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At least 253 records · Page 14

Piezoelectric domain walls in van der Waals antiferroelectric CuInP2Se6

Polar van der Waals chalcogenophosphates exhibit unique properties, such as negative electrostriction and multi-well ferrielectricity, and enable combining dielectric and 2D electronic materials. Using low temperature piezoresponse force microscopy, we revealed coexistence of piezoelectric and non-piezoelectric phases in CuInP2Se6, forming unusual domain walls with enhanced piezoelectric response. From systematic imaging experiments we have inferred the formation of a partially polarized antiferroelectric state, with inclusions of structurally distinct ferrielectric domains enclosed by the corresponding phase boundaries. The assignment is strongly supported by optical spectroscopies and density-functional-theory calculations. Enhanced piezoresponse at the ferrielectric/antiferroelectric phase boundary and the ability to manipulate this entity with electric field on the nanoscale expand the existing phenomenology of functional domain walls. At the same time, phase-coexistence in chalcogenophosphates may lead to rational strategies for incorporation of ferroic functionality into van der Waals heterostructures, with stronger resilience toward detrimental size-effects.

36 MATERIALS SCIENCE↗

Excited states in hydrogenated single-layer MoS 2

Abstract Our calculations of the excitation spectrum of single-layer MoS 2 at several hydrogen coverages, using a density-matrix based time-dependent density-functional theory (TDDFT) show that the fully hydrogenated system is metallic, while at lower coverages the spectrum consists of spin-polarized partially filled localized mid-gap states. The calculated absorption spectrum of the system reveals standard excitonic peaks corresponding to the bound valence-band hole and conduction-band electron, as well as excitonic peaks that involve the mid-gap states. Binding energies of the excitons of the hydrogenated system are found to be relatively large (few tens of meV), making their experimental detection facile and suggesting hydrogenation as a knob for tuning the optical properties of single-layer MoS 2 . Importantly, we find hydrogenation to suppress visible light photoluminescence, in agreement with experimental observations. In contrast, both Li and Na atoms transform the system into an n-doped non-magnetic semiconductor that does not allow excitonic states.

Physics↗

Anisotropic index of refraction and structural properties of hexagonal boron nitride epilayers probed by spectroscopic ellipsometry

The anisotropic index of refraction of 200 μm thick boron-10 enriched hexagonal boron nitride (h-BN) freestanding epilayers grown by metalorganic chemical vapor deposition has been measured using spectroscopic ellipsometry in the UV (4.0–5.1 eV) spectral range. It was found that the index of refraction for the polarization mode with an electric field perpendicular to the c-axis (ordinary, n o ) is much higher than that with an electric field parallel to the c-axis (extraordinary, n e ). By inclusion of turbostratic- (t-) phase layers within h-BN having an average inclination angle (θ) with respect to the ideal c-plane, a simple method for quantifying θ has been deduced. Our results revealed that the presence of t-phase layers decreases the optical anisotropy of h-BN and that a signature of improved crystalline quality is an increase in the ordinary index of refraction (n o ) as a result of the average incline angle θ approaching 0° and predicted that n o = 2.7 and n e = 1.5 at 280 nm for single crystalline h-BN epilayers. More importantly, our results demonstrated that spectroscopic ellipsometry is an effective technique for characterizing the crystalline quality of h-BN epilayers with the advantages of being noninvasive and highly sensitive.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Optical high-order harmonic generation as a structural characterization tool

Structural characterization is essential to material engineering, but few tools can detect structural properties in the time domain. High harmonic generation (HHG) emerges as a new frontier that touches the heart of condensed-matter physics from the symmetry to quantum geometrical nature of electrons, but its capability in structural characterization has not been materialized. Here, we establish a crucial connection between the symmetry of a material and the helicity of light. We employ monolayer MoS 2 as an example. In this work, we show that a linearly polarized laser pulse used in experiments is not ideal for structural characterization because it only generates in-plane anisotropy. It is the circularly polarized laser field that is capable of producing four distinctive HHG signals from the four phases of MoS 2 . This finally links the laser helicity to the crystal structure. The results are generic and are not affected by the Berry curvature, the interband or intraband contribution. Our study unleashes the power of HHG as a structural characterization tool for technologically important materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Valley-Coherent Quantum Anomalous Hall State in AB-Stacked MoTe 2 / W S e 2 Bilayers

