Synthesis of ‘unfeasible’ zeolites

R.E.M. thanks the Royal Society and the E.P.S.R.C. (Grants EP/L014475/1, EP/K025112/1 and EP/K005499/1) for funding work in this area. J.Č. and P.N. acknowledge the Czech Science Foundation for the project of the Centre of Excellence (P106/12/G015) and the European Union Seventh Framework Programme (FP7/ 2007-­‐2013) under grant agreement n°604307. The research leading to these results has received funding from the European Union Seventh Framework Programme under Grant Agreement 312483 – ESTEEM2 (Integrated Infrastructure Initiative–I3). We thank Professor Wuzong Zhou and Dr. Fengjiao Yu for their expertise in TEM and Daniel Dawson for help with NMR.Zeolites are porous aluminosilicate materials that have found applications in many different technologies. However, although simulations suggest that there are millions of possible zeolite topologies, only a little over 200 zeolite frameworks of all compositions are currently known, of which about 50 are pure silica materials. This is known as the zeolite conundrum - why have only so few of all the possible structures been made? Several criteria have been formulated to explain why most zeolites are unfeasible synthesis targets. Here we demonstrate the synthesis of two such 'unfeasible' zeolites, IPC-9 and IPC-10, through the assembly-disassembly-organization-reassembly mechanism. These new high-silica zeolites have rare characteristics, such as windows that comprise odd-membered rings. Their synthesis opens up the possibility of preparing other zeolites that have not been accessible by traditional solvothermal synthetic methods. We envisage that these findings may lead to a step change in the number and types of zeolites available for future applications.PostprintPeer reviewe

Quantifying similarity of pore-geometry in nanoporous materials

In most applications of nanoporous materials the pore structure is as important as the chemical composition as a determinant of performance. For example, one can alter performance in applications like carbon capture or methane storage by orders of magnitude by only modifying the pore structure. For these applications it is therefore important to identify the optimal pore geometry and use this information to find similar materials. However, the mathematical language and tools to identify materials with similar pore structures, but different composition, has been lacking. We develop a pore recognition approach to quantify similarity of pore structures and classify them using topological data analysis. This allows us to identify materials with similar pore geometries, and to screen for materials that are similar to given top-performing structures. Using methane storage as a case study, we also show that materials can be divided into topologically distinct classes requiring different optimization strategies

Trapping virtual pores by crystal retro-engineering

Stable guest-free porous molecular crystals are uncommon. By contrast, organic molecular crystals with guest-occupied cavities are frequently observed, but these cavities tend to be unstable and collapse on removal of the guests—this feature has been referred to as ‘virtual porosity’. Here, we show how we have trapped the virtual porosity in an unstable low-density organic molecular crystal by introducing a second molecule that matches the size and shape of the unstable voids. We call this strategy ‘retro-engineering’ because it parallels organic retrosynthetic analysis, and it allows the metastable two-dimensional hexagonal pore structure in an organic solvate to be trapped in a binary cocrystal. Unlike the crystal with virtual porosity, the cocrystal material remains single crystalline and porous after removal of guests by heating

OpenSHMEM Application Programming Interface, v1.0 Final

This document defines the elements of the OpenSHMEM Application Programming Interface. The purpose of the OpenSHMEM API is to provide programmers with a standard interface for writing parallel programs using C, C++ and Fortran with one-sided communication

First Measurement of Differential Cross Sections for Muon Neutrino Charged Current Interactions on Argon with a Two-proton Final State in the MicroBooNE Detector

We present the first measurement of differential cross sections for charged-current muon neutrino interactions on argon with one muon, two protons, and no pions in the final state. Such interactions leave the target nucleus in a two-particle two-hole state; these states are of great interest, but currently there is limited information about their production in neutrino-nucleus interactions. Detailed investigations of the production of two-particle two-hole states are vital to support upcoming experiments exploring the nature of the neutrino, and the development of the liquid-argon time-projection-chamber has made possible the isolation of such final states. The opening angle between the two protons, the angle between the total proton momentum and the muon, and the total transverse momentum of the final state system are sensitive to the underlying physics processes as embodied in a variety of models. Realistic initial-state momentum distributions are shown to be important in reproducing the data.Comment: To be submitted to PR

Measurement of triple-differential inclusive muon-neutrino charged-current cross section on argon with the MicroBooNE detector

