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.

Tabletop extreme ultraviolet reflectometer for quantitative nanoscale reflectometry, scatterometry, and imaging.

Imaging using coherent extreme-ultraviolet (EUV) light provides exceptional capabilities for the characterization of the composition and geometry of nanostructures by probing with high spatial resolution and elemental specificity. We present a multi-modal tabletop EUV imaging reflectometer for high-fidelity metrology of nanostructures. The reflectometer is capable of measurements in three distinct modes: intensity reflectometry, scatterometry, and imaging reflectometry, where each mode addresses different nanostructure characterization challenges. We demonstrate the system's unique ability to quantitatively and non-destructively measure the geometry and composition of nanostructures with tens of square microns field of view and sub-nanometer precision. Parameters such as surface and line edge roughness, density, nanostructure linewidth, and profile, as well as depth-resolved composition, can be quantitatively determined. The results highlight the applicability of EUV metrology to address a wide range of semiconductor and materials science challenges.

Optically controlling the competition between spin flips and intersite spin transfer in a Heusler half-metal on sub-100-fs time scales.

The direct manipulation of spins via light may provide a path toward ultrafast energy-efficient devices. However, distinguishing the microscopic processes that can occur during ultrafast laser excitation in magnetic alloys is challenging. Here, we study the Heusler compound Co2MnGa, a material that exhibits very strong light-induced spin transfers across the entire M-edge. By combining the element specificity of extreme ultraviolet high-harmonic probes with time-dependent density functional theory, we disentangle the competition between three ultrafast light-induced processes that occur in Co2MnGa: same-site Co-Co spin transfer, intersite Co-Mn spin transfer, and ultrafast spin flips mediated by spin-orbit coupling. By measuring the dynamic magnetic asymmetry across the entire M-edges of the two magnetic sublattices involved, we uncover the relative dominance of these processes at different probe energy regions and times during the laser pulse. Our combined approach enables a comprehensive microscopic interpretation of laser-induced magnetization dynamics on time scales shorter than 100 femtoseconds.

Bipolaronic Nature of the Pseudogap in Quasi-One-Dimensional (TaSe4)2I Revealed via Weak Photoexcitation.

The origin of the pseudogap in many strongly correlated materials has been a longstanding puzzle. Here, we present experimental evidence that many-body interactions among small Holstein polarons, i.e., the formation of bipolarons, are primarily responsible for the pseudogap in (TaSe4)2I. After weak photoexcitation of the material, we observe the appearance of both dispersive (single-particle bare band) and flat bands (single-polaron sub-bands) in the gap by using time- and angle-resolved photoemission spectroscopy. Based on Monte Carlo simulations of the Holstein model, we propose that the melting of pseudogap and emergence of new bands originate from a bipolaron to single-polaron crossover. We also observe dramatically different relaxation times for the excited in-gap states in (TaSe4)2I (∼600 fs) compared with another 1D material Rb0.3MoO3 (∼60 fs), which provides a new method for distinguishing between pseudogaps induced by polaronic or Luttinger-liquid many-body interactions.

Direct Observation of Enhanced Electron-Phonon Coupling in Copper Nanoparticles in the Warm-Dense Matter Regime.

Warm dense matter (WDM) represents a highly excited state that lies at the intersection of solids, plasmas, and liquids and that cannot be described by equilibrium theories. The transient nature of this state when created in a laboratory, as well as the difficulties in probing the strongly coupled interactions between the electrons and the ions, make it challenging to develop a complete understanding of matter in this regime. In this work, by exciting isolated ∼8 nm copper nanoparticles with a femtosecond laser below the ablation threshold, we create uniformly excited WDM. Using photoelectron spectroscopy, we measure the instantaneous electron temperature and extract the electron-ion coupling of the nanoparticle as it undergoes a solid-to-WDM phase transition. By comparing with state-of-the-art theories, we confirm that the superheated nanoparticles lie at the boundary between hot solids and plasmas, with associated strong electron-ion coupling. This is evidenced both by a fast energy loss of electrons to ions, and a strong modulation of the electron temperature induced by strong acoustic breathing modes that change the nanoparticle volume. This work demonstrates a new route for experimental exploration of the exotic properties of WDM.

A beamline for ultrafast extreme ultraviolet magneto-optical spectroscopy in reflection near the shot noise limit.

