arXiv subjects

Henry C. Kapteyn

Publications and source records attributed to Henry C. Kapteyn.

At least 37 records · Page 2Linked to original sources

arXiv2022

Ultrafast perturbation of magnetic domains by optical pumping in a ferromagnetic multilayer

Ultrafast optical pumping of spatially nonuniform magnetic textures is known to induce far-from-equilibrium spin transport effects. Here, we use ultrafast x-ray diffraction with unprecedented dynamic range to study the laser-induced dynamics of labyrinth domain networks in ferromagnetic CoFe/Ni multilayers. We detected azimuthally isotropic, odd order, magnetic diffraction rings up to 5th order. The amplitudes of all three diffraction rings quench to different degrees within 1.6 ps. In addition, all three of the detected diffraction rings both broaden by 15% and radially contract by 6% during the quench process. We are able to rigorously quantify a 31% ultrafast broadening of the domain walls via Fourier analysis of the order-dependent quenching of the three detected diffraction rings. The broadening of the diffraction rings is interpreted as a reduction in the domain coherence length, but the shift in the ring radius, while unambiguous in its occurrence, remains unexplained. In particular, we demonstrate that a radial shift explained by domain wall broadening can be ruled out. With the unprecedented dynamic range of our data, our results provide convincing evidence that labyrinth domain structures are spatially perturbed at ultrafast speeds under far-from-equilibrium conditions, albeit the mechanism inducing the perturbations remains yet to be clarified.

cond-mat.mes-hall↗

arXiv2021

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 wavefunction, 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 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.

physics.optics↗

arXiv2021

Second-harmonic generation and the conservation of spatiotemporal orbital angular momentum of light

Light with spatiotemporal orbital angular momentum (ST-OAM) is a recently discovered type of structured and localized electromagnetic field. This field carries characteristic space-time spiral phase structure and transverse intrinsic OAM. In this work, we present the generation and characterization of the second-harmonic of ST-OAM pulses. We uncovered the conservation of transverse OAM in a second-harmonic generation process, where the space-time topological charge of the fundamental field is doubled along with the optical frequency. Our experiment thus suggests a general ST-OAM nonlinear scaling rule - analogous to that in conventional OAM of light. Furthermore, we observe that the topology of a second-harmonic ST-OAM pulse can be modified by complex spatiotemporal astigmatism, giving rise to multiple phase singularities separated in space and time. Our study opens a new route for nonlinear conversion and scaling of light carrying ST-OAM with the potential for driving other secondary ST-OAM sources of electromagnetic fields and beyond.

physics.optics↗

arXiv2021

Direct observation of 3D topological spin textures and their interactions using soft x-ray vector ptychography

Magnetic topological defects are energetically stable spin configurations characterized by symmetry breaking. Vortices and skyrmions are two well-known examples of 2D spin textures that have been actively studied for both fundamental interest and practical applications. However, experimental evidence of the 3D spin textures has been largely indirect or qualitative to date, due to the difficulty of quantitively characterizing them within nanoscale volumes. Here, we develop soft x-ray vector ptychography to quantitatively image the 3D magnetization vector field in a frustrated superlattice with 10 nm spatial resolution. By applying homotopy theory to the experimental data, we quantify the topological charge of hedgehogs and anti-hedgehogs as emergent magnetic monopoles and probe their interactions inside the frustrated superlattice. We also directly observe virtual hedgehogs and anti-hedgehogs created by magnetically inert voids. We expect that this new quantitative imaging method will open the door to study 3D topological spin textures in a broad class of magnetic materials. Our work also demonstrates that magnetically frustrated superlattices could be used as a new platform to investigate hedgehog interactions and dynamics and to exploit optimized geometries for information storage and transport applications.

cond-mat.str-el↗

arXiv2021

Thermal transport from 1D- and 2D-confined nanostructures on silicon probed using coherent extreme UV light: General and predictive model yields new understanding

Heat management is crucial in the design of nanoscale devices as the operating temperature determines their efficiency and lifetime. Past experimental and theoretical works exploring nanoscale heat transport in semiconductors addressed known deviations from Fourier's law modeling by including effective parameters, such as a size-dependent thermal conductivity. However, recent experiments have qualitatively shown new behavior that cannot be modeled in this way. Here, we combine advanced experiment and theory to show that the cooling of 1D- and 2D-confined nanoscale hot spots on silicon can be described using a general hydrodynamic heat transport model, contrary to previous understanding of heat flow in bulk silicon. We use a comprehensive set of extreme ultraviolet scatterometry measurements of non-diffusive transport from transiently heated nanolines and nanodots to validate and generalize our ab initio model, that does not need any geometry-dependent fitting parameters. This allows us to uncover the existence of two distinct timescales and heat transport mechanisms: an interface resistance regime that dominates on short time scales, and a hydrodynamic-like phonon transport regime that dominates on longer timescales. Moreover, our model can predict the full thermomechanical response on nanometer length scales and picosecond time scales for arbitrary geometries, providing an advanced practical tool for thermal management of nanoscale technologies. Furthermore, we derive analytical expressions for the transport timescales, valid for a subset of geometries, supplying a route for optimizing heat dissipation.

