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At least 343 records · Page 19

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DOE OSTI2024

Poly(cyclosilane) Postpolymerization Hydrosilylation

Postpolymerization functionalization is a key strategy in the diversification of polymeric materials for the conferral of tailored properties. Poly(cyclosilane)s are structurally complex polymers with an all-silicon backbone, featuring a periodic array of hydrido (Si–H) side chains that are potentially suitable for postpolymerization functionalization via hydrosilylation. At the same time, classical methods for hydrosilylation employing Pt- or Pd-based catalysts can result in Si–Si bond scission. In this work, we demonstrate borane-catalyzed hydrosilylation reactions between α-olefins and small molecules or three distinct poly(cyclosilane) architectures. We investigate chemoselectivity for end group versus internal Si–H groups and find that 29 Si cross-polarization magic angle spinning can provide insight on site-selectivity in the functionalization of a complex poly(cyclosilane). Furthermore, we show that postpolymerization hydrosilylation, converting oxidatively sensitive Si–H groups to Si–alkyl chains, modulates solubility and physical characteristics, optical properties, pyrolytic reactivity, and air sensitivity.

36 MATERIALS SCIENCE↗

DOE OSTI2021

The spin selectivity effect in chiral materials

We overview experiments performed on the chiral induced spin selectivity (CISS) effect using various materials and experimental configurations. Through this survey of different material systems that manifest the CISS effect, we identify several attributes that are common to all the systems. Among these are the ability to observe spin selectivity for two point contact configurations, when one of the electrodes is magnetic, and the correlation between the optical activity of the chiral systems and a material’s spin filtering properties. In addition, recent experiments show that spin selectivity does not require pure coherent charge transport and the electron spin polarization persists over hundreds of nanometers in an ordered medium. Finally, we point to several issues that still have to be explored regarding the CISS mechanism. Among them is the role of phonons and electron–electron interactions.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Field-resolved space–time characterization of few-cycle structured light pulses

Accompanied by the rapid development of ultrafast laser platforms in recent decades, the spatiotemporal manipulation of ultrashort laser pulses has attracted much attention due to the potential for cutting-edge applications of structured light, including optical tweezers, optical communications, super-resolution imaging, time-resolved spectroscopy in molecules and quantum materials, and strong-field physics. Today, techniques capable of characterizing the full spatial, temporal, and polarization state properties of structured light are strongly desired. Here, we demonstrate a technique, termed 3D TIPTOE, for characterizing structured mid-infrared waveforms, which uses only a two-dimensional silicon-based image sensor as both the detector and the nonlinear medium. By combining the advantages of the sub-cycle time resolution afforded by nonlinear excitation and the spatial resolution inherent to the two-dimensional sensor, the 3D TIPTOE technique allows full characterization of structured electric fields, significantly reducing the complexity of detection compared to other techniques. The validity of the technique is established by measuring both few-cycle Bessel–Gaussian pulses and radially polarized femtosecond vector beams.

Liu, Yangyang (ORCID:0000000335205332)↗

NASA NTRS1979

Some properties of the knots in the M87 jet

Photographs taken in 1956 by Baade show the knots in the jet of M87 to be polarized. In 1978, these plates were repeated under conditions as identical as possible. A careful comparison indicates that the polarization and intensity of the knots have changed in the 22 year interval. Emission lines in the nucleus of M87 not previously seen have been revealed by extensive 5 m SIT spectroscopy. The same spectroscopy with galaxy subtracted, however, has failed to reveal any features in the jet. The known optical and radio properties of the jet are reviewed. A coincidence is found in almost all of the defining properties of BL Lacertae objects with the properties of the knots in the jet. Statistical studies of the distribution of BL Lacertae objects near bright galaxies reveals a marginally significant excess of such associations.

Sulentic, J. W.↗

NASA NTRS1984

Some photometric properties of the Martian south polar cap region during the 1971 apparition

High-quality earth-based photographs from the Lowell Observatory Planetary Research Center collection have been analyzed to derive some photometric parameters for the Martian south polar cap region during the 1971 apparition. The optical thickness of the atmosphere above the cap varied with wavelength from 0.35 + or - 0.05 in red light to 0.58 + or 0.06 in UV light. The effective geometric albedo is calculated from the 30 deg phase data assuming isotropic scattering: it varies from 0.85 + or - 0.04 (in red light) to 0.63 + or 0.05 (in UV light).

