Large Exchange Coupling Between Localized Spins and Topological Bands in MnBi2 Te4.

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 MnBi2 Te4 , 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. 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.

Interlayer magnetophononic coupling in MnBi2Te4.

The emergence of magnetism in quantum materials creates a platform to realize spin-based applications in spintronics, magnetic memory, and quantum information science. A key to unlocking new functionalities in these materials is the discovery of tunable coupling between spins and other microscopic degrees of freedom. We present evidence for interlayer magnetophononic coupling in the layered magnetic topological insulator MnBi2Te4. Employing magneto-Raman spectroscopy, we observe anomalies in phonon scattering intensities across magnetic field-driven phase transitions, despite the absence of discernible static structural changes. This behavior is a consequence of a magnetophononic wave-mixing process that allows for the excitation of zone-boundary phonons that are otherwise 'forbidden' by momentum conservation. Our microscopic model based on density functional theory calculations reveals that this phenomenon can be attributed to phonons modulating the interlayer exchange coupling. Moreover, signatures of magnetophononic coupling are also observed in the time domain through the ultrafast excitation and detection of coherent phonons across magnetic transitions. In light of the intimate connection between magnetism and topology in MnBi2Te4, the magnetophononic coupling represents an important step towards coherent on-demand manipulation of magnetic topological phases.

Nanotextured Dynamics of a Light-Induced Phase Transition in VO2.

We investigate transient nanotextured heterogeneity in vanadium dioxide (VO2) thin films during a light-induced insulator-to-metal transition (IMT). Time-resolved scanning near-field optical microscopy (Tr-SNOM) is used to study VO2 across a wide parameter space of infrared frequencies, picosecond time scales, and elevated steady-state temperatures with nanoscale spatial resolution. Room temperature, steady-state, phonon enhanced nano-optical contrast reveals preexisting "hidden" disorder. The observed contrast is associated with inequivalent twin domain structures. Upon thermal or optical initiation of the IMT, coexisting metallic and insulating regions are observed. Correlations between the transient and steady-state nano-optical textures reveal that heterogeneous nucleation is partially anchored to twin domain interfaces and grain boundaries. Ultrafast nanoscopic dynamics enable quantification of the growth rate and bound the nucleation rate. Finally, we deterministically anchor photoinduced nucleation to predefined nanoscopic regions by locally enhancing the electric field of pump radiation using nanoantennas and monitor the on-demand emergent metallicity in space and time.

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. Here, we critically assess an experimental approach using near-field imaging to probe HCP in Bi2Sr2CaCu2O8+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.

Femtosecond exciton dynamics in WSe2 optical waveguides.

Van-der Waals (vdW) atomically layered crystals can act as optical waveguides over a broad range of the electromagnetic spectrum ranging from Terahertz to visible. Unlike common Si-based waveguides, vdW semiconductors host strong excitonic resonances that may be controlled using non-thermal stimuli including electrostatic gating and photoexcitation. Here, we utilize waveguide modes to examine photo-induced changes of excitons in the prototypical vdW semiconductor, WSe2, prompted by femtosecond light pulses. Using time-resolved scanning near-field optical microscopy we visualize the electric field profiles of waveguide modes in real space and time and extract the temporal evolution of the optical constants following femtosecond photoexcitation. By monitoring the phase velocity of the waveguide modes, we detect incoherent A-exciton bleaching along with a coherent optical Stark shift in WSe2.

Photoenhanced metastable c-axis electrodynamics in stripe-ordered cuprate La1.885Ba0.115CuO4.

Quantum materials are amenable to nonequilibrium 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 La2-xBaxCuO4 (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 µJ/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 nonthermal collapse of the charge order. The photoinduced signal persists well beyond our measurement window of 300 ps and exhibits signatures of spatial inhomogeneity. The electrodynamic response of this metastable state is consistent with enhanced superconducting fluctuations. Our results reveal that La2-xBaxCuO4 is highly sensitive to nonequilibrium excitation over a wide fluence range, providing an unambiguous example of photoinduced modification of order-parameter competition.

