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DOE OSTI2022

Hybridization and deconfinement in colloidal quantum dot molecules

The structural, electronic, and optical properties of CdSe/CdS core–shell colloidal quantum dot molecules, a new class of coupled quantum dot dimers, are explored using atomistic approaches. Unlike the case of dimers grown by molecular beam epitaxy, simulated strain profile maps of free-standing colloidal dimers show negligible additional strain resulting from the attachment. Further, the electronic properties of the relaxed dimers are described within a semiempirical pseudopotential model combined with the Bethe–Salpeter equation within the static screening approximation to account for electron–hole correlations. The interplay of strain, hybridization (tunneling splitting), quantum confinement, and electron–hole binding energies on the optical properties is analyzed and discussed. The effects of the dimensions of the neck connecting the two quantum dot building blocks, as well as the shell thickness, are studied.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Quantum efficiency enhancement in simulated nanostructured negative electron affinity GaAs photocathodes

We report nanostructured negative electron affinity GaAs photocathodes for a polarized electron source are studied using finite difference time domain optical simulation. The structures studied are nanosquare columns, truncated nanocones, and truncated nanopyramids. Mie-type resonances in the 700–800 nm waveband, suitable for generation of polarized electrons, are identified. At resonance wavelengths, the nanostructures can absorb up to 99% of the incident light. For nanosquare columns and truncated nanocones, the maximum quantum efficiency (QE) at 780 nm obtained from simulation is 27%, whereas for simulated nanopyramids, the QE is ~21%. The high photocathode quantum efficiency is due to the shift of Mie resonance toward the longer wavelength, leading to increased light absorption. The field profile distribution shows the excitation of dipole and quadrupole modes within the nanostructures at resonant frequencies. This leads to enhanced photoabsorption and photoelectron generation closer to emission surfaces than for a flat photocathode. The enhanced photoabsorption and reduced electron transport distance for the nanostructured photocathode enhance its QE compared to that for the flat surface wafer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2020

Direct time-domain determination of electron-phonon coupling strengths in chromium

In this work, we report the results of an ultrafast, direct structural measurement of optically pumped phonons in a Cr thin film using ultrashort x-ray pulses from a free-electron laser. In addition to measuring and confirming the known long-wavelength dispersion relation of Cr along a particular acoustic branch, we are able to determine the relative phase of the phonons as they are generated. The Cr sample exhibits two generation mechanisms for the phonons: the releasing of a preexisting charge density wave at higher frequencies, and the creation of an acoustic strain pulse via laser heating that dominates at lower frequencies. Furthermore, for the latter mechanism, we are able to measure the frequency dependence of the time required to generate the phonons. To explain the observed magnitude and slope of the delays, we perform first-principles simulations in the framework of density functional perturbation theory and ab initio molecular dynamics to fit anharmonic phonon models. In conclusion, these results show that the wave-vector dependence of the electron-phonon coupling is the driving mechanism behind the delay times: Phase-space limitation leads to higher times near the zone center. The absolute magnitudes of the delay times measured are found to be much shorter than the equilibrium electron-phonon coupling times we compute, indicating that the coupling strength is greatly enhanced when the electronic system is out of equilibrium with the lattice, as has been seen in bismuth and other systems.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2020

Dephasingless Laser Wakefield Acceleration

Laser wakefield accelerators (LWFAs) produce significantly high gradients enabling compact accelerators and radiation sources, but face design limitations, such as dephasing, occurring when trapped electrons outrun the accelerating phase of the wakefield. In this report we combine spherical aberration with a novel cylindrically symmetric echelon optic to spatiotemporally structure an ultra-short, high-intensity laser pulse that can overcome dephasing by propagating at any velocity over any distance. The ponderomotive force of the spatiotemporally shaped pulse can drive a wakefield with a phase velocity equal to the speed of light in vacuum, preventing trapped electrons from outrunning the wake. Simulations in the linear regime and scaling laws in the bubble regime illustrate that this dephasingless LWFA can accelerate electrons to high energies in much shorter distances than a traditional LWFA—a single 4.5 m stage can accelerate electrons to TeV energies without the need for guiding structures.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2024

