Search NASA⌕ Search

SEARCH · Search NASA

Results for “Optical Probe”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 451 records · Page 25
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Photoexcitation of Fe 3 O Nodes in MOF Drives Water Oxidation at pH=1 When Ru Catalyst Is Present

Abstract Artificial photosynthesis strives to convert the energy of sunlight into sustainable, eco‐friendly solar fuels. However, systems with light‐driven water oxidation reaction (WOR) at pH=1 are rare. Broadly used [Ru(bpy) 3 ] 2+ (bpy=2,2’‐bipyridine) photosensitizer has a fixed +1.23 V potential which is insufficient to drive most water oxidation catalysts (WOCs) in acid, while Fe 2 O 3 , featuring the highly oxidizing holes, is not stable at low pH. Here, the key examples of Fe‐based metal–organic framework (MOF) water oxidation photoelectrocatalysts active at pH=1 are presented. Fe‐MIL‐126 and Fe MOF‐dcbpy structures were formed with 4,4’‐biphenyl dicarboxylate (bpdc), 2,2’‐bipyridine‐5,5’‐dicarboxylate (dcbpy) linkers and their mixtures. Presence of dcbpy linkers allows integration of metal‐based catalysts via coordination to 2,2’‐bipyridine fragments. Fe‐based MOFs were doped with Ru‐based precursors to achieve highly active MOFs bearing [Ru(bpy)(dcbpy)(H 2 O) 2 ] 2+ WOC. Materials were analyzed with X‐ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infra‐red (FTIR) spectroscopy, resonance Raman, X‐ray absorption spectroscopy, fs optical pump‐probe, electron paramagnetic resonance (EPR), diffuse reflectance and electric conductivity measurements and were modeled by band structure calculations. It is shown that under reaction conditions, Fe III and Ru III oxidation states are present, indicating rate‐limiting electron transfer in MOF. Fe 3 O nodes emerge as photosensitizers able to drive prolonged O 2 evolution in acid. Further developments are possible via MOF's linker modification for enhanced light absorption, electrical conductivity, reduced MOF solubility in acid, Ru‐WOC modification for faster WOC catalysis, or Ru‐WOC substitution to 3d metal‐based systems. The findings give further insight for development of light‐driven water splitting systems based on Earth‐abundant metals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Use of a Multiplexed Photonic Doppler Velocimetry (MPDV) System to Study Plastic Deformation of Metallic Steel Plates in High Velocity Impact

High-velocity impact experiments with a gas gun pose unique challenges, in terms of experimental setup and computational simulation, since the projectile-target interaction creates extreme pressure and temperature within few micro seconds. The objective of this study is to accurately measure the plastic deformation of plates under projectile impact that does not lead to full penetration. In this work, free surface velocities at the back side of target plates are measured using the newly developed Multiplexed Photonic Doppler Velocimetry (MPDV) system, which is an interferometric fiber-optic technique which can measure velocity from the Doppler shift of the light reflected from the moving back surface of the target. The MPDV system allows measurements of velocity from different locations on the target plate using multiple optical fiber probes oriented in specific directions and patterns. Data are reduced using a Fast Fourier transformation (FFT) technique to obtain the free surface velocity profiles. These velocity profiles can present insights into the dynamic behavior of impacted materials under shock loading conditions.

MPDV, multiplexing, high-velocity impact, velocime↗
DOE OSTI2016

A new mechanistic scale-up methodology for gas-solid spouted beds

We report a new mechanistic methodology of scale-up for gas-solid spouted beds has been proposed and validated which is based on maintaining similar radial profiles of gas holdup. Two spouted beds of 0.152 m and 0.076 m inside diameter have been used. The local measurements of the dimensionless solids velocity and holdups using an advanced optical fiber probe and pressure fluctuations using pressure transducers indicate clearly the similarity when the radial profiles of the gas holdups were kept similar in the two studied spouted beds. When the radial profiles of the gas holdups were different in the two studied spouted beds, the dimensionless of the local studied parameters mentioned above were different. The differences increase when the difference in the magnitudes and trends of the gas holdup profiles increases.

