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At least 73 records · Page 4

Direct Observation of Bandgap Oscillations Induced by Optical Phonons in Hybrid Lead Iodi.de Perovskites

Hybrid organic-inorganic perovskites such as methylammonium lead iodide have emerged as promising semiconductors for energy-relevant applications. The interactions between charge carriers and lattice vibrations, giving rise to polarons, have been invoked to explain some of their extraordinary optoelectronic properties. Here, time-resolved optical spectroscopy is performed, with off-resonant pumping and electronic probing, to examine several representative lead iodide perovskites. The temporal oscillations of electronic bandgaps induced by coherent lattice vibrations are reported, which is attributed to antiphase octahedral rotations that dominate in the examined 3D and 2D hybrid perovskites. The off-resonant pumping scheme permits a simplified observation of changes in the bandgap owing to the A(g) vibrational mode, which is qualitatively different from vibrational modes of other symmetries and without increased complexity of photogenerated electronic charges. The work demonstrates a strong correlation between the lead-iodide octahedral framework and electronic transitions, and provides further insights into the manipulation of coherent optical phonons and related properties in hybrid perovskites on ultrafast timescales.

coherent optical phonons↗

Plasma Photonics: Manipulating Light Using Plasmas (Full Technical Final Report)

In this LDRD, we made significant advances on multiple fronts on the investigation and design of plasma-based optical structures to manipulate light at extreme intensities. We have unveiled new fundamental properties of laser-plasma interaction that were leveraged to introduce transformative applications. We first investigated new ways to generate high-amplitude plasma-based optical structures, based on the auto-resonance mechanism in order to produce refractive structures in plasmas. New insights into the interaction of such plasma structures with light waves allowed us to propose new methods for polarization manipulation and control for high-intensity lasers in the nonlinear regime, i.e. allowing the manipulation of an intense laser via its interaction with a less intense “control” laser beam in plasmas. Another application that we demonstrated experimentally is the capability to manipulate the velocity of light waves in plasmas by tailoring its refractive index; we reported the first demonstration of “slow light” and supra-luminal light propagation in plasmas. We also developed a new technological concept that would allow the probing of the type of plasma structures investigated in such applications, using high-bandwidth laser probing [Ludwig Phys. Plasmas 2019]. Finally, first steps were taken towards the demonstration of a plasma-based amplifier and compressor for the National Ignition Facility, in order to achieve powers equal of greater than those delivered by the Advanced Radiographic Capability (ARC). This technique uses a plasma-based grating acting like a compressor and amplifier, which could potentially compress and amplify an 88 ps, 56 J beam from the National Ignition Facility to <10 ps and hundreds of J.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Ultrafast optically induced spin transfer in ferromagnetic alloys

The vision of using light to manipulate electronic and spin excitations in materials on their fundamental time and length scales requires new approaches in experiment and theory to observe and understand these excitations. The ultimate speed limit for all-optical manipulation requires control schemes for which the electronic or magnetic subsystems of the materials are coherently manipulated on the time scale of the laser excitation pulse. In our work, we provide experimental evidence of such a direct, ultrafast, and coherent spin transfer between two magnetic subsystems of an alloy of Fe and Ni. Our experimental findings are fully supported by time-dependent density functional theory simulations and, hence, suggest the possibility of coherently controlling spin dynamics on subfemtosecond time scales, i.e., the birth of the research area of attomagnetism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Frequency and time multiplexing for multiphoton state generation

One of the primary challenges with photonic quantum information processing is that single-photon states are created and heralded probabilistically, rather than being created on demand. One solution to this problem is multiplexing , which is attempting probabilistic generation of a single photon at multiple locations, times, or frequencies, and switching one successfully generated photon into an output mode. Motivated by the development of frequency-based photonic quantum information processing, we consider multiplexing using frequency and time as our options to use to get many photon generation opportunities. We devise an approach for generating multiphoton states, with photons populating multiple frequency modes in the same spatiotemporal mode. This method uses a variable-length optical delays to manipulate the temporal mode of the photons, and spaced fiber Bragg grating (FBG) reflectors to jointly manipulate the frequency and temporal modes of the photons. Experimental progress toward implementing this multiplexing scheme is proceeding along 2 fronts, each with different ways to achieve the variable-length optical delay. First, we will implement this scheme using a free-space optical quantum memory with multiple discretely adjustable free-space delays. For this implementation method, I calculate multiphoton generation rates, accounting for loss, that are realistically achievable with commercially available hardware. This work will appear in a theory paper, currently in preparation. Second, we will implement this multiplexing scheme in an integrated manner: the variable-length optical delay will happen on-chip using a long-lifetime Q-switchable Fabry-Perot cavity. The joint manipulation of the frequency and temporal modes of the photons will still happen off-chip in fiber with FBG reflectors. I report on experimental progress in constructing integrated Q-switchable Fabry-Perot cavities.

