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At least 901 records · Page 50
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Dynamic wavelength control of laser pulse profiles at picosecond to nanosecond timescales

We report on a novel combined laser pulse shaping and dynamic wavelength encoding capability based on a simple architecture implementing direct space to time mapping. There are several potential applications that can be enabled by the ability to control the instantaneous intensity or wavelength of an optical waveform on a picosecond-to-nanosecond timescale. To our knowledge, no known methods can access this temporal regime with a practical architecture. Here, we demonstrate an extension of the Space–Time Induced Linearly Encoded Transcription for Temporal Optimization (STILETTO) technique that can generate optical waveforms with a programmable instantaneous wavelength vs. time. We experimentally demonstrate the technique by generating self-gated spectrograms and show that it can encode dynamic wavelength vs time profiles at timescales not achievable by any other known method.

47 OTHER INSTRUMENTATION↗
DOE OSTI2019

Optimization of switch diagnostics on the MAIZE linear transformer driver

The MAIZE Linear Transformer Driver is made of 40 capacitor-switch-capacitor `bricks' connected in parallel. When these 40 bricks are charged to 100-kV and then discharged synchronously, the MAIZE facility generates a 1-MA current pulse with a 100-ns rise time into a matched load impedance. Discharging each of the capacitors in a brick is carried out by the breakdown of a spark-gap switch, a process which results in the emission of light. Monitoring this output light with a fiber optic coupled to a photomultiplier tube (PMT) and an oscilloscope channel provides information on switch performance and timing jitter– whether a switch red early, late, or in phase with the other switches. However, monitoring each switch with a dedicated detector- oscilloscope channel can be problematic for facilities where the number of switches to be monitored (e.g., 40 on MAIZE) greatly exceeds the number of detector-oscilloscope channels available. The technique of using fibers to monitor light emission from switches can be optimized by treating a PMT as a binary digit or bit and using a combinatorial encoding scheme, where each switch is monitored by a unique combination of fiber- PMT-oscilloscope channels simultaneously. By observing the unique combination of ber-PMT-oscilloscope channels that are turned on, the pre-firing or late-firing of a single switch on MAIZE can be identified by as few as six PMT-oscilloscope channels. The number of PMT-oscilloscope channels, N , required to monitor X switches can be calculated by 2 N = X + 1, where the number '2' is selected because the PMT-oscilloscope acts as a bit. Here, we demonstrate the use of this diagnostic technique on MAIZE. In conclusion, we also present an analysis of how this technique could be scaled to monitor the tens of thousands of switches proposed for various next generation pulsed power facilities.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

A prototype scintillator real‐time beam monitor for ultra‐high dose rate radiotherapy

Background: FLASH Radiotherapy (RT) is an emergent cancer RT modality where an entire therapeutic dose is delivered at more than 1000 times higher dose rate than conventional RT. For clinical trials to be conducted safely, a precise and fast beam monitor that can generate out-of-tolerance beam interrupts is required. This paper describes the overall concept and provides results from a prototype ultra-fast, scintillator-based beam monitor for both proton and electron beam FLASH applications. Purpose: A FLASH Beam Scintillator Monitor (FBSM) is being developed that employs a novel proprietary scintillator material. The FBSM has capabilities that conventional RT detector technologies are unable to simultaneously provide: (1) large area coverage; (2) a low mass profile; (3) a linear response over a broad dynamic range; (4) radiation hardness; (5) real-time analysis to provide an IEC-compliant fast beam-interrupt signal based on true two-dimensional beam imaging, radiation dosimetry and excellent spatial resolution. Methods: The FBSM uses a proprietary low mass, less than 0.5 mm water equivalent, non-hygroscopic, radiation tolerant scintillator material (designated HM: hybrid material) that is viewed by high frame rate CMOS cameras. Folded optics using mirrors enable a thin monitor profile of ∼10 cm. A field programmable gate array (FPGA) data acquisition system generates real-time analysis on a time scale appropriate to the FLASH RT beam modality: 100–1000 Hz for pulsed electrons and 10–20 kHz for quasi-continuous scanning proton pencil beams. An ion beam monitor served as the initial development platform for this work and was tested in low energy heavy-ion beams ( 86 Kr +26 and protons). A prototype FBSM was fabricated and then tested in various radiation beams that included FLASH level dose per pulse electron beams, and a hospital RT clinic with electron beams. Results: Results presented in this report include image quality, response linearity, radiation hardness, spatial resolution, and real-time data processing. Furthermore, the HM scintillator was found to be highly radiation damage resistant. It exhibited a small 0.025%/kGy signal decrease from a 216 kGy cumulative dose resulting from continuous exposure for 15 min at a FLASH compatible dose rate of 237 Gy/s. Measurements of the signal amplitude versus beam fluence demonstrate linear response of the FBSM at FLASH compatible dose rates of >40 Gy/s. Comparison with commercial Gafchromic film indicates that the FBSM produces a high resolution 2D beam image and can reproduce a nearly identical beam profile, including primary beam tails. The spatial resolution was measured at 35–40 µm. Tests of the firmware beta version show successful operation at 20 000 Hz frame rate or 50 µs/frame, where the real-time analysis of the beam parameters is achieved in less than 1 µs. Conclusions: The FBSM is designed to provide real-time beam profile monitoring over a large active area without significantly degrading the beam quality. A prototype device has been staged in particle beams at currents of single particles up to FLASH level dose rates, using both continuous ion beams and pulsed electron beams. Using a novel scintillator, beam profiling has been demonstrated for currents extending from single particles to 10 nA currents. Radiation damage is minimal and even under FLASH conditions would require ≥50 kGy of accumulated exposure in a single spot to result in a 1% decrease in signal output. Beam imaging is comparable to radiochromic films, and provides immediate images without hours of processing. Real-time data processing, taking less than 50 µs (combined data transfer and analysis times), has been implemented in firmware for 20 kHz frame rates for continuous proton beams.

