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DOE OSTI2019

Probing Trions at Chemically Tailored Trapping Defects

Trions, charged excitons that are reminiscent of hydrogen and positronium ions, have been intensively studied for energy harvesting, light-emitting diodes, lasing, and quantum computing applications because of their inherent connection with electron spin and dark excitons. However, these quasi-particles are typically present as a minority species at room temperature making it difficult for quantitative experimental measurements. Here, we show that by chemically engineering the well depth of sp 3 quantum defects through a series of alkyl functional groups covalently attached to semiconducting carbon nanotube hosts, trions can be efficiently generated and localized at the trapping chemical defects. The exciton-electron binding energy of the trapped trion approaches 119 meV, which more than doubles that of “free” trions in the same host material (54 meV) and other nanoscale systems (2–45 meV). Magnetoluminescence spectroscopy suggests the absence of dark states in the energetic vicinity of trapped trions. Unexpectedly, the trapped trions are approximately 7.3-fold brighter than the brightest previously reported and 16 times as bright as native nanotube excitons, with a photoluminescence lifetime that is more than 100 times larger than that of free trions. These intriguing observations are understood by an efficient conversion of dark excitons to bright trions at the defect sites. This work makes trions synthetically accessible and uncovers the rich photophysics of these tricarrier quasi-particles, which may find broad implications in bioimaging, chemical sensing, energy harvesting, and light emitting in the short-wave infrared.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Effects of turbulent diffusion and back-reaction on the dust distribution around two resonant planets

In evolved and dusty circumstellar discs, two planets with masses comparable to Jupiter and Saturn that migrate outwards while maintaining an orbital resonance can produce distinctive features in the dust distribution. Dust accumulates at the outer edge of the common gas gap, which behaves as a dust trap, where the local dust concentration is significantly enhanced by the planets’ outward motion. Concurrently, an expanding cavity forms in the dust distribution inside the planets’ orbits, because dust does not filter through the common gaseous gap and grain depletion in the region continues via inward drifting. There is no cavity in the gas distribution because gas can filter through the gap, although ongoing gas accretion on the planets can reduce the gas density in the inner disc. Such behaviour was demonstrated by means of simulations neglecting the effects of dust diffusion due to turbulence and of dust backreaction on the gas. Both effects may alter the formation of the dust peak at the gap outer edge and of the inner dust cavity, by letting grains filter through the dust trap. We performed high-resolution hydrodynamical simulations of the coupled evolution of gas and dust species, the latter treated as pressureless fluids, in the presence of two giant planets. We show that diffusion and backreaction can change some morphological aspects of the dust distribution but do not alter some main features, such as the outer peak and the expanding inner cavity. Furthermore, these findings are confirmed for different parametrizations of gas viscosity.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2017

Infusion of hydrogen into nanostructured bainitic steel

Highlights: • Results show that austenite is more effective in trapping hydrogen than α/γ interfaces. • The H desorption behaviour was accurately reproduced with local equilibrium model. • The trapping capacity of retained austenite originates from the austenite lattice sites. - Abstract: The trapping of hydrogen in nanostructured bainitic steel has been investigated using thermal desorption analysis, in order to determine the potency of the ferrite-retained austenite (α/γ) interfaces and retained austenite as trapping sites. Thermal desorption data showed that the volume of retained austenite is more effective in trapping hydrogen than the interfaces. There is a close correlation between the quantity of hydrogen and the retained austenite content rather than the density of interfaces. A local equilibrium model was able to reproduce the hydrogen desorption behaviour of saturated and unsaturated samples considering both retained austenite and α/γ interfaces as the trapping sites. A trap binding energy ranging from 47 to 52 kJ/mol was estimated for retained austenite, suggesting that the observed trapping capacity originates from the austenite lattice sites.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Trapped fast particle destabilization of internal kink mode for the locally flattened q-profile with an inflection point

