We propose a highly efficient atomically-resolved mode of electron magnetic chiral dichroism. This method exploits the recently introduced orbital angular momentum spectrometer to analyze the inelastically scattered electrons allowing for simultaneous dispersion in both energy and angular momentum. The technique offers several advantages over previous formulations of electron magnetic chiral dichroism as it requires much simpler experimental conditions in terms of specimen orientation and thickness. A novel simulation algorithm, based on the multislice description of the beam propagation, is used to anticipate the advantages of the new approach over current electron magnetic chiral dichroism implementations. Numerical calculations confirm an increased magnetic signal to noise ratio with in plane atomic resolution.
In this work we derive sum rules for orbital angular momentum(OAM) resolved electron magnetic chiral dichroism (EMCD) which enable the evaluation of the strength of spin and orbital components of the atomic magnetic moments in a crystalline sample. We also demonstrate through numerical simulations that these rules appear to be only slightly dependent from the dynamical diffraction of the electron beam in the sample, making possible their application without the need of additional dynamical diffraction calculations.
X-ray magnetic circular dichroism (XMCD) signals are usually absent in antiferromagnets. In this letter, we report the observation of spontaneous XMCD spectra originating from the inverse triangular spin structure, or the polarization of the cluster magnetic octupole, in the chiral antiferromagnet Mn$_{3}$Sn thin film. The result is consistent with the recent theoretical predictions that the inverse triangular spin structure can give rise to finite XMCD signals in the absence of net magnetization [J. Phys. Soc. Jpn. 89, 083703 (2020) and Phys. Rev. Lett. 126, 157402 (2021)].
Inversion-symmetric crystals are optically isotropic and thus naively not expected to show dichroism effects in optical absorption and photoemission processes. Here, we find a strong linear dichroism effect (up to 42.4%) in the conduction band of inversion-symmetric bilayer MoS$_2$, when measuring energy- and momentum-resolved snapshots of excited electrons by time- and angle-resolved photoemission spectroscopy. We model the polarization-dependent photoemission intensity in the transiently-populated conduction band using the semiconductor Bloch equations and show that the observed dichroism em…
We show, by way of tight-binding and first-principles calculations, that a one-to-one correspondence between electron's crystal momentum k and non-zero orbital angular momentum (OAM) is a generic feature of surface bands. The OAM forms a chiral structure in momentum space much as its spin counterpart in Rashba model does, as a consequence of the inherent inversion symmetry breaking at the surface but not of spin-orbit interaction. Circular dichroism (CD) angle-resolved photoemission (ARPES) experiment is an efficient way to detect this new order, and we derive formulas explicitly relating the …
This work reports on the measurement of magnetic dichroism in angular-resolved photoelectron spectroscopy from in-plane magnetized buried thin films. The high bulk sensitivity of hard X-ray photoelectron spectroscopy (HAXPES) in combination with circularly polarized radiation enables the investigation of the magnetic properties of buried layers. Angular distributions of high kinetic energy (7 to 8 keV) photoelectrons in a range of about 60 deg were recorded in parallel to the energy distribution. Depending on purpose, energy and angular resolutions of 150 to 250 meV and 0.17 to 2 deg can be ac…
This work reports the measurement of magnetic dichroism in angular-resolved photoemission from in-plane magnetized buried thin films. The high bulk sensitivity of hard X-ray photoelectron spectroscopy (HAXPES) in combination with circularly polarized radiation enables the investigation of the magnetic properties of buried layers. HAXPES experiments with an excitation energy of 8 keV were performed on exchange-biased magnetic layers covered by thin oxide films. Two types of structures were investigated with the IrMn exchange-biasing layer either above or below the ferromagnetic layer: one with …
Using circularly polarised radiation and a combination of bulk-sensitive hard X-ray photoelectron spectroscopy and X-ray-absorption spectroscopy (XAS) we studied the electronic and magnetic structure of epitaxial Mn$_{1.8}$Co$_{1.2}$Ga thin films. Spin resolved Bloch spectral functions, density of states as well as charge and magnetisation densities were investigated by a first-principles analysis of full potential, fully relativistic Korringa--Kohn--Rostoker calculations of the electronic structure. The valence states were experimentally investigated by using linear dichroism in the angular d…
We report observation of electron helical dichroism on a material with chiral structure. In analogy with circular dichroism, a common technique for molecular structural fingerprinting, we use a nanofabricated forked diffraction grating to prepare electron vortex beams with opposite orbital angular momenta incident upon metal nanoparticle clusters and post-select for a zero-orbital angular momentum final state. We observe a difference in the differential scattering probability for orbital angular momentum transfer from vortices with opposite handedness incident on chiral aluminum nanoparticle c…
Circular dichroism (CD) spectra of chiral bare and thiol-passivated gold nanoclusters have been calculated within the dipole approximation. The calculated CD spectra show features that allow us to distinguish between clusters with different indexes of chirality. The main factor responsible of the differences in the CD lineshapes is the distribution of interatomic distances that characterize the chiral cluster geometry. These results provide theoretical support for the quantification of chirality and its measurement, using the CD lineshapes of chiral metal nanoclusters.
