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Results for “Circular dichroism spectroscopy”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Origins of electronic bands in the antiferromagnetic topological insulator MnBi 2 Te 4

Despite the rapid progress in understanding the first intrinsic magnetic topological insulator MnBi 2 Te 4 , its electronic structure remains a topic under debates. In this work, we perform a thorough spectroscopic investigation into the electronic structure of MnBi 2 Te 4 via laser-based angle-resolved photoemission spectroscopy. Through quantitative analysis, we estimate an upper bound of 3 meV for the gap size of the topological surface state. Furthermore, our circular dichroism measurements reveal band chiralities for both the topological surface state and quasi-2D bands, which can be well reproduced in a band hybridization model. A numerical simulation of energy-momentum dispersions based on a four-band model with an additional step potential near the surface provides a promising explanation for the origin of the quasi-2D bands. Our study represents a solid step forward in reconciling the existing controversies in the electronic structure of MnBi 2 Te 4 , and provides an important framework to understand the electronic structures of other relevant topological materials MnBi 2n Te 3n+1 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

A fully contained sample holder capable of electron-yield detection at soft X-ray energies

A holder has been developed that enables electron yield-detected soft X-ray spectroscopy of fully contained samples at low temperature. Crucially, this design uses elements of the sample containment to collect ejected electrons, removing the need to expose samples directly to the vacuum environment of the spectrometer. The design is modular and should be adaptable to a number of different endstation configurations, enabling spectroscopy of air-sensitive, radioactive and vacuum-sensitive (biological) samples.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Mid-infrared chiral metasurface absorbers with split-ellipse structures

Natural chiral materials usually have very weak circular dichroism (CD) responses. Here, in this study, we design and demonstrate one type of mid-infrared chiral metasurface absorber with strong chiroptical effects, which can achieve high CD in absorption above 0.57 over the wavelength range of 5 to 5.9 μm. The maximum absorption of the chiral metasurface absorber under circularly polarized light can reach 0.90 and the maximum CD in absorption is 0.63. Meanwhile, the chiral resonance wavelength and the CD value can be tuned by varying the geometric parameters of the metasurface. A thermal analysis of the metasurface absorber further shows the strong connection between CD in absorption and temperature difference. The demonstrated chiral metasurface absorbers can be used in many promising applications such as molecular sensing, thermophotovoltaics and chiral spectroscopy.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Room-temperature intrinsic ferromagnetism in epitaxial CrTe 2 ultrathin films

While the discovery of two-dimensional (2D) magnets opens the door for fundamental physics and next-generation spintronics, it is technically challenging to achieve the room-temperature ferromagnetic (FM) order in a way compatible with potential device applications. Here in this paper, we report the growth and properties of single- and few-layer CrTe 2 , a van der Waals (vdW) material, on bilayer graphene by molecular beam epitaxy (MBE). Intrinsic ferromagnetism with a Curie temperature (TC) up to 300 K, an atomic magnetic moment of ~0.21 μ B /Cr and perpendicular magnetic anisotropy (PMA) constant (K u ) of 4.89 × 10 5 erg/cm 3 at room temperature in these few-monolayer films have been unambiguously evidenced by superconducting quantum interference device and X-ray magnetic circular dichroism. This intrinsic ferromagnetism has also been identified by the splitting of majority and minority band dispersions with ~0.2 eV at Г point using angle-resolved photoemission spectroscopy. The FM order is preserved with the film thickness down to a monolayer (T C ~ 200 K), benefiting from the strong PMA and weak interlayer coupling. The successful MBE growth of 2D FM CrTe 2 films with room-temperature ferromagnetism opens a new avenue for developing large-scale 2D magnet-based spintronics devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

Revealing the two-dimensional electronic structure and anisotropic superconductivity in a natural van der Waals superlattice (PbSe) 1.14 NbSe 2

