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Meredith Henstridge

Publications and source records attributed to Meredith Henstridge.

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Dynamically suppressed lattice rotations in SrTiO$_3$ as a basis for photo-induced ferroelectricity

Photo-induced ferroelectricity in the quantum paraelectric SrTiO$_3$ involves the dynamical interplay between a coherently driven Ti-O stretching vibration and multiple structural degrees of freedom, including antiferrodistortive rotations, strain, and the polar mode instability. In the high-temperature cubic phase, in the absence of average antiferrodistortion, time-resolved X-ray diffuse scattering has evidenced a correlation between a photo-induced reduction in antiferrodistortive fluctuations and the emergence of ferroelectric order. Here, we complement these measurements with time-resolved elastic X-ray diffraction in the low-temperature tetragonal phase, in which antiferrodistortive fluctuations are small but a finite average rotation has set in. In this phase, we observe a long-lived reduction of the equilibrium antiferrodistortive rotation angle. A unified theory of the nonlinear lattice dynamics based on first-principles calculations describes the dynamics in both high-temperature cubic and low-temperature tetragonal phases, providing a basis for light-induced ferroelectricity in SrTiO$_3$.

cond-mat.mtrl-sci

Nonresonant Raman control of ferroelectric polarization

Important advances have recently been made in the search for materials with complex multi-phase landscapes that host photoinduced metastable collective states with exotic functionalities. In almost all cases so far, the desired phases are accessed by exploiting light-matter interactions via the imaginary part of the dielectric function through above-bandgap or resonant mode excitation. Nonresonant Raman excitation of coherent modes has been experimentally observed and proposed for dynamic material control, but the resulting atomic excursion has been limited to perturbative levels. Here, this challenge is overcome by employing nonresonant ultrashort pulses with low photon energies well below the bandgap. Using mid-infrared pulses, ferroelectric reversal is induced in lithium niobate, and the large-amplitude mode displacements are characterized through femtosecond stimulated Raman scattering and second harmonic generation. This approach, validated by first-principle calculations, defines a novel method for synthesizing hidden phases with unique functional properties and manipulating complex energy landscapes at reduced energy consumption and ultrafast speeds.

physics.optics

Nonlocal nonlinear phononics

Nonlinear phononics relies on the resonant optical excitation of infrared-active lattice vibrations to coherently induce targeted structural deformations in solids. This form of dynamical crystal-structure design has been applied to control the functional properties of many interesting systems, including magneto-resistive manganites, magnetic materials, superconductors, and ferroelectrics. However, phononics has so far been restricted to protocols in which structural deformations occur locally within the optically excited volume, sometimes resulting in unwanted heating. Here, we extend nonlinear phononics to propagating polaritons, effectively separating in space the optical drive from the functional response. Mid-infrared optical pulses are used to resonantly drive an 18 THz phonon at the surface of ferroelectric LiNbO3. A time-resolved stimulated Raman scattering probe reveals that the ferroelectric polarization is reduced over the entire 50 micron depth of the sample, far beyond the ~ micron depth of the evanescent phonon field. We attribute the bulk response of the ferroelectric polarization to the excitation of a propagating 2.5 THz soft-mode phonon-polariton. For the highest excitation amplitudes, we reach a regime in which the polarization is reversed. In this this non-perturbative regime, we expect that the polariton model evolves into that of a solitonic domain wall that propagates from the surface into the materials at near the speed of light.

physics.app-ph

Accelerating Light with Metasurfaces

It has been recently shown that especially engineered light beams have the remarkable ability to propagate along curved trajectories in vacuum. Current methods for generating accelerating beams use phase modulators and lenses leading to length scales on the order of tens of centimeters or larger. This poses constraints and severely limits their applicability inside materials. Here, we accelerate light inside glass using a metasurface consisting of plasmonic nanoantennas. Highly-bending beams with radii of curvature on the order of a hundred microns were generated, and the imaged intensities agree well with theory. Our approach for generating accelerating beams allows for their integration into on-chip photonic systems.

physics.optics

Terahertz Spectrometer of Wavelength Dimensions Based on Extraordinary Transmission

Subwavelength-slotted parallel plate waveguides exhibit a localized electromagnetic resonance bound to the slits at a frequency slightly below the transverse electric cutoff [R. Merlin, Phys. Rev. X 2, 031015 (2012)]. The resonance is long-lived and, as opposed to the vanishingly small transmission shown by a single sub-wavelength aperture, it gives perfect transmission for perfectly-conducting plates. We show that the aperture-supported resonances of a pair of slotted copper plates have long lifetimes at THz frequencies. Finite element method calculations show that these bound resonances can have quality factors greater than 100. Effects of plate length and imperfect parallel alignment are also discussed. Using THz time domain spectroscopy, we measured the transmission of a broadband pulse through a test structure for several plate separations. These results suggest that the slotted waveguide can function as a highly compact THz spectrometer.

physics.optics