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At least 235 records · Page 13

On the statistical treatment of the Cabibbo angle anomaly

We point out that testing the equality of the Cabibbo angle as extracted from $\Gamma(K\rightarrow \pi l\nu)$, the ratio $\Gamma(K\rightarrow l\nu)/\Gamma(\pi\rightarrow l\nu)$ and nuclear $\beta$ decays is not identical to a test of first row unitarity of the Cabibbo-Kobayashi-Maskawa (CKM) matrix. The reason is that a CKM unitarity test involves only two parameters, while the degrees of freedom for the assessment of the goodness-of-fit of the universality of the Cabibbo angle entailed by the Standard Model (SM) is equal to the number of measurements minus one. Beyond the SM all different processes could in principle give different Cabibbo angles. Consequently, the difference between the two tests becomes relevant starting from three observables giving results for the Cabibbo angle that are in tension with each other. With current data, depending on the treatment of the nuclear $\beta$ decays, we find that New Physics is favored over the SM at $5.1\,\sigma$ or $3.6\,\sigma$ while CKM unitarity is rejected at $4.8\sigma$ or $3.0\sigma$, respectively. We argue that the best method to test the SM is to test the equality of the Cabibbo angle, because CKM unitarity is only one aspect of the SM.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Gravity-improved metastability bounds for the Type-I seesaw mechanism

Right-handed neutrinos (RHN) destabilize the electroweak vacuum by increasing its decay rate. In the SM, the latter is dominated by physics at the RG scale at which λ reaches its minimum, ${\mu}_{\ast}^{\textrm{SM}}$ ~10 17 GeV. For large neutrino Yukawa coupling Y ν , RHNs can push μ* beyond the Planck scale, implying that gravitational effects need to be taken into account. In this work, we perform the first comprehensive study of electroweak vacuum metastability in the type-I seesaw mechanism including these effects. Our analysis covers both low- and high-scale seesaw models, with two as well as three RHNs and for multiple values of the Higgs’ non-minimal coupling to gravity. We find that gravitational effects can significantly stabilize the vacuum, leading to weaker metastability bounds. We show that metastability sets the strongest bounds for low-scale seesaws with M N > 1 TeV. For high-scale seesaws, we find upper bounds on the allowed masses for the RHNs, which are relevant for high-scale leptogenesis. We also point out that Tr(${Y}_{\nu}^{\dagger}$Y ν ), which is commonly used to express these metastability bounds, cannot be used for all of parameter space. Instead, we argue that bounds can always be expressed reliably through Tr(${Y}_{\nu}^{\dagger}$Y ν ${Y}_{\nu}^{\dagger}$Y ν ). Lastly, we use this insight to develop a new technique for an easier RG analysis applicable to scenarios with degenerate RHN masses.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Indirect constraints on third generation baryon number violation

Abstract The non-observation of baryon number violation suggests that the scale of baryon-number violating interactions at zero temperature is comparable to the GUT scale. However, the pertinent measurements involve hadrons made of the first-generation quarks, such as protons and neutrons. One may therefore entertain the idea that new flavour physics breaks baryon number at a much lower scale, but only in the coupling to a third generation quark, leading to observable baryon-number violatingb-hadron decay rates. In this paper we show that indirect constraints on the new physics scale Λ BNV from the existing bounds on the proton lifetime do not allow for this possibility. For this purpose we consider the three dominant proton decay channelsp→$$ {\ell}^{+}{\nu}_{\ell}\overline{\nu} $$ ℓ + ν ℓ ν ¯ ,p→$$ {\pi}^{+}\overline{\nu} $$ π + ν ¯ andp→π 0 ℓ + mediated by a virtual bottom quark.