Lumme, K.↗

NASA NTRS2021

The Thermal Infrared Optical Depth of Mineral Dust Retrieved from Integrated CALIOP and IIR Observations

Recent studies reveal that a higher fraction of coarse mineral dust particles than that estimated by climate model simulations has been observed in the atmosphere, leading to a more significant positive (i.e., warming) longwave (LW) thermal infrared (TIR) direct radiative effect (DRE). However, the magnitude of this DRE remains highly uncertain because our understanding of the radiative properties, quantitatively represented by the optical depth of dust, especially information on the TIR, remains limited. This study presents a simple approach to retrieve the thermal infrared dust aerosol optical depth (DAODTIR) over oceans during nighttime using the observations from the Infrared Imaging Radiometer (IIR) and the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) onboard CALIPSO. For each cloud-free dust-laden profile identified by the IIR-CALIOP observation, a Lookup-Table (LUT) of the 10.6 μm IIR band brightness temperatures difference (dBT) under different DAODTIR with respect to their dust-free BTs is constructed based on the CALIOP retrieved dust vertical profile and pre-assumed dust scattering properties using a fast radiative transfer model. Then the DAODTIR is retrieved by projecting the IIR-observed dBT on the LUT. Sensitivity studies show that the DAODTIR retrieval at 10.6 μm is more susceptible to the dust particle size distribution (PSD) assumption than dust refractive indices. To estimate the uncertainty caused by PSD assumption, two DAODTIR retrieval products, one based on the dust PSD from the AERONET at Cape Verde and the other on an in situ measured PSD from the recent Fennec campaign, are provided. The retrieval uncertainty is mainly contributed by the BT difference between the observation and simulation using auxiliary atmospheric data. The climatology of the retrieval from 2013 to 2019 shows confident spatiotemporal variations of DAODTIR with the global-averaged value of 0.006 and 0.008 based on different pre-assumed dust PSDs. Climatological results agree reasonably well with two independent DAODTIR retrieval products based on the Infrared Atmospheric Sounding Interferometer (IASI) over the active dust transport regions, such as North and Tropical Atlantic (r = 0.904 and 0.819) and Indian Ocean (r = 0.832). The seasonal and interannual variation is also well-compared (r = 0.758) with AERONET coarse-mode AOD at 97 selected sites. The synergic CALIOP observation allows the retrieved DAODTIR to directly compare with the extrapolated DAODTIR from DAOD in visible (i.e., 532 nm), which helps evaluate the observational constraints on DAODTIR. This study offers a unique prospect of collocating active lidar and passive IR observations for retrieving dust DAODTIR.

aerosol↗

NASA NTRS1993

Sensor fusion for assured vision in space applications

By using emittance and reflectance radiation models, the effects of angle of observation, polarization, and spectral content are analyzed to characterize the geometrical and physical properties--reflectivity, emissivity, orientation, dielectric properties, and roughness--of a sensed surface. Based on this analysis, the use of microwave, infrared, and optical sensing is investigated to assure the perception of surfaces on a typical lunar outpost. Also, the concept of employing several sensors on a lunar outpost is explored. An approach for efficient hardware implementation of the fused sensor systems is discussed.

Collin, Marie-France↗

NASA NTRS2007

The Solar Ultraviolet Magnetograph Investigation Sounding Rocket Program

This paper will describe the objectives of the Marshall Space Flight Center (MSFC) Solar Ultraviolet Magnetograph Investigation (SUMI) and the unique optical components that have been developed to meet those objectives. A sounding rocket payload has been developed to test the feasibility of magnetic field measurements in the Sun's transition region. The optics have been optimized for simultaneous measurements of two magnetic sensitive lines formed in the transition region (CIV at 1550 A and MgII at 2800 A). This paper will concentrate on the polarization properties SUMI's toroidal varied-line-space (TVLS) gratings and its system level testing as we prepare to launch in the Summer of 2008.

