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At least 289 records · Page 16

Fluid Physics in a Fluctuating Acceleration Environment

Our program of research aims at developing a stochastic description of the residual acceleration field onboard spacecraft (g-jitter) to describe in quantitative detail its effect on fluid motion. Our main premise is that such a statistical description is necessary in those cases in which the characteristic time scales of the process under investigation are long compared with the correlation time of g-jitter. Although a clear separation between time scales makes this approach feasible, there remain several difficulties of practical nature: (i), g-jitter time series are not statistically stationary but rather show definite dependences on factors such as active or rest crew periods; (ii), it is very difficult to extract reliably the low frequency range of the power spectrum of the acceleration field. This range controls the magnitude of diffusive processes; and (iii), models used to date are Gaussian, but there is evidence that large amplitude disturbances occur much more frequently than a Gaussian distribution would predict. The lack of stationarity does not constitute a severe limitation in practice, since the intensity of the stochastic components changes very slowly during space missions (perhaps over times of the order of hours). A separate analysis of large amplitude disturbances has not been undertaken yet, but it does not seem difficult a priori to devise models that may describe this range better than a Gaussian distribution. The effect of low frequency components, on the other hand, is more difficult to ascertain, partly due to the difficulty associated with measuring them, and partly because they may be indistinguishable from slowly changing averages. This latter effect is further complicated by the lack of statistical stationarity of the time series. Recent work has focused on the effect of stochastic modulation on the onset of oscillatory instabilities as an example of resonant interaction between the driving acceleration and normal modes of the system, and on cavity flow as an example of how an oscillatory response under periodic driving becomes diffusive if the forcing is random instead. This paper describes three different topics that illustrate behavior that is peculiar to a stochastic acceleration field. In the first case, we show that g-jitter can induce effective attractive or repulsive forces between a pair of spherical particles that are suspended in an incompressible fluid of different density provided that the momentum diffusion length is larger than the interparticle separation (as in the case in most colloidal suspensions). Second, a stochastic modulation of the control parameter in the vicinity of a pitchfork or supercritical bifurcation is known not to affect the location of the threshold. We show, however, that resonance between the modulation and linearly stable modes close to onset can lead to a shift in threshold. Finally, we discuss the classical problem of vorticity diffusion away from a plane boundary that is being vibrated along its own plane. Periodic motion with zero average vorticity production results in an exponential decay of the vorticity away from the boundary. Random vibration, on the other hand, results in power law decay away from the boundary even if vorticity production averages to zero.

Drolet, Francois↗

Polariton-assisted incoherent to coherent excitation energy transfer between colloidal nanocrystal quantum dots

Here, we explore the dynamics of energy transfer between two nanocrystal quantum dots placed within an optical microcavity. By adjusting the coupling strength between the cavity photon mode and the quantum dots, we have the capacity to fine-tune the effective coupling between the donor and acceptor. Introducing a non-adiabatic parameter, γ, governed by the coupling to the cavity mode, we demonstrate the system’s capability to shift from the overdamped Förster regime (γ $\ll$ 1) to an underdamped coherent regime (γ $\gg$ 1). In the latter regime, characterized by swift energy transfer rates, the dynamics are influenced by decoherence time. To illustrate this, we study the exciton energy transfer dynamics between two closely positioned CdSe/CdS core/shell quantum dots with sizes and separations relevant to experimental conditions. Employing an atomistic approach, we calculate the excitonic level arrangement, exciton–phonon interactions, and transition dipole moments of the quantum dots within the microcavity. These parameters are then utilized to define a model Hamiltonian. Subsequently, we apply a generalized non-Markovian quantum Redfield equation to delineate the dynamics within the polaritonic framework.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Simulating sticky particles: A Monte Carlo method to sample a stratification

Many problems in materials science and biology involve particles interacting with strong, short-ranged bonds that can break and form on experimental timescales. Treating such bonds as constraints can significantly speed up sampling their equilibrium distribution, and there are several methods to sample probability distributions subject to fixed constraints. We introduce a Monte Carlo method to handle the case when constraints can break and form. More generally, the method samples a probability distribution on a stratification: a collection of manifolds of different dimensions, where the lower-dimensional manifolds lie on the boundaries of the higher-dimensional manifolds. We show several applications of the method in polymer physics, self-assembly of colloids, and volume calculation in high dimensions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Statics and dynamics of skyrmions interacting with disorder and nanostructures