Physics↗

Applying design principles to improve hydrogen storage capacity in nanoporous materials

Hydrogen is an attractive option for energy storage because it can be produced from renewable sources and produces environmentally benign byproducts. However, the volumetric energy density of molecular hydrogen at ambient conditions is low compared to other storage methods like batteries, so it must be compressed to attain a viable energy density for applications such as transportation. Nanoporous materials have attracted significant interest for gas storage because they can attain high storage density at lower pressure than conventional compression. Here, we examine how to improve the cryogenic hydrogen storage capacity of a series of porous aromatic frameworks (PAFs) by controlling the pore size and increasing the surface area by adding functional groups. We also explore tradeoffs in gravimetric and volumetric measures of the hydrogen storage capacity and the effects of temperature swings using grand canonical Monte Carlo simulations. We also consider the effects of adding functional groups to the metal–organic framework NU-1000 to improve its hydrogen storage capacity. We find that highly flexible alkane chains do not improve the hydrogen storage capacity in NU-1000 because they do not extend into the pores; however, rigid chains containing alkyne groups do increase the surface area and hydrogen storage capacity. Finally, we demonstrate that the deliverable capacity of hydrogen in NU-1000 can be increased from 40.0 to 45.3 g/L (at storage conditions of 100 bar and 77 K and desorption conditions of 5 bar and 160 K) by adding long, rigid alkyne chains into the pores.

08 HYDROGEN↗

Heat transport and temperature boundary-layer profiles in closed turbulent Rayleigh–Bénard convection with slippery conducting surfaces

Here, we report direct numerical simulations (DNS) of the Nusselt number Nu , the vertical profiles of mean temperature Θ(z) and temperature variance Ω(z) across the thermal boundary layer (BL) in closed turbulent Rayleigh–Bénard convection (RBC) with slippery conducting surfaces ( z is the vertical distance from the bottom surface). The DNS study was conducted in three RBC samples: a three-dimensional cuboid with length L=H and width W=H/4 ( H is the sample height), and two-dimensional rectangles with aspect ratios Γ≡L/H=1 and 10. The slip length b for top and bottom plates varied from 0 to ∞ . The Rayleigh numbers Ra were in the range 10 6 $⩽$Ra$⩽$10 10 and the Prandtl number Pr was fixed at 4.3 . As b increases, the normalised Nu/Nu 0 ( Nu 0 is the global heat transport for b =0 ) from the three samples for different Ra and Γ can be well described by the same function Nu/Nu 0 = N 0 tanh( b /λ 0 )+1 , with N 0 =0.8±0.03 . Here λ 0 ≡ L /(2 Nu 0 ) is the thermal boundary layer thickness for b =0 . Considering the BL fluctuations for Pr >1, one can derive solutions of temperature profiles Θ(z) and Ω(z) near the thermal BL for b $⩾$ 0 . When b =0 , the solutions are equivalent to those reported by Shishkina et al. ( Phys. Rev. Lett. , vol. 114, 2015, 114302) and Wang et al. ( Phys. Rev. Fluids , vol. 1, 2016, 082301(R)), respectively, for no-slip plates. For b >0, the derived solutions are in excellent agreement with our DNS data for slippery plates.

42 ENGINEERING↗

Vapor-Phase Cyclohexene Epoxidation by Single-Ion Fe(III) Sites in Metal–Organic Frameworks

Heterogeneous catalysts supported on metal–organic frameworks (MOFs), which possess uniform porosity and crystallinity, have attracted significant interest for recent years due to the ease of active-site characterization via X-ray diffraction and the subsequent relation of the active site structure to the catalytic activity. We report the syntheses, structures, and oxidation catalytic activities of single-ion iron catalysts incorporated into the zirconium MOF NU-1000. Single-ion iron catalysts with different counteranions were anchored onto the Zr node through postsynthetic solvothermal deposition. Crystallographic characterization of the resulting MOFs (NU-1000-Fe-Cl and NU-1000-Fe-NO 3 ) revealed that, while both frameworks have similar Fe coordination, the distance between Fe and the Zr 6 node differs significantly between the two. Lastly, the product rate profiles of the two catalysts for vapor-phase cyclohexene epoxidation demonstrate different initial rates and product formations, likely originating from the different Fe–O distances.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Photogenerated Charge Separation in a CdSe Nanocluster Encapsulated in a Metal–Organic Framework for Improved Photocatalysis

