arXiv subjects

Jeremy A. Johnson

Publications and source records attributed to Jeremy A. Johnson.

At least 19 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↗

arXiv2026

ZPAN: An Organic Nonlinear Optical Crystal for High Intensity THz Generation

We report an optimized synthesis and crystal growth protocol as well as structural, optical, and terahertz (THz) generation characteristics of the organic nonlinear optical crystal ZPAN ((Z)-1-(((4-Phenylamino)phenylamino)methylene)naphthalen-2(1H)-one). Noncentrosymmetric packing of ZPAN is most reliably achieved by slow evaporation from an acetone-based solvent system, producing long rectangular prisms (7 cm \times 1 cm \times 0.2 cm) with (010) as the main face and [001] as both the polar axis and the direction of elongated crystal growth. [001] is thus the most effective pump polarization direction for generating THz light via optical rectification. The THz generation characteristics of the developed ZPAN crystals are determined at different near-infrared irradiation wavelengths, crystal thicknesses, and pump powers, revealing that ZPAN can generate a peak-to-peak electric field of near 1 MV/cm with a smooth spectrum from 0.5-3.4 THz. Calculated second order nonlinear optical coefficients indicate that both the (100) and (010) faces are theoretically capable of THz generation, though (010) is consistently the dominant growth face. The large size of this face (7 cm \times 1 cm) makes it possible to scale laser power with aperture size, for use in extremely high-power laser systems.

physics.optics↗

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

Optimal Routes to Ultrafast Polarization Reversal in Ferroelectric LiNbO3

We use the frozen phonon method to calculate the anharmonic potential energy surface and to model the ultrafast ferroelectric polarization reversal in LiNbO3 driven by intense pulses of THz light. Before stable switching of the polarization occurs, there exists a region of excitation field-strengths where transient switching can occur, as observed experimentally [Physical Review Letters 118, 197601 (2017)]. By varying the excitation frequency from 4 to 20 THz, our modeling suggests that more efficient, permanent polarization switching can occur by directly exciting the soft mode at 7 THz, compared to nonlinear phononic-induced switching driven by exciting a high frequency mode at 18 THz. We also show that neglecting anharmonic coupling pathways in the modeled experiment can lead to significant differences in the modeled switching field strengths.

cond-mat.mtrl-sci↗

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↗

arXiv2023

Wavelength and phase considerations for multi-pulse plasma generation of terahertz

We present a numerical study on plasma generation of THz radiation utilizing multiple light pulses of various wavelengths in an optical scheme that is readily achievable in a tabletop environment. To achieve coherent THz emission it is necessary to carefully consider all the wavelengths involved in a multi-pulse setup. Previous theoretical work has explored ideal waveforms and electric field symmetries for optimal efficiency in generating THz from plasma [Phys. Rev. Lett. 114 183901 (2015)]. In practice such setups are quite delicate and prone to instability. We show that wavelength combinations with lower theoretical efficiency can more easily produce stable THz pulses in a tabletop environment combining readily available near-infrared wavelengths.

physics.optics↗

arXiv2022

A new standard in high-field terahertz generation: the organic nonlinear optical crystal PNPA

We report the full characterization of a new organic nonlinear optical (NLO) crystal for intense THz generation: PNPA ((E)-4-((4-nitrobenzylidene)amino)-N-phenylaniline). We discuss crystal growth and structural characteristics. We present the wavelength dependence of THz generation, the thickness dependence of the THz spectrum for PNPA crystals, and measure the efficiency. PNPA enables intense THz generation that surpasses NLO crystals DAST and OH-1, which have been the standard in organic high-field THz generators for several years.

