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NASA NTRS1978

Investigation of laser induced parametric interactions in optical waveguides and fibers

Experimental and theoretical aspects of the laser pump depletion characteristics in an optical fiber due to stimulated Raman scattering, and stimulated Brillouin scattering were studied. A review is presented of research in fiber transmission accompanied by stimulated scattering. Results of experimental work with tunable dye lasers and argon lasers are presented. The spectral profiles of the laser pump and its transmitted light through the fiber are given.

Yu, C.↗

DOE OSTI2020

Resonant propagation of x rays from the linear to the nonlinear regime

We present a theoretical study of temporal, spectral, and spatial reshaping of intense, ultrafast x-ray pulses propagating through a resonant medium. Our calculations are based on the solution of a three-dimensional time-dependent Schrodinger-Maxwell equation, with the incident x-ray photon energy on resonance with the core-level is-3p transition in neon. We study the evolution of the combined incident and medium-generated field, including the effects of stimulated emission, absorption, ionization, and Auger decay, as a function of the input pulse energy and duration. We find that stimulated Raman scattering between core-excited states 1s -1 3p and 2p -1 3p occurs at high x-ray intensity, and that the emission around this frequency is strongly enhanced when also including the similar 1s -1 -2p -1 response of the ion. We also explore the dependence of x-ray self-induced transparency (SIT) and self-focusing on the pulse intensity and duration, and we find that the stimulated Raman scattering plays an important role in both effects. Finally, we discuss how these nonlinear effects may potentially be exploited as control parameters for pulse properties of x-ray free-electron laser sources.

74 ATOMIC AND MOLECULAR PHYSICS↗

NASA NTRS1994

Physical processes in eclipsing pulsars: Eclipse mechanisms and diagnostics

We investigate how the radio emission of a pulsar interacts with plasma derived from a stellar companion. Various physical mechanisms that can cause radio pulse eclipse are discussed, and predictions are made for the polarization properties of the emergent radio wave. We consider eclipses by a wind from the stellar companion, by a stellar magnetosphere, or by material entrained in the pulsar wind. Eclipses due to refraction require either a relatively high plasma density or a sharp edge to the plasma distribution. The conditions that must prevail for free-free absorption to be effective in eclipsing a radio beam are also outlined. Pulse smearing may be important at higher frequencies; related eclipse mechanisms include pulse spreading due to a rapidly changing electron column, and scattering by Langmuir turbulence. The high brightness temperature radio beam can generate its own plasma turbulence via a number of nonlinear parametric instabilities, such as the instability associated with stimulated Raman scattering. When the plasma turbulence is heavily damped, the radio bean can still undergo induced Compton scattering. Stimulated scattering effects such as these are very sensitive to the presence of narrow-band substructure in the pulsar radio emission. Finally, we consider the possibility that plasma derived from a stellar companion may mix with the relativistic pulsar wind and cause cyclotron absorption at low radio frequencies. Even if the cyclotron optical depth is small, fluctuations in the emergent polarization of the radio beam on the timescale of a few seconds are a very sensitive probe of the spatial structure of the magnetic field in the pulsar wind. The current observational properties of two known eclipsing pulsar systems, PSR 1957+20 and PSR 1744-24A, are used to construct tentative eclipse models. The favored model for PSR 1957+20 is cyclotron or synchrotron absorption by plasma embedded in the pulsar wind combined with pulse smearing at high frequency, and the favored model for PSR 1744-24A is backscattering off plasma turbulence generated by the stimulated Raman scattering parametric instability. Pulsar eclipses promise to provide a good diagnostic of pulsar winds and possible of the pulse emission mechanism.

Thompson, C.↗

NASA NTRS1999

Coherent Pump-Probe Interactions and Terahertz Intersubband Gain in Semiconductor Quantum Wells

In recent years there has been considerable interest in intersubband-transition-based infrared semiconductor quantum well (QW) lasers because of their potential applications. In the mid-infrared range, both electrically-injected quantum cascade lasers [1] and optically-pumped multiple QW lasers [2] have been experimentally realized. In these studies, optical gain is due to population inversion between the lasing subbands. It was also proposed that stimulated Raman scattering in QW systems can produce net infrared optical gain [3j. In such a nonlinear optical scheme, the appearance of optical gain that may lead to intersubband Raman lasers does not rely on the population inversion. Since, in tile resonant Raman process (Raman gain is the largest in this case), the pump field induces population redistribution among subbands in the QW s ystem, it seems that a realistic estimate of the optical gain has to include this effect. Perturbative calculations used in the previous work [3] may overestimate the Raman gain. In this paper we present a nonperturbative calculation of terahertz gain of optically-pumped semiconductor step quantum wells. Limiting optical transitions within the conduction band of QW, we solve the pump-field-induced nonequilibrium distribution function for each subband of the QW system from a set of coupled rate equations. Both intrasubband and intersubband relaxation processes in the quantum well system are included. Taking into account the coherent interactions between pump and THz (signal) waves, we we derive the susceptibility of the QW system for the THz field. For a GaAs/AlGaAs step QW, we calculate the Thz gain spectrum for different pump frequencies and intensities. Under moderately strong pumping (approximately 0.3 MW/sq cm), a significant THz gain (approximately 300/m) is predicted. It is also shown that the coherent wave interactions (resonant stimulated Raman processes) contribute significantly to the THz gain.

