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DOE OSTI2020

High-resolution optical micro-spectroscopy extending from the near-infrared to the vacuum-ultraviolet

Optical characterization of small samples over a wide spectral range with rapid data acquisition is essential for the analysis of many material systems, such as 2D van der Waals layers and their heterostructures. In this paper, we present the design and implementation of a tabletop micro-spectroscopy system covering the near-infrared to the vacuum-ultraviolet (1.2 eV–6.8 eV or ~1.0 μm to 185 nm) using mostly off-the-shelf components. It can measure highly reproducible local reflectance spectra with a total integration time of a few minutes and a full-width-half-maximum spot size of 2.7 by 5.6 μm. For precise positioning, the design also allows simultaneous monitoring of the measurement location and the wide-field image of the sample. We demonstrate ultra-broadband reflectance spectra of exfoliated thin flakes of several wide-gap 2D materials, including ZnPS 3 , hexagonal BN, and Ca(OH) 2 .

47 OTHER INSTRUMENTATION↗

DOE OSTI2022

Comparing the shock sensitivity of insensitive energetic materials

We present a tabletop method to study the shock sensitivity of plastic-bonded explosives that are considered shock insensitive using high dynamic range optical emission spectroscopy with laser-launched km/s flyer plate impacts (2, 3, and 4 km/s), which measures the spectral radiance (the emission spectrum vs a calibrated intensity standard) every 0.8 ns in the nanosecond and microsecond regimes. The explosives were TATB (1,3,5 trinitro, 2,4,6 triamino benzene), FOX-7 (1,1-diamino-2,2-dinitroethylene), LLM-105 (2,6-diamino-3,5-dinitropyrazine-1-oxide), and NTO (nitrotriazolone), all with 20% Sylgard 182 binder. Time resolving emission from shocked explosives produces a unique fingerprint at each shock pressure, and the emission temporal profile can be used to understand each material's shock response and the underlying mechanisms within the framework of the well-known shock ignition and growth models. Ignition was characterized by the emission intensity during nanosecond hot spot ignition. The growth process, which occurs after the shock has unloaded, was characterized by the time derivative of microsecond emission intensity. Singular-value decomposition was used to determine a characteristic spectral radiance over the entire time range, and this radiance was fit to a graybody model to determine a characteristic temperature Tc. Even though these insensitive explosives have similar shock sensitivities, our method can clearly distinguish their shock response. FOX-7 and NTO were the most sensitive, with FOX-7 having the greatest shock ignition sensitivity, growth rate, and Tc. LLM-105 was much less sensitive than FOX-7 and NTO, and TATB consistently showed the lowest sensitivity by any measure.

Akhtar, Meysam (ORCID:0000000243897837)↗

DOE OSTI2023

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. Here, 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.

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

Toward streaked collective Thomson scattering measurements on an extreme ultraviolet plasma light source

Here we show through forward modeling calculations that streaked collective Thomson scattering measurements are feasible on laser-produced tin plasmas generated under conditions relevant for extreme ultraviolet lithography. Using a 532 nm probe laser beam, the feasibility of simultaneous measurements of electron plasma wave (EPW) and ion acoustic wave (IAW) spectra is investigated. Absolute photon counts for laser scattering off both waves are calculated. Probe laser electron heating and bremsstrahlung background radiation effects are accounted for. While a large spatiotemporal region can be successfully probed based on the IAW feature, only one measurement location can be accessed through the EPW as a result of the low signal to noise ratio. A portable/traveling tabletop system is proposed.

