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At least 181 records · Page 10

Entangled spin-polarized excitons from singlet fission in a rigid dimer

Abstract Singlet fission, a process that splits a singlet exciton into a biexciton, has promise in quantum information. We report time-resolved electron paramagnetic resonance measurements on a conformationally well-defined acene dimer molecule, TIPS-BP1', designed to exhibit strongly state-selective relaxation to specific magnetic spin sublevels. The resulting optically pumped spin polarization is a nearly pure initial state from the ensemble. The long-lived spin coherences modulate the signal intrinsically, allowing a measurement scheme that substantially removes noise and uncertainty in the magnetic resonance spectra. A nonadiabatic transition theory with a minimal number of spectroscopic parameters allows the quantitative assignment and interpretation of the spectra. In this work, we show that the rigid dimer TIPS-BP1' supports persistent spin coherences at temperatures far higher than those used in conventional superconducting quantum hardware.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Incident beam optics optimization for the single crystal neutron diffractometer Pioneer with a polarized beam option

Pioneer, a next-generation single-crystal neutron diffractometer, is under development for Oak Ridge National Laboratory’s Second Target Station. Designed to address a wide range of scientific questions, Pioneer will deliver homogeneous neutron beams with customizable size and divergence and provide a polarized beam option. This article introduces its incident beam optics, highlighting the optimization methodology and the simulated performance. Pioneer will utilize a modified elliptical-straight guide for neutron transport and deploy slit packages and insertable apertures to control beam size and divergence. The optimized guide geometry matches the optimal-and-full-sample-illumination condition, and the beam control system effectively filters out unwanted neutrons while preserving the desired ones. In addition, we have found that polygon-approximated guides provide satisfactory transport efficiency and beam homogeneity, eliminating the need for truly curved guides. Further, to enhance neutronics performance and reduce cost, the coatings of supermirror elements are individually optimized to the lowest half-integer m-values that are sufficient to deliver the desired neutrons. After evaluating polarizing V-cavities and 3 He spin filters over the default polarized wavelength band of 1.2–5.5 Å, we selected a translatable multichannel polarizing V-cavity as the incident beam polarizer. Strategically placed at a location where the beam divergence is low and a large in-guide gap has negligible impact on transport efficiency, the optimized V-cavity achieves an average P 2 T of ~35%.

47 OTHER INSTRUMENTATION↗

Carrier-Envelope Phase Control in Terahertz Pulse Generation Using InAs Ribbon Metasurfaces

Generation of broadband terahertz (THz) pulses with variable polarization and carrier-envelope phase can enable the tailoring of THz beam wavefronts for advanced applications in THz imaging and spectroscopy and for strong THz field optics. While metasurfaces composed of deeply subwavelength THz emitters have recently been demonstrated to define the polarization and spatial profile of the generated THz fields, precise phase control or synthesis of THz pulse waveforms remains a challenging problem. Here, we propose and demonstrate metasurfaces composed of indium arsenide (InAs) nanoscale ribbon arrays capable of generating THz pulses with variable carrier-envelope phase. We show that different THz generation mechanisms, each contributing distinct phases, can be activated in the ribbons, enabling carrier-envelope phase control spanning a range of π over a wide band of frequencies (∼1–3 THz). This is achieved solely through the ribbon array geometry using linearly polarized optical excitation of the ribbons. The arrays enable precise control of the THz phase and amplitude, opening the door to advanced structured THz wavefront synthesis using ultrathin dielectric metasurfaces.

carrier-envelope phase↗

Ultrafast strong-field absorption in gapped graphene

In this work, we study theoretically the strong-field absorption of an ultrafast optical pulse by a gapped graphene monolayer. At low field amplitudes, the absorbance in pristine graphene is equal to the universal value of 2.3%. Although the ultrafast optical absorption for low field amplitudes is independent of the polarization, linear or circular, of the applied optical pulse, for high field amplitudes, the absorption strongly depends on the pulse polarization. For a linearly polarized pulse, the optical absorbance is saturated at the value of ≈ 1.4% for the pulse's amplitude of ≥ 0.4 V/Å, but no such saturation is observed for a circularly polarized pulse. For the gapped graphene, the absorption of a linearly polarized pulse shows a weak dependence on the bandgap, while for a circularly polarized pulse, the absorption is very sensitive to the bandgap.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