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 La_{0.67}Ca_{0.33}MnO_{3}, optical excitation with a sub-100-fs pulse above 2 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 multistep 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.

Phototunable Dielectric Huygens' Metasurfaces.

Conventional dielectric metasurfaces achieve their properties through geometrical tuning and consequently are static. Although some unique properties are demonstrated, the usefulness for realistic applications is thus inherently limited. Here, control of the resonant eigenmodes supported by Huygens' metasurface (HMS) absorbers through optical excitation is proposed and demonstrated. An intensity transmission modulation depth of 99.93% is demonstrated at 1.03 THz, with an associated phase change of greater than π/2 rad. Coupled mode theory and S-parameter simulations are used to elucidate the mechanism underlying the dynamics of the metasurface and it is found that the tuning is primarily governed by modification of the magnetic dipole-like odd eigenmode, which both lifts the degeneracy, and eliminates critical coupling. The dynamic HMS demonstrates wide tunability and versatility which is not limited to the spectral range demonstrated, offering a new path for reconfigurable metasurface applications.

Analysis of the thickness dependence of metamaterial absorbers at terahertz frequencies.

Metamaterial absorbers typically consist of a metamaterial layer, a dielectric spacer layer, and a metallic ground plane. We have investigated the dependence of the metamaterial absorption maxima on the spacer layer thickness and the reflection coefficient of the metamaterial layer obtained in the absence of the ground plane layer. Specifically, we employ interference theory to obtain an analytical expression for the spacer thickness needed to maximize the absorption at a given frequency. The efficacy of this simple expression is experimentally verified at terahertz frequencies through detailed measurements of the absorption spectra of a series of metamaterials structures with different spacer thicknesses. Using an array of split-ring resonators (SRRs) as the metamaterial layer and SU8 as the spacer material we observe that the absorption peaks redshift as the spacer thickness is increased, in excellent agreement with our analysis. Our findings can be applied to guide metamaterial absorber designs and understand the absorption peak frequency shift of sensors based on metamaterial absorbers.

Nonlinear terahertz devices utilizing semiconducting plasmonic metamaterials.

The development of responsive metamaterials has enabled the realization of compact tunable photonic devices capable of manipulating the amplitude, polarization, wave vector and frequency of light. Integration of semiconductors into the active regions of metallic resonators is a proven approach for creating nonlinear metamaterials through optoelectronic control of the semiconductor carrier density. Metal-free subwavelength resonant semiconductor structures offer an alternative approach to create dynamic metamaterials. We present InAs plasmonic disk arrays as a viable resonant metamaterial at terahertz frequencies. Importantly, InAs plasmonic disks exhibit a strong nonlinear response arising from electric field-induced intervalley scattering, resulting in a reduced carrier mobility thereby damping the plasmonic response. We demonstrate nonlinear perfect absorbers configured as either optical limiters or saturable absorbers, including flexible nonlinear absorbers achieved by transferring the disks to polyimide films. Nonlinear plasmonic metamaterials show potential for use in ultrafast terahertz (THz) optics and for passive protection of sensitive electromagnetic devices.

Voltage-tunable dual-layer terahertz metamaterials.

This paper presents the design, fabrication, and characterization of a real-time voltage-tunable terahertz metamaterial based on microelectromechanical systems and broadside-coupled split-ring resonators. In our metamaterial, the magnetic and electric interactions between the coupled resonators are modulated by a comb-drive actuator, which provides continuous lateral shifting between the coupled resonators by up to 20 µm. For these strongly coupled split-ring resonators, both a symmetric mode and an anti-symmetric mode are observed. With increasing lateral shift, the electromagnetic interactions between the split-ring resonators weaken, resulting in frequency shifting of the resonant modes. Over the entire lateral shift range, the symmetric mode blueshifts by ~60 GHz, and the anti-symmetric mode redshifts by ~50 GHz. The amplitude of the transmission at 1.03 THz is modulated by 74%; moreover, a 180° phase shift is achieved at 1.08 THz. Our tunable metamaterial device has myriad potential applications, including terahertz spatial light modulation, phase modulation, and chemical sensing. Furthermore, the scheme that we have implemented can be scaled to operate at other frequencies, thereby enabling a wide range of distinct applications.

