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At least 379 records · Page 21

Floquet Prethermalization with Lifetime Exceeding 90 s in a Bulk Hyperpolarized Solid

Here, we report the observation of long-lived Floquet prethermal states in a bulk solid composed of dipolar-coupled 13 C nuclei in diamond at room temperature. For precessing nuclear spins prepared in an initial transverse state, we demonstrate pulsed spin-lock Floquet control that prevents their decay over multiple-minute-long periods. We observe Floquet prethermal lifetimes $T^{'}_{2}$≈90.9 s, extended >60 000-fold over the nuclear free induction decay times. The spins themselves are continuously interrogated for ~10 min, corresponding to the application of ≈5.8×10 6 control pulses. The 13 C nuclei are optically hyperpolarized by lattice nitrogen vacancy centers; the combination of hyperpolarization and continuous spin readout yields significant signal-to-noise ratio in the measurements. This allows probing the Floquet thermalization dynamics with unprecedented clarity. We identify four characteristic regimes of the thermalization process, discerning short-time transient processes leading to the prethermal plateau and long-time system heating toward infinite temperature. This Letter points to new opportunities possible via Floquet control in networks of dilute, randomly distributed, low-sensitivity nuclei. In particular, the combination of minutes-long prethermal lifetimes and continuous spin interrogation opens avenues for quantum sensors constructed from hyperpolarized Floquet prethermal nuclei.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

The importance of shear on the collective charge transport in CDWs revealed by an XFEL source

Charge transport in materials has an impact on a wide range of devices based on semiconductor, battery, or superconductor technology. Charge transport in sliding charge density waves (CDW) differs from all others in that the atomic lattice is directly involved in the transport process. To obtain an overall picture of the structural changes associated to the collective transport, the large coherent x-ray beam generated by an x-ray free-electron laser (XFEL) source was used. The CDW phase can be retrieved over the entire sample from diffracted intensities using a genetic algorithm. For currents below threshold, increasing shear deformation is observed in the central part of the sample while longitudinal deformation appears above threshold when shear relaxes. Shear thus precedes longitudinal deformation, with relaxation of one leading to the appearance of the other. Moreover, strain accumulates on surface steps in the sliding regime, demonstrating the strong pinning character of these surface discontinuities. The sliding process of nanometric CDW involves macroscopic sample dimensions.

36 MATERIALS SCIENCE↗

Three phase spectral interferometry for recording high dynamic range optical waveforms with <1 ps resolution over >2 ns records applied to closed-loop pulse shaping

Herein we demonstrate, to our knowledge, a novel spectral interferometry technique that simultaneously captures three spectral interferograms of a signal waveform with a reference pulse. The measured performance is robust to nonidealities and ambient drifts by implementing a precisely calibrated 3 × 3 polarization maintaining (PM) splitter that provides three phase shift differences nominally spaced 120° apart. The system can achieve long record length by implementing three, high resolution, virtually imaged phase array (VIPA) spectrometers. Here, we experimentally implement this technique and demonstrate the measurement of waveforms with >2ns of record while maintaining <1ps resolution.

42 ENGINEERING↗

Design, tuning, and blackbox optimization of laser systems

Chirped pulse amplification (CPA) and subsequent nonlinear optical (NLO) systems constitute the backbone of myriad advancements in semiconductor manufacturing, communications, biology, defense, and beyond. Accurately and efficiently modeling CPA+NLO-based laser systems is challenging because of the complex coupled processes and diverse simulation frameworks. Our modular start-to-end model unlocks the potential for exciting new optimization and inverse design approaches reliant on data-driven machine learning methods, providing a means to create tailored CPA+NLO systems unattainable with current models. To demonstrate this new, to our knowledge, technical capability, we present a study on the LCLS-II photo-injector laser, representative of a high-power and spectro-temporally non-trivial CPA+NLO system.

47 OTHER INSTRUMENTATION↗

Bell state analyzer for spectrally distinct photons

We demonstrate a Bell state analyzer that operates directly on frequency mismatch. Based on electro-optic modulators and Fourier-transform pulse shapers, our quantum frequency processor design implements interleaved Hadamard gates in discrete frequency modes. Experimental tests on entangled-photon inputs reveal fidelities of ∼ <#comment/> 98 % <#comment/> for discriminating between the | Ψ <#comment/> + ⟩ <#comment/> and | Ψ <#comment/> − <#comment/> ⟩ <#comment/> frequency-bin Bell states. Our approach resolves the tension between wavelength-multiplexed state transport and high-fidelity Bell state measurements, which typically require spectral indistinguishability.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Pulsed Magnetic Gradiometry in Earth's Field [Poster]

