arXiv subjects

Henry C. Kapteyn

Publications and source records attributed to Henry C. Kapteyn.

At least 19 recordsLinked to original sources

arXiv2025

Dynamic Imaging of Periodic Structures using Extreme Ultraviolet Scatterometry

Dynamic scattering and imaging with coherent, ultrafast, extreme ultraviolet (EUV) light sources can resolve charge, phonon and spin processes on their intrinsic length and time scales. However, full field coherent diffraction imaging requires scanning of the sample combined with computational phase retrieval, making it challenging to quickly acquire a large series of dynamic frames. In this work, we demonstrate a technique for extracting dynamic 1D images of the average unit cell in a periodic sample from traditional EUV scatterometry data by analyzing the changing intensities of the far field diffracted orders. Starting from a system of equations relating small changes in far field diffraction to phase and amplitude perturbations at the sample plane, it is shown that under certain conditions, changes to the $n$th diffracted order map exclusively onto the $n$th Fourier component of the perturbation via a closed-form relation. We show through rigorous coupled-wave analysis simulations that our method can provide a good approximation even outside the scalar diffraction theory framework in which it is derived. Finally, we experimentally demonstrate this reconstruction method by exiting 1D nickel nanowires on a diamond substrate using an infrared laser pump pulse, and measuring their relaxation using a time-delayed EUV probe pulse, to visualize nanoscale phonon dynamics.

physics.optics↗

arXiv2025

Coherent EUV scatterometry of 2D periodic structure profiles with mathematically optimal experimental design

Extreme ultraviolet (EUV) scatterometry is an increasingly important metrology that can measure critical parameters of periodic nanostructured materials in a fast, accurate, and repeatable manner and with high sensitivity to nanoscale structure and material composition. Because of this, EUV scatterometry could support manufacturing of semiconductor devices or polymer metamaterials, addressing the limitations of traditional imaging methods such as resolution and field of view, sample damage, throughput, or low sensitivity. Here we use EUV scatterometry to measure the profile of an industrially relevant 2D periodic interconnect structure, using $λ= 29$ nm light from a table-top high harmonic generation source. We show that EUV scatterometry is sensitive to out-of-plane features with single-nanometer sensitivity. Furthermore, we also apply a methodology based on the Fisher information matrix to optimize experimental design parameters, such as incidence angles and wavelength, to show how measurement sensitivity can be maximized. This methodology reveals the strong dependence of measurement sensitivity on both incidence angle and wavelength $-$ even in a simple two-parameter case. Through a simultaneous optimization of incidence angles and wavelength, we determine that the most sensitive measurement of the quantities of interest can be made at a wavelength of $\sim$14 nm. In the future, by reducing sample contamination due to sample preparation, deep sub-nanometer sensitivity to axial profiles and 2D structures will be possible. Our results are an important step in guiding EUV scatterometry towards increased accuracy and throughput with a priori computations and by leveraging new experimental capabilities.

physics.optics↗

arXiv2025

How to Measure and Model Light-Induced Spin Transfer

Femtosecond laser light can transfer spin angular momentum between magnetic subspecies that exhibit hybridized valence bands within an alloy or compound, and represents the fastest route for manipulating the magnetization of a material. To date, ultrafast spin transfer has predominantly been explained in terms of the initial and final states available for laser excitation. Here, by comparing the measured and calculated dynamics across the entire $M$-edges of two very similar Heusler compounds, $Co_2MnGa$ and $Co_2MnGe$ as well as a sample of elemental Co, we find that simply accounting for the initial and final electron states available for laser excitation cannot alone explain the experimental observations. The influence of spin lifetimes must also be included, due to the shifting of the Fermi level upon replacing Ga with Ge, or the presence of crystalline disorder. This explains why the ordered $L2_1$ phase of $Co_2MnGa$ demonstrates strong laser-induced magnetic signal enhancements across the entire Co-edge, while similar enhancements were not observed in partially disordered $Co_2MnGe$. Although intra-site spin-transfers were expected in the minority channel in pure Co due to the presence of many more available states in the minority channel above the Fermi level, no such signal was observed due to very short few-femtosecond spin lifetimes in a metal. Finally, we identify key regions in the magnetic asymmetry where a transiently enhanced signal could be misinterpreted as a light-induced spin-transfer signature.

cond-mat.mtrl-sci↗

arXiv2024

Uncovering the Timescales of Spin Reorientation in $TbMn_{6}Sn_{6}$

Kagome ferrimagnets are of fundamental interest because of their tunable magnetic, electronic and topological properties, with potential applications for quantum-enabled technologies and spintronics. Here we present the first direct measurement of the intrinsic timescale of the spin reorientation transition in the Kagome ferrimagnet $TbMn_{6}Sn_{6}$. This material exhibits a magnetic phase transition near room temperature, where spins remain collinear while the total magnetic moment rotates from out-of-plane to in-plane. This reorientation has been attributed to the competing anisotropies of Tb and Mn, whose magnetic moments have very different temperature dependencies. By probing at the Mn M-edge using high harmonic extreme ultraviolet pulses, we measure reorientation timescales between 6 and 18 ps, depending on the laser excitation fluence. Our model of the magnetization dynamics shows that this timescale is consistent with a spin reorientation driven by very large anisotropy energies, on meV energy scales. Our model also predicts a possibility of a 180$^{\circ}$ reorientation of the out-of-plane moment, that could facilitate optically controlled magnetization switching between very stable ground states, for applications in spintronics or data storage.