West, E. A.↗

NASA NTRSDate not supplied

The PACE-MAPP Polarized Ocean Bio-optical Model

The MAPP polarimeter retrieval algorithm, originally developed for the airborne NASA GISS Research Scanning Polarimeter, is being adapted to the PACE observing system to allow for a simultaneous retrieval of aerosol, thin cirrus, and ocean products using both PACE polarimeters and the OCI shortwave infrared channels. Here, we describe the polarized ocean bio-optical model we have developed for PACE-MAPP, which is designed to use a combination of homogenous and coated spheres to more accurately model the absorption and backscattering properties of algal and non-algal particles, and which also includes absorption by colored dissolved organic matter. We first use Lorenz-Mie computations to create lookup tables to accurately and efficiently characterize the optical properties of homogeneous and coated spheres embedded in water for PACE. We then use these lookup tables to develop a bio-optical model that consists of an external mixture of homogeneous (non-algal) and coated (algal) spheres. Lastly, we use the bio-optical model in forward radiative transfer computations to perform inversions of MODIS remote sensing reflectance for a variety of ocean regions. We explore the sensitivity of these inversions to ocean constituent inherent optical properties.

James Allen↗

NASA NTRSDate not supplied

Impacts of Aerosol and Cloud Variability on Satellite-Derived All-skies Direct Aerosol Radiative Effects (DARE) over the North and Southeast Atlantic

The Top-of-Atmosphere (TOA) Shortwave (SW) Direct Aerosol Radiative Effect (DARE) in all-sky conditions (i.e., aerosols in clear skies and aerosols above and below all types of clouds) is the global change in upwelling radiative flux due to aerosols. It is one of the strongest indicators of global climate change due to aerosols. SW DARE at TOA depends on the Earth’s surface albedo, cloud fraction, cloud optical properties, and aerosol optical properties, which are all challenging to accurately characterize from space. The overarching goals of our project are to provide state-of-the-art observational all-sky TOA SW DARE, along with guidance on which aerosol and/or cloud properties are the most important to measure, and at which spatio-temporal scales, for accurate DARE observations. We compute all-sky DARE based on state-of-the-art cloud and aerosol retrieval algorithms from CALIOP (Cloud–Aerosol Lidar with Orthogonal Polarization) and MODIS (Moderate Resolution Imaging spectroradiometer) satellite sensors, as well as aerosol intensive properties from MERRA-2 (Modern-Era Retrospective Analysis for Research and Applications, version 2) simulations over three specific regions of the Atlantic Ocean from 2012 to 2016. In this symposium, we present a characterization of the cloud and aerosol optical and physical properties and the observational TOA SW DARE along three individual satellite tracks in the Southeast Atlantic region -- on September 18 and 20, 2016 and August 13, 2017. We then quantify the impact of assuming homogeneous cloud or aerosol fields in space-based TOA SW DARE calculations. And, finally, the resulting space-based all-skies aerosol vertical distribution and DARE calculations are evaluated using remote sensing observations from coincident suborbital flights from the NASA ORACLES (the ObseRvations of Aerosols above CLouds and their intEractionS, ORACLES field campaign) field campaign. The NASA Atmospheric Observing System (AOS) mission addresses the NASA Aerosol, Cloud, Convection and Precipitation (ACCP) designated observables and proposes, as one of its aerosol objectives, to reduce uncertainties in estimates of global mean all-sky SW DARE at TOA. Well characterizing clouds, aerosol vertical distributions, aerosol types and associated all-skies DARE over the Atlantic Ocean will inform the AOS community on where, when, how, and how often the satellite retrievals should be performed to estimate DARE and reduce all-skies DARE uncertainties most accurately. These comprehensive characterizations will also identify the key regions and times when the AOS (or other ACCP-related) suborbital missions should be conducted to evaluate and improve the AOS space-based observations and retrievals.

aerosol↗

DOE OSTI2024

Spin-Controllable Dynamics in Defect-Engineered Carbon Nanotubes as Single Photon Emitters: Data-Driven Modeling and Computations