47 OTHER INSTRUMENTATION↗

DOE OSTI2024

Extracting the electronic structure of light elements in bulk materials through a Compton scattering method in the readily accessible hard x-ray regime

Here, our Compton profile measurements of Ti and TiH 2 using readily available hard X-ray radiation at 27.5 keV, detected by both a Hitachi Vortex silicon-drift detector and a high-resolution superconducting transition-edge sensor array, are found to be in excellent accord with state-of-the-art density functional theory based calculations. The spherically averaged difference between the Compton profiles of TiH 2 and Ti is well described by an inverted parabola, supporting an itinerant behavior of the electron gas screening the protons in the Ti matrix. Our experimental approach, validated by two different detectors, extends the applicability of Compton scattering technique to the readily accessible hard x-ray regime (below 30 keV). Our study suggests possibilities for experiments at low-flux bending magnet synchrotron beamlines and paves the way for the development of tabletop Compton experiments with x-ray tubes.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Soft x-ray high-harmonic generation in an anti-resonant hollow core fiber driven by a 3 μ m ultrafast laser

High-harmonic upconversion driven by a mid-infrared femtosecond laser can generate coherent soft x-ray beams in a tabletop-scale setup. Here, we report on a compact ytterbium-pumped optical parametric chirped pulse amplifier (OPCPA) laser system seeded by an all-fiber front-end and employing periodically poled lithium niobate (PPLN) nonlinear media operated near the pulse fluence limits of current commercially available PPLN crystals. The OPCPA delivers 3 µm wavelength pulses with 775 µJ energy at 1 kHz repetition rate, with transform-limited 120 fs pulse duration, diffraction-limited beam quality, and ultrahigh 0.33% rms energy stability over >18 h. Using this laser, we generate soft x-ray high harmonics (HHG) in argon gas by focusing into a low-loss, high-pressure gas-filled anti-resonant hollow core fiber (ARHCF), generating coherent light at photon energies up to the argon L-edge (250 eV) and carbon K-edge (284 eV), with high beam quality and ∼1% rms energy stability. This work demonstrates soft x-ray HHG in a high-efficiency guided-wave phase matched geometry, overcoming the high losses inherent to mid-IR propagation in unstructured waveguides, or the short interaction lengths of gas cells or jets. The ARHCF can operate in the long term without damage and with the repetition rate, stability, and robustness required for demanding applications in spectromicroscopy and imaging. Finally, we discuss routes for further optimizing the soft x-ray HHG flux by driving He at higher laser intensities using either the signal (1.5 μm) or idler wavelengths (3 μm).

Femtosecond lasers↗

DOE OSTI2021

Generation of isolated soft x-ray attosecond pulses with mid-infrared driving lasers via transient phase-matching gating

Abstract Isolated attosecond pulses (IAPs) in the soft x-ray (SXR) region are highly desirable for attosecond time-resolved experiments. Here we identify a transient phase matching gating method for the generation of such IAPs with mid-infrared (MIR) lasers. This gating method works when a loosely focused, long-duration MIR Gaussian driving beam is slightly reshaped during its propagation in the gas medium under the ‘critical’ ionization condition. Quantitatively, the calculated coherence length of high harmonic is used to analyze the mechanism of the gating method, by using one-dimensional plane-wave beams and by comparing 2000 nm and 800 nm lasers. The robustness of the generation method is checked by varying laser’s carrier-envelope-phase and gas pressure. This gating method provides with an alternative route to efficiently produce tabletop ultrashort attosecond SXR light sources with the emerging MIR lasers.

