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At least 109 records · Page 6

Black Carbon in Estuarine and Coastal Ocean Dissolved Organic Matter

Black carbon (BC) in ultrafiltered high-molecular-weight DOM (UDOM) was measured in surface waters of Delaware Bay, Chesapeake Bay and the adjacent Atlantic Ocean (USA) to ascertain the importance of riverine and estuarine DOM as a source of BC to the ocean. BC comprised 5-72% of UDOM-C (27+/-l7%) and on average 8.9+/-6.5% of dissolved organic carbon (DOC) with higher values in the turbid region of the Delaware Estuary and lower yields in the river and coastal ocean. The spatial and seasonal distributions of BC along the salinity gradient of Delaware Bay suggest that the higher levels of BC in surface water UDOM originated from localized sources, possibly from atmospheric deposition or released from resuspended sediments. Black carbon comprised 4 to 7% of the DOC in the coastal Atlantic Ocean, revealing that river-estuary systems are important exporters of colloidal BC to the ocean. The annual flux of BC from Delaware Bay UDOM to the Atlantic Ocean was estimated at 2.4x10(exp 10) g BC yr(exp -1). The global river flux of BC through DOM to the ocean could be on the order of 5.5x1O(exp 12)g BC yr (exp -1). These results support the hypothesis that the DOC pool is the intermediate reservoir in which BC ages prior to sedimentary deposition.

Mannino, Antonio↗

Dynamic Control System Performance during Commissioning of the Space Technology 7-Disturbance Reduction System Experiment of LISA Pathfinder

The Space Technology-7 Disturbance Reduction System (DRS) launched aboard the European Space Agency's LISA Pathfinder spacecraft on December 3, 2015, after more than a decade in development. DRS consists of three primary components: an Integrated Avionics Unit (IAU), Colloidal MicroNewton Thrusters, and Dynamic Control System (DCS) algorithms implemented on the IAU. During the portions of the mission in which the DRS was under control, the DCS was responsible for controlling the spacecraft and the free-floating test masses that were part of the LISA Test Package. The commissioning period was originally divided into two periods: before propulsion separation and after propulsion separation. A recommissioning period was added after an anomaly occurred in the thruster system. The paper will describe the activities used to commission DRS, present results from the commissioning of the DCS and the recommissioning activities per-formed after the thruster anomaly.

Hsu, Oscar↗

Turbulent-like flows in quasi two-dimensional dense suspensions of motile colloids

Dense bacterial suspensions exhibit turbulent-like flows at low Reynolds numbers, driven by the activity of the microswimmers. In this study, we develop a model system to examine these dynamics using motile colloids that mimic bacterial locomotion. The colloids are powered by the Quincke instability, which causes them to spontaneously roll in a random-walk pattern when exposed to a square-wave electric field. We experimentally investigate the flow dynamics in dense suspensions of these Quincke random walkers under quasi two-dimensional conditions, where the particle size is comparable to the gap between the electrodes. The results suggest a scaling regime in the energy spectrum ∼k −4 at high wavenumbers, observed consistently across activity levels and particle concentrations. We observe that velocity time correlations decay within a single period of the square-wave field, yet an anti-correlation appears between successive field applications, indicative of a dynamic structural memory of the ensemble.

Luo, Rui [Northwestern Univ., Evanston, IL (United↗

Dynamic Control System Performance during Commissioning of the Space Technology 7-Disturbance Reduction System Experiment of LISA Pathfinder

The Space Technology-7 Disturbance Reduction System (DRS) launched aboard the European Space Agencys LISA Pathfinder spacecraft on December 3, 2015, after more than a decade in development. DRS consists of three prima-ry components: an Integrated Avionics Unit (IAU), Colloidal MicroNewton Thrusters, and Dynamic Control System (DCS) algorithms implemented on the IAU. During the portions of the mission in which the DRS was under control, the DCS was responsible for controlling the spacecraft and the free-floating test masses that were part of the LISA Test Package. The commissioning period was originally divided into two periods: before propulsion separation and after pro-pulsion separation. A recommissioning period was added after an anomaly oc-curred in the thruster system. The paper will describe the activities used to com-mission DRS, present results from the commissioning of the DCS and the re-commissioning activities performed after the thruster anomaly.