Nanoclusters encapsulated in a metal–organic framework (MOF) are the subject of intense interest because of their high promise for photocatalysis. We show computationally that a CdSe nanocluster incorporated into NU-1000 (Cd 6 Se 6 @NU-1000) allows electron transfer from a visible-light photo-excited organic linker to the lowest unoccupied crystal orbital of the inorganic cluster, which can lead to charge separation. Substituents on the linker can be used to tune the band position and the band gap of the whole composite (Cd 6 Se 6 @NU-1000), and this makes it possible to perform the water splitting reaction under visible light. Here, the achievement of charge separation within the MOF leads to longer life of the excited states, and as a result, it can enhance the photocatalytic activity of the system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Investigating the Influence of Hexanuclear Clusters in Isostructural Metal–Organic Frameworks on Toxic Gas Adsorption

The efficient capture of toxic gases, such as ammonia (NH 3 ) and sulfur dioxide (SO 2 ), can protect the general population and mitigate widespread air pollution. Metal–organic frameworks (MOFs) comprise a tunable class of adsorbents with high surface areas that can meet this challenge by selectively capturing these gases at low concentrations. In this work, we explored how modifying the metal ions in the node of an isostructural MOF series from a transition metal to a lanthanide or actinide influences the electronic environment of the node-based active site. Next, we investigated the adsorption properties of each MOF toward the relatively basic NH 3 and relatively acidic SO 2 gases. Within the NU-907 family of MOFs, we found that Zr 6 -NU-907 exhibits the best uptake toward NH 3 at low pressures, while Th 6 -NU-907 demonstrates the best low-pressure performance for SO 2 adsorption. Here, tracking the infrared (IR) stretching frequency of the node-based μ 3 -OH groups provides insights into the electronegativity of the metal ion and suggests that the most electronegative metal ion (Zr) affords the node with the best NH 3 uptake at low pressures. In contrast, the Th 6 node contains additional coordinated water groups relative to the other M 6 nodes, which appears to yield the MOF with the greatest affinity for SO 2 uptake that occurs predominately through reversible physisorption interactions. Finally, in situ NH3 IR spectroscopic studies indicate that both NH 4 + and Lewis-bound NH 3 species form during adsorption. Combined, these results suggest that tuning the electronic properties and structure of the node-based active site in an MOF presents a viable strategy to change the affinity of an MOF toward toxic gases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Unexpected “Spontaneous” Evolution of Catalytic, MOF-Supported Single Cu(II) Cations to Catalytic, MOF-Supported Cu(0) Nanoparticles

A desirable feature of metal–organic frameworks (MOFs) is their well-defined structural periodicity and the presence of well-defined catalyst grafting sites (e.g., reactive –OH and –OH 2 groups) that can support single-site heterogeneous catalysts. However, one should not overlook the potential role of residual organic moieties, specifically formate ions that can occupy the catalyst anchoring sites during MOF synthesis. Here we show how these residual formate species in a Zr-based MOF, NU-1000, critically alter the structure, redox capability, and catalytic activity of postsynthetically incorporated Cu(II) ions. Single-crystal X-ray diffraction measurements established that there are two structurally distinct types of Cu(II) ions in NU-1000: one type with residual formate and one without. In NU-1000 with formate, Cu(II) solely binds to the node via the formate-unoccupied, bridging μ 3 –OH, whereas in the formate-free case, it displaces protons from two node hydroxo ligands and resides close to the terminal –OH 2 . Under an inert atmosphere, node-bound formate facilitates the unanticipated reduction of isolated Cu(II) to nanoparticulate Cu(0)—a behavior which is essentially absent in the formate-free analogue because no other sacrificial reductant is present. When the two MOFs were tested as benzyl alcohol oxidation catalysts, we observed that residual formate boosts the catalytic turnover frequency. Density functional calculations showed that node-bound formate acts as a sacrificial two-electron donor and assists in reducing Cu(II) to Cu(0) by a nonradical pathway. The negative Gibbs free energy of reaction (ΔG) and enthalpy of reaction (ΔH) indicate that the reduction is thermodynamically favorable. Here, the work presented here highlights how the often-neglected residual formate prevalent in nearly all zirconium-based MOFs can significantly modulate the properties of supported catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Photocatalytic Biocidal Coatings Featuring Zr 6 Ti 4 -Based Metal–Organic Frameworks