Magnetic skyrmions are topologically stable nanoscale particlelike objects that were discovered in 2009. Since that time, intense research interest in the field has led to the identification of numerous compounds that support skyrmions over a range of conditions spanning from cryogenic to room temperatures. Skyrmions can be set into motion under various types of driving, and the combination of their size, stability, and dynamics makes them ideal candidates for numerous applications. At the same time, skyrmions represent a new class of system in which the energy scales of the skyrmion-skyrmion interactions, sample disorder, temperature, and drive can compete. A growing body of work indicates that the static and dynamic states of skyrmions can be influenced strongly by pinning or disorder in the sample; thus, an understanding of such effects is essential for the eventual use of skyrmions in applications. The current state of knowledge regarding individual skyrmions and skyrmion assemblies interacting with quenched disorder or pinning is reviewed. Additionally, the microscopic mechanisms for skyrmion pinning, including the repulsive and attractive interactions that can arise from impurities, grain boundaries, or nanostructures, are outlined. This is followed by descriptions of depinning phenomena, sliding states over disorder, the effect of pinning on the skyrmion Hall angle, the competition between thermal and pinning effects, the control of skyrmion motion using ordered potential landscapes such as one- or two-dimensional periodic asymmetric substrates, the creation of skyrmion diodes, and skyrmion ratchet effects. Highlighted are the distinctions arising from internal modes and the strong gyrotropic or Magnus forces that cause the dynamical states of skyrmions to differ from those of other systems with pinning, such as vortices in type-II superconductors, charge density waves, or colloidal particles. Throughout this review future directions and open questions related to the pinning and dynamics in skyrmion systems are also discussed.

36 MATERIALS SCIENCE↗

Grimsel Test Site - A Successful International Underground Research Laboratory for Many Decades - 20429

For more than 35 years, Nagra and its partners from around the world have been conducting underground research projects at the Grimsel Test Site (GTS, www.grimsel.com) to contribute to the development and confirmation of safe geological disposal concepts and for the characterization of suitable host rock formations. Over the years, the results of this internationally recognized research program have been, and continue to be, incorporated directly into exploration programs, modelling, safety, and engineering feasibility studies on options for deep geological repositories. Each project of the GTS program involves field-testing, laboratory studies, design and modelling tasks, and integrates all scientific and technical aspects. Each project phase is planned with a duration of three to five years to facilitate practical and administrative aspects and allow flexibility for updating the overall project plans with the latest findings. Scientific and engineering interaction among the different projects is ensured via an international steering committee meeting. Hosting an IAEA level C radiation- controlled zone, which allows use of radionuclides, including actinides such as thorium, uranium, neptunium, plutonium and americium, in in-situ experiments is one of the reasons why GTS also developed as a center of excellence for work with radioactive tracers under realistic in-situ boundary conditions. Last year, a new five-year program (2019 to 2023) started which includes projects with a planning horizon of decades. The new five-year program includes a new phase of in-situ experiments using radionuclides such as migration experiments in the Colloid Formation and Migration project (CFM), the Long-Term Diffusion experiment (LTD) and the newly established C-14 and I-129 Migration in cement project (CIM). The 'High Temperature effects on Bentonite' (HotBENT) project is starting in the current phase and is studying the effects of elevated temperatures (>175 deg. C) on bentonite materials. As a generic underground research laboratory (URL) it is expected that the GTS will provide in the coming years a platform for international collaboration, knowledge development and knowledge transfer for the next generation of scientists and engineers in the area of radioactive waste disposal and geosciences. A key role regarding knowledge transfer and training is provided by the well-established Grimsel Training Center (GTC), which (beside many URL related issues) also covers many general aspects of radioactive waste management. In this paper we provide an overview of the current program at the GTS, focusing on the experiments that study the migration of radionuclides through engineered barrier materials and the geosphere. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Amine-Assisted Ligand-Exchange Method to Enhance Photovoltaic Parameters in FAPbI3 Nanocrystal Solar Cells

Perovskite colloidal nanocrystals (PeNCs) have exceptional optoelectronic properties and phase stability, making them promising for photovoltaic applications. However, insulating ligands on PeNC surfaces limit the current density and reduce the power conversion efficiency (PCE) in PeNC solar cells (SCs). This study introduces an amine-assisted ligand-exchange (ALE) strategy using 3-phenyl-1-propylamine (3P1P) to effectively remove long ligands from PeNC films. ALE reduced long-chain ligand density without increasing the number of defect states and therefore reduced the exciton-binding energy of FAPbI3 NC films. These changes facilitated exciton dissociation and charge transport in FAPbI3 PeNC SCs. The facilitation of exciton dissociation was due to the increased magnetic dipole interaction between excitons after the ALE process. The use of ALE achieved FAPbI3 PeNC SCs that had an improved short-circuit current density of 17.98 mA/cm2 and a PCE of 15.56% with improved stability after the treatment and negligible hysteresis. This work provides new insight into engineering PeNC films.

