Tetraarylcyclobutadienecyclopentadienylcobalt Complexes: Synthesis, Electronic Spectra, Magnetic Circular Dichroism, Linear Dichroism, and TD DFT Calculations
N/A
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
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Linear dichroism of DNA: Characterization of the orientation distribution function caused by hydrodynamic shear
Linear dichroism provides information on the orientation of chromophores part of, or bound to, an orientable molecule such as DNA. For molecular alignment induced by hydrodynamic shear, the principal axes orthogonal to the direction of alignment are not equivalent. Thus, the magnitude of the flow-induced change in absorption for light polarized parallel to the direction of flow can be more than a factor of two greater than the corresponding change for light polarized perpendicular to both that direction and the shear axis. The ratio of the two flow-induced changes in absorption, the dichroic increment ratio, is characterized using the orthogonal orientation model, which assumes that each absorbing unit is aligned parallel to one of the principal axes of the apparatus. The absorption of the alienable molecules is characterized by components parallel and perpendicular to the orientable axis of the molecule. The dichroic increment ratio indicates that for the alignment of DNA in rectangular flow cells, average alignment is not uniaxial, but for higher shear, as produced in a Couette cell, it can be. The results from the simple model are identical to tensor models for typical experimental configuration. Approaches for measuring the dichroic increment ratio with modern dichrometers are further discussed.
59 BASIC BIOLOGICAL SCIENCES↗
X-ray Linear Dichroism in Apatite
The recent observation in parrotfish teeth of X-ray linear dichroism motivated an in-depth investigation into this spectroscopic effect in various apatite crystals, including geologic hydroxyapatite (Ca 5 (PO 4 ) 3 OH), fluorapatite (Ca 5 (PO 4 ) 3 F), and their biogenic counterparts in human bone, mouse enamel, and in parrotfish bone, dentin, and enameloid, the equivalent of dental enamel in certain fish. These data are important because they now enable visualization of the nano- to microscale structure of apatite crystals in teeth and bone. Polarization-dependent imaging contrast (PIC) maps of lamellar bone, obtained with a new method that minimizes space-charge and charging effects, show the expected rotating apatite crystal orientations. PIC maps of mouse enamel reveal a complex arrangement of hydroxyapatite crystals perpendicular to the dentin-enamel junction, with rods arranged in a decussation pattern in inner enamel and nearly parallel to one another in outer enamel. In both inner and outer enamel crystal c-axes are not always aligned with the rod elongation direction.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
THz and Mid-Infrared Linear Dichroism in the High Tc Superconductor La2-xSrxCuO4
We measure the rotation of the linear polarization of light that is transmitted through a high Tc superconductor film as a function of sample orientation. We observe a linear dichroism signal over the entire probing range from 2 to 230 meV, which is consistent with anisotropic in-plane conductivity. The La2- xSrxCuO4 thin film sample is epitaxially constrained to be tetragonal, so the symmetry breaking is purely electronic.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Linear dichroism and the nature of charge order in underdoped cuprates
Recent experiments have addressed the nature of the charge order seen in underdoped cuprates. In this paper, I show that x-ray absorption and linear dichroism are excellent probes of such order. Ab initio calculations reveal that a d-wave charge density wave order involving the oxygen ions is a much better description of the data than alternate models.
36 MATERIALS SCIENCE↗
Observation of Giant Optical Linear Dichroism in a Zigzag Antiferromagnet FePS 3
Direct optical probing of the antiferromagnetic order parameter in atomically thin samples is challenging, for example, via magneto-optical spectroscopy, due to the lack of net magnetization. Here, we report zigzag-antiferromagnetism (AFM) induced optical linear dichroism (LD) in layered transition-metal thiophosphate FePS3 down to the monolayer limit. The observed LD is giant despite having the optical wave vector parallel to the Neel vector. The LD is at least one order of magnitude larger than those reported in other antiferromagnetic systems, where the optical wave vector is orthogonal to the Neel vector. The large LD enables the probe of 60 degrees orientated zigzag-AFM domains. The optical anisotropy in FePS 3 originates from an electronic anisotropy associated with the zigzag direction of the AFM order and is independent of the spin-pointing direction. Furthermore, our findings point to a new optical approach for the investigation and control of zigzag or stripe magnetic order in strongly correlated systems.