Cosmological Constraints from Combining Photometric Galaxy Surveys and Gravitational Wave Observatories

Spatial variations in survey properties due to selection effects generate substantial systematic errors in large-scale structure measurements in optical galaxy surveys on very large scales. On such scales, the statistical sensitivity of optical surveys is also limited by their finite sky coverage. By contrast, gravitational wave (GW) sources appear to be relatively free of these issues, provided the angular sensitivity of GW experiments can be accurately characterized. We quantify the expected cosmological information gain from combining the forecast LSST 3$\times$2pt analysis (combination of three 2-point correlations of galaxy density and weak lensing shear fields) with the large-scale auto-correlation of GW sources from proposed next-generation GW experiments. We find that in $\Lambda$CDM and $w$CDM models, there is no significant improvement in cosmological constraints from combining GW with LSST 3$\times$2pt over LSST alone, due to the large shot noise for the former; however, this combination does enable a $\sim6\%$ constraint on the linear galaxy bias of GW sources. More interestingly, the optical-GW data combination provides tight constraints on models with primordial non-Gaussianity (PNG), due to the predicted scale-dependent bias in PNG models on large scales. Assuming that the largest angular scales that LSST will probe are comparable to those in Stage III surveys ($\ell_{\rm min}\sim50$), the inclusion of next-generation GW measurements could improve constraints on the PNG parameter $f_{\rm NL}$ by up to a factor of $\simeq6.6$ compared to LSST alone, yielding $\sigma(f_{\rm NL})=8.5$. These results assume the expected capability of a network of Einstein Telescope-like GW observatories, with a detection rate of $10^6$ events/year. We investigate the sensitivity of our results to different assumptions about future GW detectors as well as different LSST analysis choices.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2020

Atmospheric Pressure Plasma Deposition of TiO2: A Review

Atmospheric pressure plasma (APP) deposition techniques are useful today because of their simplicity and their time and cost savings, particularly for growth of oxide films. Among the oxide materials, titanium dioxide (TiO2) has a wide range of applications in electronics, solar cells, and photocatalysis, which has made it an extremely popular research topic for decades. Here, we provide an overview of non-thermal APP deposition techniques for TiO2 thin film, some historical background, and some very recent findings and developments. First, we define non-thermal plasma, and then we describe the advantages of APP deposition. In addition, we explain the importance of TiO2 and then describe briefly the three deposition techniques used to date. We also compare the structural, electronic, and optical properties of TiO2 films deposited by different APP methods. Lastly, we examine the status of current research related to the effects of such deposition parameters as plasma power, feed gas, bias voltage, gas flow rate, and substrate temperature on the deposition rate, crystal phase, and other film properties. The examples given cover the most common APP deposition techniques for TiO2 growth to understand their advantages for specific applications. In addition, we discuss the important challenges that APP deposition is facing in this rapidly growing field.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Modeling and simulations of hydrodynamic shocks in a plasma flowing across randomized ICF scale laser beams

High-energy laser beams interacting with flowing plasmas can produce a plasma response that leads to deflection of the beam, beam bending. Such beams have usually a speckle structure generated by optical smoothing techniques that reduce the spatial and temporal coherence in the laser field pattern. The cumulative plasma response from laser speckles slows down the velocity of the incoming flow by momentum conservation. For slightly super-sonic flow the cumulative plasma response to the ponderomotive force exerted by the beam speckle ensemble is the strongest, such that slowing down the flow to subsonic velocities leads eventually to the generation of a shock around the cross section of the beam. This scenario has been predicted theoretically and is confirmed here by our hydrodynamic simulations in two dimensions with speckled beams and in one dimension with a reduced model. The conditions of shock generation are given in terms of the ponderomotive pressure, speckle size and the flow velocity. The nonlinear properties of the shocks are analyzed using Rankine–Hugoniot relations. According to linear theory, temporally smoothed laser beams exhibit a higher threshold for shock generation. Numerical simulations with beams that are smoothed by spectral dispersion compare well with the linear theory results, diverging from those produced by beams with only a random phase plates in the nonlinear regime. The conditions necessary for shock generation and their effects on the laser plasma coupling in inertial confinement fusion (ICF) experiments are also discussed.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2020

Charge Ordering and Low-Temperature Lattice Distortion in the {beta}'-(BDT-TTF){sub 2}CF{sub 3}CF{sub 2}SO{sub 3} Dime Mott Insulator.

