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DOE OSTI2022

Ionization-Based Optical Structures for the Control of Short-Pulse Lasers (Full LDRD Report)

High-power lasers require enormous beam sizes to avoid optics damage; without plasma control of light, future higher-power systems will have prohibitive costs. The laser-induced formation of ionization patterns in gases provides an opportunity to manipulate the spatial and temporal properties of femtosecond to picosecond beams with precise control at high intensity, providing a path towards compact multi-petawatt lasers. In this project, we proposed new concepts of diffractive optics elements relying on ionization-based structures, including a holographic lens and a compression grating. The theoretical characterization of these optical elements was supported by particle-in-cell simulations. Experiments have been carried out to achieve reflective elements (i.e., plasma-based gratings) that demonstrated high robustness and efficiencies on the order of 50%, which validates the feasibility of our new concepts and paves the way for future plasma-based high-power laser systems.

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

Vector measurements using a pulsed, optically pumped atomic magnetometer

An atomic magnetometer, and a method for using same is disclosed. The method for measuring an ambient magnetic field uses an atomic magnetometer that has a probe light beam with a probe axis that probes a polarization vector of an atomic population confined within a vapor cell. The method employs one or more measurement cycles. In each measurement cycle, the polarization vector is prepared in an initial state via an optical pumping pulse. The vapor cell is then subjected to the ambient magnetic field, which results in rotation of the polarization vector by Larmor precession. Within the measurement cycle, at a point in time after the polarization vector has been prepared in the initial state, the ambient magnetic field rotates the direction of the polarization vector, and at least one measurement is made of a projection of the Larmor-rotated polarization vector onto the probe axis during or after application of a magnetic waveform.

Schwindt, Peter↗

DOE OSTI2025

Metastable‐State Photoacids with Fast Reverse Reactions

Metastable-state photoacid (mPAH) has become a common tool for controlling and driving chemical processes with light. mPAHs with fast reverse reactions are desirable for precise temporal control or generating quick pulses of proton concentration. Here, in this work, different approaches towards fast reversing mPAHs are studied. Experimental and computational results showed that stabilizing the charge–transfer intermediate is an effective way to increase the rate. A novel mPAH with a reverse reaction ≈500 times faster than the most used mPAH in methanol is developed. Another water-soluble mPAH showed a reverse reaction with a rate constant of 7.8 s −1 , which is the fastest ever reported. The half-life of the acidic state is calculated to be 89 ms, which allowed to demonstrate sub-second switching using this mPAH.

Abbood, Rana [Florida Institute of Technology, Mel↗

DOE OSTI2025

Coherent Control over Nuclear Hyperpolarization Using an Optically Initializable Chromophore-Radical System

Chromophore radicals (CR) are emerging as important components for molecular quantum information science (QIS), especially in the context of quantum sensing. Here, we demonstrate that the optically hyperpolarized electrons in a 1,6,7,12-tetrakis(4-tert-butylphenoxy)-perylene-3,4,9,10-bis(dicarboximide) (tpPDI) covalently linked to a partially deuterated 1,3-bis(diphenylene)-d 16 -2-phenylallyl radical (BDPA-d 16 ) can be coherently manipulated via pulsed dynamic nuclear polarization (DNP) methods to transfer polarization to nuclear spins and back. Under light illumination at 85 K, electron hyperpolarization in BDPA is enhanced 2.1- to 2.4-fold over thermal polarization and lasts for more than 100 ms. By applying nuclear orientation via electron spin-locking (NOVEL) DNP, this optically amplified electron hyperpolarization was successfully transferred to a 1 H nuclear spin within the CR system and efficiently returned to the electron spin for readout via reverse-NOVEL. The NOVEL transfer efficiency of 65% amounts to a 688-fold nuclear spin hyperpolarization of the target nuclear spin, considering the 2.1-fold electron spin hyperpolarization. This reversible coherent manipulation of hyperpolarization transfer highlights the utility of CR systems to initialize and read out nuclear spin states in a disordered matrix at moderate cryogenic temperatures. Coupled with CRs’ environmental compatibility, tunability, and precise state initialization, these results highlight the promising role of nuclear spins in CRs for QIS applications, including quantum sensing and memory.

charge transfer↗

DOE OSTI2025

A profile monitor for proton radiography experiments at the Los Alamos Neutron Science Center

