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At least 343 records · Page 19

Attention Network Forecasts Time-to-Failure in Laboratory Shear Experiments

Rocks under stress deform by creep mechanisms that include formation and slip on small-scale internal cracks. Intragranular cracks and slip along grain contacts release energy as elastic waves termed acoustic emissions (AE). AEs are thought to contain predictive information that can be used for fault failure forecasting. Here, we present a method using unsupervised classification and an attention network to forecast labquakes using AE waveform features. Our data were generated in a laboratory setting using a biaxial shearing device with granular fault gouge intended to mimic the conditions of tectonic faults. Here, we analyzed the temporal evolution of AEs generated throughout several hundred laboratory earthquake cycles. We used a Conscience Self-Organizing Map (CSOM) to perform topologically ordered vector quantization based on waveform properties. The resulting map was used to interactively cluster AEs. We examined the clusters over time to identify those with predictive ability. Finally, we used a variety of LSTM and attention-based networks to test the predictive power of the AE clusters. By tracking cumulative waveform features over the seismic cycle, the network is able to forecast the time-to-failure (TTF) of lab earthquakes. Our results show that analyzing the data to isolate predictive signals and using a more sophisticated network architecture are key to robustly forecasting labquakes. In the future, this method could be applied on tectonic faults to monitor earthquakes and augment early warning systems.

58 GEOSCIENCES↗

Bridging the Transuranics with Uranium(IV) Sulfate Aqueous Species and Solid Phases

Isolating isomorphic compounds of tetravalent actinides (i.e., Th IV , U IV , Np IV , and Pu IV ) improve our understanding of the bonding behavior across the series, in addition to their relationship with tetravalent transition metals (Zr and Hf) and lanthanides (Ce). Similarities between these tetravalent metals are particularly illuminated in their hydrolysis and condensation behavior in aqueous systems, leading to polynuclear clusters typified by the hexamer [M IV 6 O 4 (OH) 4 ] 12+ building block. Prior studies have shown the predominance and coexistence of smaller species for Th IV (monomers, dimers, and hexamers) and larger species for U IV , Np IV , and Pu IV (including 38-mers and 70-mers). We show here that aqueous uranium(IV) sulfate also displays behavior similar to that of Th IV (and Zr IV ) in its isolated solidphase and solution speciation. Two single-crystal X-ray structures are described: a dihydroxide-bridged dimer (U 2 ) formulated as U 2 (OH) 2 (SO 4 ) 3 (H 2 O) 4 and a monomer-linked hexamer framework (U-U 6 ) as (U(H 2 O) 3.5 ) 2 U 6 O 4 (OH) 4 (SO 4 ) 10 (H 2 O) 9 . These structures are similar to those previously described for ThIV. Moreover, cocrystallization of monomer and dimer and of dimer and monomer–hexamer phases for both Th IV (prior) and U IV (current) indicates the coexistence of these species in solution. Because it was not possible to effectively study the sulfate-rich solutions via X-ray scattering from which U 2 and U-U 6 crystallized, we provide a parallel solution speciation study in low sulfate conditions, as a function of the pH. Raman spectroscopy, UV–vis spectroscopy, and small-angle X-ray scattering of these show decreasing sulfate binding, increased hydrolysis, increased species size, and increased complexity, with increasing pH. Furthermore, this study describes a bridge across the first half the actinide series, highlighting U IV similarities to Th IV , in addition to the previously known similarities to the transuranic elements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ce IV 70 Oxosulfate Rings, Frameworks, Supramolecular Assembly, and Redox Activity**

Abstract M IV molecular oxo‐clusters (M=Zr, Hf, Ce, Th, U, Np, Pu) are prolific in bottoms‐up material design, catalysis, and elucidating reaction pathways in nature and in synthesis. Here we introduce Ce 70 , a wheel‐shaped oxo‐cluster, [Ce IV 70 (OH) 36 (O) 64 (SO 4 ) 60 (H 2 O) 10 ] 4− . Ce 70 crystallizes into intricate high pore volume frameworks with divalent transition metals and Ce‐monomer linkers. Eight crystal‐structures feature four framework types in which the Ce 70 ‐rings are linked as propellers, in offset‐stacks, in a tartan pattern, and as isolated rings. Small‐angle X‐ray scattering of Ce 70 dissolved in butylamine, with and without added cations (Ce IV , alkaline earths, Mn II ), shows the metals‘ differentiating roles in ring linking, leading to supramolecular assemblies. The large acidic pores and abundant terminal sulfates provide ion‐exchange behavior, demonstrated with U IV and Nd III . Frameworks featuring Ce III/IV ‐monomer linkers demonstrate both oxidation and reduction. This study opens the door to mixed‐metal, highly porous framework catalysts, and new clusters for metal‐organic framework design