We present single-crystal x-ray diffraction measurements, optical investigations, and electronic structure calculations for the organic charge-transfer salt beta'-(BEDT-TTF)(2)CF3CF2SO3 synthesized by electrocrystallization. Electronic structure calculations confirm the quasi-one-dimensional behavior of the compound and optical conductivity measurements reveal the dimer-Mott insulating nature of the system. The splitting of the charge-sensitive nu(2) mode in Raman spectra demonstrates the onset of an interlayer charge-ordered phase below 25 K, also suggested by the crystal structure considerations. This transition is accompanied by clear signatures of a lattice distortion in the BEDT-TTF donor layer, as shown by a splitting of the vibrational nu(3) mode in infrared spectra. At the same time, the sharp redshift of the nu(1) mode involving the BEDT-TTF ethylene groups strongly suggests a significant modification of the hydrogen-type bonding present between the BEDT-TTF donor layer and the CF3CF2SO3- anion layer. These observations point to a subtle interplay of charge and lattice degrees of freedom at the phase transition.

Olejniczak, I.↗

DOE OSTI2024

Probing the origin of the two-component structure of broad-line region by reverberation mapping of an extremely variable quasar

ABSTRACT The physical origins of quasar components, such as the broad-line region (BLR) and dust torus, remain under debate. To gain insights into them, we focused on changing-state quasars (CSQs) which provide a unique perspective through structural changes associated with accretion disc state transitions. We targeted SDSS J125809.31+351943.0, an extremely variable CSQ, to study its central core structure and kinematics. We conducted reverberation mapping with optical spectroscopy to explore the structure of the BLR and estimate the black hole mass. The results from Hβ reverberation mapping indicated a black hole mass of $10^{9.64^{+0.11}_{-0.20}}\rm {M_\odot }$. Additionally, we analysed variations in the optical to X-ray spectral indices, αox, before and after the state transition, to investigate the accretion disc. These variations in αox and the Eddington ratio (from 0.4 per cent to 2.4 per cent) exhibitied behaviour similar to state transitions observed in X-ray binary systems. Spectral analysis of Hβ revealed a predominantly double-peaked profile during dim periods, transitioning to include a single-peaked component as the quasar brightened, suggesting that Hβ contains a mixture of two components. Each of these components has its distinct characteristics: the first is a double-peaked profile that remains stable despite changes in the accretion rate, while the second is a variable single-peaked profile. Using time-lags from reverberation mapping, we estimated the spatial relationships between these BLR components, the accretion disc, and the dust torus. Our results suggest that the BLR consists of two distinct components, each differing in location and origin.

Nagoshi, Shumpei (ORCID:0000000326504322)↗

DOE OSTI2020

Smart Adhesive Joint with High-Definition Fiber-Optic Sensing for Automotive Applications

Structural health monitoring of fiber-reinforced composite-based joints for automotive applications during their manufacturing and on-demand assessment for its durability in working environments is critically needed. High-definition fiber-optic sensing is an effective method to measure internal strain/stress development using minimally invasive continuous sensors. The sensing fiber diameters are in the same order of magnitude when compared to reinforcement (glass, basalt, or carbon fibers) used in polymer composites. They also offer a unique ability to monitor the evolution of residual stresses after repeated thermal exposure with varying temperatures for automotive components/joints during painting using an electrophoretic painting process. In this paper, a high-definition fiber-optic sensor utilizing Rayleigh scattering is embedded within an adhesive joint between a carbon fiber-reinforced thermoset composite panel and an aluminum panel to measure spatially resolved strain development, residual strain, and thermal expansion properties during the electrophoretic paint process-simulated conditions. The strain measured by the continuous fiber-optic sensor was compared with an alternate technique using thermal digital image correlation. The fiber-optic sensor was able to identify the spatial variation of residual strains for a discontinuous carbon fiber-reinforced composite with varying local fiber orientations and resin content.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Probing Self-Assembly in Arginine–Oleic Acid Solutions with Terahertz Spectroscopy and X-ray Scattering