Van der Waals superlattices are important for tailoring the electronic structures and properties of layered materials. Here we report the superconducting properties and electronic structure of a natural van der Waals superlattice (PbSe) 1.14 NbSe 2 . Anisotropic superconductivity with a transition temperature T c = 5.6 ± 0.1 K, which is higher than monolayer NbSe 2 , is revealed by transport measurements on high-quality samples. Angle-resolved photoemission spectroscopy (ARPES) measurements reveal the two-dimensional electronic structure and a charge transfer of 0.43 electrons per NbSe 2 unit cell from the blocking PbSe layer. In addition, polarization-dependent ARPES measurements reveal a significant circular dichroism with opposite contrast at K and K' valleys, suggesting a significant spin-orbital coupling and distinct orbital angular momentum. In conclusion, our work suggests natural van der Waals superlattice as an effective pathway for achieving intriguing properties distinct from both the bulk and monolayer samples.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Emergent flat band electronic structure in a VSe 2 /Bi 2 Se 3 heterostructure

Flat band electronic states are proposed to be a fundamental tool to achieve various quantum states of matter at higher temperatures due to the enhanced electronic correlations. However, materials with such peculiar electronic states are rare and often rely on subtle properties of the band structures. Here, by using angle-resolved photoemission spectroscopy, we show the emergent flat band in a VSe 2 / Bi 2 Se 3 heterostructure. Our photoemission study demonstrates that the flat band covers the entire Brillouin zone and exhibits 2D nature with a complex circular dichroism. In addition, the Dirac cone of Bi 2 Se 3 is not reshaped by the flat band even though they overlap in proximity of the Dirac point. These features make this flat band distinguishable from the ones previously found. Thereby, the observation of a flat band in the VSe 2 / Bi 2 Se 3 heterostructure opens a promising pathway to realize strongly correlated quantum effects in topological materials.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Magnetic Control of Soft Chiral Phonons in PbTe

We report PbTe crystals have a soft transverse optical phonon mode in the terahertz frequency range, which is known to efficiently decay into heat-carrying acoustic phonons, resulting in anomalously low thermal conductivity. Here, we studied this phonon via polarization-dependent terahertz spectroscopy. We observed softening of this mode with decreasing temperature, indicative of incipient ferroelectricity, which we explain through a model including strong anharmonicity with a quartic displacement term. In magnetic fields up to 25 T, the phonon mode splits into two modes with opposite handedness, exhibiting circular dichroism. Their frequencies display Zeeman splitting together with an overall diamagnetic shift with increasing magnetic field. Using a group-theoretical approach, we demonstrate that these observations are the result of magnetic field-induced morphic changes in the crystal symmetries through the Lorentz force exerted on the lattice ions. Thus, our Letter reveals a novel process of controlling phonon properties in a soft ionic lattice by a strong magnetic field.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Inhomogeneity in electronic phase and flat band in magnetic kagome metal Co 3 Sn 2 S 2

Co 3 Sn 2 S 2 has been reported to be a Weyl semimetal with c-axis ferromagnetism below a Curie temperature of 177 K. Despite the large interest in Co 3 Sn 2 S 2 , the magnetic structure is still unclear. Recent studies have challenged the magnetic phase diagram of Co 3 Sn 2 S 2 by reporting unusual magnetic phases including the presence of exchange bias. Here we show, using X-ray Magnetic Circular Dichroism, a shift in the magnetization hysteresis loop, reminiscent of exchange bias and establish that the magnetic moment in Co arises from the spin, with negligible orbital moment. At 6 K, using spatially-resolved angle-resolved photoemission spectroscopy, we detect a butterfly-shaped electronic band structure at small regions of the sample distinct from the known ferromagnetic band structure. Our density functional theory calculations suggest that the butterfly bands correspond to an antiferromagnetic phase. Separately, we detect a sharp flat band at the Fermi level at some regions in the sample, which we attribute to a surface state. These different electronic states found in a stoichiometric intermetallic invite further efforts to explore the origin and nature of the electronic inhomogeneity associated to magnetism on the mesoscale.

