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At least 181 records · Page 10

Sub-two-cycle gigawatt-peak-power LWIR OPA for ultrafast nonlinear spectroscopy of condensed state materials

The application of high-power, few-cycle, long-wave infrared (LWIR, 8–20 µm) pulses in strong-field physics is largely unexplored due to the lack of suitable sources. However, the generation of intense pulses with >6 µm wavelength range is becoming increasingly feasible with the recent advances in high-power ultrashort lasers in the middle-infrared range that can serve as a pump for optical parametric amplifiers (OPA). Here we experimentally demonstrate the feasibility of this approach by building an OPA pumped at 2.4 µm that generates 93 µJ pulses at 9.5 µm, 1 kHz repetition rate with sub-two-cycle pulse duration, 1.6 GW peak power, and excellent beam quality. The results open a wide range of applications in attosecond physics (especially for studies of condensed phase samples), remote sensing, and biophotonics.

Leshchenko, Vyacheslav (ORCID:0000000199708559)↗

Amplification of 10 μm picosecond pulses in a compact optically pumped multiatmosphere CO 2 laser

Picosecond pulses, generated by a commercial mid-IR optical parametric source (∼0.5 ps, 1-5 μJ), have been regeneratively amplified to an energy of ≤2 mJ in a palm-size high-pressure CO 2 amplifier optically pumped by a Q-switched 2.8 μm Cr:Er:YSGG laser. The characteristics of the amplified pulses have been studied as a function of seed wavelength centered around 10.3 or 10.6 μm, and the pressure in the gain medium. The measured amplified pulse length is ∼5 ps. Numerical modeling suggests that pulses as short as ∼0.5 ps with multi-GW peak power can be generated in a mixture of CO 2 isotopes. Robustness of the output of a compact CO 2 regenerative amplifier to the seed and pump fluctuations measured at 3 Hz and a perfect Gaussian beam profile indicates the potential of such laser technology for producing high-power ultrashort long-wave infrared pulses at high repetition rates.

43 PARTICLE ACCELERATORS↗

Broad Frequency Shift of Parametric Processes in Epsilon-Near-Zero Time-Varying Media

The ultrafast changes of material properties induced by short laser pulses can lead to a frequency shift of reflected and transmitted radiation. Recent reports highlight how such a frequency shift is enhanced in spectral regions where the material features a near-zero real part of the permittivity. Here, we investigate the frequency shift for fields generated by four-wave mixing. In our experiment, we observed a frequency shift of more than 60 nm (compared to the pulse width of ~40 nm) in the phase conjugated radiation generated by a 500 nm aluminium-doped zinc oxide (AZO) film pumped close to the epsilon-near-zero wavelength. Our results indicate applications of time-varying media for nonlinear optics and frequency conversion.

36 MATERIALS SCIENCE↗

Theory for anomalous terahertz emission in striped cuprate superconductors

Recent experiments in the doped cuprates La 2−𝑥 ⁢Ba 𝑥⁢ CuO 4 have revealed the emission of anomalous terahertz radiation after impulsive optical excitation. Here, we theoretically investigate the nonlinear electrodynamics of such striped superconductors and explore the origin of the observed radiation. We argue that photoexcitation is converted into a photocurrent by a second-order optical nonlinearity, which is activated by the breaking of inversion symmetry in certain stripe configurations. We point out the importance of including umklapp photocurrents modulated at the stripe periodicity itself, which impulsively drive surface Josephson plasmons and lead to a resonant structure of outgoing radiation, consistent with the experiments. We speculate on the utility of the proposed mechanism in the context of generating tunable terahertz radiation.

36 MATERIALS SCIENCE↗

Ultrafast X-Ray Scattering Reveals Composite Amplitude Collective Mode in the Weyl Charge Density Wave Material ( TaSe 4 ) 2 I

Here we report ultrafast x-ray scattering experiments of the quasi-1D charge density wave (CDW) material (TaSe 4 ) 2⁢ I following ultrafast infrared photoexcitation. From the time-dependent diffraction signal at the CDW sidebands we identify a 0.11 THz amplitude mode derived primarily from a transverse acoustic mode of the high-symmetry structure. From our measurements we determine that this mode interacts with the valence charge indirectly through another collective mode, and that the CDW system in (TaSe 4 ) 2 ⁢I has a composite nature supporting multiple dynamically active structural degrees of freedom.