2D beam imaging↗
DOE OSTI2023

Tailoring light-induced charge transfer and intersystem crossing in FeCO using time-dependent spin–orbit configuration interaction

Real-time (RT) electronic structure methods provide a natural framework for describing light–matter interactions in arbitrary time-dependent electromagnetic fields (EMF). Optically induced excited state transitions are of particular interest, which require tuned EMF to drive population transfer to and from the specific state(s) of interest. Intersystem crossing, or spin-flip, may be driven through shaped EMF or laser pulses. These transitions can result in long-lived “spin-trapped” excited states, which are especially useful for materials requiring charge separation or protracted excited state lifetimes. Time-dependent configuration interaction (TDCI) is unique among RT methods in that it may be implemented in a basis of eigenstates, allowing for rapid propagation of the time-dependent Schrödinger equation. The recent spin–orbit TDCI (TD-SOCI) enables a real-time description of spin-flip dynamics in an arbitrary EMF and, therefore, provides an ideal framework for rational pulse design. The present study explores the mechanism of multiple spin-flip pathways for a model transition metal complex, FeCO, using shaped pulses designed to drive controlled intersystem crossing and charge transfer. These results show that extremely tunable excited state dynamics can be achieved by considering the dipole transition matrix elements between the states of interest.

Chemistry↗
DOE OSTI2020

Total internal reflection enabled wide-field coherent anti-Stokes Raman scattering microscopy

Wide-field coherent anti-Stokes Raman scattering (CARS) microscopy offers an attractive means for the rapid and simultaneous acquisition of vibrationally resolved images across a large field of view. A major challenge in the implementation lies in how to achieve sufficiently strong excitation fields necessary to drive the third-order optical responses over the large focal region. Here, we report a new wide-field CARS microscope enabled by a total internal reflection excitation scheme using a femtosecond Ti:Sapphire oscillator to generate pump and broadband near-infrared Stokes pulses. The spectrally broad Stokes pulse, in combination with its inherent chirp, offers not only access to a wide range of Raman modes spanning ∼ <#comment/> 1000 to ∼ <#comment/> 3500 c m − <#comment/> 1 but also a straightforward means to select vibrational transitions within this range by simply varying the time delay between the pulses. The unique capabilities of this wide-field CARS microscope were validated by acquiring high-quality CARS images from the model and complex biological samples on conventional microscope coverslips.

Doughty, Benjamin (ORCID:0000000164299329)↗
DOE OSTI2020

Total internal reflection enabled wide-field coherent anti-Stokes Raman scattering microscopy

Wide-field coherent anti-Stokes Raman scattering (CARS) microscopy offers an attractive means for the rapid and simultaneous acquisition of vibrationally resolved images across a large field of view. A major challenge in the implementation lies in how to achieve sufficiently strong excitation fields necessary to drive the third-order optical responses over the large focal region. Here, we report a new wide-field CARS microscope enabled by a total internal reflection excitation scheme using a femtosecond Ti:Sapphire oscillator to generate pump and broadband near-infrared Stokes pulses. The spectrally broad Stokes pulse, in combination with its inherent chirp, offers not only access to a wide range of Raman modes spanning ${\sim}{1000}$ to ${\sim}{3500}\;{{\rm cm}^{- 1}}$ but also a straightforward means to select vibrational transitions within this range by simply varying the time delay between the pulses. The unique capabilities of this wide-field CARS microscope were validated by acquiring high-quality CARS images from the model and complex biological samples on conventional microscope coverslips.