Colliard, Ian↗

Merging LANDSAT Derived Land Covers into Quad-referenced Geographic Information Systems

An approach for merging multiscene LANDSAT data bases into existing geographic information systems having 5-second or smaller cells is described. The approach uses the output from the State of Maryland's UNIVAC 1180-based LANDSAT classification program ASTEP (Algorithm Simulation Test and Evaluation) developed by NASA. The structure of the technique was designed to address the problems that emerged as part of the LANDSAT classification of the 64,000 square mile Chesapeake water shed involving twelve scenes. The removal of overlap among adjacent scenes, the crossreferencing of ground control points, and the isolation of the appropriate pixels from the LANDSAT data base for subsequent positioning into a file containing ancillary data referenced to a specific USGS 7 1/2 minute quadrangle sheet are described. Examples illustrate the clustering of classified LANDSAT pixels to define the dominant land use for each of 8,100 cells within a series of quadrangle sheets distributed over the State of Maryland. The approach uses a hard copy terminal tied to an ASTEP algorithm through telephone lines. A coordinate digitizing board for inputing the position of ground control points is also valuable, although manual measurements are possible. The approach is quite efficient and should be especially attractive for use on regional scale studies.

White, J. M.↗

Characterization of Surface Heterogeneity-Induced Convection Using Cluster Analysis

Land-atmosphere interactions and boundary layer processes often control the formation of shallow clouds and subsequently deep convective precipitation over the Southern Great Plains. In this study, we examine the impacts of large-scale advection on the cloud populations and land-atmospheric coupling observed during the Holistic Interactions of Shallow Clouds, Aerosols, and Land-Ecosystems (HI-SCALE) field campaign in 2016. In this work, we performed two Large Eddy Simulations (LES) using the Weather Research and Forecasting Model for a day in which the transition from clear-sky to shallow precipitating clouds and isolated deep convection was observed. The control simulation reproduced the overall distribution of cloud populations by using realistic soil conditions with an interactive land model. In the sensitivity simulation where large-scale advection is removed, a strong relationship between the land and boundary layer is found. To study the timing, location, and intensity of convective initiation and the relationship of clouds with land surface properties, a cluster analysis of equivalent potential temperature is performed for the simulation without large-scale advection. That analysis shows that convective clouds first form over regions with higher surface sensible heat flux. Precipitation from those convective clouds likely triggers new updrafts nearby about two hours later through the lifting associated with cold pools. Furthermore, the cluster analysis also shows that in addition to the spatial pattern of soil moisture, land use and soil texture in western Oklahoma also influence the location of convective initiation.

54 ENVIRONMENTAL SCIENCES↗

Diagnostic diagrams for ram pressure stripped candidates

ABSTRACT This paper presents a method for finding ram pressure stripped (RPS) galaxy candidates by performing a morphological analysis of galaxy images obtained from the Legacy survey. We consider a sample of about 600 galaxies located in different environments such as groups and clusters, tidally interacting pairs and the field. The sample includes 160 RPS previously classified in the literature into classes from J1 to J5, based on the increasing level of disturbances. Our morphological analysis was done using the astromorphlib software followed by the inspection of diagnostic diagrams involving combinations of different parameters like the asymmetry (A), concentration (C), Sérsic index (n), and bulge strength parameters $F(G,\, M_{20})$. We found that some of those diagrams display a distinct region in which galaxies classified as J3, J4, and J5 decouples from isolated galaxies. We call this region as the morphological transition zone and we also found that tidally interacting galaxies in pairs are predominant within this zone. Nevertheless, after visually inspecting the objects in the morphological transition zone to discard obvious contaminants, we ended up with 33 bona fide new RPS candidates in the studied nearby groups and clusters (Hydra, Fornax, and CLoGS sample), of which one-third show clear evidence of unwinding arms. Future works may potentially further increase significantly the samples of known RPS using such method.