amines↗

Open and Close-Packed, Shape-Engineered Polygonal Nanoparticle Metamolecules with Tailorable Fano Resonances

In this study, a top-down lithographic patterning and deposition process is reported for producing nanoparticles (NPs) with well-defined sizes, shapes, and compositions that are often not accessible by wet-chemical synthetic methods. These NPs are ligated and harvested from the substrate surface to prepare colloidal NP dispersions. Using a template-assisted assembly technique, fabricated NPs are driven by capillary forces to assemble into size- and shape-engineered templates and organize into open or close-packed multi-NP structures or NP metamolecules. The sizes and shapes of the NPs and of the templates control the NP number, coordination, interparticle gap size, disorder, and location of defects such as voids in the NP metamolecules. The plasmonic resonances of polygonal-shaped Au NPs are exploited to correlate the structure and optical properties of assembled NP metamolecules. Comparing open and close-packed architectures highlights that introduction of a center NP to form close-packed assemblies supports collective interactions, altering magnetic optical modes and multipolar interactions in Fano resonances. Decreasing the distance between NPs strengthens the plasmonic coupling, and the structural symmetries of the NP metamolecules determine the orientation-dependent scattering response.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Optical and Magneto-Optical Properties of Donor-Bound Excitons in Vacancy-Engineered Colloidal Nanocrystals

Controlled insertion of electronic states within the band gap of semiconductor nanocrystals (NCs) is a powerful tool for tuning their physical properties. One compelling example is II–VI NCs incorporating heterovalent coinage metals in which hole capture produces acceptor-bound excitons. To date, the opposite donor-bound exciton scheme has not been realized because of the unavailability of suitable donor dopants. Here, we produce a model system for donor-bound excitons in CdSeS NCs engineered with sulfur vacancies (V S ) that introduce a donor state below the conduction band (CB), resulting in long-lived intragap luminescence. V S -localized electrons are almost unaffected by trapping, and suppression of thermal quenching boosts the emission efficiency to 85%. Magneto-optical measurements indicate that the V S are not magnetically coupled to the NC bands and that the polarization properties are determined by the spin of the valence-band photohole, whose spin flip is massively slowed down due to suppressed exchange interaction with the donor-localized electron.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Improved Fundamental Understanding of Aluminum Chemistry and Interactions of Aluminate Anion with Co-Anions: ORNL Project Progress Report

The U.S. Department of Energy (DOE)’s Hanford Site in Washington State houses 177 underground storage tanks containing millions of gallons of nuclear and chemical waste with high aluminum content. Aluminum (Al) salt reactions with strong bases produce aluminum hydroxides, like boehmite (γ-AlOOH), which are main components of insoluble nuclear waste sludge. Understanding the morphology, crystallinity, and dissolution behavior of boehmite under waste tank conditions is necessary for improving waste management and mitigation strategies. The ORNL team uses in situ multimodal analysis strategy to study Al chemistry of simulated tank waste using microfluidic reactors and advanced chemical imaging and mass spectrometry (MS) techniques. Because the SALVI device is vacuum compatible and transferrable among different platforms, we can use it in scanning electron microscopy (SEM), vacuum ultraviolet single photon mass spectrometry (VUV SPI-MS), and time-of-flight secondary ion mass spectrometry (ToF-SIMS) to study the chemical speciation and colloid stability in liquids in this project. Additionally, ex situ transmission electron microscopy (TEM) and x-ray diffraction (XRD) spectroscopy can be used to verify particle phase to further the understanding of the Al-bearing phases. This report gives a summary of the technical progress of the ORNL tasks. A plan for year 2 performance is recommended in the summary.

