arXiv subjects

Richard D. Averitt

Publications and source records attributed to Richard D. Averitt.

At least 19 recordsLinked to original sources

arXiv2025

Subgap pumping of antiferromagnetic Mott insulators: photoexcitation mechanisms and applications

We study the behavior of the 2D repulsive Hubbard model on a square lattice at half filling, under strong driving with ac electric fields, by employing a time-dependent Gaussian variational approach. Within the same theoretical framework, we analytically obtain the conventional Keldysh crossover between multiphoton and tunneling photoexcitation mechanisms, as well as two new regimes beyond the Keldysh paradigm. We discuss how dynamical renormalization of the Mott-Hubbard gap feeds back into the photoexcitation process, modulating the carrier generation rate in real time. The momentum distribution of quasiparticle excitations immediately after the drive is calculated, and shown to contain valuable information about the generation mechanism. Finally, we discuss experimental probing of the pump-induced nonequilibrium electronic state.

cond-mat.str-el↗

arXiv2024

Nonresonant nonlinear magnonics in an antiferromagnet

Antiferromagnets exhibit rapid spin dynamics in a net zero magnetic background which enables novel spintronic applications and interrogation of many-body quantum phenomena. The layered antiferromagnet Sr$_2$IrO$_4$ hosts an exotic spin one-half Mott insulating state with an electronic gap arising from on-site Coulomb repulsion and strong spin-orbit coupling. This makes Sr$_2$IrO$_4$ an interesting candidate to interrogate dynamical attributes of the magnetic order using ultrafast laser pulses. We investigate the magnetization dynamics of Sr$_2$IrO$_4$ following circularly-polarized photoexcitation with below-gap mid-infrared (mid-IR -- 9 $μm$) and above-gap near-infrared (near-IR -- 1.3 $μm$) pulses. In both cases, we observe excitation of a zone-center coherent magnon mode featuring a 0.5 THz oscillation in the pump-induced Kerr-rotation signal. However, only below-gap excitation exhibits a helicity dependent response and linear (quadratic) scaling of the coherent magnon amplitude with excitation fluence (electric field). Moreover, below-gap excitation has a magnon generation efficiency that is at least two orders of magnitude greater in comparison to above-gap excitation. Our analysis indicates that the helicity dependence and enhanced generation efficiency arises from a unique one-photon two-magnon coupling mechanism for magnon generation. Thus, preferential spin-photon coupling without photoexcitation of electrons permits extremely efficient magnon generation. Our results reveal new possibilities for ultrafast control of antiferromagnets.

cond-mat.str-el↗

arXiv2024

Terahertz Metamaterial Renormalization of Superconducting Josephson Plasmons in La$_{1.85}$Sr$_{0.15}$CuO$_4$

We investigate light-matter coupling in the cuprate superconductor La$_{1.85}$Sr$_{0.15}$Cu0$_4$ (LSCO), accomplished by adhering metamaterial resonator arrays (MRAs) to a c-axis oriented single crystal. The resonators couple to the Josephson Plasma Mode (JPM) which manifests as a plasma edge in the terahertz reflectivity in the superconducting state. Terahertz reflectivity measurements at 10K reveal a renormalization of the JPM frequency, $ω_{jpm}$, from 1.7 THz for the bare crystal to $\sim$1 THz with the MRAs. With increasing temperature, the modified $ω_{jpm}$ redshifts as expected for decreasing superfluid density, vanishing above T$_{c}$. The modification of the electrodynamic response arises from resonator induced screening of the longitudinal polariton response, reminiscent of plasmon-phonon coupling in doped semiconductors. Modeling reveals that the electrodynamic response is fully interpretable using classical electromagnetism. Future studies will have to contend with the large effects we observe which could obscure subtle changes that may indicate cavity-based manipulation of superconductivity. Finally, we note that our MRA/LSCO structure is a tunable epsilon-near-zero (ENZ) metamaterial that exhibits a nonlinear response arising from the c-axis Josephson tunneling coupled with the local fields of the resonators.