The world is currently suffering socially, economically, and politically from the recent pandemic outbreak due to the Coronavirus Disease 2019 (COVID-19), and those in hospitals, schools, and elderly nursing homes face enhanced threats. Healthcare textiles, such as masks and medical staff gowns, are susceptible to contamination of various pathogenic microorganisms, including bacteria and viruses. Here, metal–organic frameworks (MOFs) can potentially address these challenges due to their tunable reactivity and ability to be incorporated as porous coatings on textile materials. Here, we report how incorporating titanium into the zirconium-pyrene-based MOF NU-1000, denoted as NU-1012, generates a highly reactive biocidal photocatalyst. This MOF features a rare ligand migration phenomenon, and both the Ti/Zr center and the pyrene linker act synergistically as dual active centers and widen the absorption band for this material that results in enhanced reactive oxygen species (ROS) generation upon visible light irradiation. Additionally, we found the ligand migration process is generally applicable to other csq topology Zr-MOFs. Importantly, NU-1012 can be easily incorporated onto cotton textile cloths as a coating, and the resulting composite material demonstrates fast and potent biocidal activity against Gram-negative bacteria (E. coli), Gram-positive bacteria (S. epidermidis), and T7 bacteriophage virus with up to a 7-log (99.99999%) reduction within one hour under simulated daylight.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Three-state majority-vote model on small-world networks

Abstract In this work, we study the opinion dynamics of the three-state majority-vote model on small-world networks of social interactions. In the majority-vote dynamics, an individual adopts the opinion of the majority of its neighbors with probability 1- q , and a different opinion with chance q , where q stands for the noise parameter. The noise q acts as a social temperature, inducing dissent among individual opinions. With probability p , we rewire the connections of the two-dimensional square lattice network, allowing long-range interactions in the society, thus yielding the small-world property present in many different real-world systems. We investigate the degree distribution, average clustering coefficient and average shortest path length to characterize the topology of the rewired networks of social interactions. By employing Monte Carlo simulations, we investigate the second-order phase transition of the three-state majority-vote dynamics, and obtain the critical noise $$q_c$$ q c , as well as the standard critical exponents $$\beta /\nu$$ β / ν , $$\gamma /\nu$$ γ / ν , and $$1/\nu$$ 1 / ν for several values of the rewiring probability p . We conclude that the rewiring of the lattice enhances the social order in the system and drives the model to different universality classes from that of the three-state majority-vote model in two-dimensional square lattices.

99 GENERAL AND MISCELLANEOUS↗

Homogeneous versus MOF-supported catalysis: a direct comparison of catalytic hydroboration with Ni tripodal P 3 E (E = Si, Ge) complexes

The MOF material NU-1000 was employed to host Ni tripodal complexes prepared from new organometallic precursors [HNi(κ 4 (E,P,P,P)-E(o-C 6 H 4 CH 2 PPh 2 ) 3 ], E = Si (Ni-1), Ge (Ni-2). The new heterogeneous catalytic materials, Ni-1@NU-1000 and Ni-2@NU-1000, show the advantages of both homogeneous and heterogeneous catalysts. Finally, they catalyze the hydroboration of aldehydes and ketones more efficiently than the homogeneous Ni-1 and Ni-2, under aerobic conditions and show recyclability.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Toward Verification of RANS Simulations of the T-Tube Modular Divertor Using Large Eddy Simulations of Impinging Turbulent Plane Jets