97 MATHEMATICS AND COMPUTING↗

HSR transition jump optics in the September 2022 layout

Transition is crossed during acceleration in the Hadron Storage Ring (HSR) for all species other than protons. A first-order transition jump scheme manipulates the value of the optical quantity γ T and distorts the optics of the HSR around the time that the beam energy γ beam crosses the nominal transition value γ T 0 . The jump scheme in the Relativistic Heavy Ion Collider (RHIC) uses 48 jump quads, driven by 12 bi-polar power supplies that each drive 4 quads in series. Ten of those 48 are eliminated in the preliminary September 2022 HSR layout (EIC-HSR-220921a) that was developed from RHIC with no initial regard for transition crossing. This note analyzes the performance of the 38-quad HSR scheme, by comparison with the 48-quad RHIC scheme. It is concerned only with optics – the manipulation and response of Twiss functions and related quantities – and not with beams. This evaluation is a necessary first step before enhancing the transition jump scheme to restore RHIC performance in the HSR. Eventually full beam simulations of transition crossing need to be performed.

43 PARTICLE ACCELERATORS↗

Giant Enhancement of Four-Wave Mixing by Doubly Zone-Folded Nonlocal Metasurfaces

Resonant optical metasurfaces hold promise for enhancing nonlinear optical signals and manipulating their fundamental properties. However, they rarely excel at amplifying signals from nonlinear processes with two incident pump beams, such as four-wave mixing (FWM) or sum-frequency generation. Frequency-mixing experiments impose challenging requirements for metasurface design due to the need to support multiple optical resonances with compatible field profiles at specified resonant wavelengths, often across a substantial spectral separation. Here, in this work, we introduce nonlocal ‘quadromer’ metasurfaces containing four nanostructures per unit cell as the key to unlocking configurable, multiresonant metasurfaces that enhance frequency-mixing processes. As a proof of concept, we experimentally demonstrate enhanced FWM using quadromer metasurfaces made of silicon and silicon-rich silicon nitride. The results are relevant for applications such as imaging of infrared light upconverted into the visible spectrum and the generation of quantum light via spontaneous FWM.

four-wave mixing↗

Illumination-induced modulation of conductivity and Gunn oscillation properties in epitaxial GaAs

In this work, we illuminate a gallium arsenide (GaAs) Gunn device and study the light-induced changes of Gunn oscillation properties. We observe that illumination leads to the modulation of the Gunn threshold voltage, the Gunn oscillation magnitude, and the coherency of Gunn oscillation, with the nature of the modulation being closely related to the position of illumination on the device. These effects are attributed to the generation of optically excited carriers, which results in the modulation of conductivity and the electric field profile along the device. The finite element method is used to simulate the change of the field profile of the Gunn device caused by illumination. We also report an unexpected phenomenon of Gunn oscillation property manipulation with an optical chopper. In addition, wavelength-dependent, power-dependent, and pulsed illumination measurements are performed to help with further understanding the observations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Nonequilibrium phonon tuning and mapping in few-layer graphene with infrared nanoscopy

Electron-phonon interactions are fundamentally important physical processes responsible for many key discoveries in condensed matter physics and material sciences. Herein, by exploiting the scattering-type scanning near-field optical microscope (s-SNOM) excited with a femtosecond infrared (IR) laser, we explored the strong coupling between IR phonons in few-layer graphene (FLG) with ultrahot electrons, which are heated up by the intense laser field enhanced by the s-SNOM tip. More specifically, we found that the intensity of the phonon resonance can be tuned systematically by varying the laser power that controls the electron temperature. Furthermore, the high spatial resolution of s-SNOM allows us to map the local phonon characteristics at sharp boundaries and nanostructures. Our results offer insights into the intriguing physics behind the electron-phonon interactions in nonequilibrium conditions and open a pathway for manipulating phonons with optical means.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Nonlocal Metasurfaces with Lithographically Defined Vertical Symmetry Breaking

