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At least 235 records · Page 13

Characterization of light production and transport in tellurium dioxide crystals

Simultaneous measurement of phonon and light signatures is an effective way to reduce the backgrounds and increase the sensitivity of CUPID, a next-generation bolometric neutrinoless double-beta decay ($0\nu\beta\beta$) experiment. Light emission in tellurium dioxide (TeO$_2$) crystals, one of the candidate materials for CUPID, is dominated by faint Cherenkov radiation, and the high refractive index of TeO$_2$ complicates light collection. Positive identification of $0\nu\beta\beta$ events therefore requires high-sensitivity light detectors and careful optimization of light transport. A detailed microphysical understanding of the optical properties of TeO$_2$ crystals is essential for such optimization. We present a set of quantitative measurements of light production and transport in a cubic TeO$_2$ crystal, verified with a complete optical model and calibrated against a UVT acrylic standard. We measure the optical surface properties of the crystal, and set stringent limits on the amount of room-temperature scintillation in TeO$_2$ for $\beta$ and $\alpha$ particles of 5.3 and 8 photons / MeV, respectively, at 90% confidence. Finally, the techniques described here can be used to optimize and verify the particle identification capabilities of CUPID.

47 OTHER INSTRUMENTATION↗

Effects of B 2 O 3 on the Growth, Structural, and Magneto-Optical Properties of Yttrium Iron Garnet Single-Crystal Fibers

This study explores the fabrication of yttrium iron garnet (YIG) single crystal fibers using the laser heated pedestal growth (LHPG) method with the experimental addition of B 2 O 3 . The incorporation of B 2 O 3 facilitates the fiber fabrication process by lowering the required growth temperatures and likely modifying melt viscosity behavior, consistent with the established fluxing behavior of B2O3 and the comparative viscosity trend observed in the TMA−VFT analysis, thereby improving process efficiency while maintaining fiber quality. Structural characterization using EBSD and SC-XRD reveals a transition from polycrystalline to single-crystal behavior, with improved alignment along the [111] direction without altering the garnet structure. Magnetic measurements show increases in saturation magnetization in B 2 O 3 -assisted fibers. Three-dimensional anisotropy energy modeling, based on EBSD-derived Euler angles, indicates that the enhanced crystallinity and orientation contribute to reorientation of MCA energy distribution due to improved crystallographic alignment. Faraday rotation measurements show that the B 2 O 3 -assisted sample exhibits a rotation angle closer to reported values for high-quality YIG, suggesting improved phase purity and crystallographic quality. These findings demonstrate that B 2 O 3 -assisted LHPG growth is a scalable and nontoxic approach to producing high-performance YIG fibers for integrated photonic and magnetic field sensing applications.

Crystal structure↗

Highly Saturated Glassy Liquid Crystal Films Having Nano- and Microscale Thicknesses for High-Power Laser Applications

The optical properties of glassy liquid crystals (GLC’s) designed to provide high resistance to laser-induced damage are explored. GLC’s readily enable freezing of the anisotropic ordering of liquid crystals into the glassy state. This solidity avoids issues of fluid leakage while providing mechanical robustness and the promise of single-substrate coatings or stand-alone films of nanometer to micron thicknesses. A series of three increasingly saturated GLC’s was synthesized and tested for their thin-film (hundreds of nanometers to tens of micrometers) high-peak-power laser-damage resistance with nanosecond pulses at 1053 nm, 532 nm, and 351 nm, as well as their durability under continuous-wave, broadband ultraviolet illumination. As a result, the GLC’s with higher degrees of saturation demonstrated high resistance to laser-induced damage, extending from the near infrared to the ultraviolet spectral region.