cond-mat.mtrl-sci↗

arXiv2020

Creation of a novel inverted charge density wave state

Charge density wave (CDW) order is an emergent quantum phase that is characterized by a 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 over-drive the unique star-of-David lattice distortion in 1T-TaSe$_2$. We track the signature of this novel CDW state using time- and angle-resolved photoemission spectroscopy and time-dependent density functional theory, and 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.

cond-mat.mtrl-sci↗

arXiv2020

Ultrafast 1 MHz vacuum-ultraviolet source via highly cascaded harmonic generation in negative-curvature hollow-core fibers

Vacuum ultraviolet (VUV) light is critical for the study of molecules and materials, but the generation of femtosecond pulses in the VUV region at high repetition rates has proven difficult. Here, we demonstrate the efficient generation of VUV light at MHz repetition rates using highly cascaded four-wave mixing processes in a negative-curvature hollow-core fiber. Both even and odd order harmonics are generated up to the 15th harmonic (69 nm, 18.0 eV), with high energy resolution of ~40 meV. In contrast to direct high harmonic generation, this highly cascaded harmonic generation process requires lower peak intensity and therefore can operate at higher repetition rates, driven by a robust ~10 W fiber-laser system in a compact setup. Additionally, we present numerical simulations that explore the fundamental capabilities and spatiotemporal dynamics of highly cascaded harmonic generation. This VUV source can enhance the capabilities of spectroscopies of molecular and quantum materials, such as photoionization mass spectrometry and time , angle , and spin-resolved photoemission.

physics.optics↗

arXiv2019

Conservation of torus-knot angular momentum in high-order harmonic generation

High-order harmonic generation stands as a unique nonlinear optical up-conversion process, mediated by a laser-driven electron recollision mechanism, which has been shown to conserve energy, momentum, and spin and orbital angular momentum. Here we present theoretical simulations which demonstrate that this process also conserves a mixture of the latter, the torus-knot angular momentum $J_γ$, by producing high-order harmonics with driving pulses that are invariant under coordinated rotations. We demonstrate that the charge $J_γ$ of the emitted harmonics scales linearly with the harmonic order, and that this conservation law is imprinted onto the polarization distribution of the emitted spiral of attosecond pulses. We also demonstrate how the nonperturbative physics of high-order harmonic generation affect the torus-knot angular momentum of the harmonics, and we show that this configuration harnesses the spin selection rules to channel the full yield of each harmonic into a single mode of controllable orbital angular momentum.

quant-ph↗

arXiv2019

Light with a self-torque: extreme-ultraviolet beams with time-varying orbital angular momentum

Twisted light fields carrying orbital angular momentum (OAM) provide powerful capabilities for applications in optical communications, microscopy, quantum optics and microparticle rotation. Here we introduce and experimentally validate a new class of light beams, whose unique property is associated with a temporal OAM variation along a pulse: the self-torque of light. Self-torque is a phenomenon that can arise from matter-field interactions in electrodynamics and general relativity, but to date, there has been no optical analog. In particular, the self-torque of light is an inherent property, which is distinguished from the mechanical torque exerted by OAM beams when interacting with physical systems. We demonstrate that self-torqued beams in the extreme-ultraviolet (EUV) naturally arise as a necessary consequence of angular momentum conservation in non-perturbative high-order harmonic generation when driven by time-delayed pulses with different OAM. In addition, the time-dependent OAM naturally induces an azimuthal frequency chirp, which provides a signature for monitoring the self-torque of high-harmonic EUV beams. Such self-torqued EUV beams can serve as unique tools for imaging magnetic and topological excitations, for launching selective excitation of quantum matter, and for manipulating molecules and nanostructures on unprecedented time and length scales.