physics.optics↗

arXiv2021

Data Mining for Terahertz Generation Crystals

We demonstrate a data mining approach to discover and develop new organic nonlinear optical crystals that produce intense pulses of terahertz radiation. We mine the Cambridge Structural Database for non-centrosymmetric materials and use this structural data in tandem with density functional theory calculations to predict new materials that efficiently generate terahertz radiation. This enables us to (in a relatively short time) discover, synthesize, and grow large, high-quality crystals of four promising materials and characterize them for intense terahertz generation. In a direct comparison to the current state-of-the-art organic terahertz generation crystals, these new materials excel. The discovery and characterization of these novel terahertz generators validates the approach of combining data mining with density functional theory calculations to predict properties of high-performance organic materials, potentially for a host of exciting applications.

cond-mat.mtrl-sci↗

arXiv2020

Enabling High-Power, Broadband THz Generation with 800-nm Pump Wavelength

The organic terahertz (THz) generation crystal BNA has recently gained traction as a valuable source to produce broadband THz pulses. Even when pumped with 800-nm light, thin BNA crystals can produce relatively high electric fields with frequency components out to 5 THz. However, the THz output when pumped with 800-nm light is limited by the damage threshold of the organic crystal. Here we report that the damage threshold of BNA can be significantly improved by physically bonding BNA to a high-thermal conductivity sapphire window. When pumped with 800-nm light from an amplified Ti:sapphire laser system, our bonded BNA (BNA-sapphire) generates 2.5 times higher electric field strengths compared to bare BNA crystals. We characterize the average damage threshold for bare BNA and BNA-sapphire, measure peak-to-peak electric field strengths and THz waveforms, and determine the nonlinear transmission in BNA. Pumping BNA-sapphire with 800-nm light results in peak-to-peak electric fields exceeding 1 MV/cm, with strong broadband frequency components from 0.5-5 THz. Our BNA-sapphire THz source is a promising alternative to tilted pulse front LiNbO3 THz sources, which will enable many research groups without optical parametric amplifiers to perform high-field, broadband THz spectroscopy.

physics.optics↗

arXiv2020

Comprehensive Characterization of Terahertz Generation with the Organic Crystal BNA

We characterize the terahertz (THz) generation of N-benzyl-2-methyl-4-nitroaniline (BNA), with crystals ranging in thickness from 123-700 μm. We compare excitation using 800-nm and 1250 to 1500-nm wavelengths. Pumping BNA with 800-nm wavelengths and longer near-infrared wavelengths results in a broad spectrum, producing out to 6 THz using a 100-fs pump, provided the BNA crystal is thin enough. ~200 μm or thinner crystals are required to produce a broad spectrum with an 800-nm pump, whereas ~300 μm thick crystals are optimal for broadband THz generation using the longer wavelengths. We report the favorable THz generation and optical characteristics of our BNA crystals that make them attractive for broadband, high-field THz generation, and we also find significant differences to BNA results reported in other works.

physics.optics↗

arXiv2018

Enhancing terahertz generation from a two-color plasma using optical parametric amplifier waste light

We show experimentally that the terahertz (THz) emission of a plasma, generated in air by a two-color laser pulse (containing a near IR frequency and its second harmonic), can be enhanced by the addition of an 800-nm pulse. We observed enhancements of the THz electric field by a factor of up to 30. This provides a widely accessible means for researchers using optical parametric amplifiers (OPA) to increase their THz yields by simply adding the residual pump beam of the OPA to the plasma generating beam. We investigate the dependence of the THz electric field enhancement factor on the powers of the two-color beam as well as the 800-nm enhancement beam. Numerical calculations using the well-known photocurrent model are in excellent agreement with the experimental observations.

physics.plasm-ph↗

arXiv2017

Laser-induced plasma generation of terahertz radiation using three incommensurate wavelengths

We present the generation of THz radiation by focusing ultrafast laser pulses with three incommensurate wavelengths to form a plasma. The three colors include 800 nm and the variable IR signal and idler outputs from an optical parametric amplifier. Stable THz is generated when all three colors are present, with a peak-to-peak field strength of ~200 kV/cm and a relatively broad, smooth spectrum extending out to 6 THz, without any strong dependence on the selection of signal and idler IR wavelengths (in the range from 1300-2000 nm). We confirm that 3 colors are indeed needed, and comment on the polarization characteristics of the generated THz, some of which are challenging to explain with plasma current models that have had success in describing two-color plasma THz generation.