We report the first measurement of the differential cross section $d^{2}\sigma (E_{\nu})/ d\cos(\theta_{\mu}) dP_{\mu}$ for inclusive muon-neutrino charged-current scattering on argon. This measurement utilizes data from 6.4$\times10^{20}$ protons on target of exposure collected using the MicroBooNE liquid argon time projection chamber located along the Fermilab Booster Neutrino Beam with a mean neutrino energy of approximately 0.8~GeV. The mapping from reconstructed kinematics to truth quantities, particularly from reconstructed to true neutrino energy, is validated by comparing the distribution of reconstructed hadronic energy in data to that of the model prediction in different muon scattering angle bins after conditional constraint from the muon momentum distribution in data. The success of this validation gives confidence that the missing energy in the MicroBooNE detector is well-modeled in simulation, enabling the unfolding to a triple-differential measurement over muon momentum, muon scattering angle, and neutrino energy. The unfolded measurement covers an extensive phase space, providing a wealth of information useful for future liquid argon time projection chamber experiments measuring neutrino oscillations. Comparisons against a number of commonly used model predictions are included and their performance in different parts of the available phase-space is discussed

Measurement of the differential cross section for neutral pion production in charged-current muon neutrino interactions on argon with the MicroBooNE detector

We present a measurement of neutral pion production in charged-current interactions using data recorded with the MicroBooNE detector exposed to Fermilab's booster neutrino beam. The signal comprises one muon, one neutral pion, any number of nucleons, and no charged pions. Studying neutral pion production in the MicroBooNE detector provides an opportunity to better understand neutrino-argon interactions, and is crucial for future accelerator-based neutrino oscillation experiments. Using a dataset corresponding to $6.86 \times 10^{20}$ protons on target, we present single-differential cross sections in muon and neutral pion momenta, scattering angles with respect to the beam for the outgoing muon and neutral pion, as well as the opening angle between the muon and neutral pion. Data extracted cross sections are compared to generator predictions. We report good agreement between the data and the models for scattering angles, except for an over-prediction by generators at muon forward angles. Similarly, the agreement between data and the models as a function of momentum is good, except for an underprediction by generators in the medium momentum ranges, $200-400$ MeV for muons and $100-200$ MeV for pions

First measurement of η\eta production in neutrino interactions on argon with MicroBooNE

We present a measurement of $\eta$ production from neutrino interactions on argon with the MicroBooNE detector. The modeling of resonant neutrino interactions on argon is a critical aspect of the neutrino oscillation physics program being carried out by the DUNE and Short Baseline Neutrino programs. $\eta$ production in neutrino interactions provides a powerful new probe of resonant interactions, complementary to pion channels, and is particularly suited to the study of higher-order resonances beyond the $\Delta(1232)$. We measure a flux-integrated cross section for neutrino-induced $\eta$ production on argon of $3.22 \pm 0.84 \; \textrm{(stat.)} \pm 0.86 \; \textrm{(syst.)}$ $10^{-41}{\textrm{cm}}^{2}$/nucleon. By demonstrating the successful reconstruction of the two photons resulting from $\eta$ production, this analysis enables a novel calibration technique for electromagnetic showers in GeV accelerator neutrino experiments

First demonstration of O(1 ns)\mathcal{O}(1\,\text{ns}) timing resolution in the MicroBooNE liquid argon time projection chamber

MicroBooNE is a neutrino experiment located in the Booster Neutrino Beamline (BNB) at Fermilab, which collected data from 2015 to 2021. MicroBooNE's liquid argon time projection chamber (LArTPC) is accompanied by a photon detection system consisting of 32 photomultiplier tubes used to measure the argon scintillation light and determine the timing of neutrino interactions. Analysis techniques combining light signals and reconstructed tracks are applied to achieve a neutrino interaction time resolution of $\mathcal{O}(1\,\text{ns})$. The result obtained allows MicroBooNE to access the ns neutrino pulse structure of the BNB for the first time. The timing resolution achieved will enable significant enhancement of cosmic background rejection for all neutrino analyses. Furthermore, the ns timing resolution opens new avenues to search for long-lived-particles such as heavy neutral leptons in MicroBooNE, as well as in future large LArTPC experiments, namely the SBN program and DUNE

First search for dark-trident processes using the MicroBooNE detector

We present a first search for dark-trident scattering in a neutrino beam using a data set corresponding to $7.2 \times 10^{20}$ protons on target taken with the MicroBooNE detector at Fermilab. Proton interactions in the neutrino target at the Main Injector produce $\pi^0$ and $\eta$ mesons, which could decay into dark-matter (DM) particles mediated via a dark photon $A^\prime$. A convolutional neural network is trained to identify interactions of the DM particles in the liquid-argon time projection chamber (LArTPC) exploiting its image-like reconstruction capability. In the absence of a DM signal, we provide limits at the $90\%$ confidence level on the squared kinematic mixing parameter $\varepsilon^2$ as a function of the dark-photon mass in the range $10\le M_{A^\prime}\le 400$ MeV. The limits cover previously unconstrained parameter space for the production of fermion or scalar DM particles $\chi$ for two benchmark models with mass ratios $M_{\chi}/M_{A^\prime}=0.6$ and $2$ and for dark fine-structure constants $0.1\le\alpha_D\le 1$