Circular dichroism is a technologically important phenomenon contrasting the absorption and resultant emission properties between left- and right-handed circularly polarized light. While the chiral handedness of systems mainly determines the mechanism of the circular dichroism in linear optics, the counterpart in the nonlinear optical regime is nontrivial. Here, in contrast to traditional nonlinear circular dichroism responses from structured surfaces, we report on an unprecedented bulk-material-induced circular dichroism of second harmonic generation with a massive g-factor up to 1.8.
Recently it was demonstrated (Schattschneider et al., Nature 441 (2006), 486), that an analogue of the X-ray magnetic circular dichroism (XMCD) experiment can be performed with the transmission electron microscope (TEM). The new phenomenon has been named energy-loss magnetic chiral dichroism (EMCD). In this work we present a detailed ab initio study of the chiral dichroism in the Fe, Co and Ni transition elements. We discuss the methods used for the simulations together with the validity and accuracy of the treatment, which can, in principle, apply to any given crystalline specimen. The depend…
In the close vicinity of a chiral nanostructure, the circular dichroism of a biomolecule could be greatly enhanced, due to the interaction with the local superchiral fields. Modest enhancement of optical activity using a planar metamaterial, with some chiral properties, and achiral nanoparticles has been previously reported. A more substantial chirality enhancement can be achieved in the local filed of a chiral nanostructure with a three-dimensional arrangement. Using an embossed chiral nanostructure designed for chiroptical sensing, we measure the circular dichroism spectra of two biomolecule…
Observing signatures of light-induced Floquet topological states in materials has been shown to be very challenging. Angle-resolved photoemission spectroscopy (ARPES) is well suited for the investigation of Floquet physics, as it allows to directly probe the dressed electronic states of driven solids. Depending on the system, scattering and decoherence can play an important role, hampering the emergence of Floquet states. Another challenge is to disentangle Floquet side bands from laser-assisted photoemission (LAPE), since both lead to similar signatures in ARPES spectra. Here, we investigate …
Twisted bilayer graphene is a chiral system which has been recently shown to present circular dichroism. In this work we show that the origin of this optical activity is the rotation of the Dirac fermions' helicities in the top and bottom layer. Starting from the Kubo formula, we obtain a compact expression for the Hall conductivity that takes into account the dephasing of the electromagnetic field between the top and bottom layers and gathers all the symmetries of the system. Our results are based in both a continuum and a tight-binding model, and they can be generalized to any two-dimensiona…
Strong enhancement of molecular circular dichroism has the potential to enable efficient asymmetric photolysis, a method of chiral separation that has conventionally been impeded by insufficient yield and low enantiomeric excess. Here, we study experimentally how predicted enhancements in optical chirality density near resonant silicon nanodisks boost circular dichroism. We use fluorescence-detected circular dichroism spectroscopy to measure indirectly the differential absorption of circularly polarized light by a monolayer of optically active molecules functionalized to silicon nanodisk array…
The helical Dirac fermions at the surface of topological insulators show a strong circular dichroism which has been explained as being due to either the initial-state spin angular momentum, the initial-state orbital angular momentum, or the handedness of the experimental setup. All of these interpretations conflict with our data from Bi2Te3 which depend on the photon energy and show several sign changes. Our one-step photoemission calculations coupled to ab initio theory confirm the sign change and assign the dichroism to a final-state effect. The spin polarization of the photoelectrons, inste…
We revisit the formulations and simulations of angular distributions in polarization-dependent core-level photoemission spectra of strongly correlated electron systems, in order to explain the recently discovered linear dichroism (LD) in the core-level photoemission of 4f-based rare-earth compounds. Owing to the selection rules for the optical process of core-level excitations, the LD originating from the anisotropic outer localized charge distributions determined by the ground-state orbital symmetry can be observed. Our simulations show that core d-level excitations are essential for the LD i…