A new class of single-phase multiferroics: Bismuth-based layered supercell oxide thin films—Current progress and future perspectives

Multiferroic materials, where ferroelectric and magnetic orders coexist, have ignited substantial research interest due to the achievable manipulation of magnetic orders using external electric fields, a feature that has garnered serious interest for memory storage applications. Nonetheless, naturally occurring single-phase multiferroic materials are scarce, thus constraining options for practical use. Over the last decade, bismuth-based layered supercell (LSC) oxides have emerged as novel candidates for multiferroics, catalyzing extensive investigations in this domain. Additionally, these LSC systems are known for their anisotropic structures and optical properties, making them promising for application in optics such as polarizers, beam splitters, and modulators. This thorough review explores the development and current advancements in multiferroic bismuth-based LSC materials. It covers the diverse nature of LSCs, detailing their microstructure, properties, and the mechanics of self-assembly formation. It also highlights the remarkable multifunctional characteristics of LSC-based nanocomposites, with a particular focus on their applications in electronics and optics. Moreover, this review examines the significant potential of LSCs in practical applications, particularly through their integration onto silicon and flexible substrates via heteroepitaxy and film transfer techniques. Finally, it offers insights into potential future research avenues and the broader implications of these versatile LSC materials.

Materials Science↗

Tunable valleytronics with symmetry-retaining high polarization degree in SnS x Se 1–x model system

SnS has recently been shown to possess unique valleytronic capability with a large polarization degree, where non-degenerate valleys can be accessed using linearly polarized light, bestowed upon by the unique anisotropy and wavefunction symmetry. It is thus of utmost importance to demonstrate the extension of such effects for the IV–VI system in general, thereby elucidating the generality and tunability of such valleytronics. In this study, we show the highly tunable valleytronics via gradual compositional control of the tin(II) sulfo-selenide (SnS x Se 1–x ) alloy system with excellent retainment of symmetry-determined selection rules. We show the presence of both ΓY and ΓX valleys in all alloy compositions via selectivity in absorption and emission of linearly polarized light by optical reflection (R)/transmission (T) and photoluminescence measurements and tuned the bandgaps of the valleys within a range of 1.28 eV–1.05 eV and 1.48 eV–1.24 eV, respectively. This simultaneous tuning of non-degenerate valleys agrees well with theoretical calculations. We then fitted the bandgap values in compositional space, obtaining bowing parameters as a useful database. We further demonstrated the feasibility of using IV–VI valleytronics systems in general by elucidating the retainment of strong polarization degrees of as high as 91% across all compositions. The generalization of such purely symmetry-dependent valleytronics also opens up opportunities for the discovery of more multi-functional materials.

36 MATERIALS SCIENCE↗

Plasmonically assisted channels of photoemission from metals

We analyze recently measured nonlinear photoemission spectra from Ag surfaces that reveal resonances whose energies do not scale with the applied photon energy but stay pinned to multiples of bulk plasmon energy $\hbar$ω p above the Fermi level. To elucidate these unexpected and peculiar features we investigate the spectra of plasmons generated in a solid by the optically pumped electronic polarization and their effect on photoemission. By combining quadratic response formalism for calculations of photoemission yield, a nonperturbative approach to inelastic electron scattering, and first-principles calculations for the electronic structure, we demonstrate the dependence of probability amplitude for single- and multiplasmon excitations on the basic parameters characterizing the photon pulse and the system. The resulting multiexcitation spectrum evolves towards a truncated plasmonic coherent state. Analogous concept is extrapolated to interpret plasmon generation by multiphoton excited electronic polarization. Based on this we elaborate a scenario that the thus created real plasmons act as supplementary frequency-locked pump field for non-Einsteinian plasmonically assisted channels of photoemission from metals. The established paradigm enables assignment and assessment of the observed linear $\hbar$ω p and nonlinear 2$\hbar$ω p electron yields from Ag. Such effects may be exploited for selective filtering of optical energy conversion in electronic systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Direct dark matter searches with metal halide perovskites