42 ENGINEERING↗
DOE OSTI2016

An advanced evaluation of spouted beds scale-up for coating TRISO nuclear fuel particles using Radioactive Particle Tracking (RPT)

A set of dimensionless groups has been proposed in the literature by He et al. (1997) to scale-up gas-solid spouted beds while maintaining their hydrodynamics similarity. The literature reported studies do not provide conclusive assessments about this methodology. Therefore, in this work, we have applied an advanced non-invasive Radioactive Particle Tracking (RPT) technique for the first time to evaluate such scale-up methodology by measuring the local solids velocity, normal and shear stresses and the turbulent kinetic energy. The axial and azimuthal averaged radial profiles of solids velocity, normal stresses, shear stresses, and turbulent kinetic energy illustrate that the similarity of the hydrodynamics has not been attained when the proposed set of dimensionless groups has been matched using two sizes of spouted beds of 0.076 m and 0.152 m and sets of operating conditions. The conclusion is consistent with the recent reported findings by measuring cross sectional distribution and radial profiles of solids and gas holdups along the bed height using gamma-ray computed tomography and by the limited point measurements of solids velocity and holdup using optical fiber probe. It is clear that local measurements of hydrodynamic parameters are essential for detailed assessment of scale-up methodologies. Here, the presented results of our work in terms of the components profiles of the particles radial velocities and turbulent parameters are also valuable for benchmarking computational fluid dynamics codes and models.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

The importance of temporal and spatial incoherence in quantitative interpretation of 4D-STEM

Recent developments in pixelated detectors, when combined with aberration correction of probe forming optics have greatly enhanced the field of scanning electron diffraction. Differential phase contrast is now routine and deep learning has been proposed as a method to extract maximum information from diffraction patterns. This study examines the effects of temporal and spatial incoherence on convergent beam electron diffraction patterns and demonstrates that simple center of mass measurements cannot be naively interpreted. The inclusion of incoherence in deep learning data sets is also discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Time-resolved ionization measurements with intense ultrashort XUV and X-ray free-electron laser pulses

Abstract Modern free-electron lasers (FEL) operating in XUV (extreme ultraviolet) or X-ray range allow an access to novel research areas. One instance is the ultrafast ionization of a solid by an intense femtosecond FEL pulse in XUV which consequently leads to a change of the complex index of refraction on an ultrashort timescale. The photoionization and subsequent impact ionization resulting in electronic and atomic dynamics are modeled with our hybrid code XTANT(X-ray thermal and non-thermal transitions) and a Monte Carlo code XCASCADE(X-ray-induced electron cascades). The simulations predict the temporal kinetics of FEL-induced electron cascades and thus yield temporally and spatially resolved information on the induced changes of the optical properties. In a series of experiments at FERMI and LCLS, single shot measurements with spatio-temporal encoding of the ionization process have been performed by a correlation of the FEL pump pulse with an optical femtosecond probe pulse. An excellent agreement between the experiment and the simulation has been found. Furthermore, we demonstrate that such kind of experiments forms the basis for pulse duration and arrival time jitter monitoring as currently under development for XUV-FELs.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Oxygen-Vacancy-Induced Midgap States Responsible for the Fluorescence and the Long-Lasting Phosphorescence of the Inverse Spinel Mg(Mg,Sn)O 4

Samples of inverse spinel Mg 2 SnO 4 were prepared using a ceramic method, their phosphorescence phenomenon was probed by optical measurements, and its cause was explored on the basis of density functional theory calculations for model structures of Mg 2 SnO 4 with oxygen vacancies VO. Mg 2 SnO 4 exhibits long-lasting luminescence at two different wavelength regions, peaking at ~498 and ~755 nm. A Sn-VO-Sn defect plus a Mg vacancy VMg away from the VO generates the empty midgap states, σSn-Sn and σSn-Sn*, localized at the Sn-VO-Sn defect, while an oxygen vacancy VO between adjacent Sn 4+ and Mg 2+ sites creates a filled midgap state Sn 2+ (5s 2 lone pair) lying below the σ Sn-Sn level. The long-lasting luminescence at two different wavelength regions and the up-conversion photostimulated luminescence observed for undoped Mg 2 SnO 4 are well explained by considering the σ Sn-Sn * level as the trapping level for a photogenerated electron.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Nonlinear Optical Microscopy with Ultralow Quantum Light

