arXiv subjects

Megan F. Biggs

Publications and source records attributed to Megan F. Biggs.

5 recordsLinked to original sources

arXiv2026

Measuring momentum-resolved dissipation of phonon-polaritons in LiNbO$_3$ with terahertz driving

Mapping the dispersion of polaritons, hybrid quasiparticles arising from light-matter coupling, can provide key insights into the material dielectric response, coupling strength, and energy transfer pathways with other excitations. In this work, we present THz pump-Raman probe (TP-RP) as a versatile method for mapping the polariton dispersion in polar non-centrosymmetric materials, demonstrated here for the case of phonon-polaritons in LiNbO$_3$. By resonantly driving polaritonic modes with a broadband THz pump and probing them with a tunable NIR Raman pulse, TP-RP allows for the extraction of the momentum-dependence of both their frequency and damping rate with high accuracy. The spectral features observed in the pump-probe signal, including the polaritonic response as well as pulse artifacts, are reproduced within a many-body theoretical approach. Applying the technique to study the E(TO$_1$) phonon of LiNbO$_3$ enables the combined analysis of theory and experiments to uncover a nontrivial frequency dependence of the phonon intrinsic damping rate, revealing possible anharmonic couplings to other modes.

cond-mat.mtrl-sci↗

arXiv2025

Ultrafast Faraday Rotation Probe of Chiral Phonon-Polaritons in LiNbO3

Time reversal symmetry breaking motion of chiral phonon-polaritons in LiNbO3 is probed via the ultrafast Faraday effect. By combining a pair of perpendicularly polarized THz pulses with the right relative delay, we create a chiral THz driving field to excite chiral phonon-polaritons. The chiral atomic motion combines with the inverse Faraday effect from the circularly polarized THz pump to induce a magnetic moment field in the nonmagnetic material, LiNbO3. We attempt to quantify the strength of the magnetic field with Faraday rotation probe measurements. The direction of the Faraday signal flips when the input THz pulse is changed from left- to right-circular polarization, and we estimate a strong induced magnetic field strength of ~11 Tesla based on the Faraday rotation.

cond-mat.mes-hall↗

arXiv2024

High-Dynamic Range Broadband Terahertz Time-Domain Spectrometer Based on Organic Crystal MNA

We present a high power and broadband THz-TDS setup utilizing the nonlinear organic crystal MNA both as emitter and detector. The THz source is based on optical rectification of near infra-red laser pulses at a central wavelength of 1036 nm from a commercial, high-power Yb-based laser system and reaches a high THz average power of 11 mW at a repetition rate of 100 kHz and a broad and smooth bandwidth of more than 9 THz. The conversion efficiency is high (0.13%) in spite of the high excitation average power of 8 W. We validate the high dynamic range and reliability of the source for applications in linear spectroscopy by measuring the broadband THz properties of chi(2) nonlinear crystals up to 8 THz. This new high-repetition rate source is very promising for ultra-broadband THz spectroscopy at high dynamic range and/or reduced measurement times.

physics.optics↗

arXiv2024

$χ^{(2)}$-Induced Artifact Overwhelming the Third-Order Signal in 2D Raman-THz Spectroscopy of Non-Centrosymmetric Materials

Through comprehensive data analysis, we demonstrate that a $χ^{(2)}$-induced artifact, arising from imperfect balancing in the conventional electro-optic sampling (EOS) detection scheme, contributes significantly to the measured signal in 2D Raman-THz spectroscopy of non-centrosymmetric materials. The artifact is a product of two 1D responses, overwhelming the desired 2D response. We confirm that by analyzing the 2D Raman-THz response of a x-cut beta barium borate (BBO) crystal. We furthermore show that this artifact can be effectively suppressed by implementing a special detection scheme. We successfully isolate the desired third-order 2D Raman-THz response, revealing a distinct cross-peak feature, whose frequency position suggests the coupling between two crystal phonons.

physics.optics↗

arXiv2023

Pump Pulse Bandwidth-Activated Nonlinear Phononic Coupling in CdWO$_4$

To control structure-function relationships in solids with light, we must harness the shape of the potential energy surface, as expressed in anharmonic coupling coefficients. We use two-dimensional terahertz (THz) spectroscopy to identify trilinear coupling between sets of vibrational modes in CdWO$_4$. It is generally understood that efficient trilinear coupling occurs when the frequencies of two coupled modes add or subtract to the frequency of the third mode. Interestingly, we observe that this condition is not necessary: the THz driving-pulse itself can activate the coupling by contributing broad frequency content to the initial motion of the excited modes. Understanding that the bandwidth of the driving force can activate energy-flow pathways has broad implications for coherent control of collective modes using intense THz light pulses.

physics.optics↗