The destabilization of ideal internal kink modes by trapped fast particles in tokamak plasmas with a “shoulder”-like equilibrium current is investigated. It is found that energetic particle branch of the mode is unstable with the driving of fast-particle precession drifts and corresponds to a precessional fishbone. The mode with a low stability threshold is also more easily excited than the conventional precessional fishbone. This is different from earlier studies for the same equilibrium in which the magnetohydrodynamic (MHD) branch of the mode is stable. Furthermore, the stability and characteristic frequency of the mode are analyzed by solving the dispersion relation and comparing with the conventional fishbone. The results suggest that an equilibrium with a locally flattened q-profile, may be modified by localized current drive (or bootstrap current, etc.), is prone to the onset of the precessional fishbone branch of the mode.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Observation of quenching-induced magnetic flux trapping using a magnetic field and temperature mapping system

Highly efficient superconducting radio-frequency cavities exhibit low heat loss and are used as components in accelerators and superconducting devices due to their high Q-values. The precise location of magnetic flux trapping in cavities is necessary to identify its effects on the performance of superconducting cavities. In this study, we report a new combined mapping system to measure the temperature and magnetic field on the equator. The proposed system comprehensively maps local magnetic field changes as magnetic flux trapping due to quenching. Our experimental results show that magnetic flux trapping due to quenching increases the local surface resistance of superconducting cavities at 2 K. Thus, the proposed system elucidates the relationship between local flux trapping due to quenching and surface resistance in superconducting cavities and highlights the effect of quenching on the surface resistance. This system can aid in the development of superconducting cavities with higher Q values.

43 PARTICLE ACCELERATORS↗

DOE OSTI2017

Intermediate-Scale Experimental Study to Improve Fundamental Understanding of Attenuation Capacity for Leaking CO 2 in Heterogeneous Shallow Aquifers

In order to assess the risks of Geologic Carbon Sequestration (GCS), it is crucial to understand the fundamental physicochemical processes that may occur if and when stored CO 2 leaks upward from a deep storage reservoir into the shallow subsurface. Intermediate-scale experiments allow for improved understanding of the multiphase evolution processes that control CO 2 migration behaviour in the subsurface, because the boundary conditions, initial conditions, and porous media parameters can be better controlled and monitored in the laboratory than in field settings. For this study, a large experimental test bed was designed to mimic a cross-section of a shallow aquifer with layered geologic heterogeneity. As water with aqueous CO 2 was injected into the system to mimic a CO 2 -charged water leakage scenario, the spatiotemporal evolution of the multiphase CO 2 plume was monitored. Similar experiments were performed with two different sand combinations to assess the relative effects of different types of geologic facies transitions on the CO 2 evolution processes. Significant CO 2 attenuation was observed in both scenarios, but by fundamentally different mechanisms. When the porous media layers had very different permeabilities, attenuation was caused by local accumulation (structural trapping) and slow re-dissolution of gas phase CO 2 . When the permeability difference between the layers was relatively small, on the other hand, gas phase continually evolved over widespread areas near the leading edge of the aqueous plume, which also attenuated CO 2 migration. In conclusion, this improved process understanding will aid in the development of models that could be used for effective risk assessment and monitoring programs for GCS projects.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Charged particle dynamics near an X-point of a non-symmetric magnetic field with closed field lines

Understanding particle drifts in a non-symmetric magnetic field is of primary interest in designing optimized stellarators in order to minimize the neoclassical radial loss of particles. Quasisymmetry and omnigeneity, two distinct properties proposed to ensure radial localization of collisionless trapped particles in stellarators, have been explored almost exclusively for magnetic fields with nested flux surfaces. In this work, we examine radial particle confinement when all field lines are closed. We then study charged particle dynamics in the special case of a non-symmetric vacuum magnetic field with closed field lines obtained recently by Weitzner & Sengupta ( Phys. Plasmas , vol. 27, 2020, 022509). These magnetic fields can be used to construct magnetohydrodynamic equilibria for low pressure. Expanding in the amplitude of the non-symmetric fields, we explicitly evaluate the omnigeneity and quasisymmetry constraints. We show that the magnetic field is omnigeneous in the sense that the drift surfaces coincide with the pressure surfaces. However, it is not quasisymmetric according to the standard definitions.