cond-mat.supr-con↗

arXiv2023

Theory of time-crystalline behaviour mediated by phonon squeezing in Ta2NiSe5

We theoretically investigate photonic time-crystalline behaviour initiated by optical excitation above the electronic gap of the excitonic insulator candidate $\rm{Ta_2 Ni Se_5}$. We show that after electron photoexcitation, electron-phonon coupling leads to an unconventional squeezed phonon state, characterised by periodic oscillations of phonon fluctuations. Squeezing oscillations lead to photonic time crystalline behaviour. The key signature of the photonic time crystalline behaviour is THz amplification of reflectivity in a narrow frequency band. The theory is supported by experimental results on $\rm{Ta_2 Ni Se_5}$ where photoexcitation with short pulses leads to enhanced terahertz reflectivity with the predicted features. We explain the key mechanism leading to THz amplification in terms of a simplified Hamiltonian whose validity is supported by ab-initio DFT calculations. Our theory suggests that the pumped $\rm{Ta_2 Ni Se_5}$ is a gain medium, demonstrating that squeezed phonon noise may be used to create THz amplifiers in THz communication applications.

cond-mat.str-el↗

arXiv2023

Terahertz parametric amplification as a reporter of exciton condensate dynamics

Condensates are a hallmark of emergence in quantum materials with superconductors and charge density wave as prominent examples. An excitonic insulator (EI) is an intriguing addition to this library, exhibiting spontaneous condensation of electron-hole pairs. However, condensate observables can be obscured through parasitic coupling to the lattice. Time-resolved terahertz (THz) spectroscopy can disentangle such obscurants through measurement of the quantum dynamics. We target $Ta_{2}NiSe_{5}$, a putative room-temperature EI where electron-lattice coupling dominates the structural transition ($T_{c}$=326 K), hindering identification of excitonic correlations. A pronounced increase in the THz reflectivity manifests following photoexcitation and exhibits a BEC-like temperature dependence. This occurs well below the $T_{c}$, suggesting a novel approach to monitor exciton condensate dynamics. Nonetheless, dynamic condensate-phonon coupling remains as evidenced by peaks in the enhanced reflectivity spectrum at select infrared-active phonon frequencies. This indicates that parametric reflectivity enhancement arises from phonon squeezing, validated using Fresnel-Floquet theory and density functional calculations. Our results highlight that coherent dynamics can drive parametric stimulated emission with concomitant possibilities, including entangled THz photon generation.

cond-mat.str-el↗

arXiv2023

Picosecond volume expansion drives a later-time insulator-metal transition in a nano-textured Mott Insulator

Technology moves towards ever faster switching between different electronic and magnetic states of matter. Manipulating properties at terahertz rates requires accessing the intrinsic timescales of electrons (femtoseconds) and associated phonons (10s of femtoseconds to few picoseconds), which is possible with short-pulse photoexcitation. Yet, in many Mott insulators, the electronic transition is accompanied by the nucleation and growth of percolating domains of the changed lattice structure, leading to empirical time scales dominated by slow coarsening dynamics. Here, we use time-resolved X-ray diffraction and reflectivity measurements to investigate the photoinduced insulator-to-metal transition in an epitaxially strained thin film Mott insulator Ca2RuO4. The dynamical transition occurs without observable domain formation and coarsening effects, allowing the study of the intrinsic electronic and lattice dynamics. Above a fluence threshold, the initial electronic excitation drives a fast lattice rearrangement, followed by a slower electronic evolution into a metastable non-equilibrium state. Microscopic calculations based on time-dependent dynamical mean-field theory and semiclassical lattice dynamics within a recently published equilibrium energy landscape picture explain the threshold-behavior and elucidate the delayed onset of the electronic phase transition in terms of kinematic constraints on recombination. Analysis of satellite scattering peaks indicates the persistence of a strain-induced nano-texture in the photoexcited film. This work highlights the importance of combined electronic and structural studies to unravel the physics of dynamic transitions and elucidates the role of strain in tuning the timescales of photoinduced processes.

cond-mat.str-el↗

arXiv2023

Terahertz third harmonic generation in c-axis La$_{1.85}$Sr$_{0.15}$CuO$_4$

Terahertz nonlinear optics is a viable method to interrogate collective phenomena in quantum materials spanning ferroelectrics, charge-density waves, and superconductivity. In superconductors this includes the Higgs amplitude and Josephson phase modes. We have investigated the nonlinear c-axis response of optimally doped La$_{1.85}$Sr$_{0.15}$CuO$_4$ using high-field THz time domain spectroscopy (THz-TDS) at field strengths up to $\sim$80 kV/cm. With increasing field, we observe a distinct red-shift of the Josephson plasma edge and enhanced reflectivity (above the plasma edge) arising from third harmonic generation. The non-monotonic temperature dependent response is consistent with nonlinear drive of the Josephson Plasma Mode (JPM) as verified with comparison to theoretical expectations. Our results add to the understanding that, using THz light, the JPM (in addition to the Higgs mode) provides a route to interrogate and control superconducting properties.