Astronomy & Astrophysics↗

Lewis Acid Supported Nickel Nitrenoids

Abstract Metalation of the polynucleating ligand F,tbs LH 6 (1,3,5‐C 6 H 9 (NC 6 H 3 −4‐F−2‐NSiMe 2 t Bu) 3 ) with two equivalents of Zn(N(SiMe 3 ) 2 ) 2 affords the dinuclear product ( F,tbs LH 2 )Zn 2 ( 1 ), which can be further deprotonated to yield ( F,tbs L)Zn 2 Li 2 (OEt 2 ) 4 ( 2 ). Transmetalation of 2 with NiCl 2 (py) 2 yields the heterometallic, trinuclear cluster ( F,tbs L)Zn 2 Ni(py) ( 3 ). Reduction of 3 with KC 8 affords [KC 222 ][( F,tbs L)Zn 2 Ni] ( 4 ) which features a monovalent Ni centre. Addition of 1‐adamantyl azide to 4 generates the bridging μ 3 ‐nitrenoid adduct [K(THF) 3 ][( F,tbs L)Zn 2 Ni(μ 3 ‐NAd)] ( 5 ). EPR spectroscopy reveals that the anionic cluster possesses a doublet ground state ( S = ). Cyclic voltammetry of 5 reveals two fully reversible redox events. The dianionic nitrenoid [K 2 (THF) 9 ][( F,tbs L)Zn 2 Ni(μ 3 ‐NAd)] ( 6 ) was isolated and characterized while the neutral redox isomer was observed to undergo both intra‐ and intermolecular H‐atom abstraction processes. Ni K‐edge XAS studies suggest a divalent oxidation state for the Ni centres in both the monoanionic and dianionic [Zn 2 Ni] nitrenoid complexes. However, DFT analysis suggests Ni‐borne oxidation for 5 .

Juda, Cristin E.↗

Combining ToF‐SIMS and Multivariate Analysis to Resolve Active Sites on Ni‐Based HER Catalysts

Unambiguous identification of active sites in heterogeneous catalysis remains a major challenge, particularly for materials with ultrathin, chemically mixed surface layers. Here, we demonstrate a generalizable approach that combines time-of-flight secondary ion mass spectrometry (ToF-SIMS) with multivariate statistical analysis (principal component analysis [PCA] and multivariate curve resolution [MCR]) to resolve catalytically relevant motifs at the nanoscale. Using Ni electrodes as a model system, PCA distinguished hydroxide-enriched domains from oxide- and metal-rich regions, while MCR decomposed depth profiles and 3D images into hydroxide, oxide, and metallic layers with nanometer resolution. A unique secondary-ion fragment, NiO 3 H 3 − (m/z 108.94), emerged as a marker of hydroxide-rich environments and correlated with hydrogen evolution reaction (HER) activity across a series of Ni electrodes. Complementary density functional theory (DFT) calculations revealed that Ni(OH) 2 clusters adjacent to metallic Ni offer the most favorable water dissociation energetics, establishing the structural origin of the marker. While illustrated here for Ni-based HER, this workflow provides a broadly applicable framework to isolate and rank near-surface patterns that govern catalytic activity, thereby extending ToF-SIMS from a qualitative probe to a predictive tool for active site identification.

HER active sites↗

Nuclear winds in active elliptical galaxies. I - Interaction

The interaction of a supersonic wind generated by an active nucleus, a nuclear wind, with the hot interstellar medium of an elliptical host galaxy is investigated. We survey the basic time and spatial scales of this interaction through a study covering the range of probable wind and galaxy parameters. The evolving wind/ISM interaction is detailed, with the conclusion that a true equilibrium state is never possible due to long cooling times. Alteration of the wind by mass loading is considered, and a relationship between nuclear winds and central stellar clusters in this context is outlined. The nuclear wind will fundamentally alter the interstellar medium of the host galaxy. Powerful radio galaxies and quasars can evacuate the entire ISM of their host galaxy. In an isolated elliptical galaxy, winds from moderately powerful radio galaxies will either be confined to within about a kpc or evacuate the entire hot ISM. Even in the relatively high pressure ISM of elliptical galaxies winds containing only 1 percent-10 percent of the radiant luminosity of the active nucleus will extend to the narrow-line region. Therefore, nuclear winds are likely to control the properties of the narrow-line emission.