36 MATERIALS SCIENCE↗
DOE OSTI2022

A compact cold-atom interferometer with a high data-rate grating magneto-optical trap and a photonic-integrated-circuit-compatible laser system

Abstract The extreme miniaturization of a cold-atom interferometer accelerometer requires the development of novel technologies and architectures for the interferometer subsystems. Here, we describe several component technologies and a laser system architecture to enable a path to such miniaturization. We developed a custom, compact titanium vacuum package containing a microfabricated grating chip for a tetrahedral grating magneto-optical trap (GMOT) using a single cooling beam. In addition, we designed a multi-channel photonic-integrated-circuit-compatible laser system implemented with a single seed laser and single sideband modulators in a time-multiplexed manner, reducing the number of optical channels connected to the sensor head. In a compact sensor head containing the vacuum package, sub-Doppler cooling in the GMOT produces 15 μK temperatures, and the GMOT can operate at a 20 Hz data rate. We validated the atomic coherence with Ramsey interferometry using microwave spectroscopy, then demonstrated a light-pulse atom interferometer in a gravimeter configuration for a 10 Hz measurement data rate and T = 0–4.5 ms interrogation time, resulting in Δ g / g = 2.0 × 10 −6 . This work represents a significant step towards deployable cold-atom inertial sensors under large amplitude motional dynamics.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

The role of ambient gas confinement, plasma chemistry, and focusing conditions on emission features of femtosecond laser-produced plasmas

Ultrafast laser ablation coupled with optical emission spectroscopy is currently under development for standoff detection of elements and their isotopes for a wide range of application areas. In this work, we explore the role of ambient air pressure during the interaction of an ultrafast laser beam with two metallic targets (brass and uranium) with significantly different oxygen gas-phase reactivity. Plasma plumes were generated by focusing ~800 nm, ~35 fs pulses from an ultrafast laser system using a long focal length lens with f = 1 m. Two-dimensional spectral imaging was performed over the pressure range of 30 mTorr-700 Torr air to evaluate emission dynamics, plasma chemistry, signal-to-background ratio, and characteristic parameters (i.e. excitation temperature, electron density). An increase in ambient air pressure during ultrafast laser ablation leads to plume confinement and subsequent changes in the emission dynamics due to plasma chemistry as well as changes in plasma generation conditions (i.e. focused fs laser ablation versus filament ablation). Ablation crater morphologies were also investigated via scanning electron microscopy. Results indicate atomic emission intensity and signal-to-background ratios peak at moderate pressure levels (~50-100 Torr air) for both targets studied, although plasma chemistry influences uranium emission signatures. The emission features of the uranium plasma at pressures = 10 Torr showed the presence of atoms and oxide molecules which are co-located within the plume. We also find filament ablation leads to wider, more shallow craters compared to focused laser ablation. Our study provides unique insight into the interplay between plume dynamics, confinement, and oxygen chemistry of fs laser-produced plasmas and how these phenomena evolve with changing ambient air pressure.

Laser-produced plasma↗
DOE OSTI2023

Measurement of 2D density profiles using a second-harmonic, dispersion interferometer

A second-harmonic, dispersion interferometer is used to image large-area (≃5 cm 2 ) plasma-jet and gas-jet density profiles. Achromatic telescopes magnify the diameters of the primary-laser beam (1064 nm) and its second-harmonic (532 nm) before probing the sample and de-magnify the beam diameters after the sample, where the primary beam transfers its phase change to a second, second-harmonic beam, allowing the sample’s dispersive-phase change to be measured between two, orthogonally polarized second harmonic beams. The telescopes produce an azimuthally symmetric, dispersive-phase shift in the sample + background phase-change image and in the background phase-change image, which is removed by digital subtraction. The interferometer’s performance was verified using standard-optical components as dispersive elements (BK7 lenses and wedge plates), resolving a minimum, phase-change sensitivity of ΔΦ min ≳ 15 mrad and spatial resolution of Δx res ≃ 100 μm. The phase change produced by unknown-density objects (a pulsed-plasma-jet and a pulsed-gas-jet) was measured, and their data were used to recover the original, 2D density profiles using an inverse Abel transform: peak-number density, N gas ≃ 6 × 10 20 cm –3 and N e ≃ 5 × 10 16 cm –3 ; line-integrated density, ∫N gas dl ~ 2 × 10 19 cm –2 and ∫N e dl ~ 1 × 10 16 cm –2 . The techniques and methods developed here are scalable to even larger probe-beam diameters and frame-capture rates, leading to a diagnostic capability that is well-suited for applications involving the real-time measurement of density.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Atmospheric clearing of solid-particle debris using femtosecond filaments