Hsu, Oscar↗

Multi-scale organization in communicating active matter

The emergence of collective motion among interacting, self-propelled agents is a central paradigm in non-equilibrium physics. Examples of such active matter range from swimming bacteria and cytoskeletal motility assays to synthetic self-propelled colloids and swarming microrobots. Remarkably, the aggregation capabilities of many of these systems rely on a theme as fundamental as it is ubiquitous in nature: communication. Despite its eminent importance, the role of communication in the collective organization of active systems is not yet fully understood. Here we report on the multi-scale self-organization of interacting self-propelled agents that locally process information transmitted by chemical signals. We show that this communication capacity dramatically expands their ability to form complex structures, allowing them to self-organize through a series of collective dynamical states at multiple hierarchical levels. Our findings provide insights into the role of self-sustained signal processing for self-organization in biological systems and open routes to applications using chemically driven colloids or microrobots.

59 BASIC BIOLOGICAL SCIENCES↗

In Situ X-ray Scattering Reveals Coarsening Rates of Superlattices Self-Assembled from Electrostatically Stabilized Metal Nanocrystals Depend Nonmonotonically on Driving Force

Self-assembly of colloidal nanocrystals (NCs) into superlattices (SLs) is an appealing strategy to design hierarchically organized materials with promising functionalities. Mechanistic studies are still needed to uncover the design principles for SL self-assembly, but such studies have been difficult to perform due to the fast time and short length scales of NC systems. To address this challenge, we developed an apparatus to directly measure the evolving phases in situ and in real time of an electrostatically stabilized Au NC solution before, during, and after it is quenched to form SLs using small-angle X-ray scattering. By developing a quantitative model, we fit the time-dependent scattering patterns to obtain the phase diagram of the system and the kinetics of the colloidal and SL phases as a function of varying quench conditions. The extracted phase diagram is consistent with particles whose interactions are short in range relative to their diameter. We find the degree of SL order is primarily determined by fast (subsecond) initial nucleation and growth kinetics, while coarsening at later times depends nonmonotonically on the driving force for self-assembly. We validate these results by direct comparison with simulations and use them to suggest dynamic design principles to optimize the crystallinity within a finite time window. The combination of this measurement methodology, quantitative analysis, and simulation should be generalizable to elucidate and better control the microscopic self-assembly pathways of a wide range of bottom-up assembled systems and architectures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ultrafast Symmetry Control in Photoexcited Quantum Dots

Symmetry control is essential for realizing unconventional properties, such as ferroelectricity, nonlinear optical responses, and complex topological order, thus it holds promise for the design of emerging quantum and photonic systems. Nevertheless, fast and reversible control of symmetry in materials remains a challenge, especially for nanoscale systems. Here, reversible symmetry changes are unveiled in colloidal lead chalcogenide quantum dots on picosecond timescales. Using a combination of ultrafast electron diffraction and total X-ray scattering, in conjunction with atomic-scale structural modeling and first-principles calculations, it is revealed that symmetry-broken lead sulfide quantum dots restore to a centrosymmetric phase upon photoexcitation. The symmetry restoration is driven by photoexcited electronic carriers, which suppress lead off-centering for about 100 ps. Furthermore, the change in symmetry is closely correlated with the electronic properties, and the bandgap transiently red-shifts in the symmetry-restored quantum dots. Overall, this study elucidates reversible symmetry changes in colloidal quantum dots, and more broadly defines a new methodology to optically control symmetry in nanoscale systems on ultrafast timescales.

36 MATERIALS SCIENCE↗

Binary Colloidal Alloy Test-3 and 4: Critical Point

Binary Colloidal Alloy Test - 3 and 4: Critical Point (BCAT-3-4-CP) will determine phase separation rates and add needed points to the phase diagram of a model critical fluid system. Crewmembers photograph samples of polymer and colloidal particles (tiny nanoscale spheres suspended in liquid) that model liquid/gas phase changes. Results will help scientists develop fundamental physics concepts previously cloaked by the effects of gravity.