Electronic properties and materials↗
DOE OSTI2024

High-Resolution Frequency-Domain Spectroscopic and Modeling Studies of Photosystem I (PSI), PSI Mutants and PSI Supercomplexes

Photosystem I (PSI) is one of the two main pigment–protein complexes where the primary steps of oxygenic photosynthesis take place. This review describes low-temperature frequency-domain experiments (absorption, emission, circular dichroism, resonant and non-resonant hole-burned spectra) and modeling efforts reported for PSI in recent years. In particular, we focus on the spectral hole-burning studies, which are not as common in photosynthesis research as the time-domain spectroscopies. Experimental and modeling data obtained for trimeric cyanobacterial Photosystem I (PSI 3 ), PSI 3 mutants, and PSI 3 –IsiA 18 supercomplexes are analyzed to provide a more comprehensive understanding of their excitonic structure and excitation energy transfer (EET) processes. Detailed information on the excitonic structure of photosynthetic complexes is essential to determine the structure–function relationship. We will focus on the so-called “red antenna states” of cyanobacterial PSI, as these states play an important role in photochemical processes and EET pathways. The high-resolution data and modeling studies presented here provide additional information on the energetics of the lowest energy states and their chlorophyll (Chl) compositions, as well as the EET pathways and how they are altered by mutations. We present evidence that the low-energy traps observed in PSI are excitonically coupled states with significant charge-transfer (CT) character. The analysis presented for various optical spectra of PSI 3 and PSI 3 -IsiA 18 supercomplexes allowed us to make inferences about EET from the IsiA 18 ring to the PSI 3 core and demonstrate that the number of entry points varies between sample preparations studied by different groups. In our most recent samples, there most likely are three entry points for EET from the IsiA 18 ring per the PSI core monomer, with two of these entry points likely being located next to each other. Therefore, there are nine entry points from the IsiA 18 ring to the PSI 3 trimer. We anticipate that the data discussed below will stimulate further research in this area, providing even more insight into the structure-based models of these important cyanobacterial photosystems.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2024

Spontaneous Chirality Flipping in an Orthogonal Spin-Charge Ordered Topological Magnet

The asymmetric distribution of chiral objects with opposite chirality is of great fundamental interest ranging from molecular biology to particle physics. In quantum materials, chiral states can build on inversion-symmetry-breaking lattice structures or emerge from spontaneous magnetic ordering induced by competing interactions. Although the handedness of a chiral state can be changed through external fields, a spontaneous chirality flipping has yet to be discovered. We present experimental evidence of chirality flipping via changing temperature in a topological magnet EuAl 4 , which features orthogonal spin density waves (SDW) and charge density waves (CDW). Using circular dichroism of Bragg peaks in the resonant magnetic x-ray scattering, we find that the chirality of the helical SDW flips through a first-order phase transition with modified SDW wavelength. Intriguingly, we observe that the CDW couples strongly with the SDW and displays a rare commensurate-to-incommensurate transition at the chirality flipping temperature. Combining with first-principles calculations and angle-resolved photoemission spectroscopy, our results support a Fermi surface origin of the helical SDW with intertwined spin, charge, and lattice degrees of freedom in EuAl 4 . Our results reveal an unprecedented spontaneous chirality flipping and lay the groundwork for a new functional manipulation of chirality through momentum-dependent spin-charge-lattice interactions. Published by the American Physical Society 2024

3-dimensional systems↗
DOE OSTI2020

Magnetism of Ir 5 + -based double perovskites: Unraveling its nature and the influence of structure

A combination of x-ray-diffraction, x-ray absorption, x-ray magnetic circular dichroism, macroscopic magnetization, and muon-spin relaxation measurements is used to investigate the interplay between structure (both crystallography and microstructure) and magnetism in Sr 2 YIrO 6 as a function of both chemical (Ca-doping) and physical (hydrostatic) pressure. X-ray absorption spectroscopy clearly shows that the physical pressure is more effective in modifying the structure. On the other hand, the dichroic measurements evidence a constant magnetic signal with physical pressure and strong differences with Ca-doping. Muon-spin relaxation reveals the presence of magnetic order, even when this is hidden in the magnetization data. From the combined analysis, the magnetic results are explained in terms of the presence of Ir 6+ or Ir 4+ ions in magnetic clusters, most likely located at and triggered by antisite disorder. The measurements under high physical pressure indicate that the magnetic state is independent of the crystallographic details such as Ir-O distances and Ir-O-Y angles.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Probing the tunability of magnetism with external pressure in metastable Sr 2 NiIrO 6 double perovskite