Polar materials with optical phonons in the meV range are excellent candidates for both dark matter direct detection via dark photon-mediated scattering and light dark matter absorption. In this study, we propose, for the first time, the metal halide perovskites MAPbI 3 , MAPbCl 3 , and CsPbI 3 for these purposes. Our findings reveal that CsPbI 3 is the best material, significantly improving exclusion limits compared to other polar materials. For scattering, CsPbI 3 can probe dark matter masses down to the keV range. For absorption, it enhances sensitivity to detect dark photon masses below ∼10 meV. The only material that has so far been investigated and that could provide competitive bounds is CsI, which, however, demonstrates lower stability as device platform compared to CsPbI 3 . Moreover, CsI is isotropic while the anisotropic structure of CsPbI 3 enables daily modulation analysis, showing that a significant percentage of daily modulation exceeding 1% is achievable for dark matter masses below 40 keV.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Temperature-dependent optical constants of vanadium dioxide thin films deposited on polar dielectrics

Coating polar dielectrics with thin film vanadium dioxide (VO 2 ) enables one to exploit the temperature-dependent phase transition within VO 2 to actively tune and modulate surface phonon polaritons at mid-infrared. However, controlling the behavior of such systems requires intimate knowledge of the temperature-dependent optical constants of VO 2 , which depend greatly on the growth conditions and substrate material. Here, in this work, we accurately determine the complex optical constants of VO 2 on polar dielectrics across the insulator-to-metal phase transition (IMT) using only normal incident reflectance spectra by analyzing the reflectance with Kramers–Kronig relations and thin film Fresnel equations. This non-ellipsometry technique offers an advantage in determining the refractive index using a standard infrared spectrometer.

36 MATERIALS SCIENCE↗

Interstellar Extinction, Polarization, and Grain Alignment in the Sh 2-185 (IC 59 and IC 63) Region

Optical and infrared continuum polarization from the interstellar medium is driven by radiative processes aligning the grains with the magnetic field. While a quantitative, predictive theory of radiative alignment torques (RATs) exists and has been extensively tested, several parameters of the theory remain to be fully constrained. In a recent paper, Medan & Andersson showed that the polarization efficiency (and therefore grain alignment efficiency) at different locations in the wall of the Local Bubble (LB) could be modeled as proportional to the integrated light intensity from the surrounding stars and OB associations. Here we probe that relationship at high radiation field intensities by studying the extinction and polarization in the two reflection nebulae IC 59 and IC 63 in the Sh 2-185 H ii region, illuminated by the B0 IV star γ Cassiopeia. We combine archival visual polarimetry with new seven-band photometry in the Vilnius system, to derive the polarization efficiency from the material. We find that the same linear relationship seen in the LB wall also applies to the Sh 2-185 region, strengthening the conclusion from the earlier study.

47 OTHER INSTRUMENTATION↗

First-Principles Framework for the Prediction of Intersystem Crossing Rates in Spin Defects: The Role of Electron Correlation

Optically active spin defects in solids are promising platforms for quantum technologies. In this work, we present a first-principles framework to investigate intersystem crossing processes, which represent crucial steps in the optical spin-polarization cycle used to address spin defects. Considering the nitrogen-vacancy center in diamond as a case study, we demonstrate that our framework effectively captures electron correlation effects in the calculation of many-body electronic states and their spin-orbit coupling and electron-phonon interactions, while systematically addressing finite-size effects. We validate our predictions by carrying out measurements of fluorescence lifetimes, finding excellent agreement between theory and experiments. The framework presented here provides a versatile and robust tool for exploring the optical cycle of varied spin defects entirely from first principles.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Extrinsic Nonlinear Kerr Rotation in Topological Materials under a Magnetic Field