Physics↗

DOE OSTI2018

Conduction of Metal–Thin Organic Film–Metal Junctions at Low Bias

A model for the low bias electric conductance of junctions, consisting of a thin organic film (TOF) positioned between two metallic electrodes (M), has been created. In contrast with other theoretical studies, the proposed model relies on the energy band picture of M–TOF–M systems. Theoretical analysis of the band-like transport has shown that the electronic flow between metallic electrodes can exist in M–TOF–M junctions only if injected charge carriers are able to overcome the potential barrier with the thickness-dependent height. Such an obstacle to the motion of injected charges in the TOF conduction band arises due to the bending of this band caused by carriers localized in structural traps. Two regimes of the zero bias conductance of M–TOF–M junctions have been studied theoretically for situations, where charges overcome the thickness-dependent barrier undergoing either thermally activated or tunneling transitions. Analytical expressions derived for the zero bias conduction in these two regimes enable us to specify key physical parameters controlling charge transport across the film and provide results consistent with observations. On the basis of our findings, we infer that thermally activated and tunneling conductances can be distinguished by temperature and thickness dependencies. Theoretical results obtained for the electric conductance of M–TOF–M systems in the tunneling regime are compared with those obtained for assemblies in which TOF has been replaced by a single molecule. Furthermore, distinctions between transport properties of these two systems and their similarities resulting from the present model are reported on.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Point Defects in Two-Dimensional Ruddlesden–Popper Perovskites Explored with Ab Initio Calculations

Two-dimensional Ruddlesden–Popper (RP) halide perovskites stand out as excellent layered materials with favorable optoelectronic properties for efficient light-emitting, spintronic, and other spin-related applications. However, properties often determined by defects are not well understood in these perovskite systems. This work investigates the ground state electronic structure of commonly formed defects in a typical RP perovskite structure by density functional theory. Our study reveals that these 2D perovskites generally retain their defect tolerance with limited perturbation of the electronic structure in the case of neutral-type point defects. In contrast, donor/acceptor defects induce deep midgap states, potentially causing harm to the material’s electronic performance. To retain positive intrinsic properties, the halide vacancies and interstitial defects should be avoided. The observed strong electron localization results in trap states and consequently leads to reduced device performance. Finally, this understanding can guide experimental efforts that aim for improved 2D halide perovskite-based device performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Machine learning the metastable phase diagram of covalently bonded carbon

Abstract Conventional phase diagram generation involves experimentation to provide an initial estimate of the set of thermodynamically accessible phases and their boundaries, followed by use of phenomenological models to interpolate between the available experimental data points and extrapolate to experimentally inaccessible regions. Such an approach, combined with high throughput first-principles calculations and data-mining techniques, has led to exhaustive thermodynamic databases (e.g. compatible with the CALPHAD method), albeit focused on the reduced set of phases observed at distinct thermodynamic equilibria. In contrast, materials during their synthesis, operation, or processing, may not reach their thermodynamic equilibrium state but, instead, remain trapped in a local (metastable) free energy minimum, which may exhibit desirable properties. Here, we introduce an automated workflow that integrates first-principles physics and atomistic simulations with machine learning (ML), and high-performance computing to allow rapid exploration of the metastable phases to construct “metastable” phase diagrams for materials far-from-equilibrium. Using carbon as a prototypical system, we demonstrate automated metastable phase diagram construction to map hundreds of metastable states ranging from near equilibrium to far-from-equilibrium (400 meV/atom). We incorporate the free energy calculations into a neural-network-based learning of the equations of state that allows for efficient construction of metastable phase diagrams. We use the metastable phase diagram and identify domains of relative stability and synthesizability of metastable materials. High temperature high pressure experiments using a diamond anvil cell on graphite sample coupled with high-resolution transmission electron microscopy (HRTEM) confirm our metastable phase predictions. In particular, we identify the previously ambiguous structure of n -diamond as a cubic-analog of diaphite-like lonsdaelite phase.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Controlled release of entrapped nanoparticles from thermoresponsive hydrogels with tunable network characteristics