physics.optics↗

arXiv2017

High-harmonic generation in periodically poled waveguides

Optical waveguides made from periodically poled materials provide high confinement of light and enable the generation of new wavelengths via quasi-phase-matching, making them a key platform for nonlinear optics and photonics. However, such devices are not typically employed for high-harmonic generation. Here, using 200-fs, 10-nJ-level pulses of 4100 nm light at 1 MHz, we generate high harmonics up to the 13th harmonic (315 nm) in a chirped, periodically poled lithium niobate (PPLN) waveguide. Total conversion efficiencies into the visible--ultraviolet region are as high as 10 percent. We find that the output spectrum depends on the waveguide poling period, indicating that quasi-phase-matching plays a significant role. In the future, such periodically poled waveguides may enable compact sources of ultrashort pulses at high repetition rates and provide new methods of probing the electronic structure of solid-state materials.

physics.optics↗

arXiv2017

Single-Shot 3D Diffractive Imaging of Core-Shell Nanoparticles with Elemental Specificity

We report 3D coherent diffractive imaging of Au/Pd core-shell nanoparticles with 6 nm resolution on 5-6 femtosecond timescales. We measured single-shot diffraction patterns of core-shell nanoparticles using very intense and short x-ray free electron laser pulses. By taking advantage of the curvature of the Ewald sphere and the symmetry of the nanoparticle, we reconstructed the 3D electron density of 34 core-shell structures from single-shot diffraction patterns. We determined the size of the Au core and the thickness of the Pd shell to be 65.0 +/- 1.0 nm and 4.0 +/- 0.5 nm, respectively, and identified the 3D elemental distribution inside the nanoparticles with an accuracy better than 2%. We anticipate this method can be used for quantitative 3D imaging of symmetrical nanostructures and virus particles.

physics.ins-det↗

arXiv2016

High harmonic interferometry of the Lorentz force in strong mid-infrared laser fields

The interaction of intense mid-infrared laser fields with atoms and molecules leads to a range of new opportunities, from the production of bright, coherent radiation in the soft x-ray range to imaging molecular structures and dynamics with attosecond temporal and sub-angstrom spatial resolution. However, all these effects, which rely on laser-driven recollision of an electron removed by the strong laser field and the parent ion, suffer from the rapidly increasing role of the magnetic field component of the driving pulse: the associated Lorentz force pushes the electrons off course in their excursion and suppresses all recollision-based processes, including high harmonic generation, elastic and inelastic scattering. Here we show how the use of two non-collinear beams with opposite circular polarizations produces a forwards ellipticity which can be used to monitor, control, and cancel the effect of the Lorentz force. This arrangement can thus be used to re-enable recollision-based phenomena in regimes beyond the long-wavelength breakdown of the dipole approximation, and it can be used to observe this breakdown in high-harmonic generation using currently-available light sources.

physics.atom-ph↗

arXiv2016

Ptychographic hyperspectral spectromicroscopy with an extreme ultraviolet high harmonic comb

We demonstrate a new scheme of spectromicroscopy in the extreme ultraviolet (EUV) spectral range, where the spectral response of the sample at different wavelengths is imaged simultaneously. It is enabled by applying ptychographical information multiplexing (PIM) to a tabletop EUV source based on high harmonic generation, where four spectrally narrow harmonics near 30 nm form a spectral comb structure. Extending PIM from previously demonstrated visible wavelengths to the EUV/X-ray wavelengths promises much higher spatial resolution and more powerful spectral contrast mechanism, making PIM an attractive spectromicroscopy method in both the microscopy and the spectroscopy aspects. Besides the sample, the multicolor EUV beam is also imaged in situ, making our method a powerful beam characterization technique. No hardware is used to separate or narrow down the wavelengths, leading to efficient use of the EUV radiation.

physics.optics↗

arXiv2016

Quantitative Chemically-Specific Coherent Diffractive Imaging of Buried Interfaces using a Tabletop EUV Nanoscope

Characterizing buried layers and interfaces is critical for a host of applications in nanoscience and nano-manufacturing. Here we demonstrate non-invasive, non-destructive imaging of buried interfaces using a tabletop, extreme ultraviolet (EUV), coherent diffractive imaging (CDI) nanoscope. Copper nanostructures inlaid in SiO2 are coated with 100 nm of aluminum, which is opaque to visible light and thick enough that neither optical microscopy nor atomic force microscopy can image the buried interfaces. Short wavelength (29 nm) high harmonic light can penetrate the aluminum layer, yielding high-contrast images of the buried structures. Moreover, differences in the absolute reflectivity of the interfaces before and after coating reveal the formation of interstitial diffusion and oxidation layers at the Al-Cu and Al-SiO2 boundaries. Finally, we show that EUV CDI provides a unique capability for quantitative, chemically-specific imaging of buried structures, and the material evolution that occurs at these buried interfaces, compared with all other approaches.

physics.optics↗

arXiv2015

Localization of Fe d-states in Ni-Fe-Cu alloys and implications for ultrafast demagnetization