Turbulent impinging jets have been proposed to cool high heat flux plasma-facing components such as the solid tungsten target plates of the divertor in long-pulse magnetic fusion energy reactors. In particular, the T-tube modular divertor, originally developed by the ARIES Team, consists of two concentric cylindrical tubes where helium flows through a slot in the inner tube, forming an approximately planar jet that impinges upon and cools the inner surface of the pressure boundary (namely, the outer tube) and the ~15-cm 2 plasma-facing W target. The objective of this work is to demonstrate that large eddy simulations (LESs) accurately simulate the thermal transport in canonical flows that comprise the cooling flow in the T-tube, as well as validate temperatures from LES with experimental measurements in a simplified T-tube geometry. Wall‑resolved LESs, validated by experimental data and verified by direct numerical simulations (DNSs), provide benchmark data for two canonical flows in the T‑tube, namely, planar impinging and wall jets, for Reynolds numbers Re B = 4 × 10 3 to 2 × 10 4 . Our LES results are within 4% to 12% root-mean-square error (RMSE) of surface Nusselt number distributions (Nu) from experiments and DNSs. The validated LES results are then used as the ground truth to evaluate four Reynolds‑averaged Navier-Stokes (RANS) turbulence closures, namely, the k‑ω SST, realizable k‑ε, GEKO, and γ‑SST models. The k‑ω SST model has the best overall performance in terms of heat transfer, giving surface Nu within 12% RMSE of the LES results for high‑ReB impinging jets and reduced overprediction in the wall‑jet region. The GEKO model with default constants has the next best performance, providing slightly better Nu predictions for low ReB impinging jets (versus k-ω SST) but worse overall performance over the full range of ReB studied here. The realizable k‑ε turbulence model significantly overestimates turbulence near the stagnation point, while the γ‑SST model suppresses near‑wall production, biasing the simulations toward simulating laminar surface heat transfer. Simulations of the simplified T‑tube show that LES and RANS simulations with the k‑ω SST model give nearly identical average heat transfer coefficients (HTCs) over the impingement surface. The realizable k‑ε model predicts significantly lower wall temperatures due to overestimation of HTC in the outlet flow.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Use of Neutrino Scattering Events with Low Hadronic Recoil to Inform Neutrino Flux and Detector Energy Scale

Charged-current neutrino interactions with low hadronic recoil ("low-nu") have a cross-section that is approximately constant versus neutrino energy. These interactions have been used to measure the shape of neutrino fluxes as a function of neutrino energy at accelerator-based neutrino experiments such as CCFR, NuTeV, MINOS and MINERvA. In this paper, we demonstrate that low-nu events can be used to measure parameters of neutrino flux and detector models and that utilization of event distributions over the upstream detector face can discriminate among parameters that affect the neutrino flux model. From fitting a large sample of low-nu events obtained by exposing MINERvA to the NuMI medium-energy beam, we find that the best-fit flux parameters are within their a priori uncertainties, but the energy scale of muons reconstructed in the MINOS detector is shifted by 3.6% (or 1.8 times the a priori uncertainty on that parameter). These fit results are now used in all MINERvA cross-section measurements, and this technique can be applied by other experiments operating at MINERvA energies, such as DUNE.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Charge Ordering and Low-Temperature Lattice Distortion in the {beta}'-(BDT-TTF){sub 2}CF{sub 3}CF{sub 2}SO{sub 3} Dime Mott Insulator.

We present single-crystal x-ray diffraction measurements, optical investigations, and electronic structure calculations for the organic charge-transfer salt beta'-(BEDT-TTF)(2)CF3CF2SO3 synthesized by electrocrystallization. Electronic structure calculations confirm the quasi-one-dimensional behavior of the compound and optical conductivity measurements reveal the dimer-Mott insulating nature of the system. The splitting of the charge-sensitive nu(2) mode in Raman spectra demonstrates the onset of an interlayer charge-ordered phase below 25 K, also suggested by the crystal structure considerations. This transition is accompanied by clear signatures of a lattice distortion in the BEDT-TTF donor layer, as shown by a splitting of the vibrational nu(3) mode in infrared spectra. At the same time, the sharp redshift of the nu(1) mode involving the BEDT-TTF ethylene groups strongly suggests a significant modification of the hydrogen-type bonding present between the BEDT-TTF donor layer and the CF3CF2SO3- anion layer. These observations point to a subtle interplay of charge and lattice degrees of freedom at the phase transition.