Smith, Steven J.↗

Fluorescence Enhancement in the Solid State by Isolating Perylene Fluorophores in Metal–Organic Frameworks

Polycyclic aromatic hydrocarbons such as perylene, pyrene, and their derivatives are highly emissive fluorophores in solution. Furthermore, the practical applications of these materials in the field of molecular electronic and light emitting devices are often hindered by self-quenching effects due to the formation of non-fluorescent aggregates in concentrated solutions or in the solid state. Herein, we demonstrate that aggregation caused quenching of perylenes can be minimalized by molecular incorporation into metalorganic frameworks (MOFs). This study utilized a stable Zr 6 cluster-based MOF, UiO-67, as a matrix. Linear linkers containing the photo-responsive moieties were designed and incorporated into the parent UiO-67 scaffold through the partially replacement of the non-fluorescent linkers of a similar length, forming mixed-linker MOFs. Here, the average distance between perylene moieties was tuned by changing the linker ratios, thus controlling the fluorescence intensity, emission wavelength, and quantum yield. Molecular modeling was further adopted to correlate the number of isolated perylene linkers within the framework to the ratio between the two linkers, therefore rationalizing the change in the observed fluorescent properties. Taking advantage of the tunable fluorescence, inherent porosity, and high chemical stability of this MOF platform, it was applied as a fluorescent sensor for oxygen detection in the gas phase, a model reaction, showing fast response and good recyclability.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

EPR studies of ferredoxin in spinach and cyanobacterial thylakoids related to photosystem I-driven NADP + reduction

Photosynthetic light-dependent reactions occur in thylakoid membranes where embedded proteins capture light energy and convert it to chemical energy in the form of ATP and NADPH for use in carbon fixation. One of these integral membrane proteins is Photosystem I (PSI). PSI catalyzes light-driven transmembrane electron transfer from plastocyanin (Pc) to oxidized ferredoxin (Fd). Electrons from reduced Fd are used by the enzyme ferredoxin-NADP + reductase (FNR) for the reduction of NADP + to NADPH. Fd and Pc are both small soluble proteins whereas the larger FNR enzyme is associated with the membrane. To investigate electron shuttling between these diffusible and embedded proteins, thylakoid photoreduction of NADP + was studied. As isolated, both spinach and cyanobacterial thylakoids generate NADPH upon illumination without extraneous addition of Fd. These findings indicate that isolated thylakoids either (i) retain a “pool” of Fd which diffuses between PSI and membrane bound FNR or (ii) that a fraction of PSI is associated with Fd, with the membrane environment facilitating PSI-Fd-FNR interactions which enable multiple turnovers of the complex with a single Fd. To explore the functional association of Fd with PSI in thylakoids, electron paramagnetic resonance (EPR) spectroscopic methodologies were developed to distinguish the signals for the reduced Fe-S clusters of PSI and Fd. Temperature-dependent EPR studies show that the EPR signals of the terminal [4Fe-4S] cluster of PSI can be distinguished from the [2Fe-2S] cluster of Fd at > 30 K. At 50 K, the cw X-band EPR spectra of cyanobacterial and spinach thylakoids reduced with dithionite exhibit EPR signals of a [2Fe-2S] cluster with g-values g x = 2.05, g y = 1.96, and g z = 1.89, confirming that Fd is present in thylakoid preparations capable of NADP + photoreduction. Quantitation of the EPR signals of P 700 + and dithionite reduced Fd reveal that Fd is present at a ratio of ~ 1 Fd per PSI monomer in both spinach and cyanobacterial thylakoids. Light-driven electron transfer from PSI to Fd in thylakoids confirms Fd is functionally associated (< 0.4 Fd/PSI) with the acceptor end of PSI in isolated cyanobacterial thylakoids. Furthermore, these EPR experiments provide a benchmark for future spectroscopic characterization of Fd interactions involved in multistep relay of electrons following PSI charge separation in the context of photosynthetic thylakoid microenvironments.