We describe a novel pulsed magnetic gradiometer based on the optical interference of sidebands generated using two spatially separated alkali vapor cells. In contrast to traditional magnetic gradiometers, our approach provides a direct readout of the gradient field without the intermediate step of subtracting the outputs of two spatially separated magnetometers. Operation of the gradiometer in multiple field orientations is discussed. The noise floor is measured as low as 25$\frac{fT}{\sqrt{Hz-cm}}$ in a room without magnetic shielding.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Assessment of Hydroxyl Radical Reactivity in Sulfur-Containing Amino Acid Models Under Acidic pH

Methionine residues in proteins and peptides are frequently oxidized by losing one electron. The presence of nearby amide groups is crucial for this process, enabling methionine to participate in long-range electron transfer. Hydroxyl radical (HO•) plays an important role being generated in aerobic organisms by cellular metabolisms as well as by exogenous sources such as ionizing radiations. The reaction of HO• with methionine mainly affords the one-electron oxidation of the thioether moiety through two consecutive steps (HO• addition to the sulfur followed by HO− elimination). We recently investigated the reaction of HO• with model peptides mimicking methionine and its cysteine-methylated counterpart, i.e., CH3C(O)NHCHXC(O)NHCH3, where X = CH2CH2SCH3 or CH2SCH3 at pH 7. The reaction mechanism varied depending on the distance between the sulfur atom and the peptide backbone, but, for a better understanding of various suggested equilibria, the analysis of the flux of protons is required. We extended the previous study to the present work at pH 4 using pulse radiolysis techniques with conductivity and optical detection of transient species, as well as analysis of final products by LC-MS and high-resolution MS/MS following γ-radiolysis. Comparing all the data provided a better understanding of how the presence of nearby amide groups influences the one-electron oxidation mechanism.

Biochemistry & Molecular Biology↗

Laser Based Ultrasound for Verification of Circuit Card Assemblies

This IR is a follow-up conference Paper to the IR approved abstract; PNNL-SA-194096. --- Verification that equipment is authentic and not changed; even at the circuit card assembly (CCA) level will likely be an important component of future arms control treaties. This effort was an initial evaluation of the potential for laser-based ultrasound (LBU) as an inspection tool for Unique Identification (UID) of Circuit Card Assembly (CCA) boards and CCA components. The LBU system used a laser pulse for ultrasound generation and an Optical Microphone for ultrasound detection to image subsurface structures without physical contact and in a dry state. This paper described the selected CCA surrogate, CCA components that were examined, the LBU system, LBU images of the CCA components, and the initial development of UID algorithms. Receiver operating characteristics (ROC) curves indicated good performance for two algorithms as a potential means for UID of CCA boards and CCA components.

Laser Ultrasound, Equipment Verification, Arms Con↗

Phase Demodulation by Frequency Chirping in Coherence Microwave Photonic Interferometry

This paper presents a signal processing method to demodulate the optical interference phase of cascaded individual optical fiber intrinsic Fabry-Perot interferometric (IFPI) sensors in a coherent microwave-photonic interferometry (CMPI) distributed sensing system. The new method utilizes the chirp effect of electro-optic modulator (EOM) to create a quasi-quadrature optical interference phase shift between two adjacent pulses which correspond to two adjacent reflection points in the time domain. The phase shift can be controlled by adjusting the bias voltage that is applied to the EOM. The interference phase is calculated by elliptically fitting the phase shift. The interference phase change is proportional to the optical path difference (OPD) change of the interferometer, and the sign can be used to differentiate the increase or decrease of the OPD. The method is demonstrated for distributed strain sensing, showing good linearity, high resolution and large dynamic range.

42 ENGINEERING↗

Generation of 3.3-mJ, 2.45-µm, sub-2-cycle laser pulses via hollow-core fiber pulse compression

We demonstrate nonlinear compression of mid-infrared pulses from a Cr:ZnSe chirped-pulse amplifier using a gas-filled stretched hollow-core fiber followed by bulk-material compression. Starting from 90 fs, 2.45 µm pulses with 5.3 mJ energy, spectral broadening in the gas-filled capillary combined with optimized dispersion management enables compression to 15 fs, less than two optical cycles at 2.45 µm, with 3.3 mJ pulse energy, corresponding to a peak power of approximately 0.12 TW. The simplicity of the approach, based on a single hollow-core fiber stage and bulk dispersion compensation, makes it scalable to higher energies and establishes a robust route to mid-infrared drivers for high harmonic generation and attosecond applications.