cond-mat.supr-con↗

arXiv2023

On-chip time-domain terahertz spectroscopy of superconducting films below the diffraction limit

Free-space time domain THz spectroscopy accesses electrodynamic responses in a frequency regime ideally matched to interacting condensed matter systems. However, THz spectroscopy is challenging when samples are physically smaller than the diffraction limit of ~0.5 mm, as is typical, for example, in van der Waals materials and heterostructures. Here, we present an on-chip, time-domain THz spectrometer based on semiconducting photoconductive switches with a bandwidth of 200 GHz to 750 GHz. We measure the optical conductivity of a 7.5-$μ$m wide NbN film across the superconducting transition, demonstrating spectroscopic signatures of the superconducting gap in a sample smaller than 2% of the Rayleigh diffraction limit. Our spectrometer features an interchangeable sample architecture, making it ideal for probing superconductivity, magnetism, and charge order in strongly correlated van der Waals materials.

cond-mat.supr-con↗

arXiv2022

Complementary Vanadium Dioxide Metamaterials with Enhanced Modulation Amplitude at Terahertz Frequencies

One route to create tunable metamaterials is through integration with "on-demand" dynamic quantum materials, such as vanadium dioxide (VO2). This enables new modalities to create high performance devices for historically challenging applications. Indeed, dynamic materials have often been integrated with metamaterials to imbue artificial structures with some degree of tunability. Conversely, metamaterials can be used to enhance and extend the natural tuning range of dynamic materials. Utilizing a complementary split ring resonator array deposited on a VO2 film, we demonstrate enhanced terahertz transmission modulation upon traversing the insulator-to-metal transition (IMT) at ~340 K. Our complementary metamaterial increases the modulation amplitude of the original VO2 film from 42% to 68.3% at 0.47 THz upon crossing the IMT, corresponding to an enhancement of 62.4%. Moreover, temperature dependent transmission measurements reveal a redshift of the resonant frequency arising from a giant increase of the permittivity of the VO2 film. Maxwell-Garnett effective medium theory was employed to explain the permittivity change upon transitioning through the IMT. Our results highlight that symbiotic integration of metamaterial arrays with quantum materials provides a powerful approach to engineer emergent functionality.

physics.app-ph↗

arXiv2022

Large Itinerant Electron Exchange Coupling in the Magnetic Topological Insulator MnBi2Te4

Magnetism in topological materials creates phases exhibiting quantized transport phenomena with applications in spintronics and quantum information. The emergence of such phases relies on strong interaction between localized spins and itinerant states comprising the topological bands, and the subsequent formation of an exchange gap. However, this interaction has never been measured in any intrinsic magnetic topological material. Using a multimodal approach, this exchange interaction is measured in MnBi2Te4, the first realized intrinsic magnetic topological insulator. Interrogating nonequilibrium spin dynamics, itinerant bands are found to exhibit a strong exchange coupling to localized Mn spins. Momentum-resolved ultrafast electron scattering and magneto-optic measurements reveal that itinerant spins disorder via electron-phonon scattering at picosecond timescales. Localized Mn spins, probed by resonant X-ray scattering, disorder concurrently with itinerant spins, despite being energetically decoupled from the initial excitation. Modeling the results using atomistic simulations, the exchange coupling between localized and itinerant spins is estimated to be >100 times larger than superexchange interactions. This implies an exchange gap of >25 meV should occur in the topological surface states. By directly quantifying local-itinerant exchange coupling, this work validates the materials-by-design strategy of utilizing localized magnetic order to create and manipulate magnetic topological phases, from static to ultrafast timescales.