The Proton Radiography (pRad) facility at the Los Alamos Neutron Science Center utilizes pulses of protons delivered by the 800 MeV linear accelerator to produce a series of radiographic images to study the dynamic behavior of materials under extreme conditions. Radiographs taken with an empty field of view, or beam pictures, are used to normalize transmission. However, because the center of the proton beam shifts between pulses, an in situ method for measuring beam position is required to normalize images for beam movement to perform absolute radiography. The beam profile monitor described here uses an array of scintillating fibers positioned in the beam path to produce light proportional to beam intensity across the beam cross section. This light is detected using fast photodiodes and a digital oscilloscope, providing a response time of several nanoseconds—suitable for measuring the 50-ns proton pulses used in pRad. The profile monitor achieves a measured position precision of 40 μm and an intensity precision of 0.7%, allowing for beam movement corrections to be applied to images, thereby improving data accuracy and image quality.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

Ionizing photon interactions modulate the optical properties of crystals with femtosecond scale temporal resolution

In this work, we continue our study of a new method for the detection of ionizing radiation with the potential for a dramatic improvement in coincidence time resolution (CTR) for time-of-flight positron emission tomography (ToF-PET) using the modulation of a material's optical properties instead of the scintillation mechanism. Our previous work has shown that for non-scintillation materials such as bismuth silicon oxide (BSO) and cadmium telluride (CdTe), their refractive index can be modulated by annihilation photon interactions. Additionally, the ultrafast nature of this process however remains unexplored. The ionizing radiation-induced charge carriers alter the local band structure in these materials, thus changing the complex refractive index. This mechanism is routinely used at the linac coherent light source (LCLS) facility of the SLAC National Accelerator Laboratory to measure x-ray pulse arrival times with femtosecond scale resolution for photon energies between 0.5 and 10 keV. The method described here follows that example by using a frequency chirped visible continuum pulse to provide a monotonic wavelength-to-time mapping by which one can measure the time-dependent refractive index modulation. In addition, we describe an interference-based measurement setup that allows for significantly improved sensitivity while preserving a timing precision of approximately 10 fs (σ) when measuring the arrival time of below 10 keV x-ray pulses with yttrium aluminum garnet (YAG) crystal. The method is presented in the context of ToF-PET application with further discussions on the potential CTR achievable if a similar detection concept is adopted for detecting 511 keV photons. Semi-empirical analysis indicates that the predicted CTR achievable is on the order of 1 ps (FWHM).

59 BASIC BIOLOGICAL SCIENCES↗

NASA NTRS1972

Pulse excitation of bolometer bridges

Driving bolometer bridge by appropriately phased excitation pulses increases signal-to-noise ratio of bolometer sensor which operates on a chopped light beam. Method allows higher applied voltage than is possible by conventional ac or dc excitation.

Rusk, S. J.↗

NASA NTRS1972

Development of a radioisotope-fueled thruster for satellite propulsion.

Description of the design and testing of two distinct thrustor concepts which use ammonia propellant and have a specific impulse as high as 310 sec during pulsed operation. Considerations of thrustor design, material selection, and system testing are discussed in the light of performance, lifetime, and nuclear safety requirements. Results of a detailed study of the advantages and disadvantages of the use of such a thrustor are presented.

Rosen, S. G.↗

NASA NTRS1973

Photographic laboratory studies of explosions.

Description of a series of cinematographic studies of explosions made with a high-speed rotating-mirror streak camera which uses a high-frequency stroboscopic ruby laser as the light source. The results obtained mainly concern explosions initiated by focused laser irradiation from a pulsed neodymium laser in a detonating gas consisting essentially of an equimolar mixture of acetylene and oxygen at an initial pressure of 100 torr at room temperature. Among the most significant observations were observations of a spherical blast wave preceded by a Chapman-Jouguet detonation which is stabilized immediately after initiation, the merging of a spherical flame with a shock front of the blast wave in which the flame is propagating, the division of a spherical detonation front into a shock wave and flame, and the generation of shock waves by a network of spherical flames.

Kamel, M. M.↗

NASA NTRS1986

An elliptical binary orbit model of GX 1 + 4

The X-ray source GX 1 + 4 (4U 1728-24) was observed by the high-energy X-ray spectrometer on OSO 8 for five days from September 20-24, 1978, and X-rays in the energy range 16-72 keV were analyzed. Measurements of the pulse period, pulsar angular acceleration, and luminosity of GX 1 + 4 are reported. The pulsar light curves obtained in different energy ranges are presented, and it is concluded that the period is about 220 s rather than about 110 s. The observations are combined with those reported by others, and a history of GX 1 + 4 as observed in hard X-rays is presentd. A continuous function for the change in period is inferred that suggests a 304-day periodicity. It is proposed that such a period in the spin-up could be caused by an elliptical orbit of GX 1 + 4 abouts its red giant companion.