Physics↗

DOE OSTI2025

New physics search at the CEPC: a general perspective

A next generation, high-intensity electron-positron collider “Higgs factory”, such as the Circular Electron-Positron Collider (CEPC), is among the highest priority for the global high energy collider physics community. The CEPC can provide unprecedented opportunities for making fundamental discoveries and providing decisive insights in the quest for a “New Standard Model (SM)” of nature’s fundamental interactions. The CEPC could: 1) Identify the origin of matter, especially the mechanism related to the first-order phase transition in the early Universe, which could produce a detectable gravitational wave signal. 2) Discover dark matter, particularly dark matter particles with a mass between one tenth and 100 times the proton mass. 3) Observe an array of new physics smoking guns, with sensitivities orders of magnitude better than those of existing facilities. The SM of Particle Physics is a triumph of the past half a century, as it predicts and interprets almost all the phenomena observed in experiments from the highest energies with colliders to low energy “tabletop” studies. On the other hand, deep mysteries exist concerning the most fundamental interactions of matter and the space-time fabric of the Universe, including the nature of dark matter, the origin of “visible” matter, the vast hierarchy of elementary particle masses, the quantum nature of gravity, and the mechanism of inflation. These mysteries challenge us to look for “new physics” beyond the SM and General Relativity. Indeed, physicists believe that the SM is simply a low-energy effective theory that reflects aspects of the more profound theory that answers the aforementioned mysteries. Uncovering this “New SM”, the profound theory who supports the SM is the primary mission for particle physics in the post-Higgs boson era.

Ai 艾, Xiaocong 小聪 [Zhengzhou University (China); e↗

DOE OSTI2022

Considerations for a TeV collider based on dielectric laser accelerators

Particle acceleration in dielectric microstructures powered by infrared lasers, or "dielectric laser acceleration" (DLA), is a promising area of advanced accelerator research with the potential to enable more affordable and higher-gradient accelerators for energy frontier science and a variety of other applications. DLA leverages well-established industrial fabrication capabilities and the commercial availability of tabletop lasers to reduce cost, with axial accelerating fields in the GV/m range. Further, desirable luminosities would be obtained by operating with very low charge per bunch but at extremely high repetition rates. And as a consequence of its unique operating parameter regime, coupling of the laser to the accelerator can potentially be in the 50% range and with low beamstrahlung energy loss due at the interaction point, making DLA a promising approach for a future multi-TeV linear collider.

43 PARTICLE ACCELERATORS↗

DOE OSTI2026

Beam-dump ceiling and its experimental implications: The case of a portable experiment

We generalize the nature of the so-called beam-dump “ceiling” beyond which the improvement on the sensitivity reach in the search for fast-decaying mediators dramatically slows down, and we point out its experimental implications that motivate tabletop-sized beam-dump experiments for the search. Light (bosonic) mediators are well-motivated new-physics particles, as they can appear in dark-sector portal scenarios and models to explain various laboratory-based anomalies. Due to their low mass and feebly interacting nature, beam-dump-type experiments, utilizing high-intensity particle beams, can play a crucial role in probing the parameter space of such visibly decaying mediators—in particular, the “prompt decay” region, where the mediators feature relatively large coupling and mass. We present a general and semianalytic proof that the ceiling effectively arises in the prompt-decay region of an experiment and show its insensitivity to data statistics, background estimates, and systematic uncertainties, considering a concrete example, the search for axion-like particles interacting with ordinary photons at three benchmark beam facilities: PIP-II at FNAL, and SPS and LHC-dump at CERN. We then identify optimal criteria to perform a cost-effective and short-term experiment to reach the ceiling, demonstrating that very short-baseline compact experiments enable access to the parameter space unreachable thus far.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2025

Tracing Long-Lived Atomic Coherences Generated via Molecular Conical Intersections

Accessing coherences is key to fully understand and control ultrafast dynamics of complex quantum systems like molecules. Most photochemical processes are mediated by conical intersections, which generate coherences between electronic states in molecules. We show with accurate calculations performed on gas-phase methyl iodide that electronic coherences of spin-orbit-split states persist in atomic iodine after dissociation. Our simulation predicts a maximum magnitude of vibronic coherence in the molecular regime of 0.75% of the initially photoexcited state population. Upon dissociation, one-third of this coherence magnitude is transferred to a long-lived atomic coherence where vibrational decoherence can no longer occur. To trace these dynamics, we propose a tabletop experimental approach—heterodyned attosecond four-wave-mixing spectroscopy. This technique can temporally resolve small electronic coherence magnitudes and reconstruct the full complex coherence function via phase cycling. Hence, heterodyned attosecond four-wave-mixing spectroscopy leads the way to a complete understanding and optimal control of spin-orbit-coupled electronic states in photochemistry.

