Building Fluorinated Hybrid Crystals: Understanding the Role of Noncovalent Interactions

Noncovalent interactions play a key role in functional materials. Metal-organofluorine interactions are of special interest because they directly affect the structure and reactivity of hybrid fluorinated materials. In-depth understanding and modulating of these interactions would enable the rational design of functional materials from fundamental chemical principles. In this work, we propose a computational approach that enables a comprehensive and quantitative characterization of noncovalent interactions (NCIs) in hybrid fluorinated crystals. Our approach couples dispersion-corrected density functional theory to NCI analysis. Additionally, we determine electron densities at bond critical points and identify electrostatic interactions using a simple electrostatic model. The versatility of this approach to probe a wide range of NCIs is demonstrated for a series of four bimetallic fluorinated crystals incorporating alkali-manganese(II) pairs and trifluoroacetato ligands. Noncovalent interactions in these hybrid crystals include metal-oxygen, metal-fluorine, hydrogen bonds, and van der Waals forces. Using K2Mn2(tfa)6(tfaH)2·H2O as an example, we demonstrate that its two-dimensional layered structure stems from a unique balance between these four NCIs. The computational approach presented herein should have general applicability to the quantitative study of NCIs in hybrid crystals, thereby serving as a guide for crystal engineering of novel hybrid materials

Hybrid turbidite-drift channel complexes: An integrated multiscale model

The interaction of deep-marine bottom currents with episodic, unsteady sediment gravity flows affects global sediment transport, forms climate archives, and controls the evolution of continental slopes. Despite their importance, contradictory hypotheses for reconstructing past flow regimes have arisen from a paucity of studies and the lack of direct monitoring of such hybrid systems. Here, we address this controversy by analyzing deposits, high-resolution seafloor data, and near-bed current measurements from two sites where eastward-flowing gravity flows interact(ed) with northward-flowing bottom currents. Extensive seismic and core data from offshore Tanzania reveal a 1650-m-thick asymmetric hybrid channel levee-drift system, deposited over a period of ∼20 m.y. (Upper Cretaceous to Paleocene). High-resolution modern seafloor data from offshore Mozambique reveal similar asymmetric channel geometries, which are related to northward-flowing near-bed currents with measured velocities of up to 1.4 m/s. Higher sediment accumulation occurs on the downstream flank of channel margins (with respect to bottom currents), with inhibited deposition or scouring on the upstream flank (where velocities are highest). Toes of the drift deposits, consisting of thick laminated muddy siltstone, which progressively step back into the channel axis over time, result in an interfingering relationship with the sandstone-dominated channel fill. Bottom-current flow directions contrast with those of previous models, which lacked direct current measurements or paleoflow indicators. We finally show how large-scale depositional architecture is built through the temporally variable coupling of these two globally important sediment transport processes. Our findings enable more-robust reconstructions of past oceanic circulation and diagnosis of ancient hybrid turbidite-drift systems

Resummations of free energy at high temperature

We discuss resummation strategies for free energy in quantum field theories at nonzero temperatures T. We point out that resummations should be performed for the short- and long-distance parts separately in order to avoid spurious interference effects and double-counting. We then discuss and perform Pade resummations of these two parts for QCD at high T. The resummed results are almost invariant under variation of the renormalization and factorization scales. We perform the analysis also in the case of the massless scalar $\phi^4$ theory.Comment: 16 pages, revtex4, 15 eps-figures; minor typographic errors corrected; the version as it appears in Phys.Rev.

Calculations of binding energies and masses of heavy quarkonia using renormalon cancellation

We use various methods of Borel integration to calculate the binding ground energies and masses of b-bbar and t-tbar quarkonia. The methods take into account the leading infrared renormalon structure of the hard+soft part of the binding energies E(s), and of the corresponding quark pole masses m_q, where the contributions of these singularities in M(s) = 2 m_q + E(s) cancel. Beforehand, we carry out the separation of the binding energy into its hard+soft and ultrasoft parts. The resummation formalisms are applied to expansions of m_q and E(s) in terms of quantities which do not involve renormalon ambiguity, such as MSbar quark mass, and alpha_s. The renormalization scales are different in calculations of m_q, E(s) and E(us). The MSbar mass of b quark is extracted, and the binding energies of t-tbar and the peak (resonance) energies for (t+tbar) production are obtained.Comment: 23 pages, 8 double figures, revtex4; the version to appear in Phys.Rev.D; extended discussion between Eqs.(25) and (26); the paragraph between Eqs.(32) and (33) is new and explains the numerical dependence of the residue parameter on the factorization scale; several new references were added; acknowledgments were modified; the numerical results are unchange

Erratum: "The ALMA Survey of 70micron dark High-mass Clumps in Early Stages (ASHES). IV. Star formation signatures in G023.477" (2021, ApJ, 923, 147)

This is a correction for 2021 ApJ 923 147DOI 10.3847/1538-4357/ac2365Interstellar matter and star formatio

The ALMA survey of 70 μm dark high-mass clumps in early stages (ASHES): IV. Star formation signatures in G023.477

Interstellar matter and star formatio

Search for the standard model Higgs boson decaying into two photons in pp collisions at sqrt(s)=7 TeV

A search for a Higgs boson decaying into two photons is described. The analysis is performed using a dataset recorded by the CMS experiment at the LHC from pp collisions at a centre-of-mass energy of 7 TeV, which corresponds to an integrated luminosity of 4.8 inverse femtobarns. Limits are set on the cross section of the standard model Higgs boson decaying to two photons. The expected exclusion limit at 95% confidence level is between 1.4 and 2.4 times the standard model cross section in the mass range between 110 and 150 GeV. The analysis of the data excludes, at 95% confidence level, the standard model Higgs boson decaying into two photons in the mass range 128 to 132 GeV. The largest excess of events above the expected standard model background is observed for a Higgs boson mass hypothesis of 124 GeV with a local significance of 3.1 sigma. The global significance of observing an excess with a local significance greater than 3.1 sigma anywhere in the search range 110-150 GeV is estimated to be 1.8 sigma. More data are required to ascertain the origin of this excess.Comment: Submitted to Physics Letters

Search for a W' boson decaying to a bottom quark and a top quark in pp collisions at sqrt(s) = 7 TeV

Results are presented from a search for a W' boson using a dataset corresponding to 5.0 inverse femtobarns of integrated luminosity collected during 2011 by the CMS experiment at the LHC in pp collisions at sqrt(s)=7 TeV. The W' boson is modeled as a heavy W boson, but different scenarios for the couplings to fermions are considered, involving both left-handed and right-handed chiral projections of the fermions, as well as an arbitrary mixture of the two. The search is performed in the decay channel W' to t b, leading to a final state signature with a single lepton (e, mu), missing transverse energy, and jets, at least one of which is tagged as a b-jet. A W' boson that couples to fermions with the same coupling constant as the W, but to the right-handed rather than left-handed chiral projections, is excluded for masses below 1.85 TeV at the 95% confidence level. For the first time using LHC data, constraints on the W' gauge coupling for a set of left- and right-handed coupling combinations have been placed. These results represent a significant improvement over previously published limits.Comment: Submitted to Physics Letters B. Replaced with version publishe