Moiré materials provide fertile ground for the correlated and topological quantum phenomena. Among them, the quantum anomalous Hall (QAH) effect, in which the Hall resistance is quantized even under zero magnetic field, is a direct manifestation of the intrinsic topological properties of a material and an appealing attribute for low-power electronics applications. The QAH effect has been observed in both graphene and transition metal dichalcogenide (TMD) moiré materials. It is thought to arise from the interaction-driven valley polarization of the narrow moiré bands. Here, we show that the newly discovered QAH state in AB-stacked MoTe 2 / W S e 2 moiré bilayers is not valley polarized but valley coherent. The layer- and helicity-resolved optical spectroscopy measurement reveals that the QAH ground state possesses spontaneous spin (valley) polarization aligned (antialigned) in two TMD layers. In addition, saturation of the out-of-plane spin polarization in both layers occurs only under high magnetic fields, supporting a canted spin texture. Our results call for a new mechanism for the QAH effect and highlight the potential of TMD moiré materials with strong electronic correlations and spin-orbit interactions for exotic topological states. Published by the American Physical Society 2024

2-dimensional systems↗

A versatile X-ray phase retarder for lock-in XMCD measurements

X-ray magnetic circular dichroism (XMCD) is a technique commonly used to probe magnetic properties of materials with element and orbital selectivity, which requires the use of circularly polarized (CP) X-rays. It is possible to accomplish XMCD experiments with fixed CP and alternating the magnetic field orientation, but most reliable data are obtained when alternating the magnetization orientation and the polarization between right and left helicities. A versatile strategy has been developed to perform XMCD experiments using a hard X-ray quarter-wave plate, at both polychromatic dispersive and conventional monochromatic optics, in combination with synchronous data acquisition. The switching frequency waveform is fed into a lock-in amplifier to detect and amplify the XMCD signal. The results on a reference sample demonstrate an improvement in data quality and acquisition time. The instrumentation successfully generated 98% of CP X-rays switching the beam helicity at 13 Hz, with the possibility of faster helicity switching once it is installed at the new Brazilian fourth-generation source, SIRIUS.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

High-harmonic spin-shearing interferometry for spatially resolved EUV magneto-optical spectroscopy

We present a method for achieving hyperspectral magnetic imaging in the extreme ultraviolet (EUV) region based on high-harmonic generation (HHG). By interfering two mutually coherent orthogonally-polarized and laterally-sheared HHG sources, we create an EUV illumination beam with spatially-dependent ellipticity. By placing a magnetic sample in the beamline and sweeping the relative time delay between the two sources, we record a spatially resolved interferogram that is sensitive to the EUV magnetic circular dichroism of the sample. This image contains the spatially-resolved magneto-optical response of the sample at each harmonic order, and can be used to measure the magnetic properties of spatially inhomogeneous magnetic samples.

Optics↗

Comparison of scattering ratio profiles retrieved from ALADIN/Aeolus and CALIOP/CALIPSO observations and preliminary estimates of cloud fraction profiles