Through nonlinear self-focusing, femtosecond pulses can propagate several kilometers beyond diffraction limits, forming an ionization channel in air known as a laser filaments. It has been demonstrated that in the wake of the filament, aerosols can be effectively cleared to improve the transmission of subsequent laser pulses or secondary light sources, pertinent to applications in atmospheric sensing. However, the current understanding of aerosol clearing is founded on interactions with droplets to simulate fogs and clouds and thus does not extend to solid particles or atmospheric debris. Using optical trapping, we isolate both graphite and silica microparticles and directly measure the subsequent displacement caused by the filament using time-resolved shadowgraphy. The shock wave from the filament is demonstrated to propel particles away from the filament, directly contributing to atmospheric debris clearing. Particles exposed to the laser light in either the intense filament core or the surrounding energy reservoir are axially displaced along the beam path. Furthermore, it is found that the optomechanical properties of the particle largely influence the axial displacement induced by laser exposure through mechanisms such as radiation pressure, mass ejection from ablation or optical damage, and particle deagglomeration.

42 ENGINEERING↗
DOE OSTI2024

Excitation-dependent features and artifacts in 2-D terahertz spectroscopy

Recently, two-dimensional terahertz spectroscopy (2DTS) has attracted increasing attention for studying complex solids. A number of recent studies have applied 2DTS either with long pulses or away from any material resonances, situations that yield unconventional 2DTS spectra that are often difficult to interpret. Here, we clarify the generic origins of observed spectral features by examining 2DTS spectra of ZnTe, a model system with a featureless optical susceptibility at low terahertz frequencies. These results also reveal possible artifacts that may arise from electro-optic sampling in collinear 2DTS experiments, including the observation of spurious rectified or second harmonic signals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Impact of Oxygen Non-Stoichiometry on Near-Ambient Temperature Ionic Mobility in Polaronic Mixed-Ionic-Electronic Conducting Thin Films

Enhanced ionic mobility in mixed ionic and electronic conducting solids contributes to improved performance of memristive memory, energy storage and conversion, and catalytic devices. Ionic mobility can be significantly depressed at reduced temperatures, for example, due to defect association and therefore needs to be monitored. Measurements of ionic transport in mixed conductors, however, proves to be difficult due to dominant electronic conductivity. This study examines the impact of different levels of quenched-in oxygen deficiency on the oxygen vacancy mobility near room temperature as measured by a novel dynamic current-voltage analysis. A Pr 0.1 Ce 0.9 O 2-δ film was grown by pulsed laser deposition and subsequently annealed, from 400-600° C, in various oxygen partial pressures to modify its oxygen vacancy concentration while minimizing microstructural growth and cation segregation. To monitor changes in film non-stoichiometry, we leverage the existence of an optical absorption center, related to the oxidation state of Pr ions in Pr0.1Ce0.9O2-δ. The oxygen vacancy migration enthalpy was found to exhibit a small increase from 0.73± 0.04 to 0.79 ± 0.02 eV with increasing oxygen deficiency, while the pre-factor was found to increase by a factor of 135. Here, a nearly 13-fold increase in ionic mobility at 60 °C for increases in oxygen non-stoichiometry from 0.032 ± 0.001 to 0.042± 0.001 was thereby detected. Raman spectroscopy was employed to rule out changes in strain as the primary cause for the significant change in mobility. Several factors potentially contributing to the large pre-factor changes are examined and discussed. Insights into how ionic defect concentration can markedly impact ionic mobility should help in elucidating the origins of variations seen in nanoionic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Optical Spin Polarization of a Narrow-Linewidth Electron-Spin Qubit in a Chromophore/Stable-Radical System