physics.plasm-ph↗

arXiv2017

Experimentally Exploring the Interatomic Potential in a Ferroelectric Crystal via Optimal Ultrafast Lattice Control

We present a direct comparison between resonant terahertz (THz) and nonresonant impulsive stimulated Raman scattering (ISRS) excitation of phonon-polaritons in ferroelectric lithium niobate. THz excitation offers advantages of selectively driving only the forward propagating phonon-polariton mode to exceedingly high amplitudes, without complications due to nonlinear processes at the high 800 nm pump fluences used in Raman excitation. At peak-to-peak THz electric field strengths exceeding 1 MV/cm, the ferroelectric lattice is driven into the anharmonic regime, allowing experimental determination of the shape of the potential energy surface.

cond-mat.mtrl-sci↗

arXiv2017

Direct Test of Supercooled Liquid Scaling Relations

Diverse material classes exhibit practically identical behavior when made viscous upon cooling toward the glass transition, suggesting a common theoretical basis. The first-principles scaling laws that have been proposed to describe the evolution with temperature have yet to be appropriately tested due to the extraordinary range of time scales involved. We used seven different measurement methods to determine the structural relaxation kinetics of a prototype molecular glass former over a temporal range of 13 decades and over a temperature range spanning liquid to glassy states. For the material studied, our results comprise a comprehensive validation of the two scaling relations that are central to the fundamental question of whether supercooled liquid dynamics can be described universally. The ultrabroadband mechanical measurements demonstrated have fundamental and practical applications in polymer science, geophysics, multifunctional materials, and other areas.

cond-mat.soft↗

arXiv2016

Thermal transport in suspended silicon membranes measured by laser-induced transient gratings

Studying thermal transport at the nanoscale poses formidable experimental challenges due both to the physics of the measurement process and to the issues of accuracy and reproducibility. The laser-induced transient thermal grating (TTG) technique permits non-contact measurements on nanostructured samples without a need for metal heaters or any other extraneous structures, offering the advantage of inherently high absolute accuracy. We present a review of recent studies of thermal transport in nanoscale silicon membranes using the TTG technique. An overview of the methodology, including an analysis of measurements errors, is followed by a discussion of new findings obtained from measurements on both solid and nanopatterned membranes. The most important results have been a direct observation of non-diffusive phonon-mediated transport at room temperature and measurements of thickness-dependent thermal conductivity of suspended membranes across a wide thickness range, showing good agreement with first-principles-based theory assuming diffuse scattering at the boundaries. Measurements on a membrane with a periodic pattern of nanosized holes indicated fully diffusive transport and yielded thermal diffusivity values in agreement with Monte Carlo simulations. Based on the results obtained to-date, we conclude that room-temperature thermal transport in membranebased silicon nanostructures is now reasonably well understood.

cond-mat.mes-hall↗

arXiv2015

Ultrafast Laser-Induced Melting of Long-Range Magnetic Order in Multiferroic TbMnO3

We performed ultrafast time-resolved near-infrared pump, resonant soft X-ray diffraction probe measurements to investigate the coupling between the photoexcited electronic system and the spin cycloid magnetic order in multiferroic TbMnO3 at low temperatures. We observe melting of the long range antiferromagnetic order at low excitation fluences with a decay time constant of 22.3 +- 1.1 ps, which is much slower than the ~1 ps melting times previously observed in other systems. To explain the data we propose a simple model of the melting process where the pump laser pulse directly excites the electronic system, which then leads to an increase in the effective temperature of the spin system via a slower relaxation mechanism. Despite this apparent increase in the effective spin temperature, we do not observe changes in the wavevector q of the antiferromagnetic spin order that would typically correlate with an increase in temperature under equilibrium conditions. We suggest that this behavior results from the extremely low magnon group velocity that hinders a change in the spin-spiral wavevector on these time scales.

cond-mat.str-el↗