Britton, Mathew [SLAC National Accelerator Laborat↗

Ultra-high energy density relativistic plasmas from nanostructures: scaling to ultra-high intensities (Final Report)

This project investigated the ultra-high energy density (UHED) regime of matter found in the center of stars, using a compact PW-class laser. These extreme conditions are typically only obtained in the laboratory in the central hot-spot of spherically imploded capsules in inertial confinement fusion experiments driven by the world’s largest lasers. We have shown that near-solid density arrays of aligned nanostructures can be volumetrically heated to multi-keV temperatures by irradiation at relativistic intensity with ultrafast laser pulses of modest energy, opening a path for the generation of UHED plasmas with compact lasers. This new UHED plasma generation approach promises to create an environment with extreme energy densities and degrees of ionization, record conversion of optical laser light into ultrafast x-ray pulses, gigantic magnetic fields and pressures, and directed beams of high energy particles . In this project we achieved record degree of ionization in volumetric heating solid density and near-solid density plasmas. Gold plasmas which spectra is characterized by L shell transition emission from ions with charge up to the Ne-like state, Au+ 72 were generated using ultrafast laser pulses of less than 10 J of energy from a compact laser focused to an intensity of ~ 3x10 21 Wcm -2 . We also conducted measurements to determine the heat penetration depth in Ni nanowire arrays as compared to Ni foil targets by monitoring the line emission of a Co buried tracer underneath a variable amount of Ni. The measurements revealed that the nanowire plasmas are roughly six times larger in depth than the solid density target plasmas. A result of this increased plasma in nanowire arrays is a greatly increased conversion of optical laser light into > 1 KeV x-rays, a record conversion efficiency of 20 %. Critical to the realization of the proposed experiments was the generation of ultrafast laser pulses with ultra-high contrast that can deposit the energy deep into the nanowire arrays before the nanowires explode to create a continuous plasma. Supporting the proposed experiments was the recent demonstration at Colorado State University of a Petawatt-class laser that emits 30 fs pulses at high repetition rates. The experiments combined this unique laser tool with a variety of tailored nanowire arrays fabricated in house and with an extensive suite of diagnostics. The experiments were accompanied by 3-dimensional particle-in-cell simulations and detailed atomic physics simulations with transient kinetics and radiation transport. The proposed research allowed us to continue training Ph.D students and post-docs with broad experience in HEDP Science.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Second-harmonic generation in zinc blende crystals under combined action of femtosecond optical and strong terahertz fields

The influence of a short intense (with an electric field strength up to 250 kV cm{sup −1}) terahertz (THz) pulse on the generation of second harmonic (SH) of Ti : sapphire laser radiation in crystals of zinc blende type (InAs and GaAs), characterised by nonzero bulk quadratic susceptibility, is investigated. It is experimentally shown for InAs(100) that, in the case of s-polarised first and second harmonics, an application of s-polarised THz field changes significantly the SH signal. The THz field-induced azimuthal dependence of the SH signal is in good agreement with the results of theoretical calculation within a phenomenological approach. The dependence of the SH signal on the delay time between the optical and THz pulses is investigated. This dependence for the GaAs crystal repeats the envelope of the THz pulse intensity, whereas in the case of InAs crystal there is a significant discrepancy, caused by the nonlinear dynamics of strong THz field in InAs. (nonlinear optical phenomena)

36 MATERIALS SCIENCE↗

Carrier-envelope-phase characterization of ultrafast mid-infrared laser pulses through harmonic generation and interference in argon

The propagation of an intense, femtosecond, mid-infrared laser pulse in a gaseous medium results in the efficient generation of spectrally overlapping low-order harmonics, whose optical carrier phases are linked to the carrier-envelope phase (CEP) of the mid-infrared driver pulse. Random peak-power fluctuations of the driver pulses, converted to the fluctuations of the nonlinear phases, acquired by the pulses on propagation, cause this phase correlation to smear out. We show that this seemingly irreversible loss of phase can be recovered, and that the complete information needed for the phase correction is contained in the harmonic spectra itself. The optical phases of the intense driver pulse and its harmonics, as fragile as they appear to be against even weak disturbances, evolve deterministically during highly nonlinear propagation through the extended ionization region.

nonlinear optics↗

XUV-driven plasma switch for THz: new spatio-temporal overlap tool for XUV–THz pump–probe experiments at FELs

