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At least 415 records · Page 23

All-optical control of charge transfer and interlayer excitons in transition metal dichalcogenide heterostructures

An all-optical approach to control interlayer charge transfer and interlayer exciton dynamics is demonstrated using transition metal dichalcogenide heterostructures of MoSe 2 /MoS 2 and MoSe 2 /WS 2 as examples. In the three-pulse pump-probe experiments, a control pulse injects photocarriers and produces an electric field due to the interlayer charge separation. A pump pulse excites new carriers and their dynamics under the influence of the control-injected carriers and field is time-resolved by measuring differential reflectance of a third probe pulse. In MoSe 2 /MoS 2 , the interlayer electron transfer time from MoSe 2 to MoS 2 decreases with increasing the control-injected carrier density and electric field. The dipole moment of the interlayer excitons is reduced by the control pulse, which can be utilized for ultrafast and all-optical control of interlayer excitons. The recombination of the interlayer excitons is enhanced by the control pulse, which increases the spatial overlap of the electron and hole wave functions. The effect of the control pulse on the interlayer excitons is confirmed in the MoSe 2 /WS 2 heterostructure, although its effect on the electron transfer time is not resolvable. Furthermore, these results reveal useful information to understand and control interlayer charge transfer dynamics and provide tools for ultrafast manipulation of electrons in van der Waals heterostructures.

36 MATERIALS SCIENCE↗

Studies of Laser-Driven Flyer Acceleration Using Optical Fiber Coupling [Book Chapter]

An optically recording velocity interferometer system has been used to measure acceleration histories and maximum velocities for laser-driven aluminum foil targets launched from the output face of optical fibers. Peak flyer velocities have been determined as a function of various parameters, including driving laser fluence, laser pulse duration and target thickness. The results at high fluences are consistent with a nearly constant efficiency of coupling optical energy into flyer kinetic energy and a small ablated mass fraction; however, the coupling efficiency falls off rapidly at fluences < 15 J-cm -2 . Measurement of the time delay between laser pulse arrival at the target and the onset of flyer motion have also been performed. Significant delays are observed at low fluences, arising from the increased time required for plasma formation at the fiber/foil interface under these conditions.

440600 -- Optical Instrumentation-- (1990-)↗

Effects of frequency and pulse width on electron density, hydrogen peroxide generation, and perfluorooctanoic acid mineralization in a nanosecond pulsed discharge gas-liquid plasma reactor

Plasma electron density and temperature were characterized in a continuous flowing gas-liquid film reactor with argon carrier gas by time-resolved optical emission spectroscopy. The plasma parameters were studied as a function of time for varying pulse widths and frequencies. Pulse frequency was varied between 1 and 10 kHz at 16 kV (input voltage) and 40 ns (pulse width) using an Eagle Harbor Technologies, Inc. (EHT) power supply and 5–100 kHz using an Airity Technologies, LLC (AT) power supply. The pulse width was varied between 40 and 200 ns at 16 kV, 2 kHz with the EHT power supply. Optimal frequencies of 5 and 20 kHz were observed for peak electron density with EHT and AT power supplies, respectively. The peak electron density increased with increasing pulse width between 40 and 200 ns using the EHT power supply. Hydrogen peroxide exiting the reactor in the liquid phase increased with discharge power irrespective of the power supply or pulse parameters. Mineralization of 12.5, 50, and 200 ppm perfluorooctanoic acid (PFOA) dissolved in DI water to fluoride (F - ) correlated to the peak electron density. Glycerol, a liquid-phase hydroxyl radical scavenger, depleted hydrogen peroxide but did not affect PFOA mineralization. CO, a gas-phase hydroxyl radical scavenger, led to a reduction in the formation of F - production, suggesting hydroxyl radicals in the gas-liquid film play a necessary, but not singular, role in mineralization of PFOA.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Quantum Interferometric Pathway Selectivity in Difference-Frequency-Generation Spectroscopy