This paper concerns optical properties of the isotropic phase above the isotropic-cholesteric transition and of the blue phase BP III. We introduce an effective index, which describes spatial dispersion effects such as optical rotation, circular dichroism, and the modification of the average index due to the fluctuations. We derive the wavelength dependance of these spatial dispersion effects quite generally without relying on an expansion in powers of the chirality and without assuming that the pitch of the cholesteric $P$ is much shorter than the wavelength of the light $λ$, an approximation…
We present an analysis of the Hall conductivity $σ_{xy}(ω, T)$ in time reversal symmetry breaking states of exotic superconductors. We find that the dichroic signal is non-zero in systems with inter-band order parameters. This new intrinsic mechanism may explain the Kerr effect observed in strontium ruthenate and possibly other superconductors. We predict coherence factor effects in the temperature dependence of the imaginary part of the ac Hall conductivity $ Imσ_{xy}(ω, T)$, which can be tested experimentally.
We discuss the feasibility of detecting magnetic transitions with focused electron vortex probes, suggested by selection rules for the magnetic quantum number. We theoretically estimate the dichroic signal strength in the L$_{2,3}$ edge of the ferromagnetic d metals. It is shown that under realistic conditions, the dichroic signal is undetectable for nanoparticles larger than ~1 nm. This is confirmed by a key experiment with nanometer sized vortices.
Ultrashort optical pulses can trigger a variety of non-equilibrium processes in magnetic thin films affecting electrons and spins on femtosecond timescales. In order to probe the charge and magnetic degrees of freedom simultaneously, we developed an x-ray streaking technique that has the advantage of providing a jitter-free picture of absorption cross section changes. In this paper, we present an experiment based on this approach which we performed using five photon probing energies at the Ni $M_{2,3}$-edges. This allowed us to retrieve the absorption and magnetic circular dichroism time trace…
A 3-fold symmetric kagome lattice that has negative spin chirality can give a non-zero x-ray magnetic circular dichroism (XMCD) signal, despite that the total spin moment amounts to zero. This is explained by a hitherto unnoticed rule for the rotational symmetry invariance of the XMCD signal. A necessary condition is the existence of an anisotropic XMCD signal for the local magnetic atom, which can arise from a spin anisotropy either in the ground state or the final state. The angular dependence of the XMCD as a function of the beam direction has an unusual behavior. The maximum dichroism is n…
Experiments of time-resolved x-ray magnetic circular dichroism (Tr-XMCD) and resonant x-ray scattering at a beamline BL07LSU in SPring-8 with a time-resolution of under 50 ps are presented. A micro-channel plate is utilized for the Tr-XMCD measurements at nearly normal incidence both in the partial electron and total fluorescence yield (PEY and TFY) modes at the L2,3 absorption edges of the 3d transition-metals in the soft x-ray region. The ultrafast photo-induced demagnetization within 50 ps is observed on the dynamics of a magnetic material of FePt thin film, having a distinct threshold of t…
Noncollinear chiral spin textures in ferromagnetic multilayers are at the forefront of recent research in nano-magnetism with the promise for fast and energy-efficient devices. The recently demonstrated possibilities to stabilize such chiral structures in synthetic antiferromagnets (SAF) has raised interests as they are immune to dipolar field, hence favoring the stabilization of ultra small textures, improve mobility and avoid the transverse deflections of moving skyrmions limiting the efficiency in some foreseen applications. However, such systems with zero net magnetization are hence diffic…
A first principles approach, based on the real space multiple scattering Green's function method, is presented for spin- and angle-resolved resonant photoemission from magnetic surfaces. It is applied to the Fe(010) valence band photoemission excited with circularly polarized X-rays around the Fe L3 absorption edge. When the photon energy is swept through the Fe 2p-3d resonance, the valence band spectra are strongly modified in terms of absolute and relative peak intensities, degree of spin-polarization and light polarization dependence. New peaks in the spin-polarized spectra are identified a…