Photoexcited organic chromophores appended to stable radicals can serve as qubit and/or qudit candidates for quantum information applications. 1,6,7,12-Tetra-(4-tert-butylphenoxy)-perylene-3,4 : 9,10-bis(dicarboximide) (tpPDI) linked to a partially deuterated α,γ-bisdiphenylene-β-phenylallyl radical (BDPA-d 16 ) was synthesized and characterized by time-resolved optical and electron paramagnetic resonance (EPR) spectroscopies. Photoexcitation of tpPDI-BDPA-d 16 results in ultrafast radical-enhanced intersystem crossing to produce a quartet state (Q) followed by formation of a spin-polarized doublet ground state (D 0 ). Pulse-EPR experiments confirmed the spin multiplicity of Q and yielded coherence times of T m =2.1±0.1 μs and 2.8±0.2 μs for Q and D 0 , respectively. BDPA-d 16 eliminates the dominant 1 H hyperfine couplings, resulting in a single narrow line for both the Q and D 0 states, which enhances the spectral resolution needed for good qubit addressability.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Shaping attosecond pulses by controlling the minima in high-order harmonic generation through alignment of CO 2 molecules

In this paper, we report a simple method for generating shaped attosecond pulses by using a CO 2 molecule. Unlike most other molecules, owing to its unique energy and angle dependence and the presence of deep minima in the photoionization transition dipole moment, the shape of harmonic spectra, especially the position and depth of minima, can be readily controlled by tuning the degree of alignment. The sensitive alignment dependence of the minima is due to the coherent interference of a laser-induced dipole from each molecule when CO 2 molecules are moderately aligned, but not when they are well aligned or when they are isotropically distributed. Such a sensitivity offers a simple way of controlling the spectral amplitude and phase of the generated harmonics and thus shaping the generated attosecond pulses, for example, producing structured attosecond pulses by splitting a single burst into two. We illustrate how such pulses are generated and how to characterize them. This method offers a simple way to shape attosecond pulses at the generation step. It can be easily implemented experimentally to generate attosecond pulses with strong phase variations for unique applications.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Optical and photophysical properties of platinum benzoporphyrins with C 2v and D 2h symmetry

Platinum(II) mono- and di-benzoporphyrins carrying either ester or imide peripheral groups have been successfully synthesized. These benzoporphyrins possessing C 2v and D 2h symmetry were investigated using a range of techniques including UV-Vis and phosphorescence spectroscopy, differential pulse voltammetry, and transient absorption spectroscopy covering wide spatial and temporal ranges. Up to three oxidation and three reductions within the accessible potential window of dichlorobenzene were observed. Facile reductions for both mono- and dibenzoporphyrin derivatives, more so with imide peripheral substituents were witnessed. Computational studies were supportive of push-pull type interactions within these molecular systems. Here, the formation of triplet excited states within 5 ps after laser excitation was confirmed by femtosecond transient absorption studies. Nanosecond transient absorption studies coupled with phosphorescence lifetime studies revealed relatively rapid relaxation of the triplet excited states as compared to a controlled platinum porphyrin suggesting push-pull type interactions on a slower time scale.

DFT calculations↗
DOE OSTI2024

Enhancement of terahertz fields in LiTaO 3 waveguides using a conical pulse front

The development of methods for the generation of strong ultrafast electromagnetic pulses in the terahertz (THz) spectral range has led to a surge of progress in nonlinear THz spectroscopy and THz control of molecular and collective responses. For spectroscopy in the 1-THz range, the submillimeter wavelengths and associated large spot sizes, large optical elements, and short distances between final focusing elements and samples can lead to cumbersome experimental setups that are incompatible with some sample environments. Here, we introduce a novel terahertz ring excitation (TREx) optical pumping geometry to generate superposing, focusing fields in planar THz waveguides made out of the electro-optic material lithium tantalate. High THz fields, >175 kV/cm, are generated and measured optically with no free-space THz propagation. The field level achieved by pumping with a sequence of concentric rings of excitation light exceeds by about 20× the result of a single cylindrically focused line of pump light that has been used routinely in previous work. The technique opens new prospects for compact waveguide-based linear and nonlinear THz spectroscopy and signal processing.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Time reflection of light from a quantum perspective and vacuum entanglement

If a boundary between two static media is moving with a constant superluminal velocity, or there is a sudden change of the refractive index with time, this yields generation of entangled pairs of photons out of vacuum propagating in the opposite directions. Here we show that during this process, entanglement of Minkowski vacuum is transferred to the entanglement of the generated photon pairs. If initially an electromagnetic pulse is present in the medium the photon generation is stimulated into the pulse mode, and since photons are created as entangled pairs the counter-propagating photon partners produce a pulse moving in the opposite direction, which is known as time reflection. Thus, time reflection occurs due to stimulated generation of the entangled photon pairs out of entangled vacuum and no photons in the original pulse are in fact being reflected. This is different from the mechanism of light reflection from spatial inhomogeneities for which no photons are generated.

Optics↗