Quantum technologies, such as quantum computing and sensing, require efficient single-photon emission (SPE) sources that operate at room temperature in telecom wavelengths. While several materials can serve as SPE sources, no single platform meets all the criteria for efficiency, ambient operation, and scalability. Single-walled carbon nanotubes (SWCNTs) with covalently attached molecules offer a promising solution. Their SPE can be easily tuned via modifications of the SWCNT's diameter, chirality, and bonded molecules, enabling emission across near-IR to telecom wavelengths at ambient conditions. However, to fully realize the potential of SWCNTs and unlock their quantum capabilities, a deeper understanding of how structural defects from molecular adducts affect their emission and competing photoexcited processes is essential. To address this gap in our knowledge, this project combined quantum chemistry calculations with data-driven methods of cheminformatics (QSAR) and machine learning (ML). The developed computational approaches have provided several design strategies for covalent functionalization of SWCNTs to improve their optical response. The collaboration with Los Alamos National Lab (LANL) enabled direct comparison of computational and experimental data, facilitating method validation. This partnership was enhanced through access to LANL's Center for Integrated Nanotechnologies (CINT) utilizing User Facility Program and summer internships, which provided three NDSU graduate students with hands-on experience at LANL. The outcomes of this project included (1) Advancing the current stage of computational methods in accurate modeling of non-adiabatic spin-dependent photoexcited dynamics and its applicability to nanosystems consisting of thousands of atoms, realized as open-access codes linked to existing DFT-based software; (2) Establishing the relationship between the structure of adducts and SWCNTs and intrinsic excitonic and spin properties of defect states for guiding novel synthetic strategies and experimental probes of chemically functionalized SWCNTs as near-IR emitting materials; (3) Generating virtual libraries of hypothetical functionalized SWCNTs for virtual screening of their chemical structures and optical properties, leveraging new functionalities of SWCNTs; (4) Offering a unique experience for NDSU graduate students that prepared them for future scientific careers related to materials modeling and big data processing. These results were summarized in 12 published journal papers and 3 recently submitted papers. One of a key finding is that the position of defect sites on the SWCNT surface primarily drives the emission redshift (up to 100 meV), while the polarity of the defect-inducing molecules has a much smaller effect (~10 meV). However, the electron-donating or withdrawing properties of a molecule influence selecting reactivity of defect sites. These insights important for optimizing synthetic protocols for desired emissions in SWCNTs. We also revealed that the interaction between two defects at various positions on the SWCNT enhances the redshift and optical activity of states, favoring strong near-IR emission. This suggests that manipulations in defect concentrations is a promising strategy for controlling efficient emission. Mostly important, the defect position was found controllable by the spin states of photoexcited intermediates: Excited aromatic molecules form ortho defects with SWCNTs at their singlet states in the presence of oxygen, while oxygen-free conditions favor para defects via the triplet-state mechanism. Additionally, a heat-activated [2+2] cycloaddition reaction facilitates divalent defect formation with fewer bonding positions that narrows emission bands. These groundbreaking findings have been experimentally validated and significantly advance our understanding of defect chemistry in SWCNTs. Using a novel encoding technique and 3D-MoRSE descriptors, we developed highly accurate ML/QSAR models to predict both the 3D structure and optical properties of SWCNTs with chemical defects. This model enabled the creation of a virtual library of 125,556 structures, providing new insights into the relationship between SWCNT-defect structure and emission.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2023

Electrical, optical, and magnetic properties of amorphous yttrium iron oxide thin films and consequences for non-local resistance measurements

We present magnetic characterization, charge resistivity, and optical photoluminescence measurements on amorphous yttrium iron oxide thin films ( ⁠a-Y–Fe–O), with supporting comparisons to amorphous germanium (⁠ a-Ge) films. We measured magnetic properties with both SQUID magnetometry and polarized neutron reflectometry. These results not only confirm that a-Y–Fe–O is a disordered magnetic material with strong predominantly antiferromagnetic exchange interactions and a high degree of frustration, but also that it is best understood electrically as a disordered semiconductor. As with amorphous germanium, a-Y–Fe–O obeys expectations for variable-range hopping through localized electron states over a wide range of temperature. We also clarify the consequences of charge transport through such a semiconducting medium for non-local voltage measurements intended to probe spin transport in nominally insulating magnetic materials. We further compare non-local resistance measurements made with “quasi-dc” automated current reversal to ac measurements made with a lock-in amplifier. These show that the “quasi-dc” measurement has an effective ac current excitation with frequency up to approximately 22 Hz, and that this effective ac excitation can cause artifacts in these measurements including incorrect sign of the non-local resistance. Here, this comprehensive investigation of non-local resistance measurements in a-Y–Fe–O shows no evidence of spin transport on micrometer length scales, which is contrary to our original work, and in line with more recent investigations by other groups.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS1991