36 MATERIALS SCIENCE↗

Selective Enhancement of Spectroscopic Features by Quantum Optimal Control

Tailored light can be used to steer atomic motions into selected quantum pathways. In optimal control theory (OCT), the target is usually expressed in terms of the molecular wave function, a quantity that is not directly observable in experiment. In this study, we present simulations using OCT that optimize the spectroscopic signal itself. By shaping the optical pump, the x-ray stimulated Raman signal, which occurs solely during the passage through conical intersections, is temporally controlled and amplified by up to 2 orders of magnitude. This enhancement can be crucial in order to bring small coherence-based signatures above the detectable threshold. Our approach is applicable to any signal that depends on the expectation value of a positive definite operator.

74 ATOMIC AND MOLECULAR PHYSICS↗

Optical parametric amplification of spectrally incoherent pulses

The optical parametric amplification of spectrally incoherent signals is analyzed and simulated using a set of normalized equations describing phase-matched three-wave nonlinear mixing. Varying the amplifier’s properties and the seeding conditions reveals different amplification regimes. In particular, the relative temporal walk-off of the signal, idler, and pump has a strong impact on the temporal and spectral properties of the amplified signal. The amplification efficiency for spectrally incoherent signals is not significantly lower than that of a coherent monochromatic signal, provided that the phase-matching bandwidth is sufficient. Here, the results obtained with the normalized set of equations are in good agreement with simulations based on the full description of the crystals’ dispersion for high-gain LBO and BBO preamplifiers and a low-gain DKDP power amplifier.

47 OTHER INSTRUMENTATION↗

Compact fiber-coupled narrowband two-mode squeezed light source

Quantum correlated states of light, such as squeezed states, are a fundamental resource for the development of quantum technologies, as they are needed for applications in quantum metrology, quantum computation, and quantum communications. It is thus critical to develop compact, efficient, and robust sources to generate such states. Here, we report on a compact, narrowband, fiber-coupled source of two-mode squeezed states of light at 795 nm based on four-wave mixing (FWM) in an 85 Rb atomic vapor. The source is designed in a small modular form factor, with two input fiber-coupled beams, the seed and pump beams required for the FWM, and two output fibers, one for each of the modes of the squeezed state. The system is optimized for low pump power (135 mW) to achieve a maximum intensity-difference squeezing of 4.4 dB after the output of fibers at an analysis frequency of 1 MHz. Furthermore, the narrowband nature of the source makes it ideal for atomic-based quantum sensing and quantum networking configurations that rely on atomic quantum memories. Such a source paves the way for a versatile and portable platform for applications in quantum information science.

Jain, Umang [University of Oklahoma, Norman, OK (U↗

Ultrafast temporal phase-resolved nonlinear optical spectroscopy in the molecular frame

In an ultrafast nonlinear optical interaction, the electric field of the emitted nonlinear signal provides direct access to the induced nonlinear transient polarization or transient currents and thus carries signatures of ultrafast dynamics in a medium. Measurement of the electric field of such signals offers sensitive observables to track ultrafast electron dynamics in various systems. In this work, we resolve the real-time phase of the electric field of a femtosecond third-order nonlinear optical signal in the molecular frame. The electric field emitted from impulsively pre-aligned gas-phase molecules at room temperature, in a degenerate four-wave mixing scheme, is measured using a spectral interferometry technique. The nonlinear signal is measured around a rotational revival to extract its molecular-frame angle dependence from pump-probe time-delay scans. By comparing these measurements for two linear molecules, carbon dioxide and nitrogen, we show that the measured second-order phase parameter (temporal chirp) of the signal is sensitive to the valence electronic symmetry of the molecules, whereas the amplitude of the signal does not show such sensitivity. We compare measurements to theoretical calculations of the chirp observable in the molecular frame. This work is an important step towards using electric field measurements in nonlinear optical spectroscopy to study ultrafast dynamics of electronically excited molecules in the molecular frame.

47 OTHER INSTRUMENTATION↗

Metastable argon dynamics in a pulsed microplasma at 43 GHz

Short pulses of millimeter wave (MMW) radiation at 43 GHz create microplasma within a photonic crystal for pressures from 40 to 600 Torr (1.3 × 10 3 –8.0 × 10 4 Pa). Gas breakdown occurs within a photonic crystal, which acts as an electromagnetic resonator to create a strong initial electric field. The time response of the argon metastable density is experimentally determined during the pulse and in the afterglow using laser absorption. The metastable density overshoots the steady-state condition at the beginning of the pulse and during the afterglow. Modeling is presented to understand these observations. The overproduction of argon 1s5 at the beginning of each pulse is due to a concurrent overshoot in the MMW electric field within the photonic crystal. This field overheats the plasma electrons and enhances the production of excited states. The burst of argon metastables observed in the afterglow is due to the pooled energy of the plasma stored in electrons, ions, and excited states of argon. As a result, understanding metastable production is an important intermediate step to ionization and is also critical in the study of diode-pumped rare gas lasers.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