Even-order spectroscopies such as sum-frequency generation (SFG) and difference-frequency generation (DFG) can serve as direct probes of molecular chirality. Such signals are usually given by the sum of several interaction pathways that carry different information about matter. Here we focus on DFG, involving impulsive optical–optical–IR interactions, where the last IR pulse probes vibrational transitions in the ground or excited electronic state manifolds, depending on the interaction pathway. Spectroscopy with classical light can use phase matching to select the two pathways. In this theoretical study, we propose a novel quantum interferometric protocol that uses entangled photons to isolate individual pathways. Importantly, this additional selectivity originates from engineering the state of light using a Zou–Wang–Mandel interferometer combined with coincidence detection.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Hollow plasma structure during the breakdown phase of nanosecond pulsed pin–pin discharges generated with overvoltage

Atmospheric pressure nanosecond repetitive pulsed discharges are of interest for applications in combustion, material processing, plasma medicine and gas treatment. Here, the observation of a hollow structure at the ignition stage of such discharge in a pin–pin geometry is reported. Plasma images show that the phenomenon occurs in a variety of gases (helium, humid helium, argon and air) suggesting that it is in first approximation non-species specific. The phenomenon is investigated in detail in pure helium discharges for peak applied voltages between 3 and 6 kV and 200 ns voltage pulse duration by performing time-resolved optical emission spectroscopy measurements of electron density, gas temperature and electric field. All the measurements were performed at the mid-gap during the early stages of the discharge, near the breakdown. The transition from a homogeneous filament to a hollow structure occurs between 4 and 5 kV in helium. Electron density measurements by Stark broadening of the He I line at 492.2 nm show no significant difference in electron densities for the applied voltage between 3 and 6 kV. In all cases, a maximum electron density of about 3.5 × 10 21 m –3 was found. Electric field measurements performed by Stark polarization spectroscopy of the He I transition at 492.2 nm and of its forbidden counterpart show electric field strengths higher than the DC breakdown field of helium at atmospheric pressure consistent with the generation of the discharges with overvoltage. Moreover, a correlation between electric field values and the appearance of the hollow structure is observed and, remarkably, the phenomenon is not sensitive to the pre-ionization level (memory effect). Possible mechanisms for the phenomenon are discussed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Flying focus with arbitrary directionality for spatiotemporal control of laser intensity

Flying focus techniques produce laser pulses whose focal points travel at arbitrary, controllable velocities. While this flexibility can enhance a broad range of laser-based applications, existing techniques constrain the motion of the focal point to the propagation direction of the pulse. Here, we introduce a flying focus configuration that decouples the motion of the focus from the propagation direction. Here, a chirped laser pulse focused and diffracted by a diffractive lens and grating creates a focal point that can move both along and transverse to the propagation direction. The focal length of the lens, grating period, and chirp can be tuned to control the direction and velocity of the focus. Simulations demonstrate this control for a holographic configuration suited to high-power pulses, in which two off-axis pump beams with different focal lengths encode the equivalent phase of a chromatic lens and grating in a gas or plasma. For low-power pulses, conventional solid-state or adaptive optics can be used instead. Multi-dimensional control over the focal trajectory enables new configurations for applications, including laser wakefield acceleration of ions, nonlinear Thomson scattering, and surface-plasmon emission of THz radiation.

Classical optics↗

Electric-field enhancement caused by subwavelength-sized particles located on the surface of multilayer dielectric mirrors

A laser pulse impinging on the surface of an optical component can interact with particles, such as contamination debris, to produce a scattered electric field, which, either by itself or combined with the incident laser field, coherently can significantly increase the local field intensity. This effect can be of critical importance as it can reduce the laser-induced–damage threshold of the affected component. In this work, we use a field-propagation code to improve understanding regarding the factors that determine the magnitude and location of the electric-field enhancement for the case of subwavelength-sized particles located on the surface of multilayer dielectric mirrors.