cond-mat.mtrl-sci↗

arXiv2024

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.

cond-mat.mes-hall↗

arXiv2024

Sub-wavelength coherent imaging of periodic samples using a 13.5 nm tabletop high harmonic light source

Coherent diffractive imaging is unique as the only route for achieving diffraction-limited spatial resolution in the extreme ultraviolet and X-ray regions, limited only by the wavelength of the light. Recently, advances in coherent short wavelength light sources, coupled with progress in algorithm development, have significantly enhanced the power of x-ray imaging. However, to date, high-fidelity diffraction imaging of periodic objects has been a challenge because the scattered light is concentrated in isolated peaks. Here, we use tabletop 13.5nm high harmonic beams to make two significant advances. First we demonstrate high-quality imaging of an extended, nearly-periodic sample for the first time. Second, we achieve sub-wavelength spatial resolution (12.6nm) imaging at short wavelengths, also for the first time. The key to both advances is a novel technique called modulus enforced probe, which enables robust, quantitative, reconstructions of periodic objects. This work is important for imaging next generation nano-engineered devices.

physics.optics↗

arXiv2024

Phase matching of high harmonic generation in the soft and hard X-ray regions of the spectrum

We show how bright, fully coherent, hard x-ray beams can be generated through nonlinear upconversion of femtosecond laser light. By using longer-wavelength mid-infrared driving lasers of moderate peak intensity, full phase matching of the high harmonic generation process can extend, in theory, into the hard x-ray region of the spectrum. We identify the dominant phase matching mechanism for long wavelength driving lasers, and verify our predictions experimentally by demonstrating phase-matched up-conversion into the soft x-ray region of the spectrum around 330 eV using an extended, high-pressure, gas medium that is weakly ionized by the laser. Scaling of the overall conversion efficiency is surprisingly favorable as the wavelength of the driving laser is increased, making useful, fully coherent, multi-keV x-ray sources feasible. Finally, we show that the rapidly decreasing microscopic single-atom yield at longer driving wavelengths is compensated macroscopically by an increasing optimal pressure for phase matching and a rapidly decreasing reabsorption of the generated light at higher photon energies.

physics.optics↗

arXiv2024

Phase Matching of High-Order Harmonics in Hollow Waveguides

We investigate the case of phase-matched high-harmonic generation in a gas-filled capillary waveguide, comparing in detail theory with experiment. We observe three different regimes of phase matching: one where atomic dispersion balances waveguide dispersion, another corresponding to non-collinear Cerenkov phase-matching, and a third where atomic dispersion and plasma dispersion balance. The role of atomic dispersion is demonstrated by studying the dependence of the harmonic signal for several gases. We also predict and provide preliminary evidence of a regime where phase-matching occurs only at specific fractional ionization levels, leading to an output signal that is sensitive to the absolute phase of the carrier wave.

physics.optics↗

arXiv2024

Non-Destructive, High-Resolution, Chemically Specific, 3D Nanostructure Characterization using Phase-Sensitive EUV Imaging Reflectometry

Next-generation nano and quantum devices have increasingly complex 3D structure. As the dimensions of these devices shrink to the nanoscale, their performance is often governed by interface quality or precise chemical or dopant composition. Here we present the first phase-sensitive extreme ultraviolet imaging reflectometer. It combines the excellent phase stability of coherent high-harmonic sources, the unique chemical- and phase-sensitivity of extreme ultraviolet reflectometry, and state-of-the-art ptychography imaging algorithms. This tabletop microscope can non-destructively probe surface topography, layer thicknesses, and interface quality, as well as dopant concentrations and profiles. High-fidelity imaging was achieved by implementing variable-angle ptychographic imaging, by using total variation regularization to mitigate noise and artifacts in the reconstructed image, and by using a high-brightness, high-harmonic source with excellent intensity and wavefront stability. We validate our measurements through multiscale, multimodal imaging to show that this technique has unique advantages compared with other techniques based on electron and scanning-probe microscopies.

physics.optics↗

arXiv2024

Generation of Spatially Coherent Light at Extreme Ultraviolet Wavelengths

We present spatial coherence measurements of extreme-ultraviolet light generated using the process of high-harmonic upconversion of a femtosecond laser. Using a phase-matched hollow-fiber geometry, the generated beam is found to exhibit essentially full spatial coherence. The coherence of this laser-like EUV source is demonstrated by recording Gabor holograms of small objects. This work demonstrates the capability to do EUV holography using a tabletop experimental setup. Such an EUV source, with low divergence and high spatial coherence, can be used for experiments such as high-precision metrology, inspection of optical components for EUV lithography (1), and for microscopy and holography (2) with nanometer resolution. Furthermore, the short time duration of the EUV radiation (a few femtoseconds) will enable EUV microscopy and holography to be performed with ultrahigh time resolution.