High harmonic generation (HHG) makes it possible to measure spin and charge dynamics in materials on femtosecond to attosecond timescales. However, the extreme nonlinear nature of the high harmonic process means that intensity fluctuations can limit measurement sensitivity. Here we present a noise-canceled, tabletop high harmonic beamline for time-resolved reflection mode spectroscopy of magnetic materials. We use a reference spectrometer to independently normalize the intensity fluctuations of each harmonic order and eliminate long term drift, allowing us to make spectroscopic measurements near the shot noise limit. These improvements allow us to significantly reduce the integration time required for high signal-to-noise (SNR) measurements of element-specific spin dynamics. Looking forward, improvements in the HHG flux, optical coatings, and grating design can further reduce the acquisition time for high SNR measurements by 1-2 orders of magnitude, enabling dramatically improved sensitivity to spin, charge, and phonon dynamics in magnetic materials.

Universal Behavior of Highly Confined Heat Flow in Semiconductor Nanosystems: From Nanomeshes to Metalattices.

Nanostructuring on length scales corresponding to phonon mean free paths provides control over heat flow in semiconductors and makes it possible to engineer their thermal properties. However, the influence of boundaries limits the validity of bulk models, while first-principles calculations are too computationally expensive to model real devices. Here we use extreme ultraviolet beams to study phonon transport dynamics in a 3D nanostructured silicon metalattice with deep nanoscale feature size and observe dramatically reduced thermal conductivity relative to bulk. To explain this behavior, we develop a predictive theory wherein thermal conduction separates into a geometric permeability component and an intrinsic viscous contribution, arising from a new and universal effect of nanoscale confinement on phonon flow. Using experiments and atomistic simulations, we show that our theory applies to a general set of highly confined silicon nanosystems, from metalattices, nanomeshes, porous nanowires, to nanowire networks, of great interest for next-generation energy-efficient devices.

Three-dimensional topological magnetic monopoles and their interactions in a ferromagnetic meta-lattice.

Topological magnetic monopoles (TMMs), also known as hedgehogs or Bloch points, are three-dimensional (3D) non-local spin textures that are robust to thermal and quantum fluctuations due to the topology protection1-4. Although TMMs have been observed in skyrmion lattices1,5, spinor Bose-Einstein condensates6,7, chiral magnets8, vortex rings2,9 and vortex cores10, it has been difficult to directly measure the 3D magnetization vector field of TMMs and probe their interactions at the nanoscale. Here we report the creation of 138 stable TMMs at the specific sites of a ferromagnetic meta-lattice at room temperature. We further develop soft X-ray vector ptycho-tomography to determine the magnetization vector and emergent magnetic field of the TMMs with a 3D spatial resolution of 10 nm. This spatial resolution is comparable to the magnetic exchange length of transition metals11, enabling us to probe monopole-monopole interactions. We find that the TMM and anti-TMM pairs are separated by 18.3 ± 1.6 nm, while the TMM and TMM, and anti-TMM and anti-TMM pairs are stabilized at comparatively longer distances of 36.1 ± 2.4 nm and 43.1 ± 2.0 nm, respectively. We also observe virtual TMMs created by magnetic voids in the meta-lattice. This work demonstrates that ferromagnetic meta-lattices could be used as a platform to create and investigate the interactions and dynamics of TMMs. Furthermore, we expect that soft X-ray vector ptycho-tomography can be broadly applied to quantitatively image 3D vector fields in magnetic and anisotropic materials at the nanoscale.

Extension of the bright high-harmonic photon energy range via nonadiabatic critical phase matching.

The concept of critical ionization fraction has been essential for high-harmonic generation, because it dictates the maximum driving laser intensity while preserving the phase matching of harmonics. In this work, we reveal a second, nonadiabatic critical ionization fraction, which substantially extends the phase-matched harmonic energy, arising because of the strong reshaping of the intense laser field in a gas plasma. We validate this understanding through a systematic comparison between experiment and theory for a wide range of laser conditions. In particular, the properties of the high-harmonic spectrum versus the laser intensity undergoes three distinctive scenarios: (i) coincidence with the single-atom cutoff, (ii) strong spectral extension, and (iii) spectral energy saturation. We present an analytical model that predicts the spectral extension and reveals the increasing importance of the nonadiabatic effects for mid-infrared lasers. These findings are important for the development of high-brightness soft x-ray sources for applications in spectroscopy and imaging.