The space-borne active sounders have been contributing invaluable vertically resolved information of atmospheric optical properties since the launch of Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) in 2006. To build long-term records from space-borne lidars useful for climate studies, one has to understand the differences between successive space lidars operating at different wavelengths, flying on different orbits, and using different viewing geometries, receiving paths, and detectors. In this article, we compare the results of Atmospheric Laser Doppler INstrument (ALADIN) and Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) lidars for the period from 28 June to 31 December 2019. First, we build a dataset of ALADIN–CALIOP collocated profiles (Δdist<1°; Δtime<6 h). Then we convert ALADIN's 355 nm particulate backscatter and extinction profiles into the scattering ratio vertical profiles SR(z) at 532 nm using molecular density profiles from Goddard Earth Observing System Data Assimilation System, version 5 (GEOS-5 DAS). And finally, we build the CALIOP and ALADIN globally gridded cloud fraction profiles CF(z) by applying the same cloud detection threshold to the SR(z) profiles of both lidars at the same spatial resolution. Before comparing the SR(z) and CF(z) profiles retrieved from the two analyzed lidar missions, we performed a numerical experiment to estimate the best achievable cloud detection agreement CDA norm (z) considering the differences between the instruments. We define CDA norm (z) in each latitude–altitude bin as the occurrence frequency of cloud layers detected by both lidars, divided by a cloud fraction value for the same latitude–altitude bin. We simulated the SR(z) and CF(z) profiles that would be observed by these two lidars if they were flying over the same atmosphere predicted by a global model. By analyzing these simulations, we show that the theoretical limit for CDA$_{norm}^{theor}$(z) for a combination of ALADIN and CALIOP instruments is equal to 0.81±0.07 at all altitudes. In other words, 19 % of the clouds cannot be detected simultaneously by two instruments due to said differences. The analyses of the actual observed CALIOP–ALADIN collocated dataset containing ~78 000 pairs of nighttime SR(z) profiles revealed the following points: (a) the values of SR(z) agree well up to ~3 km height. (b) The CF(z) profiles show agreement below ~3 km, where ~80 % of the clouds detected by CALIOP are detected by ALADIN as expected from the numerical experiment. (c) Above this height, the CDA$_{norm}^{obs}$(z) reduces to ~50 %. (d) On average, better sensitivity to lower clouds skews ALADIN's cloud peak height in pairs of ALADIN–CALIOP profiles by ~0.5±0.6 km downwards, but this effect does not alter the heights of polar stratospheric clouds and high tropical clouds thanks to their strong backscatter signals. (e) The temporal evolution of the observed CDA$_{norm}^{obs}$(z) does not reveal any statistically significant change during the considered period. This indicates that the instrument-related issues in ALADIN L0/L1 have been mitigated, at least down to the uncertainties of the following CDA$_{norm}^{obs}$(z) values: 68±12 %, 55±14 %, 34±14 %, 39±13 %, and 42±14 % estimated at 0.75, 2.25, 6.75, 8.75, and 10.25 km, respectively.

54 ENVIRONMENTAL SCIENCES↗

Light Confinement in Twisted Single-Layer 2D+ Moiré Photonic Crystals and Bilayer Moiré Photonic Crystals

Twisted photonic crystals are photonic analogs of twisted monolayer materials such as graphene and their optical property studies are still in their infancy. This paper reports optical properties of twisted single-layer 2D+ moiré photonic crystals where there is a weak modulation in z direction, and bilayer moiré-overlapping-moiré photonic crystals. In weak-coupling bilayer moiré-overlapping-moiré photonic crystals, the light source is less localized with an increasing twist angle, similar to the results reported by the Harvard research group in References 37 and 38 on twisted bilayer photonic crystals, although there is a gradient pattern in the former case. In a strong-coupling case, however, the light source is tightly localized in AA-stacked region in bilayer PhCs with a large twist angle. For single-layer 2D+ moiré photonic crystals, the light source in Ex polarization can be localized and forms resonance modes when the single-layer 2D+ moiré photonic crystal is integrated on a glass substrate. This study leads to a potential application of 2D+ moiré photonic crystal in future on-chip optoelectronic integration.

36 MATERIALS SCIENCE↗

Light-induced electronic polarization in antiferromagnetic Cr 2 O 3

In a solid, the electronic subsystem can exhibit incipient order with lower point group symmetry than the crystal lattice. Ultrafast external fields that couple exclusively to electronic order parameters have rarely been investigated, however, despite their potential importance in inducing exotic effects. Here we show that when inversion symmetry is broken by the antiferromagnetic order in Cr 2 O 3 , transmitting a linearly polarized light pulse through the crystal gives rise to an in-plane rotational symmetry-breaking (from C 3 to C 1 ) via optical rectification. Using interferometric time-resolved second harmonic generation, we show that the ultrafast timescale of the symmetry reduction is indicative of a purely electronic response; the underlying spin and crystal structures remain unaffected. The symmetry-broken state exhibits a dipole moment, and its polar axis can be controlled with the incident light. Furthermore, our results establish a coherent nonlinear optical protocol by which to break electronic symmetries and produce unconventional electronic effects in solids.

36 MATERIALS SCIENCE↗

Measurement of the angular dependence of the spontaneous Raman scattering in anisotropic crystalline materials using spherical samples: Potassium dihydrogen phosphate as a case example

A specialized experimental configuration was created to allow for more-accurate characterization of the spontaneous Raman scattering properties in anisotropic materials. This need stems from the challenges, arising from the complexity of light propagation, in obtaining accurate measurements of the angular dependence of the Raman scattering cross section in birefringent materials. The nonlinear optical material KH 2 PO 4 (KDP) is used as a model medium. Our report is motivated by the need to improve our understanding and management of transverse stimulated Raman scattering in KDP crystals and its deuterated analog, DKDP, typically used for frequency conversion and polarization control in large-aperture laser systems. Key to this experimental platform is the use of high-quality spherical samples that enable one to measure the Raman scattering cross section in a wide range of geometries using only a single sample. The effect of polarization rotation of both the pump light and the collected Raman signal must be carefully considered in data analysis and can give rise to artifacts, which can, in part, be mitigated by reducing the input and collection cone angles.