36 MATERIALS SCIENCE↗

Towards a wavefront-preservation X-ray crystal monochromator for high-repetition-rate FELs

The wavefront preservation of coherent X-ray free-electron laser beams is pushing the requirement on the quality and performance of X-ray optics to an unprecedented level. The Strehl ratio can be used to quantify this requirement. In this paper, the criteria for thermal deformation of the X-ray optics are formulated, especially for crystal monochromators. To preserve the X-ray wavefront, the standard deviation of the height error should be sub-nm for mirrors and less than 25 pm for crystal monochromators. Cryocooled silicon crystals combined with two techniques can be used to achieve this level of performance for monochromator crystals: (1) using a focusing element to compensate the second-order component of the thermal deformation; (2) introducing a cooling pad between the cooling block and silicon crystal and optimizing the effective cooling temperature. Each of these techniques allows the thermal deformation in standard deviation of the height error to be reduced by an order of magnitude. As an example, for the LCLS-II-HE Dynamic X-ray Scattering instrument, the criteria on thermal deformation of a high-heat-load monochromator crystal can be achieved for a 100 W SASE FEL beam. Wavefront propagation simulations confirm that the reflected beam intensity profile is satisfactory on both the peak power density and focused beam size.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Deep level defects and cation sublattice disorder in ZnGeN 2

The III-nitrides have revolutionized lighting technology and power electronics. Expanding the nitride semiconductor family to include the heterovalent ternary nitrides opens up new and exciting opportunities for device design that may help overcome some of the limitations of the binary nitrides as well as new applications. However, the more complex cation sublattice also gives rise to new complexities with both native and extrinsic defects, such as disorder on the cation sublattice. Here, depth-resolved cathodoluminescence spectroscopy and surface photovoltage spectroscopy measurements of defect energy levels in ZnGeN 2 combined with transmission microscopy and crystal lattice diffraction reveal optical signatures of mid-gap states that can be associated with cation sublattice disorder. The energies of these characteristic optical signatures in ZnGeN 2 thin films grown by metal-organic chemical vapor deposition are in good agreement with energy levels predicted by density functional theory for specific thermodynamically stable native point defects. To test the dependence of these defect signatures on crystal atomic composition, we correlated spatially-resolved optical and atomic composition measurements using spatially resolved x-ray photoelectron spectroscopy with systematically varied growth conditions on the same ZnGeN 2 films. The resultant elemental maps versus defect spectral energies and intensities suggest that cation antisite complexes (Zn Ge -Ge Zn ) versus isolated native point defects form preferentially and introduce mid-gap states that dominate electron-hole pair recombination. Complexing of Zn Ge and Ge Zn antisites manifests as disorder in the cation sub-lattice and leads to the formation of wurtzitic ZnGeN 2 as indicated by transmission electron microscopy diffraction patterns and x-ray diffraction (XRD) reciprocal space maps. Furthermore, these findings emphasize the importance of growth conditions to control cation place exchange.

42 ENGINEERING↗

Exploiting universal nonlocal dispersion in optically active materials for spectro-polarimetric computational imaging

Recent years have seen significant advancements in exploring novel light-matter interactions such as hyperbolic dispersion within natural crystals. However, current studies have predominantly concentrated on local optical response of materials characterized by a dielectric tensor without spatial dispersion. Here, we investigate the nonlocal response in optically-active crystals with screw symmetries, revealing their lossless, super-dispersive properties compared to traditional optical response functions. We leverage this universal nonlocal dispersion, i.e. the dispersion of optical rotatory power, to explore a novel spectral de-multiplexing scheme compared to conventional gratings, prisms and metasurfaces. We design and demonstrate an ‘Nonlocal-Cam’ - a camera that exploits nonlocal dispersion through sampling of polarized spectral states and the application of computational spectral reconstruction algorithms. The Nonlocal-Cam captures information in both laboratory and outdoor field experiments which is unavailable to traditional intensity cameras - the spectral texture of polarization. Merging the fields of nonlocal electrodynamics and computational imaging, our work paves the way for exploiting nonlocal optics of optically active materials in a variety of applications, from biological microscopy to physics-driven machine vision and remote sensing.