Nonlinear optical (NLO) microscopy relies on multiple light–matter interactions to provide unique contrast mechanisms and imaging capabilities that are inaccessible to traditional linear optical imaging approaches, making them versatile tools to understand a wide range of complex systems. However, the strong excitation fields that are necessary to drive higher-order optical processes efficiently are often responsible for photobleaching, photodegradation, and interruption in many systems of interest. This is especially true for imaging living biological samples over prolonged periods of time or in accessing intrinsic dynamics of electronic excited-state processes in spatially heterogeneous materials. This perspective outlines some of the key limitations of two NLO imaging modalities implemented in our lab and highlights the unique potential afforded by the quantum properties of light, especially entangled two-photon absorption based NLO spectroscopy and microscopy. Here, we further review some of the recent exciting advances in this emerging filed and highlight some major challenges facing the realization of quantum-light-enabled NLO imaging modalities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Disentangling Rotational Dynamics and Ordering Transitions in a System of Self-Organizing Protein Nanorods via Rotationally Invariant Latent Representations

The dynamics of complex ordering systems with active rotational degrees of freedom exemplified by protein self-assembly is explored using a machine learning workflow that combines deep learning-based semantic segmentation and rotationally invariant variational autoencoder-based analysis of orientation and shape evolution. The latter allows for disentanglement of the particle orientation from other degrees of freedom and compensates for lateral shifts. The disentangled representations in the latent space encode the rich spectrum of local transitions that can now be visualized and explored via continuous variables. The time dependence of ensemble averages allows insight into the time dynamics of the system and, in particular, illustrates the presence of the potential ordering transition. Finally, analysis of the latent variables along the single-particle trajectory allows tracing these parameters on a single-particle level. The proposed approach is expected to be universally applicable for the description of the imaging data in optical, scanning probe, and electron microscopy seeking to understand the dynamics of complex systems where rotations are a significant part of the process.

representation learning↗
DOE OSTI2016

In-plane optical anisotropy of layered gallium telluride

Layered gallium telluride (GaTe) has attracted much attention recently, due to its extremely high photoresponsivity, short response time, and promising thermoelectric performance. Different from most commonly studied two-dimensional (2D) materials, GaTe has in-plane anisotropy and a low symmetry with the C 2h 3 space group. Investigating the in-plane optical anisotropy, including the electron–photon and electron–phonon interactions of GaTe is essential in realizing its applications in optoelectronics and thermoelectrics. In this work, the anisotropic light-matter interactions in the low-symmetry material GaTe are studied using anisotropic optical extinction and Raman spectroscopies as probes. Our polarized optical extinction spectroscopy reveals the weak anisotropy in optical extinction spectra for visible light of multilayer GaTe. Polarized Raman spectroscopy proves to be sensitive to the crystalline orientation of GaTe, and shows the intricate dependences of Raman anisotropy on flake thickness, photon and phonon energies. Such intricate dependences can be explained by theoretical analyses employing first-principles calculations and group theory. Furthermore, these studies are a crucial step toward the applications of GaTe especially in optoelectronics and thermoelectrics, and provide a general methodology for the study of the anisotropy of light-matter interactions in 2D layered materials with in-plane anisotropy.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Visualization of dynamic polaronic strain fields in hybrid lead halide perovskites

Excitation localization involving dynamic nanoscale distortions is a central aspect of photocatalysis, quantum materials and molecular optoelectronics. Experimental characterization of such distortions requires techniques sensitive to the formation of point-defect-like local structural rearrangements in real time. Here, we visualize excitation-induced strain fields in a prototypical member of the lead halide perovskites via femtosecond resolution diffuse X-ray scattering measurements. Here, this enables momentum-resolved phonon spectroscopy of the locally distorted structure and reveals radially expanding nanometre-scale strain fields associated with the formation and relaxation of polarons in photoexcited perovskites. Quantitative estimates of the magnitude and shape of this polaronic distortion are obtained, providing direct insights into the dynamic structural distortions that occur in these materials. Optical pump–probe reflection spectroscopy corroborates these results and shows how these large polaronic distortions transiently modify the carrier effective mass, providing a unified picture of the coupled structural and electronic dynamics that underlie the optoelectronic functionality of the hybrid perovskites.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Strong lattice correlation of non-equilibrium quasiparticles in a pseudospin-1/2 Mott insulator Sr 2 IrO 4

