arXiv subjects

Steven L. Johnson

Publications and source records attributed to Steven L. 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

THz-induced phonon mode mixing and collective dynamics in a polar nanolattice

Manipulating phonons through symmetry is a fundamental approach to alter the dynamic responses of materials. Most often new phases are sought through control of the unit-cell (e.g. via strain, doping, light, etc.). By comparison, there is vast potential to look beyond the unit-cell into higher-order architectures to control wave scattering and interference effects that remains less explored. We describe the THz-induced dynamics of an SrTiO$_{3}$ thin film with a nanoscale ordered interfacial dislocation network probed with 2- and 3-dimensional time-resolved x-ray diffraction and classical molecular dynamics simulations. We find that symmetry breaking at all scales is an effective approach to create a dynamical electric polarization and to control phonon mixing that generates previously unreported collective modes in the THz regime with circular vortex-like displacements. This work opens a new pathway to explore dynamical functional properties that can be extended to magnetic, electric, and ferroelectric systems by controlling the real-space topology via epitaxy.

cond-mat.str-el↗

arXiv2026

Anharmonic phonon coupling enabled by local inversion symmetry breaking at domain walls in ferroelastics

In ferroelastic materials, spontaneous symmetry breaking leads to the formation of twin domains. Although the bulk crystal typically remains centrosymmetric, inversion symmetry can be locally broken at the domain walls, potentially changing phonon selection rules and enabling local anharmonic phonon coupling. Here we report direct evidence of such anharmonic coupling in ferroelastic LaAlO$_3$ using two-dimensional Raman-terahertz spectroscopy. We attribute the cross-peaks observed in the two-dimensional spectra to both mechanical and electrical anharmonicity between the $A_{1g}$ Raman-active phonon and the $E_g$ phonon, which acquires finite infrared activity through local inversion symmetry breaking at ferroelastic domain walls. These findings provide new insight into the complex lattice dynamics of ferroelastic materials and highlight the potential of two-dimensional Raman-terahertz spectroscopy to uncover subtle symmetry breaking through the detection of intrinsically weak anharmonic signals.

cond-mat.mtrl-sci↗

arXiv2026

Evaluating Temporal Consistency in Multi-Turn Language Models

Language models are increasingly deployed in interactive settings where users reason about facts over time rather than in isolation. In such scenarios, correct behavior requires models to maintain and update implicit temporal assumptions established earlier in a conversation. We study this challenge through the lens of temporal scope stability: the ability to preserve, override, or transfer time-scoped factual context across dialogue turns. We introduce ChronoScope, a large-scale diagnostic benchmark designed to isolate temporal scope behavior in controlled multi-turn interactions, comprising over one million deterministically generated question chains grounded in Wikidata. ChronoScope evaluates whether models can correctly retain inferred temporal scope when follow-up questions omit explicit time references, spanning implicit carryover, explicit scope switching, cross-entity transfer, and longer temporal trajectories. Through extensive evaluation of state-of-the-art language models, we find that temporal scope stability is frequently violated in controlled multi-turn settings, with models often drifting toward present-day assumptions despite correct underlying knowledge. These failures intensify with interaction length and persist even under oracle context conditions, revealing a gap between single-turn factual accuracy and coherent temporal reasoning under sequential interaction. We make our dataset and evaluation suite publicly available at https://github.com/yashkumaratri/ChronoScope

cs.CL↗

arXiv2026

Ultrafast Decoherence of Charge Density Waves in K$_{0.3}$MoO$_{3}$

Recent works have suggested that transient suppression of a charge density wave (CDW) by an ultra-short excitation can lead to an inversion of the CDW phase. We experimentally investigate the dynamics of the CDW in K$_{0.3}$MoO$_{3}$ by time resolved x-ray diffraction after excitation with optical pulses. Our results indicate a transient inversion of the CDW phase close to the surface that evolves into a highly disordered state in less than one picosecond. Numerical simulations solving the Ginzburg-Landau equation including disorder from strong pinning defects reproduce our main observations. Our findings highlight the critical role of disorder in schemes for coherent control in condensed matter systems.