Visualization of guided and leaky wave behaviors in an indium tin oxide metallic slab waveguide.

We explored the use of the optically transparent semiconductor indium tin oxide (ITO) as an alternative to optically opaque metals for the fabrication of photonic structures in terahertz (THz) near-field studies. Using the polaritonics platform, we confirmed the ability to clearly image both bound and leaky electric fields underneath an ITO layer. We observed good agreement between measured waveguide dispersion and analytical theory of an asymmetric metal-clad planar waveguide with TE and TM polarizations. Further characterization of the ITO revealed that even moderately conductive samples provided sufficiently high quality factors for studying guided and leaky wave behaviors in individual transparent THz resonant structures such as antennas or split ring resonators. However, without higher conductive ITO, the limited reflection efficiency and high radiation damping measured here both diminish the applicability of ITO for high-reflecting, arrayed, or long path-length elements.

Ultrafast dynamics of surface plasmons in InAs by time-resolved infrared nanospectroscopy.

We report on time-resolved mid-infrared (mid-IR) near-field spectroscopy of the narrow bandgap semiconductor InAs. The dominant effect we observed pertains to the dynamics of photoexcited carriers and associated surface plasmons. A novel combination of pump-probe techniques and near-field nanospectroscopy accesses high momentum plasmons and demonstrates efficient, subpicosecond photomodulation of the surface plasmon dispersion with subsequent tens of picoseconds decay under ambient conditions. The photoinduced change of the probe intensity due to plasmons in InAs is found to exceed that of other mid-IR or near-IR media by 1-2 orders of magnitude. Remarkably, the required control pulse fluence is as low as 60 µJ/cm(2), much smaller than fluences of ∼ 1-10 mJ/cm(2) previously utilized in ultrafast control of near-IR plasmonics. These low excitation densities are easily attained with a standard 1.56 µm fiber laser. Thus, InAs--a common semiconductor with favorable plasmonic properties such as a low effective mass--has the potential to become an important building block of optically controlled plasmonic devices operating at infrared frequencies.

Nonlinear terahertz metamaterials via field-enhanced carrier dynamics in GaAs.

We demonstrate nonlinear metamaterial split ring resonators (SRRs) on GaAs at terahertz frequencies. For SRRs on doped GaAs films, incident terahertz radiation with peak fields of ~20-160 kV/cm drives intervalley scattering. This reduces the carrier mobility and enhances the SRR LC response due to a conductivity decrease in the doped thin film. Above ~160 kV/cm, electric field enhancement within the SRR gaps leads to efficient impact ionization, increasing the carrier density and the conductivity which, in turn, suppresses the SRR resonance. We demonstrate an increase of up to 10 orders of magnitude in the carrier density in the SRR gaps on semi-insulating GaAs. Furthermore, we show that the effective permittivity can be swept from negative to positive values with an increasing terahertz field strength in the impact ionization regime, enabling new possibilities for nonlinear metamaterials.

Terahertz-field-induced insulator-to-metal transition in vanadium dioxide metamaterial.