HERO WEC V1.0 - WEC-Sim Detailed Simulation Runs and Summary Data

Data sets from simulation runs include 144 wave cases that were run based on the WEC-Sim model (https://mhkdr.openei.org/submissions/483). The 144 wave cases represent waves with the following wave height and wave period ranges: - Significant Wave Height: 0.25 - 4.0m in 0.25m increments - Wave Period: 5 - 13 sec in 1 sec increments Each run was simulated using a Pierson-Moskowitz irregular wave spectrum with a 200 second ramp time and a total simulation time of 2,200 seconds. Summary data set includes a spreadsheet and image files with matrices that are associated with data from simulation runs. All matrices cover the same significant wave height and wave periods from the sim runs, in the same increments. The following matrices are included: - Mechanical Power Input: Absorbed power calculated using linear input velocity at PTO (power take-off) multiplied by winch tension. - Mechanical Power Output: The hydraulic power calculated at the pump output prior to the pressure relief valve dump. - Feed Pressure: Average pressure at RO (reverse osmosis) input prior to pre-filters - RO Power Input: The hydraulic power calculated at the RO system inlet, accounts for flow loss due to pressure relief valve - Water Production: Average clean water flow at RO output

16 TIDAL AND WAVE POWER↗

Novel, Middle and Long Wave Infrared Laser Sources For Accelerator Applications

The main accomplishment during Years 2020-2024 of the DOE Accelerator Stewardship Program is proof-of-principle demonstration of amplification of an ultrashort 10 µm seed pulse in a multiatmosphere CO 2 laser optically pumped by nanosecond pulses of either a ~4.3 µm Fe:ZnSe laser or a 2.8 µm electro-optically (EO) Q-switched Er: Laser. This has been accomplished at the UCLA Neptune Laboratory by using about 100 mJ, ~100 ns long pulses generated by the pump laser built for this purpose by the UAB team. Implementation of EO Q-switching regime in the solid-state Er:laser system made possible nanosecond synchronization between the pump pulse and the 0.5 ps seed pulse produced by a commercial Ti:sapphire laser based mid-IR OPA/DFG. The injection mode-locking regime realized in a compact Mult atmosphere 3 Hz CO 2 -He regenerative amplifier enabled generation of a train of ultrashort pulses separated by the cavity round-trip time of ~3.2 ns. The measured gain lifetime of ~1 µs at a total pressure of ~12-15 atm indicates that lifetime of the upper laser level is a critical limiting factor in designing high-pressure CO 2 amplifiers. A single picosecond 10 mm pulse with an energy 0.1-0.2 mJ was extracted from the amplifier’s cavity using an ultrafast Ge semiconductor switch whose reflectivity was photo-induced by a femtosecond 800 nm pulse. For direct amplification regime, nonlinear absorption in Ge at 10 mm at GW/cm 2 intensities limited the extracted energy. Therefore, the generated energy could be further increased by minimizing losses in the switch and optimizing the cavity mode size. Based on the obtained data in collaboration with BNL colleagues, we have designed a high-pressure CO 2 amplifier to be used as a preamplifier for the future experiments at the ATF BNL. The latter work is the subject of funding availability.

60 APPLIED LIFE SCIENCES↗

Enhanced Microseismicity During Production Pumping Cessation at the San Emidio Geothermal Field (Nevada, USA) in December 2016

Abstract Tectonic activity, geothermal fluids, and microseismic events (MSEs) tend to occur in similar locations as a result of spatiotemporal changes in the subsurface stress state. To quantify this association, we analyze data from a dense seismic array deployed at the San Emidio geothermal field, Nevada for 1 week in December 2016 to coincide with a 19.45‐hr shutdown of all injection and production pumping operations. 123 MSEs were detected, of which 101 occurred during the shutdown. The spatial association of the MSEs with the production wells suggests a causal relationship between the production cessation and the MSEs. Here we performed a detailed analysis to investigate reservoir material properties, distribution of seismically activated faults, and local stress state. We determined the hypocenters, magnitudes, and focal mechanisms for the MSEs, P‐wave tomographic velocity model, and local stress tensor. The results show that most MSEs occurred near the production wells. Magnitudes fall between −2.2 and 0.0 with larger events located closer to the production wells. Most MSEs occurred within a westward‐dipping normal fault zone in the reservoir associated with anomalously low P‐wave velocity values. The focal mechanism and stress inversion results show predominantly normal faulting with the maximum horizontal stress oriented north‐south. We suggest that the MSEs during shutdown were triggered on pre‐existing, small‐scale, critically stressed fault patches in the reservoir as the pore pressure increased around the production wells when the production pumping ceased. We interpret the larger MSE magnitudes closer to the production wells as a result of higher pore pressure increase.