cond-mat.mtrl-sci↗

arXiv2021

Generalized Fresnel-Floquet equations for driven quantum materials

Optical drives at terahertz and mid-infrared frequencies in quantum materials are increasingly used to reveal the nonlinear dynamics of collective modes in correlated many-body systems and their interplay with electromagnetic waves. Recent experiments demonstrated several surprising optical properties of transient states induced by driving, including the appearance of photo-induced edges in the reflectivity in cuprate superconductors, observed both below and above the equilibrium transition temperature. Furthermore, in other driven materials, reflection coefficients larger than unity have been observed. In this paper we demonstrate that unusual optical properties of photoexcited systems can be understood from the perspective of a Floquet system; a system with periodically modulated system parameters originating from pump-induced oscillations of a collective mode. We present a general phenomenological model of reflectivity from Floquet materials, which takes into account parametric generation of excitation pairs. We find a universal phase diagram of drive induced features in reflectivity which evidence a competition between driving and dissipation. To illustrate our general analysis we apply our formalism to two concrete examples motivated by recent experiments: a single plasmon band, which describes Josephson plasmons in layered superconductors, and a phonon-polariton system, which describes upper and lower polaritons in materials such as insulating SiC. Finally we demonstrate that our model can be used to provide an accurate fit to results of phonon-pump - terahertz-probe experiments in the high temperature superconductor $\rm{YBa_2Cu_3O_{6.5}}$. Our model explains the appearance of a pump-induced edge, which is higher in energy than the equilibrium Josephson plasmon edge, even if the interlayer Josephson coupling is suppressed by the pump pulse.

cond-mat.str-el↗

arXiv2021

Structurally Tunable Nonlinear Terahertz Metamaterials using Broadside Coupled Split Ring Resonators

We present an experimental and numerical study of a terahertz metamaterial with a nonlinear response that is controllable via the relative structural positioning of two stacked split ring resonator arrays. The first array is fabricated on an n-doped GaAs substrate and the second array is fabricated vertically above the first using a polyimide spacer layer. Due to GaAs carrier dynamics, the on-resonance terahertz transmission at 0.4 THz varies in a nonlinear manner with incident terahertz power. The second resonator layer dampens this nonlinear response. In samples where the two layers are aligned, the resonance disappears and total nonlinear modulation of the on-resonance transmission decreases. The nonlinear modulation is restored in samples where an alignment offset is imposed between the two resonator arrays. Structurally tunable metamaterials can therefore act as a design template for tunable nonlinear THz devices by controlling the coupling of confined electric fields to nonlinear phenomena in a complex material substrate or inclusion.

physics.optics↗

arXiv2020

On-chip terahertz modulation and emission with integrated graphene junctions

The efficient modulation and control of ultrafast signals on-chip is of central importance in terahertz (THz) communications and a promising route toward sub-diffraction limit THz spectroscopy. Two-dimensional (2D) materials may provide a platform for these endeavors. We explore this potential, integrating high-quality graphene p-n junctions within two types of planar transmission line circuits to modulate and emit picosecond pulses. In a coplanar stripline geometry, we demonstrate electrical modulation of THz signal transmission by 95%. In a Goubau waveguide geometry, we achieve complete gate-tunable control over THz emission from a photoexcited graphene junction. These studies inform the development of on-chip signal manipulation and highlight prospects for 2D materials in THz applications.

cond-mat.mes-hall↗

arXiv2019

Dynamics of a Persistent Insulator-to-Metal Transition in Strained Manganite Films

Transition metal oxides possess complex free energy surfaces with competing degrees of freedom. Photoexcitation allows shaping of such rich energy landscapes. In epitaxially strained $\mathrm{La_{0.67}Ca_{0.33}MnO_3}$, optical excitation with a sub-100 fs pulse above $2\ \mathrm{mJ/cm^2}$ leads to a persistent metallic phase below 100 K. Using single-shot optical and terahertz spectroscopy, we show that this phase transition is a multi-step process. We conclude that the phase transition is driven by partial charge order melting, followed by growth of the persistent metallic phase on longer timescales. A time-dependent Ginzburg-Landau model can describe the fast dynamics of the reflectivity, followed by longer timescale in-growth of the metallic phase.

cond-mat.str-el↗

arXiv2019

Nucleation and growth bottleneck in the conductivity recovery dynamics of nickelate thin films

We investigate THz conductivity dynamics in NdNiO$_3$ and EuNiO$_3$ thin films following a photoinduced thermal quench into the metallic state and reveal a clear contrast between first- and second-order dynamics. While in EuNiO$_3$ the conductivity recovers exponentially, in NdNiO$_3$ the recovery is non-exponential and slower than a simple thermal model. Crucially, it is consistent with first-order dynamics and well-described by a 2d Avrami model, with supercooling leading to metastable phase coexistence. The large transients seen in our films are promising for fast electronic (and magnetic) switching applications.