Super-resolved time-frequency measurements of coupled phonon dynamics in a 2D quantum material.

Methods to probe and understand the dynamic response of materials following impulsive excitation are important for many fields, from materials and energy sciences to chemical and neuroscience. To design more efficient nano, energy, and quantum devices, new methods are needed to uncover the dominant excitations and reaction pathways. In this work, we implement a newly-developed superlet transform-a super-resolution time-frequency analytical method-to analyze and extract phonon dynamics in a laser-excited two-dimensional (2D) quantum material. This quasi-2D system, 1T-TaSe2, supports both equilibrium and metastable light-induced charge density wave (CDW) phases mediated by strongly coupled phonons. We compare the effectiveness of the superlet transform to standard time-frequency techniques. We find that the superlet transform is superior in both time and frequency resolution, and use it to observe and validate novel physics. In particular, we show fluence-dependent changes in the coupled dynamics of three phonon modes that are similar in frequency, including the CDW amplitude mode, that clearly demonstrate a change in the dominant charge-phonon couplings. More interestingly, the frequencies of the three phonon modes, including the strongly-coupled CDW amplitude mode, remain time- and fluence-independent, which is unusual compared to previously investigated materials. Our study opens a new avenue for capturing the coherent evolution and couplings of strongly-coupled materials and quantum systems.

High-resolution, wavefront-sensing, full-field polarimetry of arbitrary beams using phase retrieval.

Recent advances in structured illumination are enabling a wide range of applications from imaging to metrology, which can benefit from advanced beam characterization techniques. Solving uniquely for the spatial distribution of polarization in a beam typically involves the use of two or more polarization optics, such as a polarizer and a waveplate, which is prohibitive for some wavelengths outside of the visible spectrum. We demonstrate a technique that circumvents the use of a waveplate by exploiting extended Gerchberg-Saxton phase retrieval to extract the phase. The technique enables high-resolution, wavefront-sensing, full-field polarimetry capable of solving for both simple and exotic polarization states, and moreover, is extensible to shorter wavelength light.

Temporal and spectral multiplexing for EUV multibeam ptychography with a high harmonic light source.

We demonstrate temporally multiplexed multibeam ptychography implemented for the first time in the EUV, by using a high harmonic based light source. This allows for simultaneous imaging of different sample areas, or of the same area at different times or incidence angles. Furthermore, we show that this technique is compatible with wavelength multiplexing for multibeam spectroscopic imaging, taking full advantage of the temporal and spectral characteristics of high harmonic light sources. This technique enables increased data throughput using a simple experimental implementation and with high photon efficiency.

Structural and Elastic Properties of Empty-Pore Metalattices Extracted via Nondestructive Coherent Extreme UV Scatterometry and Electron Tomography.

Semiconductor metalattices consisting of a linked network of three-dimensional nanostructures with periodicities on a length scale <100 nm can enable tailored functional properties due to their complex nanostructuring. For example, by controlling both the porosity and pore size, thermal transport in these phononic metalattices can be tuned, making them promising candidates for efficient thermoelectrics or thermal rectifiers. Thus, the ability to characterize the porosity, and other physical properties, of metalattices is critical but challenging, due to their nanoscale structure and thickness. To date, only metalattices with high porosities, close to the close-packing fraction of hard spheres, have been studied experimentally. Here, we characterize the porosity, thickness, and elastic properties of a low-porosity, empty-pore silicon metalattice film (∼500 nm thickness) with periodic spherical pores (∼tens of nanometers), for the first time. We use laser-driven nanoscale surface acoustic waves probed by extreme ultraviolet scatterometry to nondestructively measure the acoustic dispersion in these thin silicon metalattice layers. By comparing the data to finite element models of the metalattice sample, we can extract Young's modulus and porosity. Moreover, by controlling the acoustic wave penetration depth, we can also determine the metalattice layer thickness and verify the substrate properties. Additionally, we utilize electron tomography images of the metalattice to verify the geometry and validate the porosity extracted from scatterometry. These advanced characterization techniques are critical for informed and iterative fabrication of energy-efficient devices based on nanostructured metamaterials.

Single-Frame Characterization of Ultrafast Pulses with Spatiotemporal Orbital Angular Momentum.