Ni$_{80}$Fe$_{20}$ (Py) and Py-Cu exhibit intriguing ultrafast demagnetization behavior, where the Ni magnetic moment shows a delayed response relative to the Fe [S. Mathias et al., PNAS {\bf 109}, 4792 (2012)]. To unravel the mechanism responsible for this behavior, we have studied Py-Cu alloys for a wide range of Cu concentrations using X-ray magnetic circular dichroism (XMCD). The magnetic moments of Fe and Ni are found to respond very differently to Cu alloying: Fe becomes a strong ferromagnet in Py, with the magnetic moment largely unaffected by Cu alloying. In contrast, the Ni magnetic moment decreases continuously with increasing Cu concentration. Our results are corroborated by ab-initio calculations of the electronic structure, which we discuss in the framework of virtual bound states (VBSs). For high Cu concentrations, Ni exhibits VBSs below the Fermi level, which are likely responsible for an increased orbital/spin magnetic ratio at high Cu concentrations. Fe exhibits VBSs in the minority band, approximately 1 eV above the Fermi level in pure Py, that move closer to the Fermi level upon Cu alloying. A strong interaction between the VBSs and excited electrons above the Fermi level enhances the formation of localized magnons at Fe sites, which explains the different behavior between Fe and Ni during ultrafast demagnetization.

cond-mat.mtrl-sci↗

arXiv2014

Controlling the electronic structure of graphene using surface-adsorbate interactions

We show that strong coupling between graphene and the substrate is mitigated when 0.8 monolayer of Na is adsorbed and consolidated on top graphene-on-Ni(111). Specifically, the π state is partially restored near the K-point and the energy gap between the π and π* states reduced to 1.3 eV after adsorption, as measured by angle-resolved photoemission spectroscopy. We show that this change is not caused by intercalation of Na to underneath graphene but it is caused by an electronic coupling between Na on top and graphene. We show further that graphene can be decoupled to a much higher extent when Na is intercalated to underneath graphene. After intercalation, the energy gap between the π and π* states is reduced to 0 eV and these states are identical as in freestanding and n-doped graphene. We conclude thus that two mechanisms of decoupling exist: a strong decoupling through intercalation, which is the same as one found using noble metals, and a weak decoupling caused by electronic interaction with the adsorbate on top.

cond-mat.mtrl-sci↗

arXiv2014

A new regime of nanoscale thermal transport: collective diffusion counteracts dissipation inefficiency

Understanding thermal transport from nanoscale heat sources is important for a fundamental description of energy flow in materials, as well as for many technological applications including thermal management in nanoelectronics, thermoelectric devices, nano-enhanced photovoltaics and nanoparticle-mediated thermal therapies. Thermal transport at the nanoscale is fundamentally different from that at the macroscale and is determined by the distribution of carrier mean free paths in a material, the length scales of the heat sources, and the distance over which heat is transported. Past work has shown that Fourier's law for heat conduction dramatically over-predicts the rate of heat dissipation from heat sources with dimensions smaller than the mean free path of the dominant heat-carrying phonons. In this work, we uncover a new regime of nanoscale thermal transport that dominates when the separation between nanoscale heat sources is small compared with the dominant phonon mean free paths. Surprisingly, the interplay between neighboring heat sources can facilitate efficient, diffusive-like heat dissipation, even from the smallest nanoscale heat sources. This finding suggests that thermal management in nanoscale systems including integrated circuits might not be as challenging as projected. Finally, we demonstrate a unique and new capability to extract mean free path distributions of phonons in materials, allowing the first experimental validation of differential conductivity predictions from first-principles calculations.

cond-mat.mes-hall↗

arXiv2014

High flux coherent supercontinuum soft X-ray source driven by a single-stage 10 mJ, kHz, Ti:sapphire laser amplifier

We demonstrate the highest flux tabletop source of coherent soft X-rays to date, driven by a single-stage 10 mJ Ti:sapphire regenerative amplifier at 1 kHz. We first down-convert the laser to 1.3 um using a parametric amplifier, before up-converting it to soft X-rays using high harmonic generation in a high-pressure, phase matched, hollow waveguide geometry. The resulting optimally phase matched broadband spectrum extends to 200 eV, with a soft X-ray photon flux of > 10^6 photons/pulse/1% bandwidth at 1 kHz, corresponding to > 10^9 photons/s/1% bandwidth, or approximately a three order-of-magnitude increase compared with past work. Finally, using this broad bandwidth X-ray source, we demonstrate X-ray absorption spectroscopy of multiple elements and transitions in molecules in a single spectrum, with a spectral resolution of 0.25 eV, and with the ability to resolve the near edge fine structure.

physics.optics↗