A study of the formation of microstructures in the reaction of oleic acid with arginine elucidates dynamical self-assembly processes at the molecular level. Terahertz spectroscopy combined with density functional calculations reveals the initial hydrogen-bonding motifs in the assembly process, leading to the formation of micelles and vesicles. Small-angle X-ray scattering measurements allow for kinetic analysis of the growth processes of these nanostructures, revealing a prenucleation pathway of vesicles and micelles which lead to spongelike structures. This final stage of the assembly into spongelike aggregates is investigated with optical microscopy. The formed structures only occur at pH > 8 and are resistant to extreme acidic and basic conditions. Here, a mechanistic pathway to the formation of the spongelike aggregates is described.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

X-ray nanodiffraction imaging reveals distinct nanoscopic dynamics of an ultrafast phase transition

Significance Phase transitions, the changes between states of matter with distinct electronic, magnetic, or structural properties, are at the center of condensed matter physics and underlie valuable technologies. First-order phase transitions are intrinsically heterogeneous. When driven by ultrashort excitation, nanoscale phase regions evolve rapidly, which has posed a significant experimental challenge to characterize. The newly developed laser-pumped X-ray nanodiffraction imaging technique reported here has simultaneous 100-ps temporal and 25-nm spatial resolutions. This approach reveals pathways of the nanoscale structural rearrangement upon ultrafast optical excitation, different from those transitions under slowly varying parameters. The spatiotemporally resolved structural characterization provides crucial nanoscopic insights into ultrafast phase transitions and opens opportunities for controlling nanoscale phases on ultrafast time scales.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Optical transient grating pumped X-ray diffraction microscopy for studying mesoscale structural dynamics

Abstract A fundamental understanding of materials’ structural dynamics, with fine spatial and temporal control, underpins future developments in electronic and quantum materials. Here, we introduce an optical transient grating pump and focused X-ray diffraction probe technique (TGXD) to examine the structural evolution of materials excited by modulated light with a precisely controlled spatial profile. This method adds spatial resolution and direct structural sensitivity to the established utility of a sinusoidal transient-grating excitation. We demonstrate TGXD using two thin-film samples: epitaxial BiFeO 3 , which exhibits a photoinduced strain (structural grating) with an amplitude proportional to the optical fluence, and FeRh, which undergoes a magnetostructural phase transformation. In BiFeO 3 , structural relaxation is location independent, and the strain persists on the order of microseconds, consistent with the optical excitation of long-lived charge carriers. The strain profile of the structural grating in FeRh, in comparison, deviates from the sinusoidal excitation and exhibits both higher-order spatial frequencies and a location-dependent relaxation. The focused X-ray probe provides spatial resolution within the engineered optical excitation profile, resolving the spatiotemporal flow of heat through FeRh locally heated above the phase transition temperature. TGXD successfully characterizes mesoscopic energy transport in functional materials without relying on a specific transport model.

36 MATERIALS SCIENCE↗

DOE OSTI2024

3D Optical Coherence Tomography image processing in BISCAP: characterization of biofilm structure and properties

Abstract Motivation BISCAP is a state-of-the-art tool for automatically characterizing biofilm images obtained from Optical Coherence Tomography. Limited availability of other software tools is reported in the field. BISCAP’s first version processes 2D images only. Processing 3D images is a problem of greater scientific relevance since it deals with the entire structure of biofilms instead of their 2D slices. Results Building on the image-processing principles and algorithms proposed earlier for 2D images, these were adapted to the 3D case, and a more general implementation of BISCAP was developed. The primary goal concerns the extension of the initial methodology to incorporate the depth axis in 3D images; multiple improvements were also made to boost computational performance. The calculation of structural properties and visual outputs was extended to offer new insights into the 3D structure of biofilms. BISCAP was tested using 3D images of biofilms with different morphologies, consistently delivering accurate characterizations of 3D structures in a few minutes using standard laptop machines. Low user dependency is required for image analysis. Availability and implementation BISCAP is available from https://github.com/diogonarciso/BISCAP. All images used in the tutorials and the validation examples are available from https://web.fe.up.pt/∼fgm/biscap3d.