Electron paramagnetic resonance↗

Understanding the Computing and Analysis Needs for Resiliency of Power Systems from Severe Weather Impacts

As the frequency and intensity of severe weather has increased, its effect on the electric grid has manifested in the form of significantly more and larger outages in the United States. This has become especially true for regions that were previously isolated from weather extremes. In this paper, we analyze the weather impacts on the electric power grid across a variety of weather conditions, draw correlations, and provide practical insights into the operational state of these systems. High resolution computational modeling of specific meteorological variables, computational approaches to solving power system models under these conditions, and the types of resiliency needs are highlighted as goal-oriented computing approaches are being built to address grid resiliency needs. An example analysis correlating outages to 1km day-ahead weather from two historical winter storms, calculated on a large cluster using a combination of interpolated and extrapolated inputs from multiple instrumented sites to workflows that produce primary meteorological outputs, is shown as initial proof of concept.

analysis↗

Ce IV 70 oxosulfate rings, frameworks, supramolecular assembly and redox activity

M IV molecular oxo-clusters (M=Zr, Hf, Ce, Th, U, Np, Pu) are prolific in bottoms-up material design, catalysis, and elucidating reaction pathways in nature and in synthesis. Here we introduce Ce 70 , a wheel-shaped oxo-cluster, [Ce IV 70 -(OH) 36 (O) 64 (SO 4 ) 60 (H 2 O) 10 ] 4- . Ce 70 crystallizes into intricate high pore volume frameworks with divalent transition metals and Ce-monomer linkers. Eight crystal-structures feature four framework types in which the Ce 70 -rings are linked as propellers, in offset-stacks, in a tartan pattern, and as isolated rings. In this work, small-angle X-ray scattering of Ce 70 dissolved in butylamine, with and without added cations (Ce IV , alkaline earths, Mn II ), shows the metals‘ differentiating roles in ring linking, leading to supramolecular assemblies. The large acidic pores and abundant terminal sulfates provide ion-exchange behavior, demonstrated with U IV and Nd III . Frameworks featuring Ce III/IV -monomer linkers demonstrate both oxidation and reduction. Furthermore, this study opens the door to mixed-metal, highly porous framework catalysts, and new clusters for metal-organic framework design.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The role of H–H interactions and impurities on the structure and energetics of H/Pd(111)

Understanding hydrogen incorporation into palladium requires detailed knowledge of surface and subsurface structure and atomic interactions as surface hydrogen is being embedded. Using density functional theory (DFT), we examine the energies of hydrogen layers of varying coverage adsorbed on Pd(111). Here we find that H–H and H–Pd interactions promote the formation of the well-known ($\sqrt{3}$ x $\sqrt{3}$) phases but also favor an unreported (3 × 3) phase at high H coverages for which we present experimental evidence. We relate the stability of isolated H vacancies of the (3 × 3) phase to the need of H 2 molecules to access bare Pd before they can dissociate. Following higher hydrogen dosage, we observe initial steps of hydride formation, starting with small clusters of subsurface hydrogen. The interaction between H and Pd is complicated by the persistent presence of carbon at the surface. X-ray photoelectron spectroscopy experiments show that trace amounts of carbon, emerging from the Pd bulk despite many surface cleaning cycles, become mobile enough to repopulate the C-depleted surface at temperatures above 200 K. When exposed to hydrogen, these surface carbon atoms react to form benzene, as evidenced by scanning tunneling microscopy observations interpreted with DFT.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A Case Study of the Glycoside Hydrolase Enzyme Mechanism Using an Automated QM-Cluster Model Building Toolkit

Glycoside hydrolase enzymes are important for hydrolyzing the β-1,4 glycosidic bond in polysaccharides for deconstruction of carbohydrates. The two-step retaining reaction mechanism of Glycoside Hydrolase Family 7 (GH7) was explored with different sized QM-cluster models built by the Residue Interaction Network ResidUe Selector (RINRUS) software using both the wild-type protein and its E217Q mutant. The first step is the glycosylation, in which the acidic residue 217 donates a proton to the glycosidic oxygen leading to bond cleavage. In the subsequent deglycosylation step, one water molecule migrates into the active site and attacks the anomeric carbon. Residue interaction-based QM-cluster models lead to reliable structural and energetic results for proposed glycoside hydrolase mechanisms. The free energies of activation for glycosylation in the largest QM-cluster models were predicted to be 19.5 and 31.4 kcal mol −1 for the wild-type protein and its E217Q mutant, which agree with experimental trends that mutation of the acidic residue Glu217 to Gln will slow down the reaction; and are higher in free energy than the deglycosylation transition states (13.8 and 25.5 kcal mol −1 for the wild-type protein and its mutant, respectively). For the mutated protein, glycosylation led to a low-energy product. This thermodynamic sink may correspond to the intermediate state which was isolated in the X-ray crystal structure. Hence, the glycosylation is validated to be the rate-limiting step in both the wild-type and mutated enzyme.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Distinguishing isotropic and anisotropic signals for X-ray total scattering using machine learning