In Sr 2 NiIrO 6 long-range Ir-Ir antiferromagnetic exchange interactions have been reported to overcome the ferromagnetic Ni-Ir interactions hampering the otherwise expected ferromagnetic behavior. Prompted by this, a combination of x-ray absorption spectroscopy and x-ray diffraction at high pressure is used here to investigate the interplay between the magnetic structure of the Ir sublattice and lattice degrees of freedom. In this work, the compression of Sr 2 NiIrO 6 drives an unexpected nonmonotonic change of the x-ray magnetic circular dichroism (XMCD) spectra: The intensity first decreases in the 0- to 18-GPa range, then shows an increase in the 18- to 30-GPa range and again decreases for higher pressures. The XMCD intensity, a measure of the net magnetization in the Ir sublattice, however, is found to remain very low in the whole pressure range so the observed changes do not correspond with a transition from antiferromagnetic to ferromagnetic or ferrimagnetic order. The evolution of the XMCD is better explained in terms of a weakening/strengthening of the long-range antiferromagnetic (AFM) IrIr interaction between ferromagnetic planes associated with the reduction of the lattice parameters. In particular, a correlation can be established between the evolution of the b/a ratio and the weakening/strengthening of the AFM interaction.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Raman and Terahertz Spectroscopy of Low-Frequency Chiral Phonons in Amino Acids

Chiral phonons are mirror-symmetric vibrations with nonzero angular momenta that correspond to twisting and rotational motions of multiple atoms. In chiral crystals, these include low-energy terahertz (THz)-range vibrations of the molecular segments involving dozens of atoms with energies sensitive to molecular chirality. Here, we present spectral signatures of chiral phonons in circularly polarized Raman optical activity (ROA) spectra from enantiomers of amino acid crystals. Along with complementary THz circular dichroism (TCD) measurements, our ROA data reveal several vibrational bands in enantiomers of valine, alanine, tyrosine, and proline between 30 and 150 cm –1 (∼1–4.5 THz) that exhibit opposite intensities. Density functional theory calculations confirm their assignment to twisting and shearing molecular motions. The simultaneous registration of chiral phonon modes by ROA and TCD demonstrates the necessity of these complementary techniques to identify complex mirror-asymmetric vibrational modes and offers new insights into their interactions with circularly polarized light.

36 MATERIALS SCIENCE↗
DOE OSTI2024

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↗
NASA NTRS2020

UV/Vis+ Photochemistry Database: Structure, Content and Applications

The “science-softCon UV/Vis+ Photochemistry Database” (www.photochemistry.org) is a large and comprehensive collection of EUV-VUV-UV–Vis-NIR spectral data and other photochemical information assembled from published peer-reviewed papers. The database contains photochemical data including absorption, fluorescence, photoelectron, and circular and linear dichroism spectra, as well as quantum yields and photolysis related data that are critically needed in many scientific disciplines. This manuscript gives an outline regarding the structure and content of the “science-softCon UV/Vis+ Photochemistry Database”. The accurate and reliable molecular level information provided in this database is fundamental in nature and helps in proceeding further to understand photon, electron and ion induced chemistry of molecules of interest not only in spectroscopy, astrochemistry, astrophysics, Earth and planetary sciences, environmental chemistry, plasma physics, combustion chemistry but also in applied fields such as medical diagnostics, pharmaceutical sciences, biochemistry, agriculture, and catalysis. In order to illustrate this, we illustrate the use of the UV/Vis+ Photochemistry Database in four different fields of scientific endeavor.

Photochemistry↗
DOE OSTI2024

Nanoscale polarization transient gratings

Light manipulation at the nanoscale is essential both for fundamental science and modern technology. The quest to shorter lengthscales, however, requires the use of light wavelengths beyond the visible. In particular, in the extreme ultraviolet regime these manipulation capabilities are hampered by the lack of efficient optics, especially for polarization control. Here, we present a method to create periodic, polarization modulations at the nanoscale using a tailored configuration of the FERMI free electron laser and demonstrate its capabilities by comparing the dynamics induced by this polarization transient grating with those driven by a conventional intensity grating on a thin ferrimagnetic alloy. While the intensity grating signal is dominated by the thermoelastic response, the polarization grating excitation minimizes it, uncovering helicity-dependent responses previously undetected. We anticipate nanoscale polarization transient gratings to become useful for the study of physical, chemical and biological systems possessing chiral symmetry.

36 MATERIALS SCIENCE↗