Liu, Ansheng↗

DOE OSTI2020

Laser-plasma instabilities in long scale-length plasmas relevant to shock-ignition

We present 2D particle-in-cell simulations of laser-plasma instabilities (LPI) performed using conditions relevant to experiments on the OMEGA and NIF laser facilities. The laser intensity used is 2×10 15 W cm -2 , which allows comparison with previous experiments and simulations investigating shock ignition, though this is a relatively low intensity for the scheme. We find that the large convective gain of the instabilities leads to dynamics that are largely controlled by pump depletion and to scattering or absorption by LPIs predominantly occurring away from the quarter-critical density. The two-plasmon decay (TPD) instability is dominant for OMEGA-type conditions and remains important at the NIF-scale. In both cases, most absorption from TPD occurs near its Landau cutoff density, and we examine its nonlinear dynamics in this region, focusing on the ion-acoustic waves responsible for saturation. For NIF-type conditions, stimulated Raman scattering (SRS) and stimulated Brillouin scattering divert significant fractions of laser energy, and we find that SRS backscatter can occur with high gain at low densities due to kinetic effects. An in-depth analysis of hot-electron production is performed to identify the main sources and their characteristic electron temperature. For both simulations presented, the overall hot-electron temperature lies between 30 and 35 keV. This is relatively low and will likely increase shock pressure; however, the distributions also contain a significant number of high-energy (E k >100 keV) electrons that would likely cause unacceptable preheat. We, therefore, suggest some strategies that may be utilized to minimize this high-energy component. I. INTROD

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2020

Pump depletion and hot-electron generation in long-density-scale-length plasma with shock-ignition high-intensity laser

Two-dimensional particle-in-cell simulations for laser plasma interaction with laser intensity of 10 16 W/cm 2 , plasma density range of 0.01–0.28$n_c$, and scale length of 230–330 $\textit{μ}$m showed significant pump depletion of the laser energy due to stimulated Raman scattering (SRS) and stimulated Brillouin scattering (SBS) in the low-density region ($n_e$ = 0.01–0.2$n_c$). The simulations identified hot electrons generated by SRS in the low-density region with moderate energy and by two-plasmon-decay near $n_e$ = 0.25$n_c$ with higher energy. The overall hot electron temperature (46 keV) and conversion efficiency (3%) were consistent with the experiment's measurements. Further, the simulations also showed artificially reducing SBS would lead to stronger SRS and a softer hot-electron spectrum.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Single and Double Shell Ignition Targets for the National Ignition Facility at 527 nm

Converting and using the National Ignition Facility (NIF) to deliver 527 nm light instead of its current 351 nm would allow the laser to deliver more energy and power to ignition targets. We update previous 527 nm target design work to reflect more contemporary target designs using high-density carbon capsules and low density helium gas filled Hohlraums. We extend single shell capsule designs based on current experimental results to higher energy and power and also explore double shell capsules, both driven by green light. These studies were completed using detailed pulse shapes found for targets that converged with acceptable 2D implosion symmetries and then used the Lava Lamp II code to confirm their feasibility at NIF. A 1.2× dimensional scaleup of one tuned NIF target at the limit of its current 351 nm capabilities and shot 170827 uses 3.3 MJ, at the limit of the current NIF's 527 nm capability. With the less-structured pulse of a double shell target, 3.7 MJ could be delivered by the laser. Our LPI calculations do not preclude operation at 527 nm, particularly for low fill Hohlraums, and suggest that the stimulated Raman backscatter may be no worse than the small quantities seen in 170827; stimulated forward Raman scattering may be present. If Stimulated Brillouin Scattering is too great, the much greater laser bandwidth available at 527 nm could be used to decrease backscatter. These larger targets with higher energy and power may offer a better chance of achieving ignition with only modest changes to the NIF laser.