Narciso, Diogo A. C. (ORCID:0000000227767477)↗

DOE OSTI2023

Exponential vs Gaussian Correlation Functions in the Characterization of Block Copolymer Grain Structure by Depolarized Light Scattering

Block copolymer (BCP) grain structure affects the mechanical, optical, and electrical properties of BCP materials, making the accurate characterization of this grain structure an important goal. In this study, improved BCP grain parameters were obtained by employing an exponentially decaying correlation function within the ellipsoidal grain model, instead of the Gaussian correlation function that was used in previous work. The exponential correlation function provides a better fit to the experimental depolarized light scattering data, which outweighs the disadvantage that it requires numerical integration to obtain the model scattered intensity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Deep optical imaging of star-forming blue early-type galaxies: Color map structures and faint features indicative of recent mergers

Blue early-type galaxies with galaxy-scale ongoing star formation are interesting targets in order to understand the stellar mass buildup in elliptical and S0 galaxies in the local Universe. We study the star-forming population of blue early-type galaxies to understand the origin of star formation in these otherwise red and dead stellar systems. The legacy survey imaging data taken with the dark energy camera in the g, r, and z bands for 55 star-forming blue early-type galaxies were examined, and g – r color maps were created. We identified low surface brightness features near 37 galaxies, faint-level interaction signatures near 15 galaxies, and structures indicative of recent merger activity in the optical color maps of all 55 galaxies. These features are not visible in the shallow Sloan Digital Sky Survey imaging data in which these galaxies were originally identified. Low surface brightness features found around galaxies could be remnants of recent merger events. The star-forming population of blue early-type galaxies could be post-merger systems that are expected to be the pathway for the formation of elliptical galaxies. We hypothesize that the star-forming population of blue early-type galaxies is a stage in the evolution of early-type galaxies. The merger features will eventually disappear, fuel for star formation will cease, and the galaxy will move to the passive population of normal early-type galaxies.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Pulsed laser deposition and structural evolution of BaF 2 nanolayers in Eu-doped BaF 2 /Al 2 O 3 layered optical nanocomposite thin films

Here, we have developed a pulsed laser deposition (PLD) geometry for the growth of uniform BaF 2 nanoscale thin films, through control of the deposition conditions. Our goal is to use the BaF 2 layers with controllable structure as component layers in layered optical nanocomposites. The structure of the BaF 2 nanolayer evolves as a function of the layer thickness: BaF 2 grows via a layer-by-layer growth mode on Al 2 O 3 ; the layers are amorphous for a thickness < 3 nm, and then become nanocrystalline as the layer thickness increases. The BaF 2 nanocrystals have an FCC crystal structure with a weak < 111 > texture that becomes stronger for thicker films. We then demonstrate that our BaF2 films can be introduced into layered Al 2 O 3 /BaF 2 /EuO x nanocomposite films, which allows for control of the relative position of the Eu ions and the BaF 2 layer. Cross-section samples of the multilayered films show interfacial intermixing between the layers, which is related to implantation during the PLD process. This intermixing enables the incorporation of Eu ions into BaF 2 layers and form a thin Eu-doped BaF 2 nanolayer at the interface. The layered nanocomposite films show photoluminescence (PL) emission from Eu 3+ ions, and the PL intensity changes can be correlated with the crystallinity and crystal size changes in the BaF 2 layer. Our results provide guidance for achieving thin film nanocomposite materials with controllable structure and photoluminescence behavior for light emitting diodes, photovoltaics and other optical applications.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Generation of multiple obstruction-free channels for free space optical communication

Multi-filament structures produced by vortical high-power femtosecond pulses propagating through clouds and fog can simultaneously clear two channels with cylindrical and annular profile. We present a method to achieve Free Space Optical (FSO) communications through such highly scattering media by propagating appropriately shaped laser modes through these channels. As a proof of concept, we implemented a Laguerre-Gaussian beam as information signal carrier to demonstrate transmission of 543-nm CW laser beam through a 1-m long cloud chamber using both channels. The low power of the information signal in this experiment allows considering applications in Earth–satellite FSO communication.

42 ENGINEERING↗