Electron-electron interactions can render an otherwise conducting material insulating, with the insulator-metal phase transition in correlated-electron materials being the canonical macroscopic manifestation of the competition between charge-carrier itinerancy and localization. The transition can arise from underlying microscopic interactions among the charge, lattice, orbital and spin degrees of freedom, the complexity of which leads to multiple phase-transition pathways. For example, in many transition metal oxides, the insulator-metal transition has been achieved with external stimuli, including temperature, light, electric field, mechanical strain or magnetic field. Vanadium dioxide is particularly intriguing because both the lattice and on-site Coulomb repulsion contribute to the insulator-to-metal transition at 340 K (ref. 8). Thus, although the precise microscopic origin of the phase transition remains elusive, vanadium dioxide serves as a testbed for correlated-electron phase-transition dynamics. Here we report the observation of an insulator-metal transition in vanadium dioxide induced by a terahertz electric field. This is achieved using metamaterial-enhanced picosecond, high-field terahertz pulses to reduce the Coulomb-induced potential barrier for carrier transport. A nonlinear metamaterial response is observed through the phase transition, demonstrating that high-field terahertz pulses provide alternative pathways to induce collective electronic and structural rearrangements. The metamaterial resonators play a dual role, providing sub-wavelength field enhancement that locally drives the nonlinear response, and global sensitivity to the local changes, thereby enabling macroscopic observation of the dynamics. This methodology provides a powerful platform to investigate low-energy dynamics in condensed matter and, further, demonstrates that integration of metamaterials with complex matter is a viable pathway to realize functional nonlinear electromagnetic composites.

THz near-field Faraday imaging in hybrid metamaterials.

We report on direct measurements of the magnetic near-field of metamaterial split ring resonators at terahertz frequencies using a magnetic field sensitive material. Specifically, planar split ring resonators are fabricated on a single magneto-optically active terbium gallium garnet crystal. Normally incident terahertz radiation couples to the resonator inducing a magnetic dipole oscillating perpendicular to the crystal surface. Faraday rotation of the polarisation of a near-infrared probe beam directly measures the magnetic near-field with 100 femtosecond temporal resolution and (λ/200) spatial resolution. Numerical simulations suggest that the magnetic field can be enhanced in the plane of the resonator by as much as a factor of 200 compared to the incident field strength. Our results provide a route towards hybrid devices for dynamic magneto-active control of light such as isolators, and highlight the utility of split ring resonators as compact probes of magnetic phenomena in condensed matter.

Time-resolved imaging of near-fields in THz antennas and direct quantitative measurement of field enhancements.

We investigate the interaction between terahertz waves and resonant antennas with sub-cycle temporal and λ/100 spatial resolution. Depositing antennas on a LiNbO3 waveguide enables non-invasive electro-optic imaging, quantitative field characterization, and direct measurement of field enhancement (up to 40-fold). The spectral response is determined over a bandwidth spanning from DC across multiple resonances, and distinct behavior is observed in the near- and far-field. The scaling of enhancement and resonant frequency with gap size and antenna length agrees well with simulations.

Flexible metamaterial absorbers for stealth applications at terahertz frequencies.

We have wrapped metallic cylinders with strongly absorbing metamaterials. These resonant structures, which are patterned on flexible substrates, smoothly coat the cylinder and give it an electromagnetic response designed to minimize its radar cross section. We compare the normal-incidence, small-beam reflection coefficient with the measurement of the far-field bistatic radar cross section of the sample, using a quasi-planar THz wave with a beam diameter significantly larger than the sample dimensions. In this geometry we demonstrate a near-400-fold reduction of the radar cross section at the design frequency of 0.87 THz. In addition we discuss the effect of finite sample dimensions and the spatial dependence of the reflection spectrum of the metamaterial.

Silk-based conformal, adhesive, edible food sensors.

An array of passive metamaterial antennas fabricated on all protein-based silk substrates were conformally transferred and adhered to the surface of an apple. This process allows the opportunity for intimate contact of micro- and nanostructures that can probe, and accordingly monitor changes in, their surrounding environment. This provides in situ monitoring of food quality. It is to be noted that this type of sensor consists of all edible and biodegradable components, holding utility and potential relevance for healthcare and food/consumer products and markets.