cond-mat.str-el↗

arXiv2025

Decoding the Rule Book: Extracting Hidden Moderation Criteria from Reddit Communities

Effective content moderation systems require explicit classification criteria, yet online communities like subreddits often operate with diverse, implicit standards. This work introduces a novel approach to identify and extract these implicit criteria from historical moderation data using an interpretable architecture. We represent moderation criteria as score tables of lexical expressions associated with content removal, enabling systematic comparison across different communities. Our experiments demonstrate that these extracted lexical patterns effectively replicate the performance of neural moderation models while providing transparent insights into decision-making processes. The resulting criteria matrix reveals significant variations in how seemingly shared norms are actually enforced, uncovering previously undocumented moderation patterns including community-specific tolerances for language, features for topical restrictions, and underlying subcategories of the toxic speech classification.

cs.CL↗

arXiv2024

Ultrafast selective mid-infrared sublattice manipulation in the ferrimagnet $FeCr_2S_4$

$FeCr_2S_4$ is a ferrimagnet with two oppositely ordered spin sublattices (Fe and Cr), connected via superexchange interaction, giving a non-zero net magnetic moment. We show, using time-resolved measurements of the magneto-optic Kerr effect, how the magnetic dynamics of the sublattices can be selectively manipulated by resonantly perturbing the Fe sublattice with ultrashort laser pulses. The mid-infrared excitation through intra-atomic Fe $d$-$d$ transitions triggers markedly slower dynamics in comparison to an off-resonant pumping affecting both of the two sublattices simultaneously. By changing probe wavelength to move in and out of resonance with the Fe $d$-$d$ transitions, we also show the specific contributions of the Fe sublattice to these dynamics.

cond-mat.mes-hall↗

arXiv2024

High-power femtosecond mid-IR source with tunable center frequency and chirp

We present an experimental implementation of a chirped mid-infrared (mid-IR) high-power laser source with variable center frequency between 4 THz to 30 THz and continuously tunable frequency sweep of up to 20 % within one pulse, with a pulse duration of 2 ps. The peak electric field obtained at 4 THz is 1.5 MV/cm. We generate the mid-IR light using a difference-frequency generation (DFG) process with two phase-locked, chirped IR pulses. The obtained mid-IR electric field waveform is characterized using electro-optic sampling. We compare our experimental results with the predictions of numerical simulations. The results indicate the potential for efficient driving of vibrational modes into a strongly anharmomic regime, in cases where using Fourier-transform-limited pulses to achieve similar vibrational amplitudes would lead to dielectric breakdown.

physics.optics↗

arXiv2024

Roles of band gap and Kane electronic dispersion in the THz-frequency nonlinear optical response in HgCdTe

Materials with linear electronic dispersion often feature high carrier mobilities and unusually strong nonlinear optical interactions. In this work, we investigate the THz nonlinear dynamics of one such material, HgCdTe, with an electronic band dispersion heavily dependent on both temperature and stoichiometry. We show how the band gap, carrier concentration and band shape together determine the nonlinear response of the system. At low temperatures, carrier generation from Zener tunneling dominates the nonlinear response with a reduction in the overall transmission. At room temperature, quasi-ballistic electronic dynamics drive the largest observed nonlinear optical interactions, leading to a transmission increase. Our results demonstrate the sensitivity of these nonlinear optical properties of narrow-gap materials to small changes in the electronic dispersion and carrier concentration.

cond-mat.mtrl-sci↗

arXiv2024

Observation of polarization density waves in SrTiO3

The nature of the "failed" ferroelectric transition in SrTiO3 has been a long-standing puzzle in condensed matter physics. A compelling explanation is the competition between ferroelectricity and an instability with a mesoscopic modulation of the polarization. These polarization density waves, which should become especially strong near the quantum critical point, break local inversion symmetry and are difficult to probe with conventional x-ray scattering methods. Here we combine a femtosecond x-ray free electron laser (XFEL) with THz coherent control methods to probe inversion symmetry breaking at finite momenta and visualize the instability of the polarization on nanometer lengthscales in SrTiO3. We find polar-acoustic collective modes that are soft particularly at the tens of nanometer lengthscale. These precursor collective excitations provide evidence for the conjectured mesoscopic modulated phase in SrTiO3.