47 OTHER INSTRUMENTATION↗

Longitudinal shaping of plasma waveguides using diffractive axicons for laser wakefield acceleration

New techniques for the optical generation of plasma waveguides—optical fibers for ultra-intense light pulses—have become vital to the advancement of multi-GeV laser wakefield acceleration. Here, we demonstrate the fabrication and characterization of a transmissive 8-level logarithmic diffractive axicon (LDA) for the generation of meter-scale plasma waveguides. These LDAs enable the formation of a Bessel-like beam with controllable start and end locations of the focal line and near-constant intensity on axis. We present measurements of the Bessel-like focal profile produced by the LDA and of the leading end of the plasma column generated by it. One important feature is the formation of a funnel-mouthed plasma channel entrance that can act as waveguide coupler. We also compare the diffraction efficiency of our 8-level LDA to 4-level and binary versions, with measurements comparing well to theory.

Tripathi, N.↗

The Illumination of Thunderclouds by Lightning: 4. Volumetric Thunderstorm Imagery

Optical instruments such as the Geostationary Lightning Mapper (GLM) detect lightning based on transient changes in cloud illumination. The horizontal location of lightning is determined from the coordinates of the pixels on the imaging array illuminated during the flash. However, the vertical position of the lightning pulses (approximated by GLM “groups”) below the cloud top cannot be routinely measured from a single space-based instrument. In our prior work, we have developed a machine learning algorithm that can infer optical source altitude for a given pulse based on how the optical energy is distributed across the group footprint and the local Advanced Baseline Imager Cloud-Top Height (CTH). In this fourth part of our thundercloud illumination study, we leverage these source altitudes to generate volumetric GLM imagery of a Colombia thunderstorm. We find that 3D versions of the current GLM meteorological imagery products (that describe thunderstorm kinematics) and thundercloud imagery products (that depict how the flashes appear from space) provide additional insights into lightning activity in the thunderstorm that are lost in the vertical integration used to generate the current 2D GLM gridded products. This new volumetric imaging capability provides a more comprehensive picture of where lightning occurs in the storm, how its physical characteristics vary across three-dimensional space, and how its optical emissions interact with surrounding the cloud medium.

54 ENVIRONMENTAL SCIENCES↗

Octave-spanning mid-infrared femtosecond OPA in a ZnGeP 2 pumped by a 2.4 μm Cr:ZnSe chirped-pulse amplifier

We report on the highly efficient, octave-spanning mid-infrared (mid-IR) optical parametric amplification (OPA) in a ZnGeP 2 (ZGP) crystal, pumped by a 1 kHz, 2.4 μm, 250 fs Cr:ZnSe chirped-pulse amplifier. The full spectral coverage of 3−10 μm with the amplified signal and idler beams is demonstrated. The signal beam in the range of ∼3 − 5 μm is produced by either white light generation (WLG) in YAG or optical parametric generation (OPG) in ZGP using the common 2.4 μm pump laser. We demonstrate the pump to signal and idler combined conversion efficiency of 23% and the pulse energy of up to 130 μJ with ∼2 μJ OPG seeding, while we obtain the efficiency of 10% and the pulse energy of 55 μJ with ∼0.2 μJ WLG seeding. The OPA output energy is limited by the available pump pulse energy (0.55 mJ at ZGP crystal) and therefore further energy scaling is feasible with multi-stage OPA and higher pump pulse energy. The autocorrelation measurements based on random quasi-phase matching show that the signal pulse durations are ∼318 fs and ∼330 fs with WLG and OPG seeding, respectively. In addition, we show the spectrally filtered 30 μJ OPA output at 4.15 μm suitable for seeding a Fe:ZnSe amplifier. Our ultrabroadband femtosecond mid-IR source is attractive for various applications, such as strong-field interactions, dielectric laser electron acceleration, molecular spectroscopy, and medical surgery.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Attosecond Optical Orientation

Circularly polarized light offers opportunities to probe symmetry-dependent properties of matter such as chirality and spin. Circular-dichroic measurements typically require further intrinsic or extrinsic breaking of symmetry by, e.g., enantiomeric excess, orientation, magnetic fields, or direction-sensitive detectors. Here we introduce circular-dichroic attosecond transient absorption spectroscopy by leveraging the angular momentum of two circularly polarized pulses, both pump and probe, in an isotropic medium, optically orienting the angular momentum of excited states on an attosecond timescale. We investigate a circular-dichroic measurement of the attosecond transient absorption of He Rydberg states. By limiting the allowed pathways via dipole selection rules for co- and counterrotating circularly polarized near-infrared and extreme ultraviolet (XUV) pulses, different spectral reshapings of the XUV transient absorption due to the AC Stark effect are observed. Furthermore, paired with time-dependent Schrödinger equation calculations, the results show the role of selection and propensity rules and open up new opportunities to study coupling pathways of excited states as well as spin-dependent dynamics in atoms and beyond via attosecond optical orientation.

