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Ultrashort x-ray pulses can be used to disentangle magnetic and structural dynamics and are accordingly utilized here to study the photoexcitation of NdNiO3 (NNO), a model nickelate exhibiting structural and magnetic dynamics that conspire to induce an insulator-to-metal transition (IMT). During the course of the photoinduced IMT with above-gap excitation, we observe an ultrafast (<180 fs) quenching of magnetic order followed by a time delayed collapse of the insulating phase probed by x-ray absorption and THz transmission (450 fs) that correlates with the slowest optical phonon mode involved in the structural transition. A simultaneous order-disorder response at the Ni site and displacive response at the Nd site coexist in the ultrafast magnetic response. Crucially, we observe the optical phonon through its coherent coupling with Nd magnetic order, demonstrating that the magnetic and structural degrees of freedom both contribute in driving the IMT. Density functional theory calculations reveal a consistent scenario where optically driven intersite charge transfer drives a collapse of antiferromagnetic order that in turn destabilizes the charge-ordered phase resulting in an IMT. These experiments provide different modalities for the control of electronic phase transitions in quantum materials based on the ultrafast interplay between structural and magnetic orders created by femtosecond photoexcitation. © 2022 American Physical Society.

We present a detailed analysis of the conditions that result in unity absorption in metamaterial absorbers to guide the design and optimization of this important class of functional electromagnetic composites. Multilayer absorbers consisting of a metamaterial layer, dielectric spacer, and ground plane are specifically considered. Using interference theory, the dielectric spacer thickness and resonant frequency for unity absorption can be numerically determined from the functional dependence of the relative phase shift of the total reflection. Further, using transmission line theory in combination with interference theory we obtain analytical expressions for the unity absorption resonance frequency and corresponding spacer layer thickness in terms of the bare resonant frequency of the metamaterial layer and metallic and dielectric losses within the absorber structure. These simple expressions reveal a redshift of the unity absorption frequency with increasing loss that, in turn, necessitates an increase in the thickness of the dielectric spacer. The results of our analysis are experimentally confirmed by performing reflection-based terahertz time-domain spectroscopy on fabricated absorber structures covering a range of dielectric spacer thicknesses with careful control of the loss accomplished through water absorption in a semiporous polyimide dielectric spacer. Our findings can be widely applied to guide the design and optimization of the metamaterial absorbers and sensors. © 2018 American Physical Society.

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 (l /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., IST/Imaging Science and Technology, Applied Sciences