2D magnet↗
Absence of magnetic order in epitaxial RuO 2 revealed by x-ray linear dichroism
Recently the topic of altermagnetism has attracted tremendous attention, and RuO 2 has been demonstrated to be one of the most promising altermagnetic candidates. However, disputes still remain on the existence of magnetic order in RuO 2 . Here in this work, we employ x-ray linear dichroism (XLD), a widely utilized technique for characterizing antiferromagnets, in conjunction with photoemission electron microscopy and multiple scattering calculation to provide clear evidence of the absence of magnetic order in epitaxial RuO 2 films. The observed XLD signal is nearly invariant with temperature and independent of cooling-field direction, in stark contrast to the substantial magnetic-order-related XLD signal predicted by multiple scattering calculation. This finding strongly suggests a nonmagnetic origin for RuO 2 . Furthermore, we observed significantly distinct XLD signals at the Ru M 3 and O K edges in RuO 2 films grown on TiO 2 substrate with different surface orientations, which can be attributed to the low-symmetry crystal field. In conclusion, these results unequivocally demonstrate the absence of magnetic order in RuO 2 and establish XLD measurement as a robust technique for probing the low-symmetry magnetic materials.
Wang, Siyu [University of Science and Technology o↗
Linear Dichroism of the Optical Properties of SnS and SnSe Van der Waals Crystals
Abstract Tin monochalcogenides SnS and SnSe, belonging to a family of Van der Waals crystals isoelectronic to black phosphorus, are known as environmentally friendly materials promising for thermoelectric conversion applications. However, they exhibit other desired functionalities, such as intrinsic linear dichroism of the optical and electronic properties originating from strongly anisotropic orthorhombic crystal structures. This property makes them perfect candidates for polarization‐sensitive photodetectors working in near‐infrared spectral range. A comprehensive study of the SnS and SnSe crystals is presented, performed by means of optical spectroscopy and photoemission spectroscopy, supported by ab initio calculations. The studies reveal the high sensitivity of the optical response of both materials to the incident light polarization, which is interpreted in terms of the electronic band dispersion and orbital composition of the electronic bands, dictating the selection rules. From the photoemission investigation the ionization potential, electron affinity and work function are determined, which are parameters crucial for the design of devices based on semiconductor heterostructures.
Chemistry↗
Linear dichroism infrared resonance in overdoped, underdoped, and optimally doped cuprate superconductors
By measuring the polarization changes in terahertz, infrared, and visible radiation over an extended energy range (3–2330 meV), we observe symmetry breaking in cuprate high-temperature superconductors over wide energy, doping, and temperature ranges. We measure the polarization rotation (Re[$θ_F$]) and ellipticity (Im[$θ_F$]) of transmitted radiation through thin films as the sample is rotated. We observe a twofold rotational symmetry in $θ_F$, which is associated with linear dichroism (LD) and occurs when electromagnetic radiation polarized along one direction is absorbed more strongly than radiation polarized in the perpendicular direction. Such polarization anisotropies can be generally associated with symmetry breakings. We measure the amplitude of the LD signal and study its temperature, energy, and doping dependence. The LD signal shows a resonant behavior with a peak in the few hundred meV range, which is coincident with the midinfrared optical feature that has been associated with the formation of the pseudogap state. In this work, the strongest LD signal is found in underdoped films, although it is also observed in optimally and overdoped samples. The LD signal is consistent with an electronic nematic order which is decoupled from the crystallographic axes as well as novel magnetoelectric effects.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Highly Anisotropic Drude-Weight-Reduction and Enhanced Linear-Dichroism in van der Waals Weyl Semimetal T d -MoTe 2 with Coherent Interlayer Electronic Transport