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Intrinsic and Extrinsic Exciton Recombination Pathways in AgInS 2 Colloidal Nanocrystals

Ternary I-III-VI 2 nanocrystals (NCs), such as AgInS 2 and CuInS 2 , are garnering interest as heavy-metal-free materials for photovoltaics, luminescent solar concentrators, LEDs, and bioimaging. The origin of the emission and absorption properties in this class of NCs is still a subject of debate. Recent theoretical and experimental studies revealed that the characteristic Stokes-shifted and long-lived luminescence of stoichiometric CuInS 2 NCs arises from the detailed structure of the valence band featuring two sublevels with different parity. The same valence band substructure is predicted to occur in AgInS 2 NCs, yet no experimental confirmation is available to date. Here, we use complementary spectroscopic, spectro-electrochemical, and magneto-optical investigations as a function of temperature to investigate the band structure and the excitonic recombination mechanisms in stoichiometric AgInS 2 NCs. Transient transmission measurements reveal the signatures of two subbands with opposite parity, and photoluminescence studies at cryogenic temperatures evidence a dark state emission due to enhanced exchange interaction, consistent with the behavior of stoichiometric CuInS 2 NCs. Lowering the temperature as well as applying reducing electrochemical potentials further suppress electron trapping, which represents the main nonradiative channel for exciton decay, leading to nearly 100% emission efficiency.

36 MATERIALS SCIENCE↗

Gate-Tunable Single Terahertz Meta-Atom Ultrastrong Light-Matter Coupling

We study the electrical tunability of ultrastrong light-matter interactions between a single terahertz circuit-based complementary split ring resonator (cSRR) and a two-dimensional electron gas. For this purpose, transmission spectroscopy measurements are performed under the influence of a strong magnetic field at different set points for the electric gate bias. The resulting Landau polariton dispersion depends on the applied electric bias, as the gating technique confines the electrons in-plane down to extremely subwavelength dimensions as small as d = 410 nm. This confinement allows for the excitation of standing plasma waves at zero magnetic field and an effective tunability of the electron number coupled to the THz resonator. This allows the normalized coupling strength to be tuned in situ from η = 0.46 down to η = 0.18. This is the first demonstration of terahertz far-field spectroscopy of an electrically tunable interaction between a single terahertz resonator and electrons in a GaAs quantum well heterostructure.

Landau levels↗

Magnetic Vortex and Hyperthermia Suppression in Multigrain Iron Oxide Nanorings

Single-crystal iron oxide nanorings have been proposed as a promising candidate for magnetic hyperthermia application because of their unique shape-induced vortex-domain structure, which supports good colloidal stability and enhanced magnetic properties. However, the synthesis of single crystalline iron oxide has proven to be challenging. In this article, we showed that chemically synthesized multigrain magnetite nanorings disfavor a shape-induced magnetic vortex-domain structure. Our results indicate that the multigrain Fe 3 O 4 nanorings with an average outer diameter of ~110 nm and an inner to outer diameter ratio of ~0.5 do not show a shape-induced vortex-domain structure, which was observed in the single-crystal Fe 3 O 4 nanorings of similar dimensions. At 300 Ks, multigrain magnetite nanorings showed an effective anisotropy field of 440 Oe, which can be attributed to its high surface area and intraparticle interaction. Both calorimetric and AC loop measurements showed a moderate inductive heating efficiency of multigrain magnetite nanorings of ~300 W/g at 800 Oe. Our results shed light on the magnetic ground states of chemically synthesized multigrain Fe 3 O 4 nanorings.

36 MATERIALS SCIENCE↗

Self-assembly of a triply periodic continuous mesophase with Fddd symmetry in simple one-component liquids

Triply periodic continuous morphologies (networks) arising as a result of the microphase separation in block copolymer melts have so far never been observed self-assembled in systems of particles with spherically symmetric interaction. Here, we report a molecular dynamics simulation where two simple one-component liquids form upon cooling an equilibrium network with the Fddd space group symmetry. This complexity reduction in the liquid network formation in terms of the particle geometry and the number of components evidences the generic nature of this class of phase transition suggesting opportunities for producing these structures in a variety of new systems.

36 MATERIALS SCIENCE↗

Quantitative Protein Corona Composition and Dynamics on Carbon Nanotubes in Biological Environments

When nanoparticles enter biological environments, proteins adsorb to form the "protein corona" which alters nanoparticle biodistribution and toxicity. Herein, we measure protein corona formation on DNA-functionalized single-walled carbon nanotubes (ssDNA-SWCNTs), a nanoparticle used widely for sensing and delivery, in blood plasma and cerebrospinal fluid. We characterize corona composition by mass spectrometry, revealing high-abundance corona proteins involved in lipid binding, complement activation, and coagulation. We investigate roles of electrostatic and entropic interactions driving selective corona formation. Lastly, we study real-time protein binding on ssDNA-SWCNTs, obtaining agreement between enriched proteins binding strongly and depleted proteins binding marginally, while highlighting cooperative adsorption mechanisms. Knowledge of protein corona composition, formation mechanisms, and dynamics informs nanoparticle translation from in vitro design to in vivo application.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Combustion, Complex Fluids, and Fluid Physics Experiments on the ISS