Wang, Xueji [Purdue Univ., West Lafayette, IN (Uni↗

London penetration depth of electron-irradiated Ba 0 . 47 K 0 . 53 Fe 2 As 2

We have characterized an electron-irradiated Ba 1-x K x Fe 2 As 2 (x = 0.53) single-crystal using two different experimental techniques: magneto-optic measurements and microwave measurements. The crystal has been measured before as well as after the 2.5 MeV electron irradiation process. After irradiation it was annealed in a number of steps, between 90 °C and 180 °C, and measured after each annealing step. Most microwave measurements were performed by means of a copper cavity, taking advantage of the TE 011 and TM 110 modes, allowing for the determination of the London penetration depths changes δλ ab (T) and δλ c (T), ie perpendicular and parallel to the sample c-axis. Appropriate equations, based on perturbation theory, were derived to calculate the penetration depths changes δλ ab and δλ c for a rectangular prism geometry. The sample showed a full recovery of its T c , however the observed behavior of δλ c and δλ ab was not monotonic vs annealing temperature, displaying a minimum of δλ c and δλ ab at 120 °C. In conclusion, this finding was confirmed by magneto-optic measurements, where besides verifying the sample uniformity and the absence of visible defects, the lower critical field H c1 of the Ba 1-x K x Fe 2 As 2 single-crystal was obtained and the London penetration depth λab(0) was calculated.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Synthesis, disorder and Ising anisotropy in a new spin liquid candidate PrMgAl 11 O 19

Here we report the successful synthesis of large single crystals of triangular frustrated PrMgAl 11 O 19 using the optical floating zone technique. Single crystal x-ray diffraction (XRD) measurements unveiled the presence of quenched disorder within the mirror plane, specifically ~7% of Pr ions deviating from the ideal 2d site towards the 6h site. Magnetic susceptibility measurements revealed an Ising anisotropy with the c-axis being the easy axis. Despite a large spin–spin interaction that develops below ~10 K and considerable site disorder, the spins do not order or freeze down to at least 50 mK. The availability of large single crystals offers a distinct opportunity to investigate the exotic magnetic state on a triangular lattice with an easy axis out of the plane.

36 MATERIALS SCIENCE↗

High Refractive Index Adhesives for Laser Glass Cladding Applications (ABBREVIATED Report)

To eliminate parasitic light oscillations (amplified spontaneous emission (ASE)), high energy laser systems often utilize polymeric materials to adhere optically absorptive cladding materials to laser gain media (glass or crystal). Most of these polymeric optical adhesives are index matched to lower index gain media, and there was no capability to achieve refractive indices (RI) greater than 1.60 with low color, while also maintaining mechanical compliance to serve as adhesives for cladding applications. The completion of LDRD 23-FS-043 shows we can chemically develop novel suitable adhesive candidates with refractive indices above 1.64 at 532 nm while also exhibiting Shore A hardness between 50-90, with high optical clarity, low color, and minimal haze for films ~1-2 mm thick (84 %Transmission at 532 nm). This will enable us to begin mapping a process space to allow future customizable adhesive formulations for building a variety of laser systems with tunable refractive index matching for various gain and cladding media.

36 MATERIALS SCIENCE↗

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↗

Purcell-Enhanced Emissions from Diamond Color Centers in Slow Light Photonic Crystal Waveguides

Diamond color centers are promising candidates for optically addressable quantum memories, which motivates the development of efficient photonic interfaces, often using nanophotonic cavities with narrow spectral line widths and small mode volumes. However, they require perfect spectral and spatial overlap between the cavity mode and quantum emitter, which is challenging. This is especially true for solid-state quantum emitters that are often randomly positioned and suffer from inhomogeneous broadening. Another approach to enhance light-matter interaction across large optical bandwidths and areas is using slow light waveguides. Here, in this study, we demonstrate diamond slow light photonic crystal (PhC) waveguides optically coupled to embedded silicon-vacancy (SiV) color centers. We use the recently developed thin-film diamond approach to fabricate fully suspended two-dimensional PhC waveguides. We demonstrate waveguide modes with high group indices up to 70 and observe Purcell-enhanced emissions of the SiVs. Our approach represents a practical diamond platform for robust spin-photon interfaces with color centers.