In correlated oxides the coupling of quasiparticles to other degrees of freedom such as spin and lattice plays critical roles in the emergence of symmetry-breaking quantum ordered states such as high temperature superconductivity. We report a strong lattice coupling of photon-induced quasiparticles in spin-orbital coupling Mott insulator Sr 2 IrO 4 probed via optical excitation. Combining time-resolved x-ray diffraction and optical spectroscopy techniques, we reconstruct a spatiotemporal map of the diffusion of these quasiparticles. Lastly, due to the unique electronic configuration of the quasiparticles, the strong lattice correlation is unexpected but extends the similarity between Sr 2 IrO 4 and cuprates to a new dimension of electron-phonon coupling which persists under highly non-equilibrium conditions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2019

Decomposing electronic and lattice contributions in optical pump – X-ray probe transient inner-shell absorption spectroscopy of CuO

Electronic and lattice contributions to picosecond time-resolved X-ray absorption spectra (trXAS) of CuO at the oxygen K-edge are analyzed by comparing trXAS spectra, recorded using excitation wavelengths of 355 nm and 532 nm, to steady-state, temperature-dependent XAS measurements. The trXAS spectra at pump-probe time-delays ≥150 ps are dominated by lattice heating effects. Insight into the temporal evolution of lattice temperature profiles on timescales up to 100s of nanoseconds after laser excitation are reported, on an absolute temperature scale, with a temporal sensitivity and a spatial selectivity on the order of 10s of picoseconds and 10s of nanometers, respectively, effectively establishing an "ultrafast thermometer". In particular, for the 532 nm experiment at ~5 mJ cm -2 fluence, both the initial sample temperature and its dynamic evolution are well captured by a one-dimensional thermal energy deposition and diffusion model. The thermal conductivity k = (1.3 ± 0.4) W m -1 K -1 derived from this model is in good agreement with the literature value for CuO powder, k powder = 1.013 W m -1 K -1 . For 355 nm excitation, a quantitative analysis of the experiments is hampered by the large temperature gradients within the probed sample volume owing to the small UV penetration depth. The impact of the findings on mitigating or utilizing photoinduced lattice temperature changes in future X-ray free electron laser (XFEL) experiments is discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Exploring the capabilities of optical pump X-ray probe NEXAFS spectroscopy to track photo-induced dynamics mediated by conical intersections

X-ray spectroscopy is gaining a growing interest in the scientific community, as it represents a versatile and powerful experimental toolbox for probing the dynamics of both core and valence electronic excitations, nuclear motions and material structure, with element and site specificity. Among the various X-ray based techniques, near-edge X-ray absorption fine structure (NEXAFS) spectroscopy, which investigates the energy and probability of resonant core-to-valence transitions, has started to be applied to organic molecules: a recent UV-pump X-ray probe time-resolved NEXAFS experiment [Wolf et al., Nat. Commun., 2017, 8, 1] has shown the capability of the technique to provide information about the ultrafast internal conversion between the bright ππ* and the dark nπ* electronic states of the nucleobase thymine. In the present contribution we introduce an accurate theoretical approach for the simulation of NEXAFS spectra of organic molecules, employing azobenzene as a test case. The electronic structure calculations, which provide both energy levels and transition probabilities of core-to-valence excitations, were here performed with a high level multiconfigurational method, the restricted active space self consistent field (RASSCF/RASPT2). GS- and nπ*-NEXAFS spectra were obtained on the top of key molecular geometries (as the optimized cis, trans and conical intersection(s) structures) as well as along the fundamental isomerization coordinates (namely, symmetric and asymmetric bendings of the phenyl rings, and torsion around the central dihedral). We eventually characterize and explain the origin of the simulated signals, highlighting the specific signatures that make it possible to follow the excited state evolution from the nπ* Franck–Condon point, towards the conical intersection(s).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

A portable fiber optic sensor for the luminescent sensing of cobalt ions using carbon dots