15 GEOTHERMAL ENERGY↗

Thomson Scattering with Gain

Thomson-scattering signals can be significantly modified by convective gains associated with the stimulated Raman scattering and stimulated Brillouin scattering instabilities as the scattered light traverses the probe beam. Gain results in amplification and narrowing of the red-shifted (i.e., Stokes) scattered light, whereas blue-shifted (anti-Stokes) features are depleted and broadened, making the relative prominence of these features a key signature of gain. Not accounting for instability growth has been a ubiquitous source of error in previous Thomson-scattering measurements.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Utah FORGE Friction-Permeability-Seismicity Laboratory Experiments with Non-Linear Acoustics

Laboratory experimental data on saw-cut interface of Westerly Granite and Utah Forge granitoid rocks. Experiments include velocity-stepping and fluid pressure stepping experiments. Mechanical data from 3 ISCO pumps connected to a Temco pressure vessel measure axial, confining and fault: fluid pressure (kPa), fluid flow rate (mL/min) and volume remaining in pump (mL). Non-linear acoustic data acquired via Verasonics systems connected to PZTs inside the pressure vessel give the timeshift, amplitude and RMS amplitude of the passing P-wave.

15 GEOTHERMAL ENERGY↗

Laser-free GHz stroboscopic transmission electron microscope: Components, system integration, and practical considerations for pump–probe measurements

In this work a 300 keV transmission electron microscope was modified to produce broadband pulsed beams that can be, in principle, between 40 MHz and 12 GHz, corresponding to temporal resolution in the nanosecond to picosecond range without an excitation laser. The key enabling technology is a pair of phase-matched modulating and de-modulating traveling wave metallic comb striplines (pulsers). An initial temporal resolution of 30 ps was achieved with a strobe frequency of 6.0 GHz. The placement of the pulsers, mounted immediately below the gun, allows for preservation of all optical configurations, otherwise available to the unmodified instrument, and therefore makes such a post-modified instrument for dual-use, i.e., both pulsed-beam mode (i.e., stroboscopic time-resolved) and conventional continuous waveform mode. In this article, we describe the elements inserted into the beam path, challenges encountered during integration with an in-service microscope, and early results from an electric-field-driven pump–probe experiment. We conclude with ideas for making this class of instruments broadly applicable for examining cyclical and repeatable phenomena.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Perturbative theoretical model of electronic transient circular dichroism spectroscopy of molecular aggregates

A chiral analog of transient absorption spectroscopy, transient circular dichroism (TCD) spectroscopy is an emerging time-resolved method. Both spectroscopic methods can probe the electronic transitions of a sample, and TCD is additionally sensitive to the dynamic aspects of chirality, such as those induced by molecular excitons. Here, we develop a theoretical description of TCD for electronic multi-level models in which the pump pulse is linearly polarized and probe pulse is alternately left- and right-circularly polarized. We derive effective response functions analogous to those often used to describe other four-wave mixing methods and then simulate and analyze TCD spectra for three representative multi-level electronic model systems. We elaborate on the presence and detection of the spectral signatures of electronic coherences.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Photoelectron spectroscopy with entangled photons; enhanced spectrotemporal resolution

In this theoretical study, we show how photoelectron signals generated by time-energy entangled photon pairs can monitor ultrafast excited state dynamics of molecules with high joint spectral and temporal resolutions, not limited by the Fourier uncertainty of classical light. This technique scales linearly, rather than quadratically, with the pump intensity, allowing the study of fragile biological samples with low photon fluxes. Since the spectral resolution is achieved by electron detection and the temporal resolution by a variable phase delay, this technique does not require scanning the pump frequency and the entanglement times, which significantly simplifies the experimental setup, making it feasible with current instrumentation. Application is made to the photodissociation dynamics of pyrrole calculated by exact nonadiabatic wave packet simulations in a reduced two nuclear coordinate space. This study demonstrates the unique advantages of ultrafast quantum light spectroscopy.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