Angular momentum of light↗

Transitions between electron emission and gas breakdown mechanisms across length and pressure scales

This Perspective outlines theoretical, simulation, and experimental studies linking electron emission and gas breakdown. Many studies have investigated field emission-driven microscale gas breakdown, including recent reviews [Garner et al., IEEE Trans. Plasma Sci. 48, 808–824 (2020); Fu et al., Plasma Res. Express 2, 013001 (2020)]. This Perspective focuses on generalizing field emission-driven microscale gas breakdown to consider the contribution of other forms of electron emission, specifically thermionic and space-charge limited. Recent theoretical studies have unified thermionic, field, and space-charge limited emission with and without collisions to derive “nexuses” where the individual solutions match, indicating transitions in the mechanisms. Reducing device size to nanoscale at atmospheric pressure leads to a transition from field emission to space-charge limited emission for nitrogen at ~250 nm. This Perspective summarizes the derivation of these nexuses and future extensions. We next describe simulation and theoretical studies for field emission-driven microscale gas breakdown and highlight how the nexus theory may be integrated to account for temperature, space-charge, and pulse parameters. Finally, we summarize the development of optical techniques to assess microscale gas breakdown and recent nanoscale experiments at atmospheric pressure that suggest that space-charge may begin to contribute to field emission prior to gas breakdown. We highlight the combination of theory, simulation, and experiment to link electron emission and gas breakdown mechanisms across length, pressure, and temperature scales for applications that include vacuum electronics, pulsed power, and medicine.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Circularly Polarized Attosecond Pulses Enabled by an Azimuthal Phase and Polarization Grating

High-harmonic generation (HHG) is an extreme nonlinear optical process that can map the properties of an infrared driving laser beam onto short wavelength attosecond pulse trains. However, current techniques for generating circularly polarized high harmonics for probing magnetic materials and chiral systems have limitations: two-color collinear counter-rotating driving lasers result in a low cutoff photon energy, while single-color non-collinear counter-rotating schemes suffer from low conversion efficiency. In this work, we generate circularly polarized attosecond pulse trains by using a structured laser driver which has a rotating polarization and phase grating along the azimuthal coordinate. Furthermore, our experimental and numerical results demonstrate the production of left and right circularly polarized harmonics, which naturally separate upon propagation. Our approach uses a single laser color in a collinear geometry, that can be scaled for high efficiency. Simulations show this scheme can extend into the soft x-ray region when driven by mid-infrared driving lasers, while preserving the same high phase-matching cutoff photon energy as for linearly-polarized high harmonics.

attosecond science↗

Acousto-optic modulators of high-power laser radiation on the basis of KGW and KYW crystals

Different modifications of acousto-optic modulators (AOMs) based on KG(WO{sub 4}){sub 2} (KGW) and KY(WO{sub 4}){sub 2} (KYW) crystals, designed for Q switching of high-power pulsed lasers, is developed and investigated. It is shown that AOMs based on these crystals are universal, can be combined with different lasers in the wavelength range of 1 – 3 μm, and have a high radiation resistance in the absence of antireflection coatings and light input at Brewster’s angle. The operation efficiency of KGW-based AOMs is experimentally demonstrated. Solid-state lasers based on Cr : Er : YSGG (λ = 2.78 μm), Cr : Yb : Ho : YSGG (λ = 2.87 μm), Cr : Tm : Ho : YSGG (λ = 2.09 μm), and Nd : YAG (λ = 1.064 μm) crystals with active acousto-optic Q switching, operating in the repetitively pulsed regime with a high beam quality and without surface destruction, are investigated. Lasing pulses (30 – 60)-ns long with energy up to 32 mJ at a repetition rate from 1 to 1000 Hz are obtained. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Influence of Annealing and Composition on the Crystal Structure of Mixed-Halide, Ruddlesden–Popper Perovskites