Chirality in condensed matter is now a topic of the utmost importance because of its significant role in the understanding and mastering of a large variety of new fundamental physicals mechanisms. Versatile experimental approaches, capable to reveal easily the exact winding of order parameters are therefore essential. Here we report X-ray resonant magnetic scattering (XRMS) as a straightforward tool to identify directly the properties of chiral magnetic systems. We show that it can straight-forwardly and unambiguously determine the main characteristics of chiral magnetic distributions: i.e. it…
Pumping graphene with circularly polarized light is the archetype of light-tailoring topological bands. Realizing the induced Floquet-Chern insulator state and tracing clear experimental manifestions has been a challenge, and it has become clear that scattering effects play a crucial role. We tackle this gap between theory and experiment by employing microscopic quantum kinetic calculations including realistic electron-electron and electron-phonon scattering. Our theory provides a direct link to the build-up of the Floquet-Chern insulator state in light-driven graphene and its detection in tim…
Angle-resolved photoemission spectroscopy (ARPES) is the most powerful technique to investigate the electronic band structure of crystalline solids. To completely characterize the electronic structure of topological materials, one needs to go beyond band structure mapping and access information about the momentum-resolved Bloch wavefunction, namely orbitals, Berry curvature, and topological invariants. However, because phase information is lost in the process of measuring photoemission intensities, retrieving the complex-valued Bloch wavefunction from photoemission data has yet remained elusiv…
Chirality is a fundamental asymmetry phenomenon, with chiral optical elements exhibiting asymmetric response in reflection or absorption of circularly polarized light. Recent realizations of such elements include nanoplasmonic systems with broken mirror symmetry and polarization-contrasting optical absorption known as circular dichroism. An alternative route to circular dichroism is provided by spin-valley polarized excitons in atomically thin semiconductors. In the presence of magnetic fields, they exhibit an imbalanced coupling to circularly polarized photons and thus circular dichroism. Her…
It is very interesting to bring plasmonic circular dichroism spectroscopy to the mid-infrared spectral interval, and there are two reasons for this. This spectral interval is very important for thermal bio-imaging and, simultaneously, this spectral range includes vibrational lines of many chiral biomolecules. Here we demonstrate that graphene plasmons indeed offer such opportunity. In particular, we show that chiral graphene assemblies consisting of a few graphene nanodisks can generate strong circular dichroism (CD) in the mid-infrared interval. The CD signal is generated due to the plasmon-p…
We performed angle-resolved photoemission spectroscopy (ARPES) of bulk 2H-WSe$_2$ for different crystal orientations linked to each other by time-reversal symmetry. We introduce a new observable called time-reversal dichroism in photoelectron angular distributions (TRDAD), which quantifies the modulation of the photoemission intensity upon effective time-reversal operation. We demonstrate that the hidden orbital pseudospin texture leaves its imprint onto TRDAD, due to multiple orbitals interference effects in photoemission. Our experimental results are in quantitative agreement with both tight…
Non-collinear spin textures in ferromagnetic ultrathin films are attracting a renewed interest fueled by possible fine engineering of several magnetic interactions, notably the interfacial Dzyaloshinskii-Moriya interaction. This allows the stabilization of complex chiral spin textures such as chiral magnetic domain walls (DWs), spin spirals, and magnetic skyrmions. We report here on the ultrafast behavior of chiral DWs after optical pumping in perpendicularly magnetized asymmetric multilayers, probed using time-resolved circular dichroism in x-ray resonant magnetic scattering (CD-XRMS). We obs…
Electronic circular dichroism (ECD) is a powerful spectroscopical method for investigating chiral properties at the molecular level. ECD calculations with the commonly used linear-response time-dependent density functional theory (LR-TDDFT) framework can be prohibitively costly for large systems. To alleviate this problem, we present here an ECD implementation for the projector augmented-wave method in the real-time-propagation TDDFT (RT-TDDFT) framework in the open-source GPAW code. Our implementation supports both local atomic basis set and real-space finite-difference representations of wav…
