CC-BY-NC-ND - Namensnennung, nicht kommerziell, keine Bearbeitungen 4.0 International

Repository record source_url

https://publishup.uni-potsdam.de/frontdoor/index/index/docId/7162

OAI identifier oai:identifier

oai:kobv.de-opus4-uni-potsdam:7162