Weyl semimetal (WSM) states can be achieved by breaking spatial-inversion symmetry or time reversal symmetry. However, the anisotropy of the energy reduction contributing to the emergence of WSM states has seldom been investigated by experiments. A van der Waals metal MoTe 2 exhibits a type-II WSM phase below the monoclinic-to-orthorhombic-phase-transition temperature T c ~ 250 K. Here, in this work, a combined linearly polarized optical-spectroscopy and electrical-transport study of MoTe 2 is reported at different temperatures. The Drude components in the a-axis, b-axis, and c-axis optical conductivity spectra, together with the metallic out-of-plane and in-plane electrical resistivities, indicate the coherent inter-layer and in-plane charge transports. Moreover, the Drude weight in σ 1a (ω), rather than the Drude weights in σ 1b (ω) and σ 1c (ω), decreases dramatically below T c , which exhibits a highly anisotropic decrease in its Drude weight and thus suggests a strongly anisotropic reduction of the electronic kinetic energy in the WSM phase. Furthermore, below T c , due to the in-plane anisotropic spectral-weight transfer from Drude component to high-energy region, the in-plane inter-band-absorption anisotropy increases remarkably ≈770 meV, and has the largest value (≈0.68) of normalized linear dichroism among the reported type-II WSMs. The work sheds light on seeking new WSMs and developing novel photonic devices based on WSMs.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Unveiling the orbital texture of 1T-TiTe 2 using intrinsic linear dichroism in multidimensional photoemission spectroscopy
The momentum-dependent orbital character in crystalline solids, referred to as orbital texture, is of capital importance in the emergence of symmetry-broken collective phases, such as charge density waves as well as superconducting and topological states of matter. By performing extreme ultraviolet multidimensional angle-resolved photoemission spectroscopy for two different crystal orientations linked to each other by mirror symmetry, we isolate and identify the role of orbital texture in photoemission from the transition metal dichalcogenide 1T-TiTe 2 . By comparing our experimental results with theoretical calculations based on both a quantitative one-step model of photoemission and an intuitive tight-binding model, we unambiguously demonstrate the link between the momentum-dependent orbital orientation and the emergence of strong intrinsic linear dichroism in the photoelectron angular distributions. Our results represent an important step towards going beyond band structure (eigenvalues) mapping and learning about electronic wavefunction and orbital texture of solids by exploiting matrix element effects in photoemission spectroscopy.
36 MATERIALS SCIENCE↗
Mid-wave and Long-Wave Infrared Linear Dichroism in a Hexagonal Perovskite Chalcogenide
Not provided.
Chemistry↗
Charge Carrier Screening in Photoexcited Epitaxial Semiconductor Nanorods Revealed by Transient X-ray Absorption Linear Dichroism
Not Available
77 NANOSCIENCE AND NANOTECHNOLOGY↗
Direct observation of temperature dependent magnetic domain structure of the multiferroic La{sub 0.66}Sr{sub 0.34}MnO{sub 3}/BiFeO{sub 3} bilayer system by x-ray linear dichroism- and x-ray magnetic circular dichroism-photoemission electron microscopy
Low-thickness La{sub 0.66}Sr{sub 0.34}MnO{sub 3} (LSMO)/BiFeO{sub 3} (BFO) thin film samples deposited on SrTiO{sub 3} were imaged by high resolution x-ray microscopy at different temperatures. The ultra-thin thickness of the top layer allows to image both the ferromagnetic domain structure of LSMO and the multiferroic domain structure of the buried BFO layer, opening a path to a direct observation of coupling at the interface on a microscopic level. By comparing the domain size and structure of the BFO and LSMO, we observed that, in contrast to LSMO single layers, LSMO/BFO multilayers show a strong temperature dependence of the ferromagnetic domain structure of the LSMO. Particularly, at 40 K, a similar domain size for BFO and LSMO is observed. This indicates a persistence of exchange coupling on the microscopic scale at a temperature, where the exchange bias as determined by magnetometer measurements is vanishing.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Insights into the electronic structure of Co 2 FeSi from x-ray magnetic linear dichroism
Not Available
Meinert, Markus↗
Testing the possibility of magnetic domain imaging based on circular & linear dichroism using photoemission electron microscopy
