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At least 649 records · Page 36
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Experimental Characterization of Photoemission from Plasmonic Nanogroove Arrays

Metal photocathodes are an important source of high-brightness electron beams, ubiquitous in the operation of both large-scale accelerators and table-top microscopes. When the surface of a metal is nanoengineered with patterns on the order of the optical wavelength, it can lead to the excitation and confinement of surface-plasmon-polariton waves that drive nonlinear photoemission. In this work, we aim to evaluate gold plasmonic nanogrooves as a concept for producing bright electron beams for accelerators via nonlinear photoemission. Here, we do this by first comparing their optical properties to numerical calculations from first principles to confirm our ability to fabricate these nanoscale structures. Their nonlinear photoemission yield is found by measuring emitted photocurrent as the intensity of their driving laser is varied. Finally, the mean transverse energy of this electron source is found using the solenoid-scan technique. Our data demonstrate the ability of these cathodes to provide a tenfold enhancement in the efficiency of photoemission over flat metals driven with a linear process. We find that these cathodes are robust and capable of reaching sustained average currents over 100 nA at optical intensities larger than 2 GW cm –2 with no degradation of performance. The emittance of the generated beam is found to be highly asymmetric, a fact we can explain with calculations involving the also asymmetric roughness of the patterned surface. These results demonstrate the use of nanoengineered surfaces as enhanced photocathodes, providing a robust air-stable source of high-average-current electron beams hopefully with great potential for industrial and scientific applications.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Transient Second-Order Nonlinear Media: Breaking the Spatial Symmetry in the Time Domain via Hot-Electron Transfer

Second-order optical effects are essential to the active control of light and the generation of new spectral components. The inversion symmetry, however, prevents achieving a bulk $χ^{(2)}$ response, limiting the portfolio of the second-order nonlinear materials. Here, we demonstrate subpicosecond conversion of a statically passive dielectric to a transient second-order nonlinear medium upon the ultrafast transfer of hot electrons. Induced by an optical switching signal, the amorphous dielectric with vanishing intrinsic $χ^{(2)}$ develops dynamically tunable second-order nonlinear responses. By taking the second-harmonic generation as an example, we show that breaking the inversion symmetry through hot-electron dynamics can be leveraged to address the critical need for all-optical control of second-order nonlinearities in nanophotonics. We report our approach can be generically adopted in a variety of material and device platforms, offering a new class of complex nonlinear media with promising potentials for all-optical information processing.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Multi-pass cell spectral broadening at high pulse energies

We simulate experimental conditions for nonlinear spectral broadening and compression of multi-joule, sub-picosecond, and femtosecond laser systems focusing on 1 μm center wavelength. The spatial, spectral, and temporal properties of two distinct cases are investigated in detail. The first system is a short multi-pass cell with 0.1–0.5 J pulse energy operated at higher helium pressures, used to illustrate the transition between Kerr-effect induced spectral broadening and spectral broadening in plasma. The second case is a long ten-joule multi-pass cell operated at few Pascal pressure range. These examples cover the operational extent of plasma spectral broadening in a multi-pass cell. Here effects pertaining to plasma spectral broadening, including imperfect spatial beam profiles and initial non-zero nonlinear phase, are investigated, as well as scalability.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Dynamics near equilibrium for intense beams in a nonlinear integrable focusing channel

Accelerator storage ring designs based on nonlinear integrable Hamiltonian systems provide a novel test-bed for studying the interplay between nonlinear dynamics and space charge at high intensity. In this work, the structure of beam Vlasov equilibria is explored for a constant focusing channel based on the nonlinear focusing potential of the Integrable Optics Test Accelerator. Finally, the dynamics of the single-particle orbits is explored in the combined space charge and external focusing fields as a function of beam current, and the self-consistent relaxation of a mismatched beam to equilibrium is characterized.

43 PARTICLE ACCELERATORS↗
DOE OSTI2023

Reanalysis of Experimental Determinations of Polariton-Polariton Interactions in Microcavities

The polariton-polariton interaction strength is an important parameter for all kinds of applications using the nonlinear properties of polaritons, such as optical switching and single-photon blockade devices. In this paper, we review and compare the results of a series of experiments on polariton-polariton interactions in GaAs/AlxGa1-xAs microcavity polariton structures and present an updated analysis of these experiments. We show that not just the energy shift of the spectral lines but also the results of measurements sensitive to the polariton scattering rate are important for the calibration of the interaction parameter at low excitation density. We find that when adjustments are made to correct for recent understanding of the experiments, the value of the interaction parameter at low density is lower than previous reported, but still significantly higher than theoretically predicted.

CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SU↗
DOE OSTI2020

Quantum Statistics of Vortices from a Dual Theory of the X Y Ferromagnet

In this work, we extend the well-known mapping between the easy-plane ferromagnet and electrostatics in d = 2 spatial dimensions to dynamical and quantum phenomena in a d = 2+1 spacetime. Ferromagnetic vortices behave like quantum particles with an electric charge equal to the vortex number and a magnetic flux equal to the transverse spin of the vortex core. Vortices with half-integer core spin exhibit fermionic statistics.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Light-induced magnetization from magnonic rectification

Rectification describes the conversion of an oscillating field or current into a quasi-static one and the most basic example of a rectifier is an AC/DC converter in electronics. This principle can be translated to nonlinear light-matter interactions, where optical rectification converts the oscillating electric field component of light into a quasi-static polarization and phononic rectification converts a lattice vibration into a quasi-static structural distortion. Here, we present a rectification mechanism for magnetism that we call magnonic rectification, where a spin precession is converted into a quasi-static magnetization through the force exerted by a coupled chiral phonon mode. The transiently induced magnetic state resembles that of a canted antiferromagnet, opening an avenue toward creating dynamical spin configurations that are not accessible in equilibrium.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Temporal reflection from short pump pulses inside a dispersive nonlinear medium: the impact of pump parameters

We have studied, through a series of experiments and numerical simulations, how temporal reflection from an intense pump pulse inside a photonic crystal fiber is affected by parameters of the pump pulse used to form a moving high-index boundary. We used femtosecond pump pulses, which slow down inside the fiber as their spectrum red-shifts because of intrapulse Raman scattering. Temporal reflection of probe pulses occurs from such decelerating pump pulses. We changed the width and chirp of our pump pulses with a 4f pulse shaper capable of providing both spectral filtering and frequency chirping. We found that temporal refection exhibited novel features, to our knowledge, when pump pulses were made wider or chirped. In both cases, two or more reflected pulses were produced at different wavelengths in a specific range of the initial pump-probe delays. Furthermore, numerical simulations reveal that the origin of such novel features is related to the complex nonlinear evolution of pump pulses inside optical fibers.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Kramers–Kronig relation in attosecond transient absorption spectroscopy

The Kramers–Kronig relation (KKR) has a wide range of applications in extreme ultraviolet (XUV) and x-ray spectroscopy. However, the validity of KKR for many of these applications has not been systematically studied, while it is known to require careful attention in nonlinear and pump–probe experiments in optical domain spectroscopy. Here, we study the validity of KKR in XUV attosecond transient absorption spectroscopy pump–probe measurements both experimentally and theoretically using argon Fano resonances as a case study. Experiments are enabled by a phase-resolved method dubbed Complex Attosecond Transient-absorption Spectroscopy (CATS). Although the estimations based on the rotating-wave approximation suggest that KKR violation could be expected in the studied case, our results validate KKR and provide a solid basis for its application in a broad range of attosecond spectroscopy experiments.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2026

Optimization and stabilization of Fermilab Booster using hybrid Bayesian/RL framework

PIPII project will raise Fermilab Booster intensity and ramp rate. Beam losses will limit average power and are hard to simulate. Presently, Booster uses operator-guided empirical tuning. This task is challenging due to high dimensionality, multiple objectives, critical safety constraints, and drifts. We developed a synergistic suite of Bayesian optimization (BO) and reinforcement learning (RL) tools to optimize and stabilize beam losses. First, active learning was used to build a rough model. Data was collected parasitically using two novel safety constraint types – nonlinear input space restrictions (based on optics model), and uncertainty constraints (to stop bad steps/beam aborts). We then applied online multi-objective BO with scalarized objectives and fitting to improve/rebalance losses, increasing safety margins by 25%. Using BO model as a safety veto, we tried several on/off-policy RL agents for long term stabilization; SAC had best performance. We found that adding contextual (state) information further improved performance, eventually integrating key knobs like linac phase and temperature into the parameter space. Long term testing is ongoing to enable operational use.