Topological properties in quantum materials are often governed by symmetry and tuned by crystal structure and external fields, and hence, symmetry-sensitive nonlinear optical measurements in a magnetic field are a valuable probe. Here, we report nonlinear magneto-optical second harmonic generation (SHG) studies of nonmagnetic topological materials including bilayer WTe 2 , monolayer WSe 2 , and bulk TaAs. The polarization-resolved patterns of optical SHG under a magnetic field show nonlinear Kerr rotation in these time-reversal symmetric materials. For materials with 3-fold rotational symmetric lattice structure, the SHG polarization pattern rotates just slightly in a magnetic field, whereas in those with mirror or 2-fold rotational symmetry, the SHG polarization pattern rotates greatly and distorts. Further, these different magneto-SHG characters can be understood by considering the superposition of the magnetic field-induced time-noninvariant nonlinear optical tensor and the crystal-structure-based time-invariant counterpart. The situation is further clarified by scrutinizing the Faraday rotation, whose subtle interplay with crystal symmetry accounts for the diverse behavior of the extrinsic nonlinear Kerr rotation in different materials. Our work illustrates the application of magneto-SHG techniques to directly probe nontrivial topological properties, and underlines the importance of minimizing extrinsic nonlinear Kerr rotation in polarization-resolved magneto-optical studies.

36 MATERIALS SCIENCE↗

The effects of field history on magnetic skyrmion formation in [Pt/Co/Ir] 3 multilayers

Here, we report on the formation of Néel-type magnetic bubble skyrmions at room temperature in [Pt/Co/Ir] 3 multilayered thin films after an in-plane magnetic field treatment. Polar magneto-optical Kerr Effect (p-MOKE) microscopy images show that the dendritic magnetic configurations observed after AC demagnetization evolve into magnetic bubble skyrmions after the application and subsequent removal of an in-plane magnetic field. Micromagnetic simulations were used to systematically investigate the role of the in-plane magnetic field magnitude, misalignment of the sample, and the Dzyaloshinskii-Moriya interactions (DMI) in generating bubble skyrmions during the field treatment. The simulations show that in-plane fields slightly below the saturation field are the most effective at producing skyrmions, and, furthermore, a small field angle away from the sample plane not only leads to improved skyrmion formation but also provides a means to select the skyrmion polarity where the direction of the out-of-plane component of the field is opposite to the direction of the skyrmion cores. This field treatment scheme leads to a simple and reliable way to create magnetic bubble skyrmions in multilayered thin films with DMI.

36 MATERIALS SCIENCE↗

Implementation of quantum key distribution and quantum clock synchronization via time bin encoding

Quantum key distribution allows for a provably secure transmission of cryptographic keys over an optical channel. Encoded polarization states or time-bin degree of freedom have been used for successful demonstrations. However, photon losses in long fibers, slow single photon detectors, and detector dark counts significantly limit the overall bit rate. Improving key throughput and reducing the overhead of key reconciliation remain as major challenges. Methods which utilize multiple time bins allow for multiple key bits to be encoded in a single photon, thus increasing the fidelity of transmitted keys and decreasing the overhead of key reconciliation in real-world conditions. Previous implementations of these methods required that Alice and Bob share a time reference by sharing a dedicated classical channel used for synchronization. This work presents a technique that allows two parties to exchange time-bin encoded photons without the need for synchronized time references. Our technique uses a framing protocol which allows Alice to encode a time reference along with a key which is determined by Alice before transmission. Security can be achieved by monitoring the visibility of a pair of Franson interferometers, using decoy pulses and measuring the round trip time between Alice and Bob. The bit rate of this technique is limited only by the recovery time of the detector and the speed of the modulation electronics. We experimentally demonstrate a raw bit rate of 5Mb/s over an optical channel with 55dB of loss, which is competitive with current research. We also demonstrate absolute timing synchronization with an accuracy of 20ps.

