21 Search Results

The transformative impact of modern computational paradigms and technologies, such as high-performance computing (HPC), quantum computing, and cloud computing, has opened up profound new opportunities for scientific simulations. Scalable computational chemistry is one beneficiary of this technological progress. The main focus of this paper is on the performance of various quantum chemical formulations, ranging from low-order methods to high-accuracy approaches, implemented in different computational chemistry packages and libraries, such as NWChem, NWChemEx, Scalable Predictive Methods for Excitations and Correlated Phenomena, ExaChem, and Fermi–Löwdin orbital self-interaction correction on Azure Quantum Elements, Microsoft's cloud services platform for scientific discovery. We pay particularmore » attention to the intricate workflows for performing complex chemistry simulations, associated data curation, and mechanisms for accuracy assessment, which is demonstrated with the Arrows automated workflow for high throughput simulations. Finally, we provide a perspective on the role of cloud computing in supporting the mission of leadership computational facilities.« less

The twilight zone is an important depth of the ocean where particulate organic matter (POM) remineralization takes place, and prokaryotes contribute to more than 70% of the estimated remineralization. However, little is known about the microbial community and metabolic activity associated with different particles in the twilight zone. The composition and distribution of particle-attached prokaryotes in the twilight zone of the South China Sea (SCS) were investigated using high-throughput sequencing and quantitative PCR, together with the Biolog Ecoplate™ microplates culture to analyze the microbial metabolic activity. We found that α- and γ-Proteobacteria dominating at the lower and upper boundary ofmore » the twilight zone, respectively; Methanosarcinales and Halobacteriales of the Euyarchaeota occupied in the larger particles at the upper boundary. Similar microbial community existed between euphotic layer and the upper boundary. Higher amount of shared Operational Taxonomic Units (OTUs) in the larger particles along the water depths, might be due to the fast sinking and major contribution of carbon flux of the larger particles from the euphotic layer. In addition to polymers as the major carbon source, carbohydrates and amino acids were preferentially used by microbial community at the upper and lower boundary, respectively. This could potentially be attributed to the metabolic capabilities of attached microbial groups in different particles, and reflected the initial preference of the carbon source by the natural microbes in the twilight zone as well. The microbial structure and carbon metabolic profiles could be complemented with metatranscriptomic analysis in future studies to augment the understanding of the complex carbon cycling pathways in the twilight zone.« less

Quantum chemical calculations on atomistic systems have evolved into a standard approach to studying molecular matter. These calculations often involve a significant amount of manual input and expertise, although most of this effort could be automated, which would alleviate the need for expertise in software and hardware accessibility. Here, we present the AutoRXN workflow, an automated workflow for exploratory high-throughput electronic structure calculations of molecular systems, in which (i) density functional theory methods are exploited to deliver minimum and transition-state structures and corresponding energies and properties, (ii) coupled cluster calculations are then launched for optimized structures to provide more accuratemore » energy and property estimates, and (iii) multi-reference diagnostics are evaluated to back check the coupled cluster results and subject them to automated multi-configurational calculations for potential multi-configurational cases. All calculations are carried out in a cloud environment and support massive computational campaigns. Key features of all components of the AutoRXN workflow are autonomy, stability, and minimum operator interference. We highlight the AutoRXN workflow with the example of an autonomous reaction mechanism exploration of the mode of action of a homogeneous catalyst for the asymmetric reduction of ketones.« less

Quasi‐2D perovskites are attractive because of their improved stability compared with 3D perovskites counterparts; however, they suffer from poor performance due to the insulating organic cation spacers. To resolve this issue, a strategy of replacing the insulating spacer with conducting spacer is proposed which successfully converts the spacer from a charge‐transporting “barrier” to charge‐transporting “bridge.” Specifically, an alkyl linker‐free, fully conjugated aromatic 2,2′‐biimidazolium (BIDZ) cation is introduced as a spacer to compose quasi‐2D perovskites. Density functional theory (DFT) simulation results show that the lowest unoccupied molecular orbital (LUMO) level localizes on BIDZ and the highest occupied molecular orbital (HOMO) levelmore » is on the perovskite. However, both HOMO and LUMO levels localize on perovskite slabs for the well‐known phenethylammonium (PEA)‐based 2D perovskites. The strong electronic coupling between BIDZ and 3D perovskite slabs improves carrier mobilities even for a low‐weak‐crystallinity and random‐orientated quasi‐2D perovskite film. As a result, a remarkable power conversion efficiency up to 11.4% ( n  = 5) is achieved, which is much higher than that of PEA‐based random‐orientated quasi‐2D perovskites with the same processing condition (6.5%). The strategy paves the way to highly efficient and stable quasi‐2D perovskites solar cells through designing new organic spacer cations.« less

The combination of measurements of the W boson polarization in top quark decays performed by the ATLAS and CMS collaborations is presented. The measurements are based on proton-proton collision data produced at the LHC at a centre-of-mass energy of 8 TeV, and corresponding to an integrated luminosity of about 20 fb$$^{−1}$$ for each experiment. The measurements used events containing one lepton and having different jet multiplicities in the final state. The results are quoted as fractions of W bosons with longitudinal (F$$_{0}$$), left-handed (F$$_{L}$$), or right-handed (F$$_{R}$$) polarizations. The resulting combined measurements of the polarization fractions are F$$_{0}$$ = 0.693more » ± 0.014 and F$$_{L}$$ = 0.315 ± 0.011. The fraction F$$_{R}$$ is calculated from the unitarity constraint to be F$$_{R}$$ = −0.008 ± 0.007. These results are in agreement with the standard model predictions at next-to-next-to-leading order in perturbative quantum chromodynamics and represent an improvement in precision of 25 (29)% for F$$_{0}$$ (F$$_{L}$$) with respect to the most precise single measurement. A limit on anomalous right-handed vector (V$$_{R}$$), and left- and right-handed tensor (g$$_{L}$$, g$$_{R}$$) tWb couplings is set while fixing all others to their standard model values. The allowed regions are [−0.11, 0.16] for V$$_{R}$$, [−0.08, 0.05] for g$$_{L}$$, and [−0.04, 0.02] for g$$_{R}$$, at 95% confidence level. Limits on the corresponding Wilson coefficients are also derived.[graphic not available: see fulltext]« less

The Phase-I upgrade of the trigger readout electronics for the ATLAS Liquid Argon (LAr) calorimeters will be installed during the second long shutdown of the Large Hadron Collider (LHC) in 2019-2020 which will enable enhanced instantaneous luminosities during LHC Run 3 from 2021 through 2023. In this trigger upgrade, so-called supercells are introduced to provide higher granularity, higher resolution and longitudinal shower shape information from the LAr calorimeters to the Level-1 trigger processors. A new LAr Trigger Digitizer Board (LTDB) will process and digitize up to 320 channels of supercell signals, and transmit them via 40 fiber optical links tomore » the back end where the data are further processed and transmitted to the trigger processors. Five pairs of bidirectional GBT links are used for slow control and monitoring between LTDB and the Front-End LInk eXchange (FELIX) in the ATLAS Trigger and Data Acquisition (TDAQ) system. Here, the LTDB also outputs 64 summed analog legacy signals to the current Tower Builder Board via a new baseplane. A test system for the production of 124 LTDBs has been developed, supporting configuration and calibration of all ASICs« less