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Averitt, Richard D.

Publications and source records attributed to Averitt, Richard D..

Photonic time-crystalline behaviour mediated by phonon squeezing in T a 2 NiSe 5

Photonic time crystals refer to materials whose dielectric properties are periodic in time, analogous to a photonic crystal whose dielectric properties is periodic in space. Here, we theoretically investigate photonic time-crystalline behaviour initiated by optical excitation above the electronic gap of the excitonic insulator candidate Ta 2 NiSe 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 terahertz (THz) amplification of reflectivity in a narrow frequency band. The theory is supported by experimental results on Ta 2 NiSe 5 where photoexcitation with short pulses leads to enhanced THz reflectivity with the predicted features. We explain the key mechanism leading to THz amplification in terms of a simplified electron-phonon Hamiltonian motivated by ab-initio DFT calculations. Our theory suggests that the pumped Ta 2 NiSe 5 is a gain medium, demonstrating that squeezed phonon noise may be used to create THz amplifiers in THz communication applications.

36 MATERIALS SCIENCE↗

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

There is significant technological interest in developing ever faster switching between different electronic and magnetic states of matter. Manipulating properties at terahertz rates requires accessing the intrinsic timescales of both electrons and associated phonons, which is possible with short-pulse photoexcitation. However, 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 timescales dominated by slowly coarsening dynamics. Here, in this study, we use time-resolved X-ray diffraction and reflectivity measurements to show that the photoinduced insulator-to-metal transition in an epitaxially strained Mott insulating thin film 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, which is followed by a slower electronic evolution into a metastable nonequilibrium state. Microscopic model calculations based on time-dependent dynamical mean-field theory and semiclassical lattice dynamics explain the threshold behaviour and elucidate the delayed onset of the electronic phase transition. This work highlights the importance of combined electronic and structural studies in unravelling the physics of dynamic transitions and the timescales of photoinduced processes. During a photoinduced phase transition, electronic rearrangements are usually faster than lattice ones. Time-resolved measurements now show that the insulator-to-metal transition in a thin-film Mott insulator is preceded by lattice reconfiguration.

36 MATERIALS SCIENCE↗

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. In conclusion, our results highlight that coherent dynamics can drive parametric stimulated emission with concomitant possibilities, including entangled THz photon generation.

36 MATERIALS SCIENCE↗

Large Exchange Coupling Between Localized Spins and Topological Bands in MnBi 2 Te 4

Magnetism in topological materials creates phases exhibiting quantized transport phenomena with potential technological applications. The emergence of such phases relies on strong interaction between localized spins and the topological bands, and the consequent formation of an exchange gap. However, this remains experimentally unquantified in intrinsic magnetic topological materials. Here, this interaction is quantified in MnBi 2 Te 4 , a topological insulator with intrinsic antiferromagnetism. This is achieved by optically exciting Bi-Te p states comprising the bulk topological bands and interrogating the consequent Mn 3d spin dynamics, using a multimodal ultrafast approach. Ultrafast electron scattering and magneto-optic measurements show that the p states demagnetize via electron-phonon scattering at picosecond timescales. Despite being energetically decoupled from the optical excitation, the Mn 3d spins, probed by resonant X-ray scattering, are observed to disorder concurrently with the p spins. Together with atomistic simulations, this reveals that the exchange coupling between localized spins and the topological bands is at least 100 times larger than the superexchange interaction, implying an optimal exchange gap of at least 25 meV in the surface states. Here, by quantifying this exchange coupling, this study validates the materials-by-design strategy of utilizing localized magnetic order to manipulate topological phases, spanning static to ultrafast timescales.

36 MATERIALS SCIENCE↗

Active and tunable nanophotonic metamaterials

Abstract Metamaterials enable subwavelength tailoring of light–matter interactions, driving fundamental discoveries which fuel novel applications in areas ranging from compressed sensing to quantum engineering. Importantly, the metallic and dielectric resonators from which static metamaterials are comprised present an open architecture amenable to materials integration. Thus, incorporating responsive materials such as semiconductors, liquid crystals, phase-change materials, or quantum materials (e.g., superconductors, 2D materials, etc.) imbue metamaterials with dynamic properties, facilitating the development of active and tunable devices harboring enhanced or even entirely novel electromagnetic functionality. Ultimately, active control derives from the ability to craft the local electromagnetic fields; accomplished using a host of external stimuli to modify the electronic or optical properties of the responsive materials embedded into the active regions of the subwavelength resonators. We provide a broad overview of this frontier area of metamaterials research, introducing fundamental concepts and presenting control strategies that include electronic, optical, mechanical, thermal, and magnetic stimuli. The examples presented range from microwave to visible wavelengths, utilizing a wide range of materials to realize spatial light modulators, effective nonlinear media, on-demand optics, and polarimetric imaging as but a few examples. Often, active and tunable nanophotonic metamaterials yield an emergent electromagnetic response that is more than the sum of the parts, providing reconfigurable or real-time control of the amplitude, phase, wavevector, polarization, and frequency of light. The examples to date are impressive, setting the stage for future advances that are likely to impact holography, beyond 5G communications, imaging, and quantum sensing and transduction.

36 MATERIALS SCIENCE↗

Structural tuning of 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 arrangement 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 the 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 and metasurfaces 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.

36 MATERIALS SCIENCE↗

Hyperbolic Cooper-Pair Polaritons in Planar Graphene/Cuprate Plasmonic Cavities

Hyperbolic Cooper-pair polaritons (HCP) in cuprate superconductors are of fundamental interest due to their potential for providing insights into the nature of unconventional superconductivity. In this study, we critically assess an experimental approach using near-field imaging to probe HCP in Bi 2 Sr 2 CaCu 2 O 8+x (Bi-2212) in the presence of graphene surface plasmon polaritons (SPP). Our simulations show that inherently weak HCP features in the near-field can be strongly enhanced when coupled to graphene SPP in layered graphene/hexagonal boron nitride (hBN)/Bi-2212 heterostructures. This enhancement arises from our multilayered structures effectively acting as plasmonic cavities capable of altering collective modes of a layered superconductor by modifying its electromagnetic environment. The degree of enhancement can be selectively controlled by tuning the insulating spacer thickness with atomic precision. Finally, we verify the expected renormalization of room-temperature graphene SPP using near-field infrared imaging. Our modeling, augmented with data, attests to the validity of our approach for probing HCP modes in cuprate superconductors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