43 PARTICLE ACCELERATORS↗

NASA NTRS2014

A New Differential Absorption Lidar to Measure Sub-Hourly Fluctuation of Tropospheric Ozone Profiles in the Baltimore - Washington D.C. Region

Tropospheric ozone profiles have been retrieved from the new ground based National Aeronautics and Space Administration (NASA) Goddard Space Flight Center TROPospheric OZone DIfferential Absorption Lidar (GSFC TROPOZ DIAL) in Greenbelt, MD (38.99 N, 76.84 W, 57 meters ASL) from 400 m to 12 km AGL. Current atmospheric satellite instruments cannot peer through the optically thick stratospheric ozone layer to remotely sense boundary layer tropospheric ozone. In order to monitor this lower ozone more effectively, the Tropospheric Ozone Lidar Network (TOLNet) has been developed, which currently consists of five stations across the US. The GSFC TROPOZ DIAL is based on the Differential Absorption Lidar (DIAL) technique, which currently detects two wavelengths, 289 and 299 nm. Ozone is absorbed more strongly at 289 nm than at 299 nm. The DIAL technique exploits this difference between the returned backscatter signals to obtain the ozone number density as a function of altitude. The transmitted wavelengths are generated by focusing the output of a quadrupled Nd:YAG laser beam (266 nm) into a pair of Raman cells, filled with high pressure hydrogen and deuterium. Stimulated Raman Scattering (SRS) within the focus generates a significant fraction of the pump energy at the first Stokes shift. With the knowledge of the ozone absorption coefficient at these two wavelengths, the range resolved number density can be derived. An interesting atmospheric case study involving the Stratospheric-Tropospheric Exchange (STE) of ozone is shown to emphasize the regional importance of this instrument as well as assessing the validation and calibration of data. The retrieval yields an uncertainty of 16-19 percent from 0-1.5 km, 10-18 percent from 1.5-3 km, and 11-25 percent from 3 km to 12 km. There are currently surface ozone measurements hourly and ozonesonde launches occasionally, but this system will be the first to make routine tropospheric ozone profile measurements in the Baltimore-Washington DC area.

Stimulated Raman Scattering↗

DOE OSTI2023

Time-dependent saturation and physics-based nonlinear model of cross-beam energy transfer

The nonlinear physics of cross-beam energy transfer (CBET) for multi-speckled laser beams is examined using large-scale particle-in-cell simulations for a range of laser and plasma conditions relevant to indirect-drive inertial confinement fusion (ICF) experiments. The time-dependent growth and saturation of CBET involve complex, nonlinear ion and electron dynamics, including ion trapping-induced enhancement and detuning, ion acoustic wave (IAW) nonlinearity, oblique forward stimulated Raman scattering (FSRS), and backward stimulated Brillouin scattering (BSBS) in a CBET-amplified seed beam. Ion-trapping-induced detuning of CBET is captured in the kinetic linear response by a new δf-Gaussian-mixture algorithm, enabling an accurate characterization of trapping-induced non-Maxwellian distributions. Ion trapping induces nonlinear processes, such as changes to the IAW dispersion and nonlinearities (e.g., bowing and self-focusing), which, together with pump depletion, FSRS, and BSBS, determine the time-dependent nature and level of CBET gain as the system approaches a steady state. Using VPIC simulations at intensities at and above the onset threshold for ion trapping and the insight from the time-dependent saturation analyses, we construct a nonlinear CBET model from local laser and plasma conditions that predicts the CBET gain and the energy deposition into the plasma. This model is intended to provide a more accurate, physics-based description of CBET saturation over a wide range of conditions encountered in ICF hohlraums compared with linear CBET gain models with ad hoc saturation clamps often used in laser ray-based methods in multi-physics codes.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Raman Interferometry between Autoionizing States to Probe Ultrafast Wave-Packet Dynamics with High Spectral Resolution

Photoelectron interferometry with femtosecond and attosecond light pulses is a powerful probe of the fast electron wave-packet dynamics, albeit it has practical limitations on the energy resolution. We show that one can simultaneously obtain both high temporal and spectral resolution by stimulating Raman interferences with one light pulse and monitoring the modification of the electron yield in a separate step. Applying this spectroscopic approach to the autoionizing states of argon, we experimentally resolved its electronic composition and time evolution in exquisite detail. Theoretical calculations show remarkable agreement with the observations and shed light on the light-matter interaction parameters. Using appropriate Raman probing and delayed detection steps, this technique enables highly sensitive probing and control of electron dynamics in complex systems.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2023

Suppressing parametric instabilities in direct-drive inertial-confinement-fusion plasmas using broadband laser light