Weitz, David A.↗

Progress on LISA Colloid Microthruster Technology Development

Colloid microthrusters have been operated successfully in flight, providing drag-free and precision control for spacecraft that can be used for future applications such as gravity wave and exoplanet observatories. The Space Technology 7 Disturbance Reduction System (ST7- DRS) technology demonstration payload included eight Busek Colloid Micro-Newton Thrusters (CMNTs) as part of the Laser Interferometer Space Antenna (LISA) Pathfinder mission that launched in December of 2015. The CMNTs provided full attitude and precision drag-free control of the spacecraft with <10 nm/√Hz stability along the most sensitive axis during commissioning, nominal, and extended mission phases through April of 2017. Performance requirements (≤0.1 μN/√Hz) were met and models were validated based on on- orbit measurements of test mass motion and actuation during the 60-day nominal and 30-day extended missions. In 2018, the European Space Agency (ESA) selected LISA to be the agency’s next “large-class” mission, currently in Phase A, with a launch scheduled for 2034 and a 12.5-year duration, including the transfer (1.5 years), commissioning (1 year), nominal (4 or 6 years), and extended (6 or 4 years) phases of the mission, which sets the lifetime and consumables requirement. NASA is considering a significant contribution of hardware to the ESA-led mission, potentially including colloid microthrusters. In preparation, NASA is developing five technologies to TRL 5 and 6, including the colloid microthrusters, to be ready for infusion into LISA by the mission adoption review (MAR), currently scheduled for 2024. While ST7-DRS effectively brought the CMNTs to TRL 7, additional lower-TRL flow control components must be developed for full redundancy, reducing the system-level TRL back to 4. Key to the future of the colloid microthruster technology will be to use lessons learned and keep as much of the heritage from the ST7 design as possible while updating the system to support redundancy and lifetime requirements of a flagship-class mission. This paper describes the technology plan and progress to reach TRL 6 by the MAR, focusing on near- term plans to reach TRL 5 by the end of March 2022 for the LISA Colloid Microthrusters (CMTs). Work includes requirements development and sizing studies, breadboard and brassboard hardware developments at Busek, including relevant lifetime and environment testing, and lifetime modeling, verification and validation efforts at JPL, UCLA, and UCI.

Gamero-Castaño, Manuel↗

Physics of Colloids in Space--Plus (PCS+) Experiment Completed Flight Acceptance Testing

The Physics of Colloids in Space--Plus (PCS+) experiment successfully completed system-level flight acceptance testing in the fall of 2003. This testing included electromagnetic interference (EMI) testing, vibration testing, and thermal testing. PCS+, an Expedite the Process of Experiments to Space Station (EXPRESS) Rack payload will deploy a second set of colloid samples within the PCS flight hardware system that flew on the International Space Station (ISS) from April 2001 to June 2002. PCS+ is slated to return to the ISS in late 2004 or early 2005.

Doherty, Michael P.↗

Scintillation of colloidal nanocrystals

Scintillators are materials that convert ionizing radiation in the form of particles or photons into low-energy photons in the ultraviolet to near-infrared spectral range. Here, this work reviews efforts to use colloidal nanocrystals as scintillator materials. To date, research on colloidal nanocrystals as scintillators has focused on doped phosphor systems, quantum dots and related structures, and perovskite-based nanocrystals. Among various material classes and forms, colloidal semiconductor nanocrystals stand out thanks to their appealing fluorescence properties, yet understanding of their radioluminescence and cathodoluminescence is incomplete. This review discusses fundamental limits and material design challenges toward achieving high brightness, fast speed, and durable scintillator performance with nanocrystal scintillators. First, this review describes the basic principles and efficiency limitations of scintillation, particularly the large influence of multiple exciton generation in many nanocrystal species, as well as performance metrics. Second, methods for measurement are described. Third, we review the results of the main classes of nanocrystal scintillators, including quantum dots and related particles, perovskites, and doped-phosphor particles. Fourth, scintillation imaging is discussed in terms of the relevant performance metrics and results obtained using nanocrystal materials. Finally, we note the strengths and weaknesses of nanocrystal scintillators and discuss potential areas of further development.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Self-oscillating synchronematic colloids