encryption↗

Tunable, Homoepitaxial Hyperbolic Metamaterials Enabled by High Mobility CdO

We report propagating light exhibits hyperbolicity in strongly anisotropic materials where the principal components of the dielectric tensor are opposite in sign. While hyperbolicity occurs naturally in anisotropic polar dielectrics, wherein optical phonons along orthogonal crystal axes are nondegenerate, such optical anisotropy can also be engineered in hyperbolic metamaterials (HMMs): thin film superlattices of alternating dielectric and metallic layers. Contrasted with the severely limited tunability of natural hyperbolic materials, the hyperbolic behavior of HMMs can be tailored significantly both through superlattice design and material selection. However, so far HMMs have suffered from high optical losses, hindering their performance. In this report, broadly tunable (λ = 2–5 µm) Type I and II hyperbolic modes with low losses (quality (Q)-factors up to 19.7) are observed through attenuated total reflectance measurements of monolithic, homoepitaxial superlattices of high- and low-doped cadmium oxide (CdO). Further, the low losses offered by CdO enable the first demonstration of real-space imaging of hyperbolic plasmon polaritons in nanoresonators by scattering-type scanning near-field optical microscopy—previously only possible for hyperbolic phonon polariton materials. Tunable, low-loss CdO HMMs promise designability for applications such as on-chip photonics, super-resolution imaging (hyperlensing), enhanced emission, novel emitter designs, and possibly quantum nanophotonic and time variant metasurfaces.

36 MATERIALS SCIENCE↗

Chemical Control of Symmetry and Bandgap in Tungsten Oxyhalide van der Waals Semiconductors

Tunability in solid-state materials is essential for testing theory, discovering quantum phases, and enabling functionality. Layered van der Waals (vdW) semiconductors offer a unique platform, providing new degrees of freedom at the two-dimensional (2D) limit through exfoliation and external controls. Here, in this study, we demonstrate tunability of symmetry and electronic structure via halogen substitution in a family of layered vdW tungsten oxyhalides. Substituting the halogens in WO 2 X 2 (X = I, Br, Cl) tunes the bandgap across a broad energy range and modifies the structural symmetry from centrosymmetric to noncentrosymmetric. By alloying WO 2 I 2– y Br y , we continuously tune the polar distortion and optical gap across the visible range. These insights into halogen substitution effects on symmetry and electronic structure lay the foundation for new tunable vdW semiconductors for optoelectronics and nonlinear optics.

36 MATERIALS SCIENCE↗

Mapping the magnetic field in the Taurus/B211 filamentary cloud with SOFIA HAWC + and comparing with simulation

ABSTRACT Optical and infrared polarization mapping and recent Planck observations of the filametary cloud L1495 in Taurus show that the large-scale magnetic field is approximately perpendicular to the long axis of the cloud. We use the HAWC + polarimeter on SOFIA to probe the complex magnetic field in the B211 part of the cloud. Our results reveal a dispersion of polarization angles of 36°, about five times that measured on a larger scale by Planck. Applying the Davis–Chandrasekhar–Fermi (DCF) method with velocity information obtained from Institut de Radioastronomie Millimétrique 30 m C18O(1-0) observations, we find two distinct sub-regions with magnetic field strengths differing by more than a factor 3. The quieter sub-region is magnetically critical and sub-Alfv$\acute{\rm e}$nic; the field is comparable to the average field measured in molecular clumps based on Zeeman observations. The more chaotic, super-Alfv$\acute{\rm e}$nic sub-region shows at least three velocity components, indicating interaction among multiple substructures. Its field is much less than the average Zeeman field in molecular clumps, suggesting that the DCF value of the field there may be an underestimate. Numerical simulation of filamentary cloud formation shows that filamentary substructures can strongly perturb the magnetic field. DCF and true field values in the simulation are compared. Pre-stellar cores are observed in B211 and are seen in our simulation. The appendices give a derivation of the standard DCF method that allows for a dispersion in polarization angles that is not small, present an alternate derivation of the structure function version of the DCF method, and treat fragmentation of filaments.

79 ASTRONOMY AND ASTROPHYSICS↗

Phase control of spin waves in the van der Waals antiferromagnet NiPS 3

Here we demonstrate phase control of magnons in the van der Waals antiferromagnet NiPS3 using optical excitation by polarized light. The sign of the coherent precession of spin amplitude changes upon (i) reversing the helicity of a circularly polarized pump beam, or (ii) rotating the polarization of a linearly polarized pump by π/2. Because these two excitation pathways have comparable generation efficiency, the phase of spin precession can be continuously tuned from 0 to 2π by controlling the polarization state of the pump pulse. The ability to excite magnons with a desired phase has potential applications in the design of a spin-wave phased array and ultrafast spin information processing.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