2D photonic crystal waveguide↗

Dynamics of self-hybridized exciton–polaritons in 2D halide perovskites

Abstract Excitons, bound electron–hole pairs, in two-dimensional hybrid organic inorganic perovskites (2D HOIPs) are capable of forming hybrid light-matter states known as exciton-polaritons (E–Ps) when the excitonic medium is confined in an optical cavity. In the case of 2D HOIPs, they can self-hybridize into E–Ps at specific thicknesses of the HOIP crystals that form a resonant optical cavity with the excitons. However, the fundamental properties of these self-hybridized E–Ps in 2D HOIPs, including their role in ultrafast energy and/or charge transfer at interfaces, remain unclear. Here, we demonstrate that >0.5 µm thick 2D HOIP crystals on Au substrates are capable of supporting multiple-orders of self-hybridized E–P modes. These E–Ps have high Q factors (>100) and modulate the optical dispersion for the crystal to enhance sub-gap absorption and emission. Through varying excitation energy and ultrafast measurements, we also confirm energy transfer from higher energy E–Ps to lower energy E–Ps. Finally, we also demonstrate that E–Ps are capable of charge transport and transfer at interfaces. Our findings provide new insights into charge and energy transfer in E–Ps opening new opportunities towards their manipulation for polaritonic devices.

42 ENGINEERING↗

Dynamically patterning x-ray beam by a femtosecond optical laser

Modern science and technology have greatly benefitted from our ability to precisely manipulate light waves, in both their spatial and temporal degrees of freedom. In the x-ray region, however, spatial control has been virtually static mainly due to stringent requirements for realizing high-performance optical elements. The lack of dynamic spatial control of x-ray beam has prevented researchers from realizing more sophisticated use of the wave field, which has rapidly advanced in the optical region in the past decades. In this study, we propose a practical scheme to dynamically control local x-ray reflectivity of a perfect silicon crystal by a femtosecond optical laser and demonstrate a programmable spatial x-ray modulator. Our modulator aims for spatial manipulation of the x-ray amplitude and is shown to produce arbitrary grayscale patterns with spatial frequencies up to 25 per millimeter. The proposed modulation scheme opens up a platform to enable advanced x-ray sensing and imaging techniques that can fully harness the wave nature of x-rays.

47 OTHER INSTRUMENTATION↗

Ultrafast photo-induced phonon hardening due to Pauli blocking in MAPbI 3 single-crystal and polycrystalline perovskites

Metal-halide perovskite semiconductors have attracted intense interest over the past decade, particularly for applications in photovoltaics. Low-energy optical phonons combined with significant crystal anharmonicity play an important role in charge-carrier cooling and scattering in these materials, strongly affecting their optoelectronic properties. We have observed optical phonons associated with Pb–I stretching in both MAPbI 3 single crystals and polycrystalline thin films as a function of temperature by measuring their terahertz conductivity spectra with and without photoexcitation. An anomalous bond hardening was observed under above-bandgap illumination for both single-crystal and polycrystalline MAPbI 3 . First-principles calculations reproduced this photo-induced bond hardening and identified a related lattice contraction (photostriction), with the mechanism revealed as Pauli blocking. For single-crystal MAPbI 3 , phonon lifetimes were significantly longer and phonon frequencies shifted less with temperature, compared with polycrystalline MAPbI 3 . We attribute these differences to increased crystalline disorder, associated with grain boundaries and strain in the polycrystalline MAPbI 3 . Thus we provide fundamental insight into the photoexcitation and electron–phonon coupling in MAPbI 3 .

