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A light-induced topological phase transition is realized in the Dirac semimetal ZrTe 5 by coherently driving symmetry-breaking phonons.

Symmetry plays a central role in conventional and topological phases of matter, making the ability to optically drive symmetry changes a critical step in developing future technologies that rely on such control. Topological materials, like topological semimetals, are particularly sensitive to a breaking or restoring of time-reversal and crystalline symmetries, which affect both bulk and surface electronic states. While previous studies have focused on controlling symmetry via coupling to the crystal lattice, we demonstrate here an all-electronic mechanism based on photocurrent generation. Using second harmonic generation spectroscopy as a sensitive probe of symmetry changes, we observe an ultrafast breaking of time-reversal and spatial symmetries following femtosecond optical excitation in the prototypical type-I Weyl semimetal TaAs. Our results show that optically driven photocurrents can be tailored to explicitly break electronic symmetry in a generic fashion, opening up the possibility of driving phase transitions between symmetry-protected states on ultrafast timescales. The authors demonstrate ultrafast symmetry breaking by optically driven photocurrents.

The chiral helimagnet Cr 1/3 NbS 2 hosts exotic spin textures, whose influence on the magneto-transport properties make this material an ideal candidate for future spintronic applications. To date, the interplay between macroscopic magnetic and transport degrees of freedom is believed to result from a reduction in carrier scattering following spin order. Here, we present electronic structure measurements across the helimagnetic transition temperature T C that challenges this view. We show that the Fermi surface is comprised of strongly hybridized Nb- and Cr-derived electronic states, and that spectral weight close to the Fermi level increases anomalously as the temperature is lowered below T C . These findings are rationalized on the basis of first principle density functional theory calculations, which reveal a large nearest-neighbor exchange energy, suggesting the interaction between local spin moments and hybridized Nb- and Cr-derived itinerant states to go beyond the perturbative interaction of Ruderman-Kittel-Kasuya-Yosida, suggesting instead a mechanism rooted in a Hund’s exchange interaction. In the chiral helimagnet Cr 1/3 NbS 2 , spin moments localized at Cr sites are believed to play a passive role in the material’s electronic and transport properties. Here, this interpretation is challenged by experimental observation of hybridization between local magnetic moments and itinerant electrons, and changes in the electronic structure with the onset of magnetism.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

We investigate the static and ultrafast magneto-optical response of the hexagonal chiral helimagnet \\(Cr_{1/3}NbS_{2}\\) above and below the helimagnetic ordering temperature. The presence of a magnetic easy plane contained within the crystallographic ab-plane is confirmed, while degenerate optical pump-probe experiments reveal significant differences in the dynamic between the parent, \\(NbS_{2}\\), and Cr-intercalated compounds. Time resolved magneto-optical Kerr effect measurements show a two-step demagnetization process, where an initial, sub-ps relaxation and subsequent buildup (\\(\\tau > 50\\) ps) in the demagnetization dynamic scale similarly with increasing pump fluence. Despite theoretical evidence for partial gapping of the minority spin channel, suggestive of possible half metallicity in \\(Cr_{1/3}NbS_{2}\\), such a long demagnetization dynamic likely results from spin lattice-relaxation as opposed to minority state blocking. However, comparison of the two-step demagnetization process in \\(Cr_{1/3}NbS_{2}\\) with other 3d intercalated transition metal dichalcogenides reveals a behavior that is unexpected from conventional spin-lattice relaxation, and may be attributed to the complicated interaction of local moments with itinerant electrons in this material system.

We use an x-ray free-electron laser to study the ultrafast lattice dynamics following above band-gap photoexcitation of the incipient ferroelectric potassium-tantalate, \\kto. % We use ultrafast near-UV (central wavelength 266\\,nm and 50 fs pulse duration) laser light to photoexcite charge carriers across the gap and probe the ultrafast lattice dynamics by recording the x-ray diffuse intensity throughout multiple Brillouin zones using pulses from the Linac Coherent Light Source (LCLS) (central wavelength 1.3\\,\\AA\\, and \\(< 10\\)~fs pulse duration). We observe changes in the diffuse intensity that we conclude are associated with a hardening of the soft transverse optical and transverse acoustic phonon branches along \\(\\Gamma\\) to \\(X\\) and \\(\\Gamma\\) to \\(M\\). Using ground- and excited-state interatomic force constants from density functional theory (DFT) and assuming the phonon populations can be described by a time-dependent temperature, we fit the quasi-equilibrium thermal diffuse intensity to the experimental time-dependent intensity. We obtain the instantaneous lattice temperature and density of photoexcited charge carriers as a function of time delay. The DFT calculations demonstrate that photoexcitation transfers charge from oxygen \\(2p\\) derived \\(\\pi\\)-bonding orbitals to Ta \\(5d\\) derived antibonding orbitals, further suppressing the ferroelectric instability and increasing the stability of the cubic, paraelectric structure.