Chemical Physics↗

DOE OSTI2022

State-selective probing of CO 2 autoionizing inner valence Rydberg states with attosecond extreme ultraviolet four-wave-mixing spectroscopy

Nonlinear spectroscopies can disentangle spectra that are congested due to inhomogeneous broadening. Here, in conjunction with theoretical calculations, attosecond extreme ultraviolet (XUV) four-wave-mixing (FWM) spectroscopy is utilized to probe the dynamics of autoionizing inner valence excited Rydberg states of the polyatomic molecule, CO 2 . This tabletop nonlinear technique employs a short attosecond XUV pulse train and two noncollinear, few-cycle near-infrared pulses to generate background-free XUV wave-mixing signals. FWM emission is observed from the n=5-7 states of the Henning sharp ndσ g Rydberg series that converges to the ionic $\widetilde{B}$ 2 Σ$^{+}_{u}$ state. However, these transient emission signals decay with lifetimes of 33 ± 6, 53 ± 2, and 94 ± 2 fs, respectively, which calculations show are consistent with the lifetimes of the short-lived n=6-8 members of the nsσ g character Henning diffuse Rydberg series. The oscillator strengths of transitions between states involved in all possible resonant FWM processes are calculated, verifying that the nonlinear spectra are dominated by pathways described by an initial excitation to the diffuse nsσ g Rydberg series and emission from the sharp ndσ g Rydberg series. The results substantiate not only that attosecond XUV FWM spectroscopy produces rigorous and meaningful measurements of ultrafast dynamics in polyatomic systems, but also that nonlinear spectroscopic techniques are versatile tools to selectively probe dynamics that are otherwise difficult to access.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Procrustean entanglement concentration in quantum-classical networking

The success of a future quantum internet will rest in part on the ability of quantum and classical signals to coexist in the same optical fiber infrastructure, a challenging endeavor given the orders of magnitude differences in flux of single-photon-level quantum fields and bright classical traffic. Here, we theoretically describe and experimentally implement Procrustean entanglement concentration for polarization-entangled states contaminated with classical light, showing significant mitigation of crosstalk noise in dense wavelength-division multiplexing. Our approach leverages a pair of polarization-dependent loss emulators to attenuate highly polarized crosstalk that results from imperfect isolation of conventional signals copropagating on shared fiber links. We demonstrate our technique both on the tabletop and over a deployed quantum local area network, finding a substantial improvement of two-qubit entangled state fidelity from approximately 75% to over 92%. This local filtering technique could be used as a preliminary step to reduce asymmetric errors, potentially improving the overall efficiency when combined with more complex error-mitigation techniques in future quantum repeater networks.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2022

Crystallography of hyperbolic lattices

Hyperbolic lattices are a revolutionary platform for tabletop simulations of holography and quantum physics in curved space and facilitate efficient quantum error correcting codes. Their underlying geometry is non-Euclidean, and the absence of Bloch's theorem precludes the straightforward application of the often indispensable energy band theory to study model Hamiltonians on hyperbolic lattices. Motivated by recent insights into hyperbolic band theory, we initiate a crystallography of hyperbolic lattices. Here we show that many hyperbolic lattices feature a hidden crystal structure characterized by unit cells, hyperbolic Bravais lattices, and associated symmetry groups. Using the mathematical framework of higher-genus Riemann surfaces and Fuchsian groups, we derive a list of example hyperbolic {p,q} lattices and their hyperbolic Bravais lattices, including five infinite families and several graphs relevant for experiments in circuit quantum electrodynamics and topolectrical circuits. This dramatically simplifies the computation of energy spectra of tight-binding Hamiltonians on hyperbolic lattices, from exact diagonalization on the graph to solving a finite set of equations in terms of irreducible representations. The significance of this achievement needs to be compared to the all-important role played by conventional Euclidean crystallography in the study of solids. We exemplify the high potential of this approach by constructing and diagonalizing finite-dimensional Bloch wave Hamiltonians.