36 MATERIALS SCIENCE↗

High-Temperature Observation of Intralayer, Interlayer, and Rydberg Excitons in Bulk Van Der Waals Alloy Single Crystals

Transition metal dichalcogenides exhibit remarkable optical properties due to the diverse number of strongly bound excitons, which can be fine-tuned by alloying. Despite a flurry of research activity in characterizing these excitons, a comprehensive and profound understanding of their behavior with temperature is lacking. Here, we report the rich spectrum of excitonic features within bulk van der Waals alloy Mo0.5 W0.5 S2 and Mo0.5 W0.5 Se2 single crystals through temperature-dependent reflectance spectroscopy and first-principles calculations. We observed Rydberg excitons and interlayer excitons in both the single crystals. Notably, we provide the first experimental evidence of highly energetic A' and B' excitons in Mo0.5 W0.5 S2 at room temperature. The strong carrier-phonon scattering significantly broadens the A', B', and interlayer excitons at room temperature in bulk Mo0.5 W0.5 S2 single crystal compared to its selenide. Our findings, supported by density functional theory and Bethe-Salpeter equation calculations, signify the crucial role of carrier-phonon interactions. These results open pathways for next-generation optoelectronic devices and quantum technologies operating at high temperature.

excitons↗

Centimeter-Scale Pillared-Layer Metal–Organic Framework Thin Films Mediated by Hydroxy Double Salt Intermediates for CO 2 Sensor Applications

Fabrication of metal–organic framework (MOF) thin films over macroscopic surface areas is a subject of great interest for gas sensor application platforms such as optics and microelectronics. However, a direct synthesis of MOF films at ambient conditions, in particular pillared-layer MOF films due to their anisotropic structures, remains a significant challenge. Herein, we demonstrate for the first time a facile construction of dense and continuous pillared-layer MOF thin films on a centimeter scale via an aluminum-doped zinc oxide template and hydroxy double salt (HDS) intermediates at room temperature. A series of Cu(II)-based pillared MOFs with different 1,4-benzenedicarboxylic acid (bdc) ligands were explored for optimizing MOF film formation for CO 2 sensor applications. Nonpolar ligands with lower water solubility preferentially formed crystalline pillared MOF structures from HDS intermediates. A Cu 2 (ndc) 2 (dabco) (ndc = 1,4-naphthalene-bdc; dabco = 1,4-diazabicyclo[2.2.2]octane) MOF demonstrated the most dense and uniform film growth with micrometer thickness over one square centimeter area. This synthetic approach for growing Cu 2 (ndc) 2 (dabco) MOF thin films was successfully translated toward two sensing platforms: a quartz crystal microbalance and an optical fiber sensor. These Cu 2 (ndc) 2 (dabco) MOF-coated sensors displayed sensitivity toward CO 2 and response/recovery time on the scale of seconds, even at moderate humidity levels. Finally, this work provides a road map for producing continuous and anisotropic crystalline MOF thin films over a centimeter scale area on various substrates, which will greatly facilitate their utilization in MOF-based sensor devices, among other applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A position and pulse shape discriminant p -terphenyl detector module

We present the development of a neutron detector array module made with para-terphenyl, a bright, fast, n/γ discriminating crystalline organic scintillator. The module is comprised of 2 cm × 2 cm × 2 cm p-terphenyl crystals that have been optically coupled together to create a pseudo-bar module. While only relying on two photo detectors, the module is capable of distinguishing interactions between up to eight crystals. Furthermore, the module retains the p-terphenyl’s pulse shape discrimination (PSD) capability. Together this makes the pseudo-bar module a promising position-sensitive neutron detector. Here we present characteristics of the pseudo-bar module - its timing resolution as well as its pulse shape and position discrimination capabilities, and briefly discuss future plans for utilizing an array of pseudo-bar modules in a useful neutron detector system.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