A new type of objective lens has recently been proposed for use in X-ray photoemission electron microscopes (XPEEMs) and momentum microscopes. Adding a ring electrode concentric with the extractor allows the field in the gap between the sample and the extractor to be shaped. Forming a lens field in this gap reduces the field strength at the sample by up to an order of magnitude. This mitigates the risk of field emission, particularly for cleaved samples with sharp edges. A retarding field can redirect all slow electrons, thus eliminating the primary contribution to the space-charge interaction. Here we present the first experimental investigation of the new lens, examining its performance at photon energies ranging from the extreme ultraviolet produced by a high-harmonic generation (HHG)-based source to soft and hard X-rays at two synchrotron facilities. The gap lens in a region without electrodes enables large working distances up to 23 mm. Reduced aberrations allow for larger fields of view in both k-space and real-space imaging, with resolutions comparable to those of conventional cathode lenses. However, field strengths are an order of magnitude smaller. The zero-field mode enables the study of 3D structured objects and is therefore beneficial for small cleaved samples as well as for operando devices involving top electrodes. The repeller mode reduces space-charge effects, but results in a smaller k-field diameter. This reduction ranges from 10% at hard X-ray energies to 50% in the XUV range. The usable energy interval is also reduced by a factor of two. In time-of-flight XPEEM mode the raw data show a resolution of 250 nm, which can be improved to better than 100 nm through data processing.

Using femtosecond time-resolved X-ray diffraction, we investigated optically excited coherent acoustic phonons in the Weyl semimetal TaAs. The low symmetry of the (112) surface probed in our experiment enables the simultaneous excitation of longitudinal and shear acoustic modes, whose dispersion closely matches our simulations. We observed an asymmetry in the spectral lineshape of the longitudinal mode that is notably absent from the shear mode, suggesting a time-dependent frequency chirp that is likely driven by photoinduced carrier diffusion. We argue on the basis of symmetry that these acoustic deformations can transiently alter the electronic structure near the Weyl points and support this with model calculations. Our study underscores the benefit of using off-axis crystal orientations when optically exciting acoustic deformations in topological semimetals, allowing one to transiently change their crystal and electronic structures.

We present the design and current status of SPLENDOR, a novel detector platform that combines narrow-gap semiconductor targets with low-noise charge readout to achieve sensitivity to dark matter energy deposits well below the eV scale. SPLENDOR is designed to be a modular and scalable system able to accommodate different target materials and signal readout technologies. SPLENDOR's present strategy entails: (i) the use of strongly correlated f-electron semiconductors with anisotropic electronic structures to enable not only sub-eV energy thresholds, but also directional sensitivity to the incoming dark matter flux, allowing for signal-background discrimination via daily modulation, and (ii) custom charge readout based on cryogenic high-electron-mobility transistor (cryoHEMT) amplifiers approaching single-electron resolution. We report on the selection and characterization of Eu\\(_5\\)In\\(_2\\)Sb\\(_6\\) as the target material for SPLENDOR's first prototype detector, as well as the development and calibration of the prototype amplifier chain, achieving a measured charge resolution of 20\\(\\pm\\)7 electrons in silicon test samples, consistent with predicted performance. This provides a demonstration of the detector architecture, which is now ready for deployment in a dark matter search campaign to deliver SPLENDOR's first science results. Finally, we present estimates of sensitivity reach in the parameter space of athermally produced relic dark matter under high- and low-background environments, and for various amplifier technology upgrades with increasing performance, including planned quantum sensing upgrades in order to achieve our ultimate goal of sub-electron resolution in optimized systems. SPLENDOR provides a novel approach to dark matter direct detection, combining quantum sensing with material's design to open new avenues of exploration in the sub-MeV mass range of dark matter parameter space.

Symmetry plays a central role in conventional and topological phases of matter, making the ability to optically drive symmetry change a critical step in developing future technologies that rely on such control. Topological materials, like the newly discovered topological semimetals, are particularly sensitive to a breaking or restoring of time-reversal and crystalline symmetries, which affect both bulk and surface electronic states. While previous studies have focused on controlling symmetry via coupling to the crystal lattice, we demonstrate here an all-electronic mechanism based on photocurrent generation. Using second-harmonic generation spectroscopy as a sensitive probe of symmetry change, we observe an ultrafast breaking of time-reversal and spatial symmetries following femtosecond optical excitation in the prototypical type-I Weyl semimetal TaAs. Our results show that optically driven photocurrents can be tailored to explicitly break electronic symmetry in a generic fashion, opening up the possibility of driving phase transitions between symmetry-protected states on ultrafast time scales.