Optical and structural characterization of InAs/GaAs quantum wells

Three InAs/GaAs single quantum wells of two-, three-, and four-monolayer thickness were characterized using optical and structural techniques. The results of high-resolution transmission electron (HRTEM) microscopy and optical studies which combine absorption, photoluminescence (PL), photoreflectance, and cathodoluminescence are presented. Using the polarization modulated absorptance technique, we observed two absorption features in our samples at 77 K. On the basis of their polarization properties and comparison with an envelope function calculation, these structures are assigned to transitions between the confined heavy-hole and confined and unconfined electron levels. Photoreflectance spectra of the three-monolayer sample in 77-300 K range show only the fundamental quantum well transition. The temperature dependence of this transition is approximately linear with a slope of 2.2 x 10 exp -4 eV/K, which is significantly lower than in both constituent materials. Comparison to the absorption data reveals that the PL spectra are affected by the carrier diffusion and therefore do not provide direct measure of the exciton density of states. The HRTEM images indicate that, while the interfaces of the two-monolayer sample are smooth and the well thickness is uniform, the four-monolayer sample has uneven interfaces and contains domains of two, three, and four monolayers.

Ksendzov, A.↗

NASA NTRSDate not supplied

CALIGOLA: A New Spaceborne Lidar Mission

Agenzia Spaziale Italiana (ASI) and NASA are partnering on an exciting new spaceborne lidar mission known as CALIGOLA (i.e., the Cloud and Aerosol Lidar for Global Scale observations of the Ocean-Land-Atmosphere) that seeks to significantly advance our understanding of Earth’s coupled ocean-land-atmosphere systems. By flying an innovative multi-wavelength, polarization-sensitive Raman lidar that will simultaneously acquire elastic backscatter and fluorescence measurements, CALIGOLA will provide new insights into the processes that influence climate, weather, and air quality by vertically profiling microphysical and optical properties of clouds and aerosols. The mission will also probe phytoplankton biomass and zooplankton dynamics and provide observations of surface vegetation, ice, and snow. The mission is planned for launch early next decade and baselined to fly in an orbit that is compatible with NASA’s AOS-Sky mission. This formation flying configuration will enable synergistic retrievals between observations from CALIGOLA and the polarimeter and radar measurements planned for AOS-Sky and thus greatly enhance our ability to explore and characterize the intricate processes that govern the interactions between different components of the Earth system. The presentation will highlight CALIGOLA’s significant science objectives and describe the pioneering instrument that will enable us to achieve these objectives.

Chip Trepte↗

DOE OSTI2023

Voltage‐Modulated Untwist Deformations and Multispectral Optical Effects from Ion Intercalation into Chiral Ceramic Nanoparticles

Abstract Reconfiguration of chiral ceramic nanostructures after ion intercalation should favor specific nanoscale twists leading to strong chiroptical effects. In this work, V 2 O 3 nanoparticles are shown to have “built‐in” chiral distortions caused by binding of tartaric acid enantiomers to the nanoparticle surface. As evidenced by spectroscopy/microscopy techniques and calculations of nanoscale chirality measures, the intercalation of Zn 2+ ions into the V 2 O 3 lattice results in particle expansion, untwist deformations, and chirality reduction. Coherent deformations in the particle ensemble manifest as changes in sign and positions of circular polarization bands at ultraviolet, visible, mid‐infrared (IR), near‐IR (NIR), and IR wavelengths. The g‐ factors observed for IR and NIR spectral diapasons are ≈100–400 times higher than those for previously reported dielectric, semiconductor, and plasmonic nanoparticles. Nanocomposite films layer‐by‐layer assembled (LBL) from V 2 O 3 nanoparticles reveal cyclic‐voltage‐driven modulation of optical activity. Device prototypes for IR and NIR range problematic for liquid crystals and other organic materials are demonstrated. High optical activity, synthetic simplicity, sustainable processability, and environmental robustness of the chiral LBL nanocomposites provide a versatile platform for photonic devices. Similar reconfigurations of particle shapes are expected for multiple chiral ceramic nanostructures, leading to unique optical, electrical, and magnetic properties.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Ti‐Modified Imogolite Nanotubes as Promising Photocatalyst 1D Nanostructures for H 2 Production