47 OTHER INSTRUMENTATION↗

A long path-length optical property measurement device for highly transparent detector media

Measurements of the optical properties of highly transparent liquids are necessary for large-scale detectors that seek to detect optical signatures in kiloton-scale or larger volumes. Detailed understanding of the attenuation and scattering properties of fill media is critical to the ability to accurately simulate detector performance, and yet is often unavailable until in-situ measurements can be performed. Moreover, in-situ measurements may rely on effective attenuation lengths or other approximations to characterize performance, rather than absolute measurements of attenuation and scattering. To better understand the optical properties of potential fill media and purification schemes, a system has been developed which provides simultaneous attenuation and differential scattering cross-section measurements for highly transparent liquids. This horizontal, adjustable path-length “long-arm” system provides excellent isolation from the atmosphere, a high degree of vibration insensitivity, and a simple and reliable method of calibration. Further, scattering measurements can be carried out simultaneously at ports along the beamline equipped with optics allowing the selection of scatter angle and polarization. This enables both reliable quantitative scatter measurements and phase-function separation. This system has been extensively tested using deionized (DI) water as a benchmark, and has demonstrated repeatable measurements of attenuation lengths exceeding 100 m and scattering lengths approaching 1 km.

47 OTHER INSTRUMENTATION↗

Altermagnetic polar metallic phase in ultrathin epitaxially strained RuO 2 films

Altermagnetism refers to a wide class of magnetic orders featuring magnetic sublattices with opposite spins related by rotational symmetries, resulting in nontrivial spin splitting and magnetic multipoles. However, the direct observation of the altermagnetic transition remains elusive. Here, by combining theoretical analysis, electrical transport, X-ray, and optical spectroscopies, we establish a phase diagram in hybrid molecular beam epitaxy-grown RuO 2 /TiO 2 (110) films, mapping symmetries along with altermagnetic/electronic/structural phase transitions as functions of film thickness and temperature. This features an altermagnetic metallic polar phase in epitaxially strained 2 nm films, suggesting a potential link between polar metals and altermagnetic materials. Such a clear signature of a magnetic phase transition at ~500 K is observed exclusively in ultrathin strained films, unlike in bulk RuO 2 single crystals. These results highlight the power of epitaxial heterostructure engineering to induce altermagnetism in systems initially nonmagnetic, opening avenues for realizing emergent quantum phases with multifunctional properties.

RuO2 thin film↗

Integration of layered group IV selenides: From SnSe–SnSe 2-x S x core-shell crystals to complex (SnSe–SnSe 2-x S x )-GeSe van der waals heterostructures

The layered semiconductor tin selenide (SnSe) has received extensive interest due to its promising thermoelectric and ferroelectric properties. Integrating SnSe with other layered crystals in heterostructures can enable the modification of charge- and thermal transport, electrical polarization, and other properties such as chemical stability, optoelectronics, and photonics. Here, we demonstrate the vapor transport synthesis of single-crystalline SnSe monochalcogenide flakes that are spontaneously encapsulated in a thin layered SnSe 2-x S x dichalcogenide shell. In a second growth step, such SnSe-SnSe 2-x S x heterostructures are integrated with the monochalcogenide GeSe, which is laterally stitched to the SnSe side facets while preserving the dichalcogenide shell across the basal facets. This architecture is confirmed by optical microscopy, electron microscopy and diffraction, energy dispersive X-ray and Raman spectroscopies, as well as cathodoluminescence spectroscopy. Furthermore, the results extend our capabilities for materials integration by forming complex heterostructures with both vertical van der Waals interfaces and covalent lateral interfaces between layered semiconductors.