Olejniczak, I.↗

Improved Limit on Neutrinoless Double-Beta Decay in Te 130 with CUORE

We report new results from the search for neutrinoless double-beta decay in $^{130}$Te with the CUORE detector. This search benefits from a four-fold increase in exposure, lower trigger thresholds and analysis improvements relative to our previous results. We observe a background of $(1.38\pm0.07)\cdot10^{-2}$ counts$/($keV$\cdot$kg$\cdot$yr$)$ in the $0\nu\beta\beta$ decay region of interest and, with a total exposure of 372.5 kg$\cdot$yr, we attain a median exclusion sensitivity of $1.7\cdot10^{25}$ yr. We find no evidence for $0\nu\beta\beta$ decay and set a $90\%$ CI Bayesian lower limit of $3.2\cdot10^{25}$ yr on the $^{130}$Te half-life for this process. In the hypothesis that $0\nu\beta\beta$ decay is mediated by light Majorana neutrinos, this results in an upper limit on the effective Majorana mass of 75-350 meV, depending on the nuclear matrix elements used.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Balancing volumetric and gravimetric uptake in highly porous materials for clean energy

A huge challenge facing scientists is the development of adsorbent materials that exhibit ultrahigh porosity but maintain balance between gravimetric and volumetric surface areas for the onboard storage of hydrogen and methane gas—alternatives to conventional fossil fuels. Here we report the simulation-motivated synthesis of ultraporous metal–organic frameworks (MOFs) based on metal trinuclear clusters, namely, NU-1501-M (M = Al or Fe). Relative to other ultraporous MOFs, NU-1501-Al exhibits concurrently a high gravimetric Brunauer–Emmett–Teller (BET) area of 7310 m 2 g -1 and a volumetric BET area of 2060 m 2 cm -3 while satisfying the four BET consistency criteria. The high porosity and surface area of this MOF yielded impressive gravimetric and volumetric storage performances for hydrogen and methane: NU-1501-Al surpasses the gravimetric methane storage U.S. Department of Energy target (0.5 g g -1 ) with an uptake of 0.66 g g -1 [262 cm 3 (standard temperature and pressure, STP) cm -3 ] at 100 bar/270 K and a 5- to 100-bar working capacity of 0.60 g g -1 [238 cm 3 (STP) cm -3 ] at 270 K; it also shows one of the best deliverable hydrogen capacities (14.0 weight %, 46.2 g liter -1 ) under a combined temperature and pressure swing (77 K/100 bar → 160 K/5 bar).

Science & Technology - Other Topics↗

A first-in-human phase 0 clinical study of RNA interference–based spherical nucleic acids in patients with recurrent glioblastoma

Glioblastoma (GBM) is one of the most difficult cancers to effectively treat, in part because of the lack of precision therapies and limited therapeutic access to intracranial tumor sites due to the presence of the blood-brain and blood-tumor barriers. We have developed a precision medicine approach for GBM treatment that involves the use of brain-penetrant RNA interference–based spherical nucleic acids (SNAs), which consist of gold nanoparticle cores covalently conjugated with radially oriented and densely packed small interfering RNA (siRNA) oligonucleotides. On the basis of previous preclinical evaluation, we conducted toxicology and toxicokinetic studies in nonhuman primates and a single-arm, open-label phase 0 first-in-human trial ( NCT03020017 ) to determine safety, pharmacokinetics, intratumoral accumulation and gene-suppressive activity of systemically administered SNAs carrying siRNA specific for the GBM oncogene Bcl2Like12 (Bcl2L12). Patients with recurrent GBM were treated with intravenous administration of siBcl2L12-SNAs (drug moniker: NU-0129), at a dose corresponding to 1/50th of the no-observed-adverse-event level, followed by tumor resection. Safety assessment revealed no grade 4 or 5 treatment–related toxicities. Inductively coupled plasma mass spectrometry, x-ray fluorescence microscopy, and silver staining of resected GBM tissue demonstrated that intravenously administered SNAs reached patient tumors, with gold enrichment observed in the tumor-associated endothelium, macrophages, and tumor cells. NU-0129 uptake into glioma cells correlated with a reduction in tumor-associated Bcl2L12 protein expression, as indicated by comparison of matched primary tumor and NU-0129–treated recurrent tumor. Our results establish SNA nanoconjugates as a potential brain-penetrant precision medicine approach for the systemic treatment of GBM.

60 APPLIED LIFE SCIENCES↗