Kuklev, Nikita [Fermilab]↗
DOE OSTI2024

Guided Mode Evolution and Ionization Injection in Meter-Scale Multi-GeV Laser Wakefield Accelerators

Here, we show that multi-GeV laser wakefield electron accelerators in meter-scale, low density hydrodynamic plasma waveguides operate in a new nonlinear propagation regime dominated by sustained beating of lowest order modes of the ponderomotively modified channel; this occurs whether or not the injected pulse is linearly matched to the guide. For a continuously doped gas jet, this emergent mode beating effect leads to axially modulated enhancement of ionization injection and a multi-GeV energy spectrum of multiple quasimonoenergetic peaks; the same process in a locally doped jet produces single multi-GeV peaks with <10% energy spread. A three-stage model of drive laser pulse evolution and ionization injection characterizes the beating effect and explains our experimental results.

43 PARTICLE ACCELERATORS↗
DOE OSTI2023

Thermalization of the Kerr index of refraction in acetone and methanol using femtosecond pump-probe scattering spectroscopy

Femtosecond time-resolved pump-probe scattering is used to temporally investigate the index thermalization Δn(t) of the molecular motions associated with the Kerr nonlinear index n 2 . This is done using an intense 300 fs 1034 nm pump pulse and temporally probed by a 517 nm and supercontinuum pulse in acetone and methanol. The optically pumped molecular states change the index of refraction and through the processes of Raman and Rayleigh scattering are shown to engage in a 4-step energy relaxation process. Here, the pump first initiates the Kerr effect as well as populate resonant vibrational molecular motions, which act as a “mother” energy state. The electronic component of the Kerr effect is shown to couple with these vibrational modes through the process of Born-Oppenheimer coupling, which can be measured through the Raman scattering of the probe. The “mother” coupled state then decays into “daughter” anharmonic non-resonant states, which then further decay into “granddaughter” and thermal bath states. The population of these states alter the index of refraction in time, Δn(t), and can be measured through the changing in the probe beam’s Rayleigh scattering. This thermalization process takes ~5.5 ps in acetone and ~3.7 ps in methanol. The scattering signals from each Δn(t) thermalization stage in the localized region, (“mother”, to “daughter”, to “granddaughter”, to the bath states, to the ground state), are fitted to theoretical decay equations that show the rise and fall times of the energy decay routes.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Photonic circuits for laser stabilization with integrated ultra-high Q and Brillouin laser resonators

The integration of stabilized lasers, sources that generate spectrally pure light, will provide compact, low-cost solutions for applications including quantum information sciences, precision navigation and timing, metrology, and high-capacity fiber communications. We report a significant advancement in this field, demonstrating stabilization of an integrated waveguide Brillouin laser to an integrated waveguide reference cavity, where both resonators are fabricated using the same CMOS-compatible integration platform. We demonstrate reduction of the free running Brillouin laser linewidth to a 292 Hz integral linewidth and carrier stabilization to a 4.9 × 10 –13 fractional frequency at 8 ms reaching the cavity-intrinsic thermorefractive noise limit for frequencies down to 80 Hz. We achieve this level of performance using a pair of 56.4 x 10 6 quality factor Si 3 N 4 waveguide ring-resonators that reduce the high-frequency noise by the nonlinear Brillouin process and the low-frequency noise by Pound–Drever–Hall locking to the ultra-low loss resonator. These results represent an important step toward integrated stabilized lasers with reduced sensitivity to environmental disturbances for atomic, molecular, and optical physics (AMO), quantum information processing and sensing, and other precision scientific, sensing, and communications applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Linear and Nonlinear X-ray Spectra of Chiral Molecules: X-ray Circular Dichroism, Sum- and Difference-Frequency Generation of Fenchone and Cysteine

Recent advancements in X-ray light sources enable element-sensitive nonlinear spectroscopies for probing molecular chirality. We simulate X-ray absorption spectroscopy, X-ray circular dichroism (XCD), and nonlinear optical/X-ray SFG and DFG (OX SFG/DFG) signals for two prototypical chiral molecules, fenchone and cysteine. Furthermore, our multireference simulations reproduce experimental data and reveal how novel X-ray spectroscopies exploit the site- and element-sensitivity of X-rays to uncover molecular asymmetry. The XCD spectra show strong asymmetries at chiral centers, while distant atoms contribute weaker signals. The OX SFG/DFG signals, under fixed resonant optical excitation, strongly depend on the core and valence excitations. This allows us to introduce two-dimensional (2D) chirality-sensitive valence-core spectroscopy, which provides insight into the overlap between valence orbitals and local molecular asymmetry. Finally, our estimates using realistic laser and X-ray pulse parameters demonstrate that such nonlinear experiments are feasible at XFELs, offering a promising tool for investigating chiral molecules.