From the very early days of human spaceflight, NASA has been conducting experiments in space to understand the effect of weightlessness on physical and chemically reacting systems. NASA Glenn Research Center (GRC) in Cleveland, Ohio has been at the forefront of this research looking at both fundamental studies in microgravity as well as experiments targeted at reducing the risks to long duration human missions to the moon, Mars, and beyond. In the current International Space Station (ISS) era, we now have an orbiting laboratory that provides the highly desired condition of long-duration microgravity. This allows continuous and interactive research similar to Earth-based laboratories. Because of these capabilities, the ISS is an indispensible laboratory for low gravity research. NASA GRC has been actively involved in developing and operating facilities and experiments on the ISS since the beginning of a permanent human presence on November 2, 2000. As the lead Center for combustion, complex fluids, and fluid physics; GRC has led the successful implementation of the Combustion Integrated Rack (CIR) and the Fluids Integrated Rack (FIR) as well as the continued use of other facilities on the ISS. These facilities have supported combustion experiments in fundamental droplet combustion; fire detection; fire extinguishment; soot phenomena; flame liftoff and stability; and material flammability. The fluids experiments have studied capillary flow; magneto-rheological fluids; colloidal systems; extensional rheology; pool and nucleate boiling phenomena. In this paper, we provide an overview of the experiments conducted on the ISS over the past 12 years.

Motil, Brian↗

Combustion, Complex Fluids, and Fluid Physics Experiments on the ISS

From the very first days of human spaceflight, NASA has been conducting experiments in space to understand the effect of weightlessness on physical and chemically reacting systems. NASA Glenn Research Center (GRC) in Cleveland, Ohio has been at the forefront of this research looking at both fundamental studies in microgravity as well as experiments targeted at reducing the risks to long duration human missions to the moon, Mars, and beyond. In the current International Space Station (ISS) era, we now have an orbiting laboratory that provides the highly desired condition of long-duration microgravity. This allows continuous and interactive research similar to Earth-based laboratories. Because of these capabilities, the ISS is an indispensible laboratory for low gravity research. NASA GRC has been actively involved in developing and operating facilities and experiments on the ISS since the beginning of a permanent human presence on November 2, 2000. As the lead Center both Combustion, Fluid Physics, and Acceleration Measurement GRC has led the successful implementation of an Acceleration Measurement systems, the Combustion Integrated Rack (CIR), the Fluids Integrated Rack (FIR) as well as the continued use of other facilities on the ISS. These facilities have supported combustion experiments in fundamental droplet combustion fire detection fire extinguishment soot phenomena flame liftoff and stability and material flammability. The fluids experiments have studied capillary flow magneto-rheological fluids colloidal systems extensional rheology pool and nucleate boiling phenomena. In this paper, we provide an overview of the experiments conducted on the ISS over the past 12 years. We also provide a look to the future development. Experiments presented in combustion include areas such as droplet combustion, gaseous diffusion flames, solid fuels, premixed flame studies, fire safety, and super critical oxidation processes. In fluid physics, experiments are discussed in multiphase flows, capillary phenomena, and heat pipes. Finally in complex fluids, experiments in rheology and soft condensed materials will be presented.

Motil, Brian↗

Nanoparticle Superlattices through Template-Encoded DNA Dendrimers

The chemical interactions that lead to the emergence of hierarchical structures are often highly complex and difficult to program. In this paper, the synthesis of a series of superlattices based upon 30 different structurally reconfigurable DNA dendrimers is reported, each of which presents a well-defined number of single-stranded oligonucleotides (i.e., sticky ends) on its surface. Such building blocks assemble with complementary DNA-functionalized gold nanoparticles (AuNPs) to yield five distinct crystal structures, depending upon choice of dendrimer and defined by phase symmetry. These DNA dendrimers can associate to form micelle-dendrimers, whereby the extent of association can be modulated based upon surfactant concentration and dendrimer length to produce a low-symmetry Ti5Ga4-type phase that has yet to be reported in the field of colloidal crystal engineering. Taken together, colloidal crystals that feature three different types of particle bonding interactions.template-dendron, dendrimer-dendrimer, and DNA-modified AuNP-dendrimer.are reported, illustrating how sequence-defined recognition and dynamic association can be combined to yield complex hierarchical materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