Thermoresponsive hydrogels have been studied intensively for creating smart drug carriers and controlled drug delivery. Understanding the drug release kinetics and corresponding transport mechanisms of nanoparticles (NPs) in a thermoresponsive hydrogel network is the key to the successful design of smart drug delivery systems. Here, we construct a mesoscopic model of rigid NPs entrapped in a hydrogel network in an aqueous solution, where the hydrogel network is formed by cross-linked semiflexible polymers of thermoresponsive poly(N-isopropylacrylamide) (PNIPAM). By varying the temperature crossing the lower critical solution temperature of PNIPAM, we can significantly change the hydrogel network characteristics. We systematically investigate how the matrix porosity and the nanoparticle size affect the transport kinetics of NPs at different temperatures. Quantitative results on the mean-squared displacement and the van Hove displacement distributions of NPs show that all NPs entrapped in the smart hydrogels undergo subdiffusion at both low and high temperatures. For a coil state, the transport of NPs in the hydrogels can be enhanced by decreasing the matrix porosity of the polymer network and NPs' size. However, when the solution temperature is increased above the critical temperature, the hydrogel network collapses following the coil-to-globule transition, with the NPs tightly trapped in some local regions inside the hydrogels. Consequently, the NP diffusion coefficient can be reduced by two orders of magnitude, or the diffusion processes can even be completely stopped. These findings provide new insights for designing controlled drug release from stimuli-responsive hydrogels, including autonomously switch on/off drug release in response to physical and chemical stimuli.

42 ENGINEERING↗

DOE OSTI2023

Spectral widths and Stokes shifts in InP-based quantum dots

InP-based quantum dots (QDs) have Stokes shifts and photoluminescence (PL) line widths that are larger than in II–VI semiconductor QDs with comparable exciton energies. The mechanisms responsible for these spectral characteristics are investigated in this paper. Upon comparing different semiconductors, we find the Stokes shift decreases in the following order: InP > CdTe > CdSe. We also find that the Stokes shift decreases with core size and decreases upon deposition of a ZnSe shell. We suggest that the Stokes shift is largely due to different absorption and luminescent states in the angular momentum fine structure. The energy difference between the fine structure levels, and hence the Stokes shifts, are controlled by the electron–hole exchange interaction. Luminescence polarization results are reported and are consistent with this assignment. Spectral widths are controlled by the extent of homogeneous and inhomogeneous broadening. Here, we report PL and PL excitation (PLE) spectra that facilitate assessing the roles of homogeneous and different inhomogeneous broadening mechanisms in the spectra of zinc-treated InP and InP/ZnSe/ZnS particles. There are two distinct types of inhomogeneous broadening: size inhomogeneity and core–shell interface inhomogeneity. The latter results in a distribution of core–shell band offsets and is caused by interfacial dipoles associated with In–Se or P–Zn bonding. Quantitative modeling of the spectra shows that the offset inhomogeneity is comparable to but somewhat smaller than the size inhomogeneity. The combination of these two types of inhomogeneity also explains several aspects of reversible hole trapping dynamics involving localized In 3+ /V Zn 2– impurity states in the ZnSe shells.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Amplification of primordial perturbations from the rise or fall of the inflaton

The next generation of cosmic microwave background, gravitational wave, and large scale structure, experiments will provide an unprecedented opportunity to probe the primordial power spectrum on small scales. An exciting possibility for what lurks on small scales is a sharp rise in the primordial power spectrum: this can lead to the formation of primordial black holes, providing a dark matter candidate or the black holes observed by the LIGO-Virgo collaboration. In this study we develop a mechanism for the amplification of the small-scale primordial power spectrum, in the context of single-field inflation with a step-like feature in the inflaton potential. Specifically, we consider both the upward and the downward step in the potential. We also discuss the possibility of the strong coupling between perturbations because the rapid changes of the potential derivatives with the time-dependent field value, caused by the step-like feature, could make the coupling stronger. As a result, we find that the perturbations can remain weakly coupled yet sufficiently enhanced if the step realizes the rapid changes of the potential derivatives in some fraction of an e-fold, Script O(P R 1/2) ≲ ΔN < 1, where P R is the power spectrum of the curvature perturbation at that time. We also discuss the PBH formation rate from the inflaton trapping at the local minimum, which can occur in the potential with an upward step.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2020

