Publications by authors named "Margaret M Murnane"

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.

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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.

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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 CoMnGa, a material that exhibits very strong light-induced spin transfers across the entire M-edge.

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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.

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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 with deep nanoscale feature size and observe dramatically reduced thermal conductivity relative to bulk.

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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 protection. Although TMMs have been observed in skyrmion lattices, spinor Bose-Einstein condensates, chiral magnets, vortex rings and vortex cores, 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.

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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.

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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.

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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.

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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.

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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.

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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.

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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 1-TaSe. 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.

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High-harmonic generation (HHG) is a unique tabletop light source with femtosecond-to-attosecond pulse duration and tailorable polarization and beam shape. Here, we use counter-rotating femtosecond laser pulses of 0.8 µm and 2.

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Understanding nanoscale thermal transport is critical for nano-engineered devices such as quantum sensors, thermoelectrics, and nanoelectronics. However, despite overwhelming experimental evidence for nondiffusive heat dissipation from nanoscale heat sources, the underlying mechanisms are still not understood. In this work, we show that for nanoscale heat source spacings that are below the mean free path of the dominant phonons in a substrate, close packing of the heat sources increases in-plane scattering and enhances cross-plane thermal conduction.

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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 parameters, such as a size-dependent thermal conductivity. However, recent experiments have qualitatively shown behavior that cannot be modeled in this way.

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Defect inspection on lithographic substrates, masks, reticles, and wafers is an important quality assurance process in semiconductor manufacturing. Coherent Fourier scatterometry (CFS) using laser beams with a Gaussian spatial profile is the standard workhorse routinely used as an in-line inspection tool to achieve high throughput. As the semiconductor industry advances toward shrinking critical dimensions in high volume manufacturing using extreme ultraviolet lithography, new techniques that enable high-sensitivity, high-throughput, and in-line inspection are critically needed.

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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.

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Biominerals such as seashells, coral skeletons, bone, and tooth enamel are optically anisotropic crystalline materials with unique nanoscale and microscale organization that translates into exceptional macroscopic mechanical properties, providing inspiration for engineering new and superior biomimetic structures. Using coral skeleton as a model, here, we experimentally demonstrate X-ray linear dichroic ptychography and map the -axis orientations of the aragonite (CaCO) crystals. Linear dichroic phase imaging at the oxygen K-edge energy shows strong polarization-dependent contrast and reveals the presence of both narrow (<35°) and wide (>35°) -axis angular spread in the coral samples.

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Metalattices are artificial 3D solids, periodic on sub-100 nm length scales, that enable the functional properties of materials to be tuned. However, because of their complex structure, predicting and characterizing their properties is challenging. Here we demonstrate the first nondestructive measurements of the mechanical and structural properties of metalattices with feature sizes down to 14 nm.

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Heusler compounds are exciting materials for future spintronics applications because they display a wide range of tunable electronic and magnetic interactions. Here, we use a femtosecond laser to directly transfer spin polarization from one element to another in a half-metallic Heusler material, CoMnGe. This spin transfer initiates as soon as light is incident on the material, demonstrating spatial transfer of angular momentum between neighboring atomic sites on time scales < 10 fs.

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Light fields carrying orbital angular momentum (OAM) provide powerful capabilities for applications in optical communications, microscopy, quantum optics, and microparticle manipulation. We introduce a property of light beams, manifested as a temporal OAM variation along a pulse: the self-torque of light. Although self-torque is found in diverse physical systems (i.

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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, linear momentum, and spin and orbital angular momentum. Here, we present theoretical simulations that 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.

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