2D layered crystals↗

Boron phosphide as a p-type transparent conductor: Optical absorption and transport through electron-phonon coupling

Boron phosphide has recently been identified as a potential high-hole-mobility transparent conducting material. This promise arises from its low hole effective masses. However, boron phosphide has a relatively small, 2 eV, indirect bandgap which will affect its transparency. In this study, we computationally study both optical absorption across the indirect gap and phonon-limited electronic transport to quantify the potential of boron phosphide as a p-type transparent conductor. We find that phonon-mediated indirect optical absorption is weak in the visible spectrum and that the phonon-limited hole mobility is very high (around 900 cm 2 /Vs) at room temperature. This exceptional mobility comes from the combination of a low hole effective mass and very weak scattering by polar phonon modes. We rationalize the weak scattering by the less ionic bonding in boron phosphide compared to oxides. We suggest that this could be a general advantage of nonoxides for p-type transparent conducting applications. Using our computed properties, we assess the transparent conductor figure of merit of boron phosphide and show that it exceeds by one order of magnitude that of established p-type transparent conductors, confirming the potential of this material.

36 MATERIALS SCIENCE↗

Excitonic Anisotropy in Single‐Crystalline 2D Silver Phenylchalcogenides

2D materials exhibiting in‐plane anisotropy enable new applications in directional energy transport and polarized optical response. Silver phenylchalcogenides (AgEPh) – including mithrene (AgSePh), tethrene (AgTePh), and thiorene (AgSPh) – represent an exciting new addition to this family, with optical response spanning the visible to near‐UV. Here, excitonic anisotropy is predicted and characterized in this family of materials using a combination of ab initio theory and optical micro‐spectroscopy of single‐crystalline flakes. Using density functional theory and GW with the Bethe–Salpeter equation calculations, it is revealed that all AgEPh compounds exhibit anisotropic electronic band structure and host multiple delocalized excitons with in‐plane anisotropy. Room‐temperature polarization‐resolved optical micro‐spectroscopy shows that orthogonally polarized excitons with similar energy lead to nearly isotropic absorption in AgSPh, whereas energy separation between excitonic resonances in AgSePh and AgTePh leads to strong absorption and emission anisotropy. Cryogenic reflectance micro‐spectroscopy further reveals exciton fine structure in AgSePh, reconciling the discrepancies between room‐temperature experiments and theoretical predictions. Finally, it is demonstrated that the optical response of thicker AgEPh crystals is influenced by photonic effects arising from finite crystal size. Overall, this work advances the understanding of the relationship between anisotropic structure, composition, and excitonic properties in AgEPh, providing a foundation for technological integration.

2D↗

Rectified Rotational Dynamics of Mobile Inclusions in Two-Dimensional Active Nematics

We investigate the dynamics of mobile inclusions embedded in 2D active nematics. The interplay between the inclusion shape, boundary-induced nematic order, and autonomous flows powers the inclusion motion. Disks and achiral gears exhibit unbiased rotational motion, but with distinct dynamics. In comparison, chiral gear-shaped inclusions exhibit long-term rectified rotation, which is correlated with dynamics and polarization of nearby +1/2 topological defects. Furthermore, the chirality of defect polarities and the active nematic texture around the inclusion correlate with the inclusion’s instantaneous rotation rate. Inclusions provide a promising tool for probing the rheological properties of active nematics and extracting ordered motion from their inherently chaotic motion.

36 MATERIALS SCIENCE↗

Quantifying Twist Angles in Cuprate Heterostructures with Anisotropic Raman Signatures

Artificially engineered twisted van der Waals (vdW) heterostructures have unlocked new pathways for exploring emergent quantum phenomena and strongly correlated electronic states. Many of these phenomena are highly sensitive to the twist angle, which can be deliberately tuned to tailor the interlayer interactions. This makes the twist angle a critical tunable parameter, emphasizing the need for precise control and accurate characterization during device fabrication. In particular, twisted cuprate heterostructures based on Bi 2 Sr 2 CaCu 2 O 8 + x (BSCCO) have demonstrated angle-dependent superconducting properties, positioning the twist angle as a key tunable parameter. However, the twisted interface is highly unstable under ambient conditions and vulnerable to damage from conventional characterization tools such as electron microscopy or scanning probe techniques. In this work, a fully non-invasive, polarization-resolved Raman spectroscopy approach is introduced for determining twist angles in artificially stacked BSCCO heterostructures. By analyzing twist-dependent anisotropic vibrational Raman modes, particularly utilizing the out-of-plane A 1g vibrational mode of Bi/Sr at ≈116 cm −1 , clear optical fingerprints of the rotational misalignment between cuprate layers are identified. The high-resolution confocal Raman setup, equipped with polarization control and RayShield filtering down to 10 cm −1 , allows for reliable and reproducible measurements without compromising the material's structural integrity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