Nonlocal metasurfaces have garnered significant interest for applications that require customized and enhanced light–matter interactions in a flat form factor. These metasurfaces are distinctive for their ability to systematically control some of the fundamental properties of optical resonances by manipulating the in-plane symmetry of the lattice. Recent theoretical works have suggested that engineering the symmetry of a metasurface not just within the plane of the metasurface but also in the vertical or out-of-plane direction enables improved control of additional fundamental properties, especially chirality. However, standard nanofabrication processes cannot readily support elaborate vertical symmetry breaking such as nanostructure heights or slopes that deliberately vary across the footprint of a metasurface. Here, in this work, we experimentally demonstrate a scalable method to lithographically define the vertical symmetry of nonlocal metasurfaces by selectively eroding the etch mask during the etch process. Moreover, as the etch mask erosion rates depend on the in-plane size of individual nanostructures, we introduce and experimentally demonstrate a compatible design framework that enables versatile control over the properties of optical resonances. The results hold promise for chiral nonlocal metasurfaces with highly customized behavior.

metamaterial↗

Light-driven nanoscale vectorial currents

Controlled charge flows are fundamental to many areas of science and technology, serving as carriers of energy and information, as probes of material properties and dynamics and as a means of revealing or even inducing broken symmetries. Emerging methods for light-based current control offer particularly promising routes beyond the speed and adaptability limitations of conventional voltage-driven systems. However, optical generation and manipulation of currents at nanometre spatial scales remains a basic challenge and a crucial step towards scalable optoelectronic systems for microelectronics and information science. Here we introduce vectorial optoelectronic metasurfaces in which ultrafast light pulses induce local directional charge flows around symmetry-broken plasmonic nanostructures, with tunable responses and arbitrary patterning down to subdiffractive nanometre scales. Local symmetries and vectorial currents are revealed by polarization-dependent and wavelength-sensitive electrical readout and terahertz (THz) emission, whereas spatially tailored global currents are demonstrated in the direct generation of elusive broadband THz vector beams 17 . We show that, in graphene, a detailed interplay between electrodynamic, thermodynamic and hydrodynamic degrees of freedom gives rise to rapidly evolving nanoscale driving forces and charge flows under the extremely spatially and temporally localized excitation. These results set the stage for versatile patterning and optical control over nanoscale currents in materials diagnostics, THz spectroscopies, nanomagnetism and ultrafast information processing.

36 MATERIALS SCIENCE↗

Polarization‐Engineered Near‐Field Generation Using a Hybrid Tip–Antenna System

Precise control of light polarization at the nanoscale is critical for accessing chiral optical responses and manipulating spin–photon interactions in advanced materials. Yet, conventional scattering-type near-field probes predominantly generate out-of-plane linear polarization and offer little control over phase or polarization state. Here, in this study, we introduce a polarization-engineered near-field methodology based on a combined metallic tip and planar dipole nanoantenna system. Using full-wave electromagnetic simulations, we show that the tip acts as a vertically oriented plasmonic resonator, while the antenna supports an in-plane dipolar mode. By tuning the tip–antenna geometry and tip height, the two orthogonal field components attain comparable amplitudes and a controllable ∼90° phase offset, producing circularly polarized nano-light in the antenna gap. The proposed system effectively functions as a nanoscale quarter-wave plate, converting linearly polarized illumination into circularly polarized hotspots without external polarization optics. This method establishes an experimentally accessible route toward polarization-programmable near-field nanoscopy, enabling chiral spectroscopy, selective excitation of spin/valley degrees of freedom, and quantum optical investigations at the nanoscale.

36 MATERIALS SCIENCE↗

Trapping light in air with membrane metasurfaces for vibrational strong coupling

Optical metasurfaces can manipulate electromagnetic waves in unprecedented ways at ultra-thin engineered interfaces. Specifically, in the mid-infrared (mid-IR) region, metasurfaces have enabled numerous biochemical sensing, spectroscopy, and vibrational strong coupling (VSC) applications via enhanced light-matter interactions in resonant cavities. However, mid-IR metasurfaces are usually fabricated on solid supporting substrates, which degrade resonance quality factors (Q) and hinder efficient sample access to the near-field electromagnetic hotspots. Besides, typical IR-transparent substrate materials with low refractive indices, such as CaF 2 , NaCl, KBr, and ZnSe, are usually either water-soluble, expensive, or not compatible with low-cost mass manufacturing processes. Here, we present novel free-standing Si-membrane mid-IR metasurfaces with strong light-trapping capabilities in accessible air voids. We employ the Brillouin zone folding technique to excite tunable, high-Q quasi-bound states in the continuum (qBIC) resonances with our highest measured Q-factor of 722. Leveraging the strong field localizations in accessible air cavities, we demonstrate VSC with multiple quantities of PMMA molecules and the qBIC modes at various detuning frequencies. Our new approach of fabricating mid-IR metasurfaces into semiconductor membranes enables scalable manufacturing of mid-IR photonic devices and provides exciting opportunities for quantum-coherent light-matter interactions, biochemical sensing, and polaritonic chemistry. The authors introduce a mid-IR metasurface fabricated by decorating a free-standing Si-membrane with air holes. The enhanced light-matter interactions in such air cavities enable vibrational strong coupling and advanced biochemical sensing.