Cutler, E. P.↗

DOE OSTI2023

Exploration of Optimizing FPGA-based Qubit Controller for Experiments on Superconducting Quantum Computing Hardware

This work explores avenues and target areas for optimizing FPGA-based control hardware for experiments conducted on superconducting quantum computing systems and serves as an introduction to some of the current research at the intersection of classical and quantum computing hardware. With the promise of building larger-scale error-corrected quantum computers based on superconducting qubit architecture, innovations to room-temperature control electronics are needed to bring these quantum realizations to fruition. The QICK (Quantum Instrumentation Control Kit) is one leading experimental FPGA-based implementations. However, its integration into other experimental quantum computing architectures, especially those using superconducting radiofrequency (SRF) cavities, is largely unexplored. We identify some key target areas for optimizing control electronics for superconducting qubit architectures and provide some preliminary results to the resolution of a control pulse waveform. With optimizations targeted at 3D superconducting qubit setups, we hope to bring to light some of the requirements in classical computational methodologies to bring out the full potential of this quantum computing architecture, and to convey the excitement of progress in this research.

43 PARTICLE ACCELERATORS↗

NASA NTRS1975

Investigation of laser dynamics, modulation and control by means of intra-cavity time varying perturbation

The generation of tunable visible, infrared, and ultraviolet light is examined, along with the control of this light by means of novel mode-locking and modulation techniques. Transient mode-locking of the Nd:YAG laser and generation of short tunable pulses in the visible and the alkali metal inert gas excimer laser systems were investigated. Techniques for frequency conversion of high power and high energy laser radiation are discussed, along with high average power blue and UV laser light sources.

Harris, S. E.↗

NASA NTRS1982

Photoelectric detection system

A photoelectric beam system for the detection of the arrival of an object at a discrete station wherein artificial light, natural light, or no light may be present is described. A signal generator turns on and off a signal light at a selected frequency. When the object in question arrives on station, ambient light is blocked by the object, and the light from the signal light is reflected onto a photoelectric sensor which has a delayed electrical output but is of the frequency of the signal light. Outputs from both the signal source and the photoelectric sensor are fed to inputs of an exclusively OR detector which provides as an output the difference between them. The difference signal is a small width pulse occurring at the frequency of the signal source. By filter means, this signal is distinguished from those responsive to sunlight, darkness, or 120 Hz artificial light. In this fashion, the presence of an object is positively established.

Currie, J. R.↗

DOE OSTI2025

Time-resolved momentum imaging of UV photodynamics in structural isomers of iodopropane probed by site-selective XUV ionization

The photodynamics of 1- and 2-iodopropane (1 and 2-IP) were studied in a time-resolved scheme incorporating ultraviolet (UV) excitation and extreme ultraviolet (XUV) probing, which initiates photoionization selectively from the I 4d core orbital. UV absorption in the A-band of both isomers leads to prompt C–I bond fission, with significant disposal of internal energy into the propyl radical product. Site-selective ionization enables a range of charge transfer (CT) processes between the nascent highly charged iodine ions and neutral propyl radicals, dependent on the interfragment distance at the instant of ionization. Subtle differences in the dynamics of these CT processes between the two isomers are observed. In 1-IP, the kinetic energies of iodine ions produced by UV photodissociation and subsequent XUV multiple ionization increased notably over the first few hundred femtoseconds, which could be understood in terms of differing gradients along the photodissociation coordinates of the neutral and polycationic states involved in the pump and probe steps, respectively. Led by a recent report of HI elimination in UV photoexcited 2-IP [Todt et al., Phys. Chem. Chem. Phys., 22(46), 27338 (2020)], we also model the most likely signatures of this process in the present experiment, and can identify signal in the 2-IP data (that is absent or significantly weaker in the data from the unbranched 1-IP isomer) that is consistent with such a process occurring on ultrafast timescales.