Self-oscillators that sustain periodic dynamics under constant input are ubiquitous in natural and engineered systems, where their interactions enable spatiotemporal coordination among many individual units. New forms of organization can emerge when these self-oscillating units are free to move and rotate, coupling their spatial arrangement and alignment with their oscillation frequencies and phases. Here, we report experiments and simulations on populations of Quincke colloids that behave as self-oscillating units with position, orientation, frequency, and phase. Depending on the initial distribution, these active oscillators spontaneously organize into distinct collective states characterized by temporal synchronization and directional alignment, which we term synchronematic order. In fluid-like clusters, this order is short-ranged and decays over a length scale set by the competition between hydrodynamic interactions and athermal noise. In crystalline clusters, these interactions drive flobal synchronization and circular alignment-synchronematic crystals-whose collective frequency increases with cluster size due to non-reciprocal interactions. Our results establish self-oscillating colloids as a model system for active oscillatory matter and reveal fundamental principles by which synchronization, alignment, and structure co-emerge, offering new pathways for designing adaptive, frequency-tunable materials.

colloids↗

Hydrogen Adsorption, Reactivity, and Catalysis on Colloidal Iron Carbide Nanoparticles

Supported iron carbide particles have long served as catalysts for CO hydrogenation (the Fischer Tropsch synthesis, FTS) and continue to be attractive. Despite this, little is known about their chemistry. Reported here is a colloidal Fe x C nanoparticle (NP) model system that allows direct observation of surface hydrogen and CO, as well as quantification of the surface H. Dodecylamine-capped Fe x C NPs (DDA-Fe x C NPs) were synthesized through solution-phase carburization of Fe NPs and form stable colloids in low-polarity organic solvents. Treatment of these colloids with H 2 or D 2 produced highly hydrogenated materials, and FTIR spectra of DDA-Fe x C-D n showed that most of the D binds to carbides, with at least four distinct v(C-D) modes. The surface C-H(D) bonds were all reactive, transferring hydrogen to alkenes and other reagents in solution. Titration and ICP measurements showed a 0.17:1 ratio of added H:total Fe, or roughly. 40 H per 1.8 nm DDA-Fe x C NP. Conversely, CO was preferentially bound to surface Fe sites, with FTIR spectra showing a single broad v(CO) that shifted with CO coverage or co-adsorption of H 2 . The DDA-Fe x C NPs were active catalysts for both olefin hydrogenation and the FTS, under mild conditions and without catalyst pre-treatment. The CO hydrogenation reactions yielded a broad distribution of long-chain linear paraffins and olefins. Though quantitative comparisons with typical FTS results are not possible because of our use of sealed batch reactors and other factors, the observations of high catalytic reactivity demonstrate the relevance of this model system to iron-carbide catalysis. DFT calculations on model slab surfaces with varying iron carbide stoichiometries revealed that the thermodynamically preferred surface adsorption sites are C for H ads and Fe for CO ads . A variety of binding sites and binding energies were found for each adsorbate. We are unaware of previous studies indicating that a diverse array of C-H bonds is the primary source of reactive H on iron carbides. Experimentally, the diversity of *C-H sites was evident in reactions with H-atom donors and abstractors of different strengths, from both the reaction stoichiometries and IR spectra. The different surface–H binding energies correlate with the v(C-D) stretching frequencies. Furthermore, these insights into complex iron carbide surfaces and catalysis could assist catalyst design, and they showcase the importance of stoichiometric studies of reaction intermediates.