Circular dichroism spectroscopy↗
DOE OSTI2021

Structure Tuning, Strong Second Harmonic Generation Response, and High Optical Stability of the Polar Semiconductors Na 1- x K x AsQ 2

We report the mixed cation compounds Na 1-x K x AsSe 2 (x = 0.8, 0.65, 0.5) and Na 0.1 K 0.9 AsS 2 crystallize in the polar noncentrosymmetric space group Cc. The AAsQ(2) (A = alkali metals, Q = S, Se) family features one-dimensional (1D) 1 / ∞ [AQ 2 - ] chains comprising corner-sharing pyramidal AQ 3 units in which the packing of these chains is dependent on the alkali metals. The parallel 1 / ∞ [AQ(2) - ] chains interact via short As ∙∙∙Se contacts, which increase in length when the fraction of K atoms is increased. The increase in the As ∙∙∙Se interchain distance increases the band gap from 1.75 eV in γ-NaAsSe 2 to 2.01 eV in Na 0.35 K 0.65 AsSe 2 , 2.07 eV in Na 0.2 K 0.8 AsSe 2 , and 2.18 eV in Na 0.1 K 0.9 AsS 2 . The Na 1-x K x AsSe 2 (x = 0.8, 0.65) compounds melt congruently at approximately 316 °C. Wavelength-dependent second harmonic generation (SHG) measurements on powder samples of Na 1-x K x AsSe 2 (x = 0.8, 0.65, 0.5) and Na 0.1 K 0.9 AsS 2 suggest that Na 0.2 K 0.8 AsSe 2 and Na 0.1 K 0.9 AsS 2 have the highest SHG response and exhibit significantly higher laser-induced damage thresholds (LIDTs). Theoretical SHG calculations on Na 0.5 K 0.5 AsSe 2 confirm its SHG response with the highest value of d 33 = 22.5 pm/V χ 333 (2) = 45.0 pm/V). The effective nonlinearity for a randomly oriented powder is calculated to be d eff = 18.9 pm/V χ eff (2) = 37.8 pm/V), which is consistent with the experimentally obtained value of d eff = 16.5 pm/V χ eff (2) = 33.0 pm/V). Three-photon absorption is the dominant mechanism for the optical breakdown of the compounds under intense excitation at 1580 nm, with Na 0.2 K 0.8 AsSe 2 exhibiting the highest stability.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Eshelby-twisted three-dimensional moiré superlattices

Twisted bilayers of van der Waals materials have recently attracted great attention due to their tunable, strongly correlated phenomena. In this work, we investigate the chirality-specific physics in three-dimensional moiré superlattices induced by Eshelby twist. Our direct density functional theory calculations reveal helical rotation leads to optical circular dichroism and chirality-specific nonlinear Hall effect, even though there is no magnetization or magnetic field. Both these phenomena can be reversed by changing the structural chirality. This provides a path to constructing chirality-specific materials.

2-dimensional systems↗
DOE OSTI2022

All-dielectric multi-resonant bullseye antennas

Integrated devices that generate multiple optical resonances in the same volume can enhance on-chip nonlinear frequency generation, nonlinear spectroscopy, and quantum sensing. Here, we demonstrate circular Bragg antennas that exhibit multiple spatially overlapping, polarization-selective optical resonances. Using templated atomic layer deposition of TiO 2 , these devices can be fabricated on arbitrary substrates, making them compatible with a wide range of nonlinear materials and sensing targets, and couple efficiently to underlying films. In this work, we detail the design, simulation, and fabrication of all-dielectric multi-resonant bullseye antennas and characterize their performance using polarized broadband reflection spectroscopy.

47 OTHER INSTRUMENTATION↗