Light that carries spatiotemporal orbital angular momentum (ST-OAM) makes possible new types of optical vortices arising from transverse OAM. ST-OAM pulses exhibit novel properties during propagation, transmission, refraction, diffraction, and nonlinear conversion, attracting growing experimental and theoretical interest and studies. However, one major challenge is the lack of a simple and straightforward method for characterizing ultrafast ST-OAM pulses. Using spatially resolved spectral interferometry, we demonstrate a simple, stationary, single-frame method to quantitatively characterize ultrashort light pulses carrying ST-OAM. Using our method, the presence of an ST-OAM pulse, including its main characteristics such as topological charge numbers and OAM helicity, can be identified easily from the unique and unambiguous features directly seen on the raw data-without any need for a full analysis of the data. After processing and reconstructions, other exquisite features, including pulse dispersion and beam divergence, can also be fully characterized. Our fast characterization method allows high-throughput and quick feedback during the generation and optical alignment processes of ST-OAM pulses. It is straightforward to extend our method to single-shot measurement by using a high-speed camera that matches the pulse repetition rate. This new method can help advance the field of spatially and temporally structured light and its applications in advanced metrologies.

Spatially homogeneous few-cycle compression of Yb lasers via all-solid-state free-space soliton management.

The high power and variable repetition-rate of Yb femtosecond lasers makes them very attractive for ultrafast science. However, for capturing sub-200 fs dynamics, efficient, high-fidelity and high-stability pulse compression techniques are essential. Spectral broadening using an all-solid-state free-space geometry is particularly attractive, as it is simple, robust and low-cost. However, spatial and temporal losses caused by spatio-spectral inhomogeneities have been a major challenge to date, due to coupled space-time dynamics associated with unguided nonlinear propagation. In this work, we use all-solid-state free-space compressors to demonstrate compression of 170 fs pulses at a wavelength of 1030nm from a Yb:KGW laser to ∼9.2 fs, with a highly spatially homogeneous mode. This is achieved by ensuring that the nonlinear beam propagation in periodic layered Kerr media occurs in spatial soliton modes, and by confining the nonlinear phase through each material layer to less than 1.0 rad. A remarkable spatio-spectral homogeneity of ∼0.87 can be realized, which yields a high efficiency of >50% for few-cycle compression. The universality of the method is demonstrated by implementing high-quality pulse compression under a wide range of laser conditions. The high spatiotemporal quality and the exceptional stability of the compressed pulses are further verified by high-harmonic generation. Our predictive method offers a compact and cost-effective solution for high-quality few-cycle-pulse generation from Yb femtosecond lasers, and will enable broad applications in ultrafast science and extreme nonlinear optics.

Necklace-structured high-harmonic generation for low-divergence, soft x-ray harmonic combs with tunable line spacing.

The extreme nonlinear optical process of high-harmonic generation (HHG) makes it possible to map the properties of a laser beam onto a radiating electron wave function and, in turn, onto the emitted x-ray light. Bright HHG beams typically emerge from a longitudinal phased distribution of atomic-scale quantum antennae. Here, we form a transverse necklace-shaped phased array of linearly polarized HHG emitters, where orbital angular momentum conservation allows us to tune the line spacing and divergence properties of extreme ultraviolet and soft x-ray high-harmonic combs. The on-axis HHG emission has extremely low divergence, well below that obtained when using Gaussian driving beams, which further decreases with harmonic order. This work provides a new degree of freedom for the design of harmonic combs-particularly in the soft x-ray regime, where very limited options are available. Such harmonic beams can enable more sensitive probes of the fastest correlated charge and spin dynamics in molecules, nanoparticles, and materials.

Creation of a novel inverted charge density wave state.

Charge density wave (CDW) order is an emergent quantum phase that is characterized by periodic lattice distortion and charge density modulation, often present near superconducting transitions. Here, we uncover a novel inverted CDW state by using a femtosecond laser to coherently reverse the star-of-David lattice distortion in 1T-TaSe2. We track the signature of this novel CDW state using time- and angle-resolved photoemission spectroscopy and the time-dependent density functional theory to validate that it is associated with a unique lattice and charge arrangement never before realized. The dynamic electronic structure further reveals its novel properties that are characterized by an increased density of states near the Fermi level, high metallicity, and altered electron-phonon couplings. Our results demonstrate how ultrafast lasers can be used to create unique states in materials by manipulating charge-lattice orders and couplings.