physics.optics↗

arXiv2024

Bright Coherent Ultrahigh Harmonics in the keV X-Ray Regime from Mid-Infrared Femtosecond Lasers

High harmonic generation traditionally combines ~100 near-infrared laser photons, to generate bright, phase matched, extreme ultraviolet beams when the emission from many atoms adds constructively. Here we show that by guiding a mid-infrared femtosecond laser in a high pressure gas, ultrahigh harmonics can be generated up to orders > 5000, that emerge as a bright supercontinuum that spans the entire electromagnetic spectrum from the ultraviolet to > 1.6 keV, allowing in-principle the generation of pulses as short as 2.5 attoseconds. The multi-atmosphere gas pressures required for bright, phase matched emission also supports laser beam self-confinement, further enhancing the x-ray yield. Finally, the x-ray beam exhibits high spatial coherence, even though at high gas density, the recolliding electrons responsible for high harmonic generation encounter other atoms during the emission process.

physics.optics↗

arXiv2024

Phase-Matched Generation of Coherent Soft-X-Rays

Phase-matched harmonic conversion of visible laser light into soft x-rays was demonstrated. The recently developed technique of guided-wave frequency conversion was used to upshift light from 800 nanometers to the range from 17 to 32 nanometers. This process increased the coherent x-ray output by factors of 10^2 to 10^3 compared to the non-phase-matched case. This source uses a small-scale (sub-millijoule) high repetition-rate laser and will enable a wide variety of new experimental investigations in linear and nonlinear x-ray science.

physics.optics↗

arXiv2024

Phase-Matching of High-Order Harmonics Driven by Mid- Infrared Light

We demonstrate that phase-matched frequency upconversion of ultrafast laser light can be extended to shorter wavelengths by using longer driving laser wavelengths. Experimentally, we show that the phase-matching cutoff for harmonic generation in argon increases from 45 to 100 eV when the driving laser wavelength is increased from 0.8 to 1.3 micrometers. Phase matching is also obtained at higher pressures using a longer-wavelength driving laser, mitigating the unfavorable scaling of the single-atom response. Theoretical calculations suggest that phase-matched high harmonic frequency upconversion driven by mid-infrared pulses could be extended to extremely high photon energies.

physics.optics↗

arXiv2024

Visualizing Magnetic Order in Self-Assembly of Superparamagnetic Nanoparticles

We use soft x-ray vector-ptychographic tomography to determine the three-dimensional magnetization field in superparamagnetic nanoparticles self-assembled at the liquid-liquid interface and reveal the magnetic order induced by layered structure. The spins in individual nanoparticles become more aligned with increasing number of layers, resulting in a larger net magnetization. Our experimental results show a magnetic short-range order in the monolayer due to the proliferation of thermally induced magnetic vortices and a magnetic long-range order in the bilayer and trilayer, stemming from the strengthened dipolar interactions that effectively suppress thermal fluctuations. We also observe a screening effect of magnetic vortices and the attractive interaction between the magnetic vortices with opposite topological charges. Our work demonstrates the crucial role of layered structure in shaping the magnetization of nanoparticle assemblies, providing new opportunities to modulate these properties through strategic layer engineering.

cond-mat.mes-hall↗

arXiv2023

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

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 timescales shorter than 100 fs.

cond-mat.mtrl-sci↗

arXiv2023

High-fidelity ptychographic imaging of highly periodic structures enabled by vortex high harmonic beams

Ptychographic Coherent Diffractive Imaging enables diffraction-limited imaging of nanoscale structures at extreme ultraviolet and x-ray wavelengths, where high-quality image-forming optics are not available. However, its reliance on a set of diverse diffraction patterns makes it challenging to use ptychography to image highly periodic samples, limiting its application to defect inspection for electronic and photonic devices. Here, we use a vortex high harmonic light beam driven by a laser carrying orbital angular momentum to implement extreme ultraviolet ptychographic imaging of highly periodic samples with high fidelity and reliability. We also demonstrate, for the first time to our knowledge, ptychographic imaging of an isolated, near-diffraction-limited defect in an otherwise periodic sample using vortex high harmonic beams. This enhanced metrology technique can enable high-fidelity imaging and inspection of highly periodic structures for next-generation nano, energy, photonic and quantum devices.

physics.optics↗

arXiv2022

Direct observation of enhanced electron-phonon coupling in copper nanoparticles in the warm-dense matter regime

Warm-dense matter (WDM) is a highly-excited state that lies at the confluence 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 nanoparticles with a femtosecond laser below the ablation threshold, we create uniformly-excited WDM. We then use photoelectron spectroscopy to track the instantaneous electron temperature and directly extract the strongest electron-ion coupling observed experimentally to date. By directly 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 the fast energy loss of electrons to ions, as well as a strong modulation of the electron temperature by acoustic oscillations in the nanoparticle. This work demonstrates a new route for experimental exploration and theoretical validation of the exotic properties of WDM.

physics.plasm-ph↗

arXiv2022

Single-frame characterization of ultrafast pulses with spatiotemporal orbital angular momentum

Light carrying 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.

physics.optics↗