Imogolite nanotubes (INTs) are predicted as a unique 1D material with spatial separation of conduction and valence band edges but their large band gaps have inhibited their use as photocatalysts. The first step toward using these NTs in photocatalysis and exploiting the polarization-promoted charge separation across their walls is to reduce their band gap. Here, the modification of double-walled aluminogermanate INTs by incorporation of titanium into the NT walls is explored. The precursor ratio x = [Ti]/([Ge]+[Ti]) is modulated between 0 and 1. Structural and optical properties are determined at different scales and the photocatalytic performance is evaluated for H 2 production. Although the incorporation of Ti atoms into the structure remains limited, the optimal condition is found around x = 0.4 for which the resulting NTs reveal a remarkable hydrogen production of ≈1500 µmol g −1 after 5 h for a noble metal-free photocatalyst, a 65-fold increase relative to a commercial TiO 2 -P25. This is correlated to a lowering of the recombination rate of photogenerated charge carriers for the most active structures. These results confirm the theoretical predictions regarding the potential of modified INTs as photoactive nanoreactors and pave the way for investigating and exploiting their polarization properties for energy applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Properties of V-defect injectors in long wavelength GaN LEDs studied by near-field electro- and photoluminescence

The efficiency of multiple quantum well (QW) light emitting diodes (LEDs) to a large degree depends on uniformity of hole distribution between the QWs. Typically, transport between the QWs takes place via carrier capture into and thermionic emission out of the QWs. In InGaN/GaN QWs, the thermionic hole transport is hindered by the high quantum confinement and polarization barriers. To overcome this drawback, hole injection through semipolar QWs located at sidewalls of V-defects had been proposed. However, in the case of the V-defect injection, strong lateral emission variations take place. In this work, we explore the nature of these variations and the impact of the V-defects on the emission spectra and carrier dynamics. The study was performed by mapping electroluminescence (EL) and photoluminescence (PL) with a scanning near-field optical microscope in LEDs that contain a deeper well that can only be populated by holes through the V-defects. Applying different excitation schemes (electrical injection and optical excitation in the far- and near-field), we have shown that the EL intensity variations are caused by the lateral nonuniformity of the hole injection. We have also found that, in biased structures, the PL intensity and decay time in the V-defect regions are only moderately lower that in the V-defect-free regions thus showing no evidence of an efficient Shockley-–Read–Hall recombination. In the V-defect regions, the emission spectra experience a red shift and increased broadening, which suggests an increase of the In content and well width in the polar QWs close to the V-defects.

Electroluminescence↗

DOE OSTI2024

Phase-Selective Synthesis of Rhombohedral WS 2 Multilayers by Confined-Space Hybrid Metal–Organic Chemical Vapor Deposition

Rhombohedral polytype transition metal dichalcogenide (TMDC) multilayers exhibit non-centrosymmetric interlayer stacking, which yields intriguing properties such as ferroelectricity, a large second-order susceptibility coefficient χ (2) , giant valley coherence, and a bulk photovoltaic effect. These properties have spurred significant interest in developing phase-selective growth methods for multilayer rhombohedral TMDC films. Here, in this study, we report a confined-space, hybrid metal–organic chemical vapor deposition method that preferentially grows 3R-WS 2 multilayer films with thickness up to 130 nm. We confirm the 3R stacking structure via polarization-resolved second-harmonic generation characterization and the 3-fold symmetry revealed by anisotropic H 2 O 2 etching. The multilayer 3R WS 2 shows a dendritic morphology, which is indicative of diffusion-limited growth. Multilayer regions with large, stepped terraces enable layer-resolved evaluation of the optical properties of 3R-WS 2 via Raman, photoluminescence, and differential reflectance spectroscopy. These measurements confirm the interfacial quality and suggest ferroelectric modification of the exciton energies.

3R-WS2↗