08 HYDROGEN↗

Optically Excited Lasing in a Cavity‐Based, High‐Current‐Density Quantum Dot Electroluminescent Device

Abstract Laser diodes based on solution‐processable materials can benefit numerous technologies including integrated electronics and photonics, telecommunications, and medical diagnostics. An attractive system for implementing these devices is colloidal semiconductor quantum dots (QDs). The progress towards a QD laser diode has been hampered by rapid nonradiative Auger decay of optical‐gain‐active multicarrier states, fast device degradation at high current densities required for laser action, and unfavorable competition between optical gain and optical losses in a multicomponent device stack. Here we resolve some of these challenges and demonstrate optically excited lasing from fully functional high‐current density electroluminescent (EL) devices with an integrated optical resonator. This advance has become possible due to excellent optical gain properties of continuously graded QDs and a refined device architecture, which allows for highly efficient light amplification in a thin, EL‐active QD layer.

36 MATERIALS SCIENCE↗

Biomolecular condensates form spatially inhomogeneous network fluids

The functions of biomolecular condensates are thought to be influenced by their material properties, and these will be determined by the internal organization of molecules within condensates. However, structural characterizations of condensates are challenging, and rarely reported. Here, we deploy a combination of small angle neutron scattering, fluorescence recovery after photobleaching, and coarse-grained molecular dynamics simulations to provide structural descriptions of model condensates that are formed by macromolecules from nucleolar granular components (GCs). We show that these minimal facsimiles of GCs form condensates that are network fluids featuring spatial inhomogeneities across different length scales that reflect the contributions of distinct protein and peptide domains. The network-like inhomogeneous organization is characterized by a coexistence of liquid- and gas-like macromolecular densities that engenders bimodality of internal molecular dynamics. These insights suggest that condensates formed by multivalent proteins share features with network fluids formed by systems such as patchy or hairy colloids.

59 BASIC BIOLOGICAL SCIENCES↗

Delivery of Colloid Micro-Newton Thrusters for the Space Technology 7 Mission

Two flight-qualified clusters of four Colloid Micro-Newton Thruster (CMNT) systems have been delivered to the Jet Propulsion Laboratory (JPL). The clusters will provide precise spacecraft control for the drag-free technology demonstration mission, Space Technology 7 (ST7). The ST7 mission is sponsored by the NASA New Millennium Program and will demonstrate precision formation flying technologies for future missions such as the Laser Interferometer Space Antenna (LISA) mission. The ST7 disturbance reduction system (DRS) will be on the ESA LISA Pathfinder spacecraft using the European gravitational reference sensor (GRS) as part of the ESA LISA Technology Package (LTP). Developed by Busek Co. Inc., with support from JPL in design and testing, the CMNT has been developed over the last six years into a flight-ready and flight-qualified microthruster system, the first of its kind. Recent flight-unit qualification tests have included vibration and thermal vacuum environmental testing, as well as performance verification and acceptance tests. All tests have been completed successfully prior to delivery to JPL. Delivery of the first flight unit occurred in February of 2008 with the second unit following in May of 2008. Since arrival at JPL, the units have successfully passed through mass distribution, magnetic, and EMI/EMC measurements and tests as part of the integration and test (I&T) activities including the integrated avionics unit (IAU). Flight software sequences have been tested and validated with the full flight DRS instrument successfully to the extent possible in ground testing, including full functional and 72 hour autonomous operations tests. Delivery of the cluster assemblies along with the IAU to ESA for integration into the LISA Pathfinder spacecraft is planned for the summer of 2008 with a planned launch and flight demonstration in late 2010.

Precision Formation Flying↗

18-Degree-of-Freedom Controller Design for the ST7 Disturbance Reduction System

The Space Technology 7 experiment will perform an on-orbit system-level validation of a Disturbance Reduction System employing gravitational reference sensors and micronewton colloidal thrusters to maintain a spacecraft s position with respect to free-floating test masses in the gravitational reference sensors to less than 10 nm/dHz over the frequency range 1 to 30 mHz. This paper presents the design and analysis of the control system that closes the loop between the gravitational reference sensors and the micronewton thrusters while incorporating star tracker data at low frequencies. The effects of disturbances and actuation and measurement noise are evaluated in a eighteen-degree-of-freedom model.

Markley, F. L.↗