cond-mat.str-el↗

arXiv2019

Photo-enhanced metastable c-axis electrodynamics in stripe ordered cuprate La$_{1.885}$Ba$_{0.115}$CuO$_{4}$

Quantum materials are amenable to non-equilibrium manipulation with light, enabling modification and control of macroscopic properties. Light-based augmentation of superconductivity is particularly intriguing. Copper-oxide superconductors exhibit complex interplay between spin order, charge order and superconductivity, offering the prospect of enhanced coherence by altering the balance between competing orders. We utilize terahertz time domain spectroscopy to monitor the c-axis Josephson Plasma Resonance (JPR) in La$_{2-x}$Ba$_{x}$CuO$_{4}$ (x = 0.115) as a direct probe of superconductivity dynamics following excitation with near infrared pulses. Starting from the superconducting state, c-axis polarized excitation with a fluence of 100 $μ$J/cm2 results in an increase of the far-infrared spectral weight by more than an order of magnitude as evidenced by a blueshift of the JPR, interpreted as resulting from non-thermal collapse of the charge order. The photo-induced signal persists well beyond our measurement window of 300 ps and exhibits signatures of spatial inhomogeneity. The electrodynamic response of this new metastable state is consistent with enhanced superconducting fluctuations. Our results reveal that La$_{2-x}$Ba$_{x}$CuO$_{4}$ is highly sensitive to non-equilibrium excitation over a wide fluence range, providing an unambiguous example of photo-induced modification of order-parameter competition.

cond-mat.supr-con↗

arXiv2019

Quasiparticle Relaxation Dynamics in URu$_{2-x}$Fe$_{x}$Si$_{2}$ Single Crystals

We investigate quasiparticle relaxation dynamics in URu$_{2-x}$Fe$_{x}$Si$_{2}$ single crystals using ultrafast optical-pump optical-probe (OPOP) spectroscopy as a function of temperature ($T$) and Fe substitution ($x$), crossing from the hidden order (HO) phase ($x$ = 0) to the large moment antiferromagnet (LMAFM) phase ($x$ = 0.12). At low $T$, the dynamics for $x$ = 0 and $x$ = 0.12 are consistent with the low energy electronic structure of the HO and LMAFM phases that emerge from the high $T$ paramagnetic (PM) phase. In contrast, for $x$ = 0.1, two transitions occur over a narrow $T$ range (from ~15.5 - 17.5 K). A PM to HO transition occurs at an intermediate $T$ followed by a transition to the LMAFM phase at lower $T$. While the data at low $T$ are consistent with the expected coexistence of LMAFM and HO, the data in the intermediate $T$ phase are not, and instead suggest the possibility of an unexpected coexistence of HO and PM. Additionally, the dynamics in the PM phase reflect the presence of a hybridization gap as well as strongly interacting spin and charge degrees of freedom. OPOP yields insights into meV-scale electrodynamics with sub-Kelvin $T$ resolution, providing a complementary approach to study low energy electronic structure in quantum materials.

cond-mat.str-el↗

arXiv2019

Ultrafast quasiparticle dynamics in correlated semimetal Ca$_3$Ru$_2$O$_7$

The correlated polar semimetal Ca$_3$Ru$_2$O$_7$ exhibits a rich phase diagram including two magnetic transitions ($T_N$=56 K and $T_C$=48 K) with the appearance of an insulating-like pseudogap (at $T_C$). In addition, there is a crossover back to metallic behavior at $T^*$=30 K, the origin of which is still under debate. We utilized ultrafast optical pump optical probe spectroscopy to investigate quasiparticle dynamics as a function of temperature in this enigmatic quantum material. We identify two dynamical processes, both of which are influenced by the onset of the pseudogap. This includes electron-phonon relaxation and, below $T_C$, the onset of a phonon bottleneck hindering the relaxation of quasiparticles across the pseudogap. We introduce a gap-modified two-temperature model to describe the temperature dependence of electron-phonon thermalization, and use the Rothwarf-Taylor to model the phonon bottleneck. In conjunction with density functional theory, our experimental results synergistically reveal the origin of the $T$-dependent pseudogap. Further, our data and analysis indicate that $T^*$ emerges as a natural consequence of $T$-dependent gapping out of carriers, and does not correspond to a separate electronic transition. Our results highlight the value of low fluence ultrafast optics as a sensitive probe of low energy electronic structure, thermodynamic parameters, and transport properties of Ruddlesden-Popper ruthenates.

cond-mat.str-el↗