Data optimization for large batch distributed training of deep neural networks

Distributed training in deep learning (DL) is common practice as data and models grow. The current practice for distributed training of deep neural networks faces the challenges of communication bottlenecks when operating at scale, and model accuracy deterioration with an increase in global batch size. Present solutions focus on improving message exchange efficiency as well as implementing techniques to tweak batch sizes and models in the training process. The loss of training accuracy typically happens because the loss function gets trapped in a local minima. We observe that the loss landscape minimization is shaped by both the model and training data and propose a data optimization approach that utilizes machine learning to implicitly smooth out the loss landscape resulting in fewer local minima. Our approach filters out data points which are less important to feature learning, enabling us to speed up the training of models on larger batch sizes to improved accuracy.

Gahlot, Shubhankar↗

DOE OSTI2016

WE-AB-209-09: Optimization of Rotational Arc Station Parameter Optimized Radiation Therapy

Purpose: To develop a fast optimization method for station parameter optimized radiation therapy (SPORT) and show that SPORT is capable of improving VMAT in both plan quality and delivery efficiency. Methods: The angular space from 0° to 360° was divided into 180 station points (SPs). A candidate aperture was assigned to each of the SPs based on the calculation results using a column generation algorithm. The weights of the apertures were then obtained by optimizing the objective function using a state-of-the-art GPU based Proximal Operator Graph Solver (POGS) within seconds. Apertures with zero or low weight were thrown out. To avoid being trapped in a local minimum, a stochastic gradient descent method was employed which also greatly increased the convergence rate of the objective function. The above procedure repeated until the plan could not be improved any further. A weighting factor associated with the total plan MU also indirectly controlled the complexities of aperture shapes. The number of apertures for VMAT and SPORT was confined to 180. The SPORT allowed the coexistence of multiple apertures in a single SP. The optimization technique was assessed by using three clinical cases (prostate, H&N and brain). Results: Marked dosimetric quality improvement was demonstrated in the SPORT plans for all three studied cases. Prostate case: the volume of the 50% prescription dose was decreased by 22% for the rectum. H&N case: SPORT improved the mean dose for the left and right parotids by 15% each. Brain case: the doses to the eyes, chiasm and inner ears were all improved. SPORT shortened the treatment time by ∼1 min for the prostate case, ∼0.5 min for brain case, and ∼0.2 min for the H&N case. Conclusion: The superior dosimetric quality and delivery efficiency presented here indicates that SPORT is an intriguing alternative treatment modality.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2016

Optimization of rotational arc station parameter optimized radiation therapy

Purpose: To develop a fast optimization method for station parameter optimized radiation therapy (SPORT) and show that SPORT is capable of matching VMAT in both plan quality and delivery efficiency by using three clinical cases of different disease sites. Methods: The angular space from 0° to 360° was divided into 180 station points (SPs). A candidate aperture was assigned to each of the SPs based on the calculation results using a column generation algorithm. The weights of the apertures were then obtained by optimizing the objective function using a state-of-the-art GPU based proximal operator graph solver. To avoid being trapped in a local minimum in beamlet-based aperture selection using the gradient descent algorithm, a stochastic gradient descent was employed here. Apertures with zero or low weight were thrown out. To find out whether there was room to further improve the plan by adding more apertures or SPs, the authors repeated the above procedure with consideration of the existing dose distribution from the last iteration. At the end of the second iteration, the weights of all the apertures were reoptimized, including those of the first iteration. The above procedure was repeated until the plan could not be improved any further. The optimization technique was assessed by using three clinical cases (prostate, head and neck, and brain) with the results compared to that obtained using conventional VMAT in terms of dosimetric properties, treatment time, and total MU. Results: Marked dosimetric quality improvement was demonstrated in the SPORT plans for all three studied cases. For the prostate case, the volume of the 50% prescription dose was decreased by 22% for the rectum and 6% for the bladder. For the head and neck case, SPORT improved the mean dose for the left and right parotids by 15% each. The maximum dose was lowered from 72.7 to 71.7 Gy for the mandible, and from 30.7 to 27.3 Gy for the spinal cord. The mean dose for the pharynx and larynx was reduced by 8% and 6%, respectively. For the brain case, the doses to the eyes, chiasm, and inner ears were all improved. SPORT shortened the treatment time by ∼1 min for the prostate case, ∼0.5 min for brain case, and ∼0.2 min for the head and neck case. Conclusions: The dosimetric quality and delivery efficiency presented here indicate that SPORT is an intriguing alternative treatment modality. With the widespread adoption of digital linac, SPORT should lead to improved patient care in the future.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2021