2-dimensional systems↗

DOE OSTI2024

Laser Excitation of the Th-229 Nucleus

The 8.4 eV nuclear isomer state in Th-229 is resonantly excited in Th-doped CaF 2 crystals using a tabletop tunable laser system. A resonance fluorescence signal is observed in two crystals with different Th-229 dopant concentrations, while it is absent in a control experiment using Th-232. The nuclear resonance for the Th 4 + ions in Th: CaF 2 is measured at the wavelength 148.3821(5) nm, frequency 2020.409(7) THz, and the fluorescence lifetime in the crystal is 630(15) s, corresponding to an isomer half-life of 1740(50) s for a nucleus isolated in vacuum. These results pave the way toward Th-229 nuclear laser spectroscopy and realizing optical nuclear clocks. Published by the American Physical Society 2024

Physics↗

DOE OSTI2025

Enhanced Isomer Population via Direct Irradiation of Solid-Density Targets Using a Compact Laser-Plasma Accelerator

Excitation of long-lived states in bromine nuclei using a tabletop laser-plasma accelerator providing pulsed (<100 fs) electron beams provided a sensitive probe of γ strength and level densities in the nuclear quasicontinuum and may indicate angular momentum coupling through electron-nuclear interactions. Solid-density active $LaBr_{3}$ targets absorb real and virtual photons up to 35 ± 2.5 MeV and deexcite through γ cascade into different states. Here, a factor of 4.354 ± 0.932 enhancement of the $^{80}Br^{m}/^{80}Br^{g}$ isomeric ratio was observed following electron irradiation, as compared to bremsstrahlung. Additional angular momentum transfer could possibly occur through nuclear-plasma or electron-nuclear interactions enabled by the ultrashort electron beam. Further investigation of these mechanisms could have far-reaching impact including decreased storage of long-term nuclear waste and an improved understanding of heavy element formation in astrophysical settings.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

Structural transformation of dusty plasma crystal in dc discharge plasma by changing confinement ring bias

We report an experimental study of the structural transition of a stable complex plasma crystal to a solid-liquid phase coexistence by the controlled adjustment of the confinement potential, while keeping all other parameters constant. The experiments are carried out on a tabletop linear dusty plasma experimental device, which consists of a circular powered electrode and an extended grounded cathode plate. A stationary crystal of melamine formaldehyde particles is formed in a background of argon plasma inside a confining ring that is isolated from the cathode by a ceramic cover. The stable crystal structure breaks in the core region and transitions to a coexistent state by carefully changing the confining potential, thereby modifying the sheath structure. The transition is confirmed by evaluating the variation in different characteristic parameters such as the pair correlation function, local bond order parameter, and dust kinetic temperature as a function of confining bias potential. It is found that melting in the core is due to the onset of dust fluctuations in the layers beneath the topmost layer, which grow in amplitude as the confining bias potential is reduced below a threshold value. The present technique of changing confinement provides a unique feature to study structural transitions of plasma crystals without affecting the overall plasma parameters.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2024

Imaging the dynamics of initial laser-driven shocks and blowoff plasmas in polystyrene under laser-direct-drive fusion conditions

The dynamics of laser-driven shock propagation in solid ablator material, along with the concomitant processes of shinethrough and blowoff plasma plume expansion, at conditions relevant to laser-direct-drive fusion are measured using a tabletop system capable of supporting rapid dataset development with significantly higher resolution compared to existing methods. The experimental results are directly compared with current radiation-hydrodynamic simulations using the two-dimensional code . Discrepancies between experiments and simulations are evidenced and attributed to limitation of simulation to account for important processes involved in the solid-to-plasma transition. Published by the American Physical Society 2024

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