It has long been recognized that broadband laser light has the potential to control parametric instabilities in inertial-confinement-fusion (ICF) plasmas. Here, we use results from laser-plasma-interaction simulations to estimate the bandwidth requirements for mitigating the three predominant classes of instabilities in direct-drive ICF implosions: cross-beam energy transfer (CBET), two-plasmon decay (TPD), and stimulated Raman scattering (SRS). We find that for frequency-tripled, Nd:glass laser light, a bandwidth of 8.5 THz can significantly increase laser absorption by suppressing CBET, while ∼13 THz is needed to mitigate absolute TPD and SRS on an ignition-scale platform. None of the glass lasers used in contemporary ICF experiments, however, possess a bandwidth greater than 1 THz and reaching larger values requires the use of an auxiliary broadening technique such as optical parametric amplification or stimulated-rotational-Raman scattering. An arguably superior approach is the adoption of an argon-fluoride (ArF) laser as an ICF driver. Besides having a broad bandwidth of ∼10 THz, the ArF laser also possesses the shortest wavelength (193 nm) that can scale to the high energy/power required for ICF—a feature that helps to mitigate parametric instabilities even further. We show that these native properties of ArF laser light are sufficient to eliminate nearly all CBET scattering in a direct-drive target and also raise absolute TPD and SRS thresholds well above those for broadband glass lasers. The effective control of parametric instabilities with broad bandwidth is potentially a “game changer” in ICF because it would enable higher laser intensities and ablation pressures in future target designs.

Bates, J. W. (ORCID:0000000188087240)↗

DOE OSTI2024

High-throughput chemical imaging for optimizing biofuel synthesis using synthetic biology (Final Technical Report)

Fatty acids can be produced biosynthetically in microbes and these compounds can serve as precursors to biodiesels and other high value oleochemicals. However, progress on engineering fatty acid biosynthesis, and biofuel synthesis more generally, has been hindered by current quantification methods that are either indirect or not amenable to high-throughput or single-cell resolution screening. In this project, we assembled an interdisciplinary team with complimentary expertise in synthetic biology and microscopy, metabolic engineering, and chemical imaging to address these challenges. We used chemical imaging to directly measure lipid biosynthesis in Escherichia coli engineered to produce fatty acids, obtaining detailed single-cell resolution measurements. We deployed stimulated Raman scattering (SRS) microscopy in concert with multiplexed genome engineering and gene circuit design strategies from synthetic biology to optimize production of fatty acids. These results provided novel insight into cell-to-cell heterogeneity present in biofuel production strains. In addition, we introduced new chemical imaging methods which are label-free and do not require fluorescent reporters. These efforts were complemented by other studied developing foundational tools for regulation and control, which offer excellent potential for advancing researchers’ ability to rapidly design, build, and test strains for enhanced biofuel synthesis.

09 BIOMASS FUELS↗

DOE OSTI2025

Lignin Removal in Subcellular Location of Poplar Cell Wall During Pretreatment Significantly Impacts Cellulose Digestibility

The γ-valerolactone (GVL) pretreatment is one of the leading solvent-based methods for producing high-quality lignin under mild conditions. However, the glucan conversion yield from GVL pretreated biomass remains unsatisfactory. To explore the discrepancies between the relatively low glucan conversion and high lignin extraction, we conducted GVL−HCl and NaOH pretreatments on poplar and investigated their effects on lignin content and location, as well as on enzymatic hydrolysis of poplar cell walls at the subcellular level. Under designated pretreatment conditions of GVL−HCl (90% GVL, 0.1 M HCl, 100 °C, 1 h) and NaOH (1 M, 121 °C, 2 h), the glucan conversion yields were 69.4% and 95.8%, with lignin removal rates of 67.8% and 47.7%, respectively. Four types of GFP-labeled carbohydrate binding modules were used to identify different forms of cellulose in the pretreated cell walls. The overall binding intensities to pretreated poplar were stronger for NaOH compared to GVL−HCl pretreatment. Stimulated Raman scattering microscopy imaging revealed that GVL−HCl preferentially extracted lignin from the compound middle lamella and cell corner areas, while NaOH effectively dissolved lignin in the secondary cell walls. Real-time imaging of cellulase degradation of pretreated cell walls further indicated that digestion started from both the cell lumen and the compound middle lamella areas for GVL, whereas it occurred uniformly across the secondary cell walls for NaOH. Our findings suggest that the location of lignin removal during pretreatment is crucial for enzymatic cellulose degradation, in addition to the total amount of lignin extraction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1994

Pressure broadening of vibrational Raman lines in N2 at temperatures below 300 K

Using quasi-cw stimulated Raman gain spectroscopy, the pressure broadening coefficients for the N2 vibrational Q-branch transitions have been measured over the temperature range 113-297 K for the rotational components J = 4, 6, 8, 10, and 12. The experimental results are fit to a simple power law to give an empirical formula for the temperature dependence of the pressure broadening over the 100-300 K range. These results are also compared to previously published scaling laws that are based on collision induced rotational transition rates.