Allum, Felix [Deutsches Elektronen-Synchrotron (DE↗

NASA NTRS1974

Application of holography to flow visualization within rotating compressor blade row

Two holographic interblade row flow visualization systems were designed to determine the three-dimensional shock patterns and velocity distributions within the rotating blade row of a transonic fan rotor, utilizing the techniques of pulsed laser transmission holography. Both single- and double-exposure bright field holograms and dark field scattered-light holograms were successfully recorded. Two plastic windows were installed in the rotor tip casing and outer casing forward of the rotor to view the rotor blade passage. The viewing angle allowed detailed investigation of the leading edge shocks and shocks in the midspan damper area; limited details of the trailing edge shocks also were visible. A technique was devised for interpreting the reconstructed holograms by constructing three dimensional models that allowed identification of the major shock systems. The models compared favorably with theoretical predictions and results of the overall and blade element data. Most of the holograms were made using the rapid double-pulse technique.

Wuerker, R. F.↗

NASA NTRS1983

Apparatus for processing electromagnetic radiation and method

Measuring apparatus including a ruled member having alternate transparent and opaque zones. An optical coupler connecting the ruled member with electromagnetic radiation-conversion apparatus. The conversion apparatus may include a photomultiplier and a discriminator. Radiation impinging on the ruled member will, in part, be converted to electrical pulses which correspond to the intensity of the radiation. A method of processing electromagnetic radiation includes providing a member having alternating dark and light zones, establishing movement of the member through the beam of electromagnetic radiation with the dark zones interrupting passage of radiation through the rule, providing an optical coupler to connect a portion of the radiation with a conversion station where the radiation portion is converted into an electrical pulse which is related to the intensity of the radiation received at the conversion station. The electrical pulses may be counted and the digitized signals stored or permanently recorded to produce positional information.

Gatewood, George D.↗

DOE OSTI2024

Photoinduced Magnetic Exchange-Jump Promotes Ground State Biradical Electron Spin Polarization

Photoinduced electron spin polarization (ESP) is reported in the electronic ground states of three Pt(II) complexes that are comprised of two S = ½ nitronyl nitroxide (NN) radicals attached through different length para-phenylethynyl bridges to the 3,6 positions of a catecholate (CAT, donor) and 4,4’-di-tert-butyl-2,2’-bipyridine (bpy, acceptor). Complexes 1-3 have from 17 to 41 bonds separating NN radicals, and display cw-EPR spectra consistent with |J NN-NN | >> |a N |, |J NN-NN | ≥ |a N |, and |J NN-NN | < |a N |, respectively, where J NN-NN is the magnetic exchange coupling between NN radicals in the electronic ground state, and a N is the isotropic 14 N hyperfine coupling constant. Light-induced transient EPR spectra characterized as enhanced ground-state absorption were observed for all three complexes using 532 nm pulsed laser excitation into the ligand-to-ligand charge transfer (LL’CT) band of the (CAT)Pt(bpy) chromophore. The magnitude of the observed ESP increases in the order 1 < 2 < 3 and is inversely correlated with the magnitude of ground-state J NN-NN . In addition to the experimental observation net absorptive polarization in 1-3, light excitation also produces multiplet polarization in 2. Since the weak dipolar coupling leads to strong spectral overlap of the absorptive and emissive components, the multiplet polarization is not observed in 1 and 3 and is very weak in 2. Here, the ability to spin polarize multiple radical spins with a single photon is anticipated to advance new photoinduced multi qubit/qudit ESP protocols for quantum information science applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Molecular bond stabilization in the strong-field dissociation of O 2 +

We theoretically examine the rotational and vibrational dynamics of O 2 + molecular ions exposed to intense, short laser pulses for conditions realized in contemporary pump-probe experiments. We solve the time-dependent Schrödinger equation within the Born-Oppenheimer approximation for an initial distribution of randomly aligned molecular ions. For fixed peak intensities, our numerical results show that total, angle-integrated O 2 + → O( 3 P) + O + ( 4 S 0 ) dissociation yields do not monotonically increase with increasing infrared-probe pulse duration. We find this pulse-duration-dependent stabilization to be consistent with the transient trapping of nuclear probability density in a light-induced (bond-hardening) potential-energy surface and robust against rotational excitation. We analyze this stabilization effect and its underlying bond-hardening mechanism (i) in the time domain, by following the evolution of partial nuclear probability densities associated with the dipole-coupled O 2 + (a 4 Π u ) and O 2 + (f 4 Π g ) cationic states, and (ii) in the frequency domain, by examining rovibrational quantum-beat spectra for the evolution of the partial nuclear probability densities associated with these states. In this work, our analysis reveals the characteristic timescale for the bond-hardening mechanism in O 2 + and explains the onset of bond stabilization for sufficiently long pulse durations.

74 ATOMIC AND MOLECULAR PHYSICS↗