Distinct Ultrafast Electronic and Magnetic Response in M-edge Magnetic Circular Dichroism
Kelvin Yao, Felix Willems, Clemens von Korff Schmising, Ilie Radu, Christian Strueber, Daniel Schick, Dieter Engel, Arata Tsukamoto, J. K. Dewhurst, Sangeeta Sh… 展开作者
Kelvin Yao, Felix Willems, Clemens von Korff Schmising, Ilie Radu, Christian Strueber, Daniel Schick, Dieter Engel, Arata Tsukamoto, J. K. Dewhurst, Sangeeta Sharma, Stefan Eisebitt
Experimental investigations of ultrafast magnetization dynamics increasingly employ resonant magnetic spectroscopy in the ultraviolet spectral range. Besides allowing to disentangle the element-specific transient response of functional magnetic systems, these techniques also promise to access attosecond to few-femtosecond dynamics of spin excitations. Here, we report on a systematic study of transient magnetic circular dichroism (MCD) on the transition metals Fe, Co and Ni as well as on a FeNi and GdFe alloy and reveal a delayed onset between the electronic and magnetic response. Supported by \textit{ab-initio} calculations, we attribute our observation to a transient energy shift of the absorption and MCD spectra at the corresponding elemental resonances due to non-equilibrium changes of electron occupations.
Over the past two decades, metamaterials have led to an increasing number of biosensing and nanophotonic applications due to the possibility of a careful control of light propagating through subwavelength features. Chiral nanostructures (characterized by the absence of any mirror symmetry), in particular, give rise to unique chiro-optical properties such as circular dichroism and optical activity. Here, we present a gyroid optical metamaterial with a periodicity of 65 nm exhibiting a strong circular dichroism at visible wavelengths. Our bottom-up approach, based on metallic replication of the …
Optical metasurfaces have come into the spotlight as a promising platform for light manipulation at the nanoscale, including ultrafast all-optical control via excitation with femtosecond laser pulses. Recently, dichroic metasurfaces have been exploited to modulate the polarization state of light with unprecedented speed. Here, we theoretically predict and experimentally demonstrate by pump-probe spectroscopy the capability to reconfigure the ultrafast dichroic signal of a gold metasurface by simply acting on the polarization of the pump pulse, which is shown to reshape the spatio-temporal dist…
Quantitatively analyzing the mechanism of giant circular dichroism in extrinsic plasmonic chiral nanostructures by the interplay of electric and magnetic dipoles
Ultrafast nanophotonics is an emerging research field aimed at the development of nanodevices capable of light modulation with unprecedented speed. A promising approach exploits the optical nonlinearity of nanostructured materials (either metallic or dielectric) to modulate their effective permittivity via interaction with intense ultrashort laser pulses. While the ultrafast temporal dynamics of such nanostructures following photoexcitation has been studied in depth, sub-ps transient spatial inhomogeneities taking place at the nanoscale have been so far almost ignored. Here we theoretically pr…
Experimental and theoretical investigation of the co-occurrence of linear and circular dichroisms for oblique incidence of light on chiral sculptured thin films
Sometimes it appears, sometimes it does not. We present a theoretical study of circular dichroism in the second-harmonic signal of single dielectric nanostructures with different symmetries and noncentrosymmetric materials. We show that this effect is not fully identified only by macroscopic and lattice symmetries, but their relative orientation as well. Based on the cumbersome symmetry and modal analysis, we provide a general and very simple formula to determine whether the dichroism exists, and a table with the most significant cases.
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.
Giant and Broadband Circular Dichroism from Particle-Hole Symmetry Breaking in Weyl Semimetals
East China Normal University（华东师范大学）；Fudan University（复旦大学）；Sun Yat-sen University（中山大学）；Southern University of Science and Technology (SUSTech)（南方科技大学）
We study nonlinear response of a dimer composed of two identical Mie-resonant dielectric nanoparticles illuminated normally by a circularly polarized light. We develop a general theory describing hybridization of multipolar modes of the coupled nanoparticles, and reveal nonvanishing nonlinear circular dichroism (CD) in the second-harmonic generation (SHG) signal enhanced by the multipolar resonances in the dimer provided its axis is oriented under an angle to the crystalline lattice of the dielectric material. We present experimental results for this SHG-CD effect obtained for the AlGaAs dimer…
Enhancement of Circular Dichroism in Chiral Dielectric Metasurfaces by Ion Beam Irradiation
Friedrich-Schiller-University Jena（耶拿弗里德里希·席勒大学）；Abbe Center of Photonics（阿贝光学中心）；ARC Centre of Excellence for Transformative Meta-Optical Systems (TMOS)（变革性超光学系统卓越研究中心）；Department of Electronic Materials Engineering, Research School of Physics Australian National University（澳大利亚国立大学物理研究学院电子材料工程系）；Max Planck School of Photonics（马普光子学高等研究院）
Circular dichroism (CD) is absorption difference of right-hand and left-hand circularly polarized light by components. CD spectroscopy technique is an important tool for detecting molecular chirality, but the molecular circular dichroism (MCD) is weak and always appears in the ultraviolet (UV) region that is more noisy than visual range (VR). Induced circular dichroism (ICD) arisen from near-field interaction of plasmonic nanostructures and chiral molecules enhances the detection limit of molecular chirality and usually appears in VR. In this study, quadrilateral arranged nanoholes (QAN) are p…
Large optical chirality in the vicinity of achiral high index dielectric nanostructures has been recently demonstrated as useful means of enhancing molecular circular dichroism. We theoretically study the spatial dependence of optical chirality enhancement in the vicinity of high index dielectric nanodisks and highlight its importance for the design of nanophotonic platforms for circular dichroism enhancement. Using a T-matrix framework, we demonstrate that depending on disk aspect ratio chirality is enhanced preferentially along different directions. We employ various statistical procedures (…