Raman Spectroscopy to Detect and Measure NOW Pheromones. Annual Report [Jan 2021]

47 OTHER INSTRUMENTATION↗

DOE OSTI2021

Advancing Enhanced Raman Spectroscopy to Detect and Measure NOW Pheromones (CPRB 2022 proposal)

Insect sex pheromones are chemical compounds that insects release to attract their partners over distances of hundreds of meters or even kilometers, in complete darkness and without any audible signals. Use of synthetic forms of key compounds have in some cases become an essential component of monitoring and/or managing key pests of agricultural crops, including navel orangeworm (Amyelois transitella) (NOW) in California tree nuts. These pheromone-based strategies can include monitoring, mating disruption, mass trapping, attract-and-kill and push-pull. There are currently multiple commercially available mating disruption products available for NOW and recent studies have demonstrated that they can be effectively used to reduce crop damage by this pest. Just how mating disruption works is not fully established and likely varies across products and target species. For instance, the extent to which synthetic pheromones compete with natural pheromone is not well understood, or in the case of monitoring, how efficaciously the insect follows the diffusing plumes, especially across large blocks and at plot borders. Furthermore, there may be specific conditions under which poor or impeded diffusion of synthetic pheromone diminishes the disruption effect, which could result in some males effectively locating females for reproduction. At the same time, many commercially available synthetic lures are also available, and growers have been effectively using them to track population development – although the attractive range of these lures remains unclear. That is, while pheromone lures can attract many moths, the relationship between trap capture and local populations, much less crop damage, remains unclear. Regardless of the emission source (aerosol puffers, meso emitters, lures etc.), we currently lack the ability to fully understand how these synthetic pheromone compounds diffuse away from their point-source of emission – and subsequently how this might affect the efficacy of mating disruption and/or the accuracy of monitoring efforts. Raman spectroscopy (RS) may offer a means to detect synthetic pheromone because of its analytical properties and recent technological advancements. In combination with nanostructured probes, RS has a demonstrated capability to detect volatiles at extremely low concentrations. While other methods for detecting pheromones have proven to be successful, such analytical methods like mass spectrometry (MS) gas chromatography (GC) require sampling in the fields and are not real-time. Other methods such as EAG/ EAD are also invasive (use antennas) but are of course valuable. Opto-electronic, micro and nano sensors just recently enticed interest. We fall in this latter category, proposing the use of optical spectroscopy (Raman) in a fiber aided by nanostructures to provide a chemical fingerprint without transductions and in real-time (i.e. no sampling). To date, we have been able to generate Raman signatures for the main chemicals in synthetic pheromones (a first for science, to the best of our knowledge), observe their trends at different concentrations, and also provide a clear distinction of such signatures in mixed samples via Principal Component Analysis (PCA) – all of which strengthens our conclusions on the ability of RS to detect emissions in more realistic conditions. We also established processes to enhance the detection sensitivity via preconcentration with Solid Phase Micro Extraction (SPME) fibers and Surface Enhanced Raman Spectroscopy (SERS) to increase the overall optical signals. Furthermore, we explored limitations and requirements for detecting from dispensers, lures, or live moths, including Dept. of Energy and CA State regulatory approvals. Finally, we setup some of our first “orchard in a box” experiments to measure pheromone diffusion along with developing appropriate models.

42 ENGINEERING↗