infrared spectroscopy↗

Doping-driven topological polaritons in graphene/$\alpha$-MoO 3 heterostructures

Control over charge carrier density provides an efficient way to trigger phase transitions and modulate the optoelectronic properties of materials. This approach can also be used to induce topological transitions in the optical response of photonic systems. Here we report a topological transition in the isofrequency dispersion contours of hybrid polaritons supported by a two-dimensional heterostructure consisting of graphene and α-phase molybdenum trioxide. By chemically changing the doping level of graphene, we observed that the topology of polariton isofrequency surfaces transforms from open to closed shapes as a result of doping-dependent polariton hybridization. Moreover, when the substrate was changed, the dispersion contour became dominated by flat profiles at the topological transition, thus supporting tunable diffractionless polariton propagation and providing local control over the optical contour topology. We achieved subwavelength focusing of polaritons down to 4.8% of the free-space light wavelength by using a 1.5-μm-wide silica substrate as an in-plane lens. Our findings could lead to on-chip applications in nanoimaging, optical sensing and manipulation of energy transfer at the nanoscale.

36 MATERIALS SCIENCE↗

Ultrafast optical melting of trimer superstructure in layered 1T′-TaTe2

Abstract Quasi-two-dimensional transition-metal dichalcogenides are a key platform for exploring emergent nanoscale phenomena arising from complex interactions. Access to the underlying degrees-of-freedom on their natural time scales motivates the use of advanced ultrafast probes sensitive to self-organised atomic-scale patterns. Here, we report the ultrafast investigation of TaTe 2 , which exhibits unique charge and lattice trimer order characterised by a transition upon cooling from stripe-like chains into a (3 × 3) superstructure of trimer clusters. Utilising MeV-scale ultrafast electron diffraction, we capture the photo-induced TaTe 2 structural dynamics – exposing a rapid ≈ 1.4 ps melting of its low-temperature ordered state followed by recovery via thermalisation into a hot cluster superstructure. Density-functional calculations indicate that the initial quench is triggered by intra-trimer Ta charge transfer which destabilises the clusters, unlike melting of charge density waves in other TaX 2 compounds. Our work paves the way for further exploration and ultimately rapid optical and electronic manipulation of trimer superstructures.

36 MATERIALS SCIENCE↗

Scintillator-based Timepix3 detector for neutron spin-echo techniques using intensity modulation

A scintillator-based Timepix3 (TPX3) detector was developed to resolve the high-frequency modulation of a neutron beam in both spatial and temporal domains, as required for neutron spin-echo experiments. In this system, light from a scintillator is manipulated with an optical lens and is intensified using an image intensifier, making it detectable with the TPX3 chip. Two different scintillators, namely, 6 LiF:ZnS(Ag) and 6 LiI:Eu, were investigated to achieve the high resolution needed for spin-echo modulated small-angle neutron scattering (SEMSANS) and modulation of intensity with zero effort (MIEZE). The methodology for conducting event-mode analysis is described, including the optimization of clustering parameters for both scintillators. The detector with both scintillators was characterized with respect to detection efficiency, spatial resolution, count rate, uniformity, and γ-sensitivity. The 6 LiF:ZnS(Ag) scintillator-based detector achieved a spatial resolution of 200 μm and a count rate capability of 1.1 × 10 5 cps, while the 6 LiI:Eu scintillator-based detector demonstrated a spatial resolution of 250 μm and a count rate capability exceeding 2.9 × 10 5 cps. Furthermore, high-frequency intensity modulations in both spatial and temporal domains were successfully observed, confirming the suitability of this detector for SEMSANS and MIEZE techniques, respectively.

47 OTHER INSTRUMENTATION↗