cond-mat.mtrl-sci↗

arXiv2023

Ultrafast all-optical manipulation of the charge-density-wave in VTe$_{2}$

The charge-density wave (CDW) phase in the layered transition-metal dichalcogenide VTe$_{2}$ is strongly coupled to the band inversion involving vanadium and tellurium orbitals. In particular, this coupling leads to a selective disappearance of the Dirac-type states that characterize the normal phase, when the CDW phase sets in. Here, by means of broadband time-resolved optical spectroscopy (TR-OS), we investigate the ultrafast reflectivity changes caused by collective and single particle excitations in the CDW ground state of VTe$_{2}$. Remarkably, our measurements show the presence of two collective (amplitude) modes of the CDW ground state. By applying a double-pulse excitation scheme, we show the possibility to manipulate these modes, demonstrating a more efficient way to control and perturb the CDW phase in VTe$_{2}$.

cond-mat.str-el↗

arXiv2022

Impact ionization in low-band-gap semiconductors driven by ultrafast THz excitation: beyond the ballistic regime

Using two-dimensional THz spectroscopy in combination with numerical models, we investigate the dynamics linked to carrier multiplication caused by high-field THz excitation of the low-gap semiconductor InSb. In addition to previously observed dynamics connected with quasi-ballistic carrier dynamics, we observe other spectral and temporal features that we attribute to impact ionization for peak fields above 60 kV/cm, which continue up to the maximum investigated peak field of 430 kV/cm. At the highest fields we estimate a carrier multiplication factor greater than 10 due to impact ionization, which is well-reproduced by a numerical simulation of the impact ionization process which we have developed.

cond-mat.other↗

arXiv2022

Solid-State Biased Coherent Detection of Ultra-Broadband Terahertz Pulses for high repetition rate, low pulse energy lasers

We report the coherent generation and detection of terahertz (THz) pulses covering the bandwidth of 0.1-9 THz in a high repetition rate, low pulse energy laser system. In this work we demonstrate the application and evaluation of solid-state biased coherent detection in combination with a spintronic emitter. This combination was used to generate and detect THz pulses in a time-domain spectroscopy (TDS) setup and tested on bulk nonlinear crystals. These results establish a new promising candidate to extend the possibilities for compact, broadband THz TDS systems driven by high repetition rate lasers.

physics.optics↗

arXiv2022

Photoinduced structural dynamics of multiferroic TbMnO$_3$

We use time-resolved hard x-ray diffraction to investigate the structural dynamics of the multiferroic insulator TbMnO$_3$ in the low temperature antiferromagnetic and ferroelectrically ordered phase. The lattice response following photoexcitation at 1.55 eV is detected by measuring the (0 2 4) and (1 3 -5) Bragg reflections. A 0.02% tensile strain, normal to the surface, is seen to arise within 20 - 30 ps. The magnitude of this transient strain is over an order of magnitude lower than that predicted from laser-induced heating, which we attribute to a bottleneck in the energy transfer between the electronic and lattice subsystems. The timescale for the transient expansion is consistent with that of previously reported demagnetization dynamics. We discuss a possible relationship between structural and demagnetization dynamics in TbMnO$_3$, in which photoinduced atomic motion modulates the exchange interaction, leading to a destruction of the magnetic order in the system.

cond-mat.str-el↗

arXiv2021

Evidence of a hidden flux phase in the topological kagome metal CsV$_3$Sb$_5$

Phase transitions governed by spontaneous time reversal symmetry breaking (TRSB) have long been sought in many quantum systems, including materials with anomalous Hall effect (AHE), cuprate high temperature superconductors, Iridates and so on. However, experimentally identifying such a phase transition is extremely challenging because the transition is hidden from many experimental probes. Here, using zero-field muon spin relaxation (ZF-$μ$SR) technique, we observe strong TRSB signals below 70 K in the newly discovered kagome superconductor CsV$_3$Sb$_5$. The TRSB state emerges from the 2 x 2 charge density wave (CDW) phase present below ~ 95 K. By carrying out optical second-harmonic generation (SHG) experiments, we also find that inversion symmetry is maintained in the temperature range of interest. Combining all the experimental results and symmetry constraints, we conclude that the interlayer coupled chiral flux phase (CFP) is the most promising candidate for the TRSB state among all theoretical proposals of orbital current orders. Thus, this prototypical kagome metal CsV3Sb5 can be a platform to establish a TRSB current-ordered state and explore its relationship with CDW, giant AHE, and superconductivity.