A simple and robust tool for spatio-temporal overlap of THz and XUV pulses in in-vacuum pump–probe experiments is presented. The technique exploits ultrafast changes of the optical properties in semiconductors (i.e. silicon) driven by ultrashort XUV pulses that are probed by THz pulses. This work demonstrates that this tool can be used for a large range of XUV fluences that are significantly lower than when probing by visible and near-infrared pulses. This tool is mainly targeted at emerging X-ray free-electron laser facilities, but can be utilized also at table-top high-harmonics sources.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Performance of microchannel plate based detectors for <25 keV x rays: Monte Carlo simulations and comparisons with experimental results

We present the results of Monte Carlo simulations of the microchannel plate (MCP) response to x rays in the 250 eV to 25 keV energy range as a function of both x-ray energy and impact angle and their comparisons with the experimental results from the X8A beamline at the National Synchrotron Light Source at Brookhaven National Laboratory. Incoming x rays interact with the lead glass of the microchannel plate, producing photoelectrons. Transport of the photoelectrons is neglected in this model, and it is assumed that photoelectrons deposit all their energy at the point they are created. This deposition leads to the generation of many secondary electrons, some fraction of which diffuse to the MCP pore surface where they can initiate secondary electron cascades in the pore under an external voltage bias. X-ray penetration through multiple MCP pore walls is increasingly important above 5 keV, and the effect of this penetration on MCP performance is studied. In agreement with past measurements, we find that the dependence of MCP sensitivity with angle relative to the pore bias changes from a cotangent dependence to angular independence and then proceeds to a secant dependence as the x-ray energy increases. We also find that with the increasing x-ray energy, the MCP gain sensitivity as a function of bias voltage decreases. The simulations also demonstrate that for x rays incident normal to the MCP surface, spatial resolution shows little dependence on the x-ray energy but degrades with the increasing x-ray energy as the angle of incidence relative to the surface normal increases. This agrees with experimental measurements. Simulation studies have also been completed for MCPs gated with a subnanosecond voltage pulse. In this work, we find that the optical gate profile width increases as the x-ray energy is increased above 5 keV, a consequence of increased x-ray penetration at energies >5 keV. Simulations of the pulsed dynamic range show that the dynamic range varies between ~100 and 1000 depending on x-ray energy and peak voltage.

47 OTHER INSTRUMENTATION↗

Optical stark effect on CdSe nanoplatelets with mid-infrared excitation for large amplitude ultrafast modulation

The optical Stark effect is a universal response of the electronic structure to incident light. In semiconductors, particularly nanomaterials, the optical Stark effect achieved with sub-band gap photons can drive large, narrowband, and potentially ultrafast changes in the absorption or reflection at the band gap through excitation of virtual excitons. Rapid optical modulation using the optical Stark effect is ultimately constrained, however, by the generation of long-lived excitons through multiphoton absorption. This work compares the modulation achievable using the optical Stark effect on CdSe nanoplatelets with several different pump photon energies, from the visible to mid-infrared. Despite expected lower efficiencies for spectrally-remote pump energies, infrared pump pulses can ultimately drive larger sub-picosecond optical Stark shifts of virtual excitons without creation of real excitons. Importantly, the CdSe nanoplatelets show subpicosecond shifts of the lowest excitonic resonance of up to 22 meV, resulting in change in absorption as large as 0.32 OD (49% increase in transmission), with a long-lived offset from real excitons less than 1% of the peak signal.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Controlled Injection of Electrons for Improved Performance of Laser-Wakefield Acceleration

Our lab performed a series of experiments on controlled injection of LWFA with two extreme laser pulses: one laser pulse was used to drive LWFA. In contrast, the other precisely controls the injection of electrons into the wakefield plasma wave. We have demonstrated an efficient reduction of electron beam emittance by optical injection and novel spatio-temporal manipulation of the electron beam by the extreme laser-plasma waves. Moreover, the optical injection process involves unprecedented new physics, which will benefit studies in astrophysics, inertial confinement fusion, laser-driven x-ray light sources, and ultrafast science. We further improved the performance of LWFA by a better understanding and control of the extreme laser-plasma wave dynamics for optical injection. Three novel mechanisms were identified in the optical injection process: (1) collision of two laser pulses, (2) collision of a laser pulse with a wakefield plasma wave, and (3) collision of two laser wakefields. All three methods improved electron-beam energy spread, emittance, stability, and reproducibility. First, we identified, compared, and independently controlled these different injection mechanisms by controlling the polarization of the injector laser pulse. Second, we manipulated the spatiotemporal splitting of LWFA electron beams to reduce their emittance. Third, we applied the same laser-plasma-wave dynamics and the same experimental setup for improved performance of ion acceleration, which has also been predicted by the recent simulations.

43 PARTICLE ACCELERATORS↗