Cobalt is critical to energy-relevant technologies, and demand for cobalt will increase significantly with growing global adoption of renewables. However, supply chain stability is threatened by economic and geopolitical factors, incentivizing domestic cobalt production from alternative resources such as coal, coal utilization byproducts (e.g., ash, acid mine drainage) and electronic waste. Rapid, inexpensive, and portable characterization techniques are needed to reduce production costs associated with cobalt prospecting and process monitoring. Here, in this research, we develop a compact, portable fiber optic luminescent probe for cobalt using phosphorus and nitrogen co-doped carbon dots as the sensing material. The carbon dot emission overlaps well with the cobalt absorption band at ~510 nm, leading to a selective decrease in emission as a function of cobalt concentration. The system responds nearly instantly to the presence of cobalt, with detection limits of 0.7 and 3.5 ppm in water and pH 1.68 buffer, respectively, providing comparable performance to a commercial spectrometer at a significantly lower cost. Moreover, the sensor is selective for cobalt in the presence of 13 of the most common metal ions encountered in coal utilization byproducts and is responsive to cobalt when spiked into an acid mine drainage leachate sample, highlighting the sensor's potential for real-world deployment in challenging matrices. In addition, integrating the carbon dots with a filter paper substrate produced ‘test strip’ sensors that exhibited a selective and sensitive visual response to cobalt using a handheld UV lamp. Taken together, the sensing system represents a significant step forward in the development of low-cost practical sensors for high-value metals in complex streams.

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

Carrier recombination parameters in diamond after surface boron implantation and annealing

In this study, an optical pump–probe technique was used to detect spatial distribution of carrier lifetimes across the thickness of a high-quality diamond device structure. Two samples with as-received and boron implanted surfaces were compared to assess the role of implantation and related processing on carrier recombination mechanisms. It was found that the two implanted surfaces show very different behaviors despite undergoing the same treatment. At one of the surfaces, carrier lifetimes remained relatively unchanged, indicating surface recombination rates in the 102–103 cm/s range. At the other surface, carrier lifetimes were almost a magnitude lower and correlated with the locally detected nitrogen vacancy defect that was attributed to the elevated concentration of residual nitrogen.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

High thermal conductivity and ultrahigh thermal boundary conductance of homoepitaxial AlN thin films

Wurtzite aluminum nitride (AlN) has attracted increasing attention for high-power and high-temperature operations due to its high piezoelectricity, ultrawide-bandgap, and large thermal conductivity k. The k of epitaxially grown AlN on foreign substrates has been investigated; however, no thermal studies have been conducted on homoepitaxially grown AlN. In this study, the thickness dependent k and thermal boundary conductance G of homoepitaxial AlN thin films were systematically studied using the optical pump–probe method of frequency-domain thermoreflectance. Our results show that k increases with the thickness and k values are among the highest reported for film thicknesses of 200 nm, 500 nm, and 1 μm, with values of 71.95, 152.04, and 195.71 W/(mK), respectively. Our first-principles calculations show good agreement with our measured data. Remarkably, the G between the epilayer and the substrate reported high values of 328, 477, 1180, and 2590 MW/(m 2 K) for sample thicknesses of 200 nm, 500 nm, 1 μm, and 3 μm, respectively. The high k and ultrahigh G of homoepitaxially grown AlN are very promising for efficient heat dissipation, which helps in device design and has advanced applications in micro-electromechanical systems, ultraviolet photonics, and high-power electronics.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Ultrafast laser-induced spin–lattice dynamics in the van der Waals antiferromagnet CoPS 3

CoPS 3 stands out in the family of the van der Waals antiferromagnets XPS 3 (X = Mn, Ni, Fe, and Co) due to the unquenched orbital momentum of the magnetic Co 2+ ions, which is known to facilitate the coupling of spins to both electromagnetic waves and lattice vibrations. Here, using a time-resolved magneto-optical pump–probe technique, we experimentally study the ultrafast laser-induced dynamics of mutually correlated spins and lattice. It is shown that a femtosecond laser pulse acts as an ultrafast heater and, thus, results in the melting of the antiferromagnetic order. At the same time, the resonant pumping of the 4 T 1g → 4 T 2g electronic transition in Co 2+ ions effectively changes their orbital momentum, giving rise to a mechanical force that moves the ions in the direction parallel to the orientation of their spins, thus generating a coherent B g phonon mode at the frequency of about 4.7 THz.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