cond-mat.supr-con↗

arXiv2020

Comparison of coherent phonon generation by electronic and ionic Raman scattering in LaAlO$_3$

In ionic Raman scattering, infrared-active phonons mediate a scattering process that results in the creation or destruction of a Raman-active phonon. This mechanism relies on nonlinear interactions between phonons and has in recent years been associated with a variety of emergent lattice-driven phenomena in complex transition-metal oxides, but the underlying mechanism is often obscured by the presence of multiple coupled order parameters in play. Here, we use time-resolved spectroscopy to compare coherent phonons generated by ionic Raman scattering with those created by more conventional electronic Raman scattering on the nonmagnetic and non-strongly-correlated wide band-gap insulator LaAlO$_3$. We find that the oscillatory amplitude of the low-frequency Raman-active $E_g$ mode exhibits a sharp peak when we tune our pump frequency into resonance with the high-frequency infrared-active $E_u$ mode, consistent with first-principles calculations. Our results suggest that ionic Raman scattering can strongly dominate electronic Raman scattering in wide band-gap insulating materials. We also see evidence of competing scattering channels at fluences above 28~mJ/cm$^2$ that alter the measured amplitude of the coherent phonon response.

cond-mat.mtrl-sci↗

arXiv2020

Ultrafast modulation of covalency in GeTe driven by a ferroelectric soft mode

The general idea of using ultrashort light pulses to control ferroic order parameters has recently attracted attention as a means to achieve control over material properties on unprecedented time scales. Much of the challenge in such work is in understanding the mechanisms by which this control can be achieved, and in particular how observables can be connected to structural and electronic properties. Here we report on a combination of experimental and computational methods to study the electronic structure of the semiconducting ferroelectric GeTe when driven out of equilibrium by absorption of a femtosecond pulse of light. We observe coherent modulations of second harmonic generations on the order of 50%, which we attribute to a combination of atomic and electronic structure changes due to a coherently excited soft mode. Comparison of the observed experimental data with model calculations indicates that this effect is predominantly due to an ultrafast modulation of the covalency of the bonding between Ge and Te ions. This stands in contrast to previously held assumptions in other systems, indicating that care should be exercised in using indirect measurements of electronic structure to make strong conclusions about the magnitude of nuclear motions.

cond-mat.str-el↗

arXiv2020

Structurally assisted melting of excitonic correlations in 1T-TiSe2

The simultaneous condensation of electronic and structural degrees of freedom gives rise to new states of matter, including superconductivity and charge-density-wave formation. When exciting such a condensed system, it is commonly assumed that the ultrafast laser pulse disturbs primarily the electronic order, which in turn destabilizes the atomic structure. Contrary to this conception, we show here that structural destabilization of few atoms causes melting of the macroscopic ordered charge-density wave in 1T-TiSe2. Using ultrafast pump-probe non-resonant and resonant X-ray diffraction, we observe full suppression of the Se 4p orbital order and the atomic structure at excitation energies more than one order of magnitude below the suggested excitonic binding energy. Complete melting of the charge-density wave occurs 4-5 times faster than expected from a purely electronic charge-screening process, strongly suggesting a structurally assisted breakup of excitonic correlations. Our experimental data clarifies several questions on the intricate coupling between structural and electronic order in stabilizing the charge-density-wave in 1T-TiSe2. The results further show that electron-phonon-coupling can lead to different, energy dependent phase-transition pathways in condensed matter systems, opening new possibilities in the conception of non-equilibrium phenomena at the ultrafast scale.

cond-mat.str-el↗