This publication presents a novel interferometric method for the simultaneous spatially resolved analysis of an object under test regarding the phase transmission function and the magnitude and orientation of dichroism. Analogous to the classical phase shifting interferometry the measurement strategy is based on the variation of phase and polarization in an interferometer. This procedure allows to analyse simultaneously and spatially resolved the dichroic properties of the object and its impact on the phase of the incoming light in one measurement cycle. The theoretical description of the inve…
We use numerical simulations to demonstrate third-harmonic generation with near-unity nonlinear circular dichroism (CD) and high conversion efficiency ($ 10^{-2}\ \text{W}^{-2}$) in asymmetric Si-on-SiO$_2$ metasurfaces. The working principle relies on the selective excitation of a quasi-bound state in the continuum, characterized by a very high ($>10^5$) quality-factor. By tuning multi-mode interference with the variation of the metasurface geometrical parameters, we show the possibility of independent control of linear CD and nonlinear CD. Our results pave the way for the development of all-…
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 near-field interaction of plasmonic nanostructures and chiral molecules induces circular dichroism in achiral nanostructure. The induced circular dichroism (ICD) strength is several orders greater than the molecular inherent CD (MCD), and it generally appears at visual range (VR) where the CD signal is easily detectable. Therefore, the ICD is considered as a potential method to detect single molecular chirality. In this study, cross shaped nanohole (CSN) is proposed for enhancing the MCD signal. The maximum enhancement of the structure reached 450 folds of molecular inherent MCD. Through a…
Increasing the sensitivity of chiral spectroscopic techniques such as circular dichroism (CD) spectroscopy is a current aspiration in the research field of nanophotonics. Enhancing CD spectroscopy depends upon of two complementary requirements: the enhancement of the electromagnetic fields perceived by the molecules under study and the conservation of the helicity of those fields, guaranteed by duality symmetry. In this work, we introduce a systematic method to design nanostructured dual periodic photonic systems capable of enhancing molecular CD spectroscopy resonantly. As an illustration, we…
X-ray magnetic circular dichroism (XMCD) is generally not observed for antiferromagnetic (AFM) states because XMCD signals from the antiparallelly coupled spins cancel each other. In this letter, we theoretically show the presence of an XMCD signal from compensated two-dimensional triangle AFM structures on a Kagome lattice. The calculation reveals the complete correspondence between the XMCD spectra and the sign of the spin chirality: the XMCD signal only appears when the spin chirality is negative. This XMCD signal originates from the different absorption coefficients of the three sublattice…
Polariton states with high levels of chiral dissymmetry offer exciting prospects for quantum information, sensing, and lasing applications. Such dissymmetry must emanate from either the involved optical resonators or the quantum emitters. Here, we theoretically demonstrate how chiral polaritons can be realized by combining (high quality factor) achiral Fabry-Perot cavities with samples exhibiting a phenomenon known as "apparent circular dichroism" (ACD), which results from an interference between linear birefringence and dichroic interactions. By introducing a quantum electrodynamical theory o…
Polarization-dependent photon spectroscopy (dichroism) using signal-enhancing superchiral beams is shown to be sensitive to magnetic properties of the sample, whereas previous investigations explored charge-like electronic properties of chiral samples. In the process of unveiling the potential to observe magnetic circular dichroism (MCD), we underline an affinity between spectroscopies using the Borrmann effect, twisted beams and superchiral beams. Use of an effective wavevector in a quantum-mechanical theory unites the aforementioned spectroscopies and vastly improves our understanding of the…
We propose a Babinet-invertible chiral metasurface for achieving dynamically reversible and strong circular dichroism (CD). The proposed metasurface is composed of VO$_2$-metal hybrid structure, and when VO$_2$ transits between the dielectric state and the metallic state, the metasurface unit cell switches between complementary structures that are designed according to the Babinet principle. This leads to a large and reversible CD tuning range between $\pm 0.5$ at 0.97~THz, which is larger than the literature. We attribute the CD effect to extrinsic chirality of the proposed metasurface. We en…
We describe the development of a broadband magneto-optical spectrometer with femtosecond temporal resolution. The absorption spectrometer is based on a white-light supercontinuum (ca. 320 - 750 nm) using shot-to-shot temporal and spectral referencing at 1 kHz. Static and transient absorption spectra using circularly polarised light are collected in a magnetic field. The difference spectra with respect to the external field direction give the static and transient magneto-optical Faraday rotation (magnetic optical rotary dispersion) and ellipticity (magnetic circular dichroism) spectra. An achro…
Photoelectron circular dichroism results from one-photon ionization of chiral molecules by circularly polarized light and manifests itself in forward-backward asymmetry of electron emission in the direction orthogonal to the light polarization plane. To expose the physical mechanism responsible for asymmetric electron ejection, we first establish a rigorous relation between the responses of unaligned and partially or perfectly aligned molecules. Next, we identify a propensity field, which is responsible for the chiral response in the electric-dipole approximation, i.e. a chiral response withou…