Herring, G. C.↗

NASA NTRS1967

Coherent Raman amplification.

Coherent Raman amplification dynamics, considering pump depletion and coupling saturation and stimulated Raman scattering by polarization waves

POLARIZATION CHARACTERISTICS↗

DOE OSTI2022

Raman gain control in optical fibers with orbital-angular-momentum-induced chirality of light

Stimulated Raman scattering is a particularly robust nonlinearity, occurring in virtually every material because its spectral linewidth and associated frequency shift do not typically depend on phases or directions (i.e. wavevectors) of the interacting light beams. In amorphous materials such as glass fibers, Raman bandwidths are large, enabling its use as a broadband gain element. This ubiquity makes it a versatile means for achieving optical amplification or realizing lasers over a large range of pulsewidths at user-defined colors. However, this ease of deploying the effect also presents itself as a stubborn source of noise in fiber-based quantum sources or parasitic emission in fiber lasers. Here, we show that orbital angular momentum carrying light beams experiencing spin-orbit interactions yield novel phase-matching criteria for Raman scattering. This enables tailoring its spectral shape (by over half the Raman shift in a given material) as well as strength (by ∼ 100×) simply by controlling light’s topological charge – a capability of utility across the multitude of applications where modulating Raman scattering is desired.

Liu, Xiao (ORCID:000000032239762X)↗

NASA NTRS1990

Optimization of a Raman shifted dye laser system for DIAL applications

An efficient Raman shifted dye laser system that generates tunable radiation at 765 and 940 nm with a bandwidth of 0.03/cm is described. Operating a Raman cell at hydrogen pressure below 14 atm, optimum first Stokes energy conversions of 45 percent and of 37 percent at 765 and 940 nm, respectively, were recorded. Optical depth measurements made at the centers of twenty-five absorption lines in the P branch of the oxygen A band imply a high spectral purity for both the laser and the Raman shifted radiation, and thus indicate the feasibility of using the stimulated Raman scattered radiation for differential absorption lidar (DIAL) measurements.

Singh, Upendra N.↗

NASA NTRS1993

Non-intrusive measurements in a rocket engine combustor

In recent years analytical tools to characterize combustor flow have been developed in order to support design. To facilitate anchoring of combustion related physical models and the CFD codes in which they are incorporated, considerable development and application of non-intrusive combustion diagnostic capabilities has occurred. Raman spectroscopy can be used to simultaneously detect all polyatomic molecules present in significant concentrations and to determine gas temperature. This is because all molecules possess a distinct temperature dependent Raman spectrum. A multi-point diagnostic system for non-intrusive temperature and species profiling in rocket engines has been developed at Rocketdyne. In the present effort, the system has been undergoing validation for application to rocket engine component testing. A 4 inch diameter windowed combustor with a coaxial gas-gas injector was chosen for this series of validation experiments. Initially an excimer-pumped tunable dye laser and later a solid state Nd-Yag laser served as excitation sources. The Raman signal was dispersed by a monochromator and detected by a gated, intensified Charged Coupled Device (CCD) array. Experiments were carried out prior to each series of hot fire tests to ensure that the Raman signal detected was due to a spontaneous rather than a stimulated Raman emission process. Over sixty hot fire tests were conducted during the first series of tests with the excimer/dye laser. All hot fire testing was at a mixture ratio of 0.5 and chamber pressures of approximately 100 and approximately 300 psia. The Raman spectra of hydrogen, water vapor and oxygen recorded during single element hot fire tests were reduced and analyzed. A significant achievement was the attainment of single shot Raman spectra in cold flow tests. Unfortunately, the single shot signal-to-noise ratio deteriorated to an unacceptable level during the hot fire testing. Attempts to obtain temperature data from the hydrogen Q1-branch profiles obtained in hot fire tests suggest that potentially complicating factors may render the approach of averaging data on the photodiode array invalid. A second series of hot fire tests was conducted with a 4 element coaxial injector using the Nd-Yag laser. A very compact and portable diagnostics set up was assembled for ease of alignment, relocation and flexibility. Measurements were made at several regions in the chamber in order to map concentration profiles. High spatial resolution and improved signal to noise characteristics were demonstrated.

Farhangi, S.↗