Understanding structure–property relationships is essential for advancing technologies based on thin films. X-ray pair distribution function (PDF) analysis can access relevant atomic structure details spanning local-, mid- and long-range structure. While X-ray PDF has been adapted for thin films on amorphous substrates, measurements on single-crystal substrates are necessary to accurately determine structure origins for some thin film materials, especially those for which the substrate changes the accessible structure and properties. However, when measuring films on single-crystal substrates, high-intensity anisotropic Bragg spots saturate 2D detector images, overshadowing the thin films' isotropic scattering signal. This renders previous data processing methods for films on amorphous substrates unsuitable for films on single-crystal substrates. To address this measurement need, we developed IsoDAT2D, an innovative data processing approach using unsupervised machine learning algorithms. The program combines dimensionality reduction and clustering algorithms to separate thin film and single-crystal substrate X-ray scattering signals. We use SimDAT2D , a program we developed to generate simulated thin film data, to validate IsoDAT2D . Here we also use IsoDAT2D to isolate X-ray total scattering signal from a thin film on a single-crystal substrate. The resulting PDF data are compared with similar data processed using previous methods, especially substrate subtraction for single-crystal and amorphous substrates. PDF data from IsoDAT2D -identified X-ray total scattering data are significantly better than from single-crystal substrate subtraction, but not as reliable as PDF data from amorphous substrate subtraction. With IsoDAT2D , there are new opportunities to expand PDF to a wider variety of thin films, including those on single-crystal substrates, with which new structure–property relationships can be elucidated to enable fundamental understanding and technological advances.

36 MATERIALS SCIENCE↗

Aggregation of solutes in bosonic versus fermionic quantum fluids

Quantum fluid droplets made of helium-3 ( 3 He) or helium-4 ( 4 He) isotopes have long been considered as ideal cryogenic nanolabs, enabling unique ultracold chemistry and spectroscopy applications. The droplets were believed to provide a homogeneous environment in which dopant atoms and molecules could move and react almost as in free space but at temperatures close to absolute zero. Here, we report ultrafast x-ray diffraction experiments on xenon-doped 3 He and 4 He nanodroplets, demonstrating that the unavoidable rotational excitation of isolated droplets leads to highly anisotropic and inhomogeneous interactions between the host matrix and enclosed dopants. Superfluid 4 He droplets are laced with quantum vortices that trap the embedded particles, leading to the formation of filament-shaped clusters. In comparison, dopants in 3 He droplets gather in diffuse, ring-shaped structures along the equator. The shapes of droplets carrying filaments or rings are direct evidence that rotational excitation is the root cause for the inhomogeneous dopant distributions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Drop clustering and drop size correlations from holographic imagery suggest cloud droplet spectral broadening via entrainment-mixing

The question of how droplets rapidly grow large enough to initiate collision-coalescence has persisted for decades. Many theories explaining the production of sufficiently large drops (i.e., those in the “bottleneck” size range; ∼ 25–50 µm diameters) involve drop clustering on millimeter scales. A novel method is introduced to evaluate drop clustering trends particle-by-particle (i.e., the number/proximity of neighboring drops for given droplets; defined as drop clustering fields) which are diagnosed relative to drops within their shared drop environments – in contrast to previous studies which diagnose drop clustering of defined sample volumes, or in terms of absolute length scales. Specifically, this study evaluates the statistical likelihood that drops of a given size are associated with either a significant number of neighboring drops, or are significantly isolated from neighboring drops. Observations are acquired from the HOLODEC during the Cloud System Evolution in the Trades campaign, which sampled subtropical marine clouds. The HOLODEC measures drop size distributions and the 3D spatial coordinates of droplets. Results show drops within the bottleneck size range (diameters of ∼ 25–50 µm) are most likely to be significantly isolated from neighboring drops. This “isolated large drop trend” is primarily observed at subsaturated conditions, suggesting entrainment is the contributing factor. Holograms associated with this trend are more likely to have broader drop size distributions, larger maximum drop sizes and overly regions where precipitation reaches the lowest altitudes from the sampled cloud, suggesting entrainment-mixing drop size distribution broadening is a relevant precipitation-initiation mechanism.

D'Alessandro, John J. [Univ. of Washington, Seattl↗