In recent years, an increasing number of memory and spintronic devices have been developed exploiting the combination of ferromagnetic (FM) and anti-ferromagnetic (aFM) materials. Consequently, magnetic imaging based on continuous-wave (CW) ultraviolet (UV) (λ = 266nm and longer wavelength) photoemission electron microscopy (PEEM) is gaining considerable attention due to the possibility of determining magnetizations for FM and aFM materials with 10 nm lateral resolution at video rate image acquisition. This PEEM-based approach exploits the polarization-dependent photoemission yield, which is subject to the polarization vector and the FM or aFM magnetization direction. Because of this unique attribute, magnetic imaging using PEEM when coupled to a laser with multiple illumination geometries allows for characterizing in-plane and out-of-plane magnetizations. This concept, however, has not been tested using a deep-UV laser (λ = 213nm), which has a much broader application space than the longer wavelength excitation used in previous reports. The purpose of this project in FY17 was to show the proof-of-concept of magnetic circular dichroism (MCD)-PEEM imaging using a λ = 210nm pulsed laser. Our results demonstrated the feasibility of in-plane and out-of-plane magnetic imaging with the limitations in the lateral resolution, data acquisition time, and signal-to-noise ratio anticipated for using a pulsed laser of moderate power. The project goal for FY18 is to construct the automated polarization-controlled data acquisition, and to establish the new lab facility in anticipation of acquiring a state-of-the-art high-power 213nm CW laser, planned to be installed in FY19. We successfully demonstrate the former by measuring dielectric stacks with polarization-dependent photoemission yield. Extrapolating from our result, we conclude that the capability of PEEM-based magnetic imaging using a CW deep UV laser could be a potential game-changer for scientific investigations and technological developments of magnetic materials and spintronic devices. In addition, polarization controlled PEEM imaging shows the potential for ellipsometry imaging of embedded nanomaterials exploiting their subtle differences in optical constants with respect to their surrounding dielectrics.
36 MATERIALS SCIENCE↗
Tunable chiral and nematic states in the triple-Q antiferromagnet Co 1/3 TaS 2
Complex spin configurations in magnetic materials, ranging from collinear single-Q to non-coplanar multi-Q states, exhibit rich symmetry and chiral properties. However, their detailed characterization is often hindered by the limited spatial resolution of neutron diffraction techniques. Here we employ magnetic circular dichroism and magnetic linear dichroism to investigate the triangular lattice antiferromagnet Co 1/3 TaS 2 , revealing three-state (Z 3 ) nematicity and also spin chirality across its multi-Q magnetic phases. At intermediate temperatures, the presence of linear dichroism identifies nematicity arising from a single-Q stripe phase, while at high magnetic fields and low temperatures, a phase characterized solely by circular dichroism emerges, signifying a purely chiral non-coplanar triple-Q state. Notably, at low temperatures and small fields, we discover a unique phase where both chirality and nematicity coexist. A theoretical analysis based on a continuous multi-Q manifold captures the emergence of these distinct magnetic phases, as a result of the interplay between four-spin interactions and weak magnetic anisotropy. Additionally, both circular and linear dichroism microscopy spatially resolves the chiral and nematic domains. Our findings establish Co 1/3 TaS 2 as a rare platform hosting diverse multi-Q states with distinct combinations of spin chirality and nematicity while demonstrating the effectiveness of polarized optical techniques in characterizing complex magnetic textures.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Differential absorption of circularly polarized light by a centrosymmetric crystal
Crystalline solids are governed by universal structure-property relationships derived from their crystal symmetry, leading to paradigmatic rules on what properties they can and cannot exhibit. A long-held structure-property relationship is that centrosymmetric crystals cannot differentially absorb circularly polarized light. In this study, we demonstrate the design, synthesis, and characterization of the centrosymmetric material Li 2 Co 3 (SeO 3 ) 4 , which violates this relationship not by defying symmetry-imposed selection rules but by invoking a photophysical process not previously characterized for crystalline solids. This process originates from an interference between linear dichroism and linear birefringence, referred to as LD-LB, and involves strong chiroptical signals that invert upon sample flipping. Here, in addition to enabling a chiroptical response under centrosymmetry, this process opens up photonic engineering opportunities based on crystalline solids.
36 MATERIALS SCIENCE↗