Mixed-halide two-dimensional (2D) hybrid organic–inorganic perovskites offer an important opportunity to control the band gap for applications in optoelectronic devices. In this study, we focus on phenethylammonium lead halide [(PEA) 2 Pb(I 1– x Br x ) 4 ] films, the pure iodide form of which is one of the most widely studied optically active 2D perovskite systems. Resonant infrared, matrix-assisted pulsed laser evaporation is used to grow films to explore the effects of post-growth annealing and mixed-halide composition. The composition, crystal structure, and optical properties are studied for as-grown and annealed films of (PEA) 2 Pb(I 1– x Br x ) 4 for x = 0, 0.25, 0.5, 0.75, and 1. First-principles calculations are used in conjunction with the experimental data to explain the mixed-halide behavior that does not trend monotonically with the bromide content. Important results of this work are as follows: (i) X-ray diffraction reveals evidence for halide phase separation around x = 0.25, consistent with first-principles calculations, whereas no phase separation is observed for x = 0.5 and above and (ii) a unique photoluminescence (PL) peak splitting is observed for x = 0.75, a composition for which no compositional phase separation is observed. The PL splitting is tentatively explained by the coexistence of two distinct types of halide short-range ordering at x = 0.75. Overall, this study demonstrates that mixed-halide n = 1 Ruddlesden–Popper perovskites are not simple random alloys but that instead, they display distinct sites and ordering preferences of the different halide anions. These preferences are critical to understand and rationally tune the properties of the materials.

36 MATERIALS SCIENCE↗

Identification of contamination in the pulse-compression chamber of the OMEGA EP Laser System originating from clean room garments

The contamination of optical components with microscopic particles strongly impacts their ability to handle high-power or high-intensity laser pulses via an array of mechanisms. This work explores the nature and origin of a subset of contamination particles found inside the pulse-compression chamber of the OMEGA EP Laser System. Using Raman microscopy accompanied by other analytical methods, it was shown that sodium nitrate constitutes a significant fraction of the particles that possess diameters on the order of a few micrometers. Further investigation aiming to reveal the origin of these particles suggests that these sodium nitrate particles are deposited via shedding from the reusable clean room garments worn in the Laser Bay and compression chamber. Raman microscopy also revealed various plastic particles such as polystyrene, polyethylene, and poly(diallyl isophthalate).

Raman spectroscopy↗

A cryogenic torsion balance using a liquid-cryogen free, ultra-low vibration cryostat

We describe a liquid-cryogen free cryostat with ultra-low vibration levels, which allows for continuous operation of a torsion balance at cryogenic temperatures. The apparatus uses a commercially available two-stage pulse-tube cooler and passive vibration isolation. Here, the torsion balance exhibits torque noise levels lower than room temperature thermal noise by a factor of about four in the frequency range of 3–10 mHz, limited by residual seismic motion and by radiative heating of the pendulum body. In addition to lowering thermal noise below room-temperature limits, the low-temperature environment enables novel torsion balance experiments. Currently, the maximum duration of a continuous measurement run is limited by accumulation of cryogenic surface contamination on the optical elements inside the cryostat.

47 OTHER INSTRUMENTATION↗

Technology of thin-rod Yb : YAG amplifiers with a high pulse energy and average power

Technology for producing thin-rod Yb : YAG laser amplifiers is improved, which is aimed at increasing the output pulse energy and includes the development of a new method for mounting active elements into a cooling system and employment of more persistent dielectric coatings of rod ends. An influence of a thermal lens on the beam size in an active element is theoretically studied and the parameters are found, which provide equal beam sizes at input and output rod ends. The output pulse energy of 4 mJ is obtained without optical breakdown of the output end, which substantially exceeds the previously obtained results. The amplifier demonstrates an average power of 60 W and maintains a high beam quality. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