rmc-discord: reverse Monte Carlo refinement of diffuse scattering and correlated disorder from single crystals

A user-friendly program has been developed to analyze diffuse scattering from single crystals with the reverse Monte Carlo method. The approach allows for refinement of correlated disorder from atomistic supercells with magnetic or structural (occupational and/or displacive) disorder. The program is written in Python and optimized for performance and efficiency. Refinements of two user cases obtained with legacy neutron-scattering data demonstrate the effectiveness of the approach and the developed program. It is shown with bixbyite, a naturally occurring magnetic mineral, that the calculated three-dimensional spin-pair correlations are resolved with finer real-space resolution compared with the pair distribution function calculated directly from the reciprocal-space pattern. With the triangular lattice Ba3Co2O6(CO3)0.7, refinements of occupational and displacive disorder are combined to extract the one-dimensional intra-chain correlations of carbonate molecules that move toward neighboring vacant sites to accommodate strain induced by electrostatic interactions. The program is packaged with a graphical user interface and extensible to serve the needs of single-crystal diffractometer instruments that collect diffuse-scattering data.

Fitting the magnetoresponses of the OLED using polaron pair model to obtain spin-pair dynamics and local hyperfine fields

Organic light-emitting diode (OLED) displays a sign reversal magnetic field effect (MFE) when the applied magnetic field range is reduced to the sub-milliTesla range and the Polaron Pair Model has been successful in explaining the ultra-small MFE. Here, we obtained high resolution (~ 1 µT) magnetoconductance (MC) and magnetoelectroluminescence (MEL) of a tris-(8-hydroxyquinoline)aluminium-based (Alq3) OLED within the magnetic field range of ± 500 µT with the earth magnetic field components cancelled. A clear “W” shaped MC with a dip position of ± 250 µT and a monotonic MEL were observed. We demonstrate a fitting technique using the polaron pair model to the experimentally obtained MC and MEL. The fitting process extracts physically significant parameters within a working OLED: the local hyperfine fields for electron and hole in Alq3: Bhf1 = (0.63 ± 0.01) mT (electron), Bhf2 = (0.24 ± 0.01) mT (hole); the separation rates for singlet and triplet polaron pairs: kS,s = (44.59 ± 0.01) MHz, kT,s = (43.97 ± 0.01) MHz, and the recombination rate for singlet polaron pair kS,r = (88 ± 6) MHz. The yielded parameters are highly reproducible across different OLEDs and are in broad agreement with density functional theory (DFT) calculations and reported experimental observations. This demonstrates the feasibility of this fitting technique to approach any working OLED for obtaining significant microscopic parameters.

Solution NMR readily reveals distinct structural folds and interactions in doubly 13C- and 19F-labeled RNAs

RNAs form critical components of biological processes implicated in human diseases, making them attractive for small-molecule therapeutics. Expanding the sites accessible to nuclear magnetic resonance (NMR) spectroscopy will provide atomic-level insights into RNA interactions. Here, we present an efficient strategy to introduce 19F-13C spin pairs into RNA by using a 5-fluorouridine-5′-triphosphate and T7 RNA polymerase–based in vitro transcription. Incorporating the 19F-13C label in two model RNAs produces linewidths that are twice as sharp as the commonly used 1H-13C spin pair. Furthermore, the high sensitivity of the 19F nucleus allows for clear delineation of helical and nonhelical regions as well as GU wobble and Watson-Crick base pairs. Last, the 19F-13C label enables rapid identification of a small-molecule binding pocket within human hepatitis B virus encapsidation signal epsilon (hHBV ε) RNA. We anticipate that the methods described herein will expand the size limitations of RNA NMR and aid with RNA-drug discovery efforts.

The GHSZ Argument: A Gedankenexperiment Requiring More Denken

I reassess the gedankenexperiment of Greenberger, Horne, Shimony, and Zeilinger after twenty-five years, finding their influential claim to the discovery of an inconsistency inherent in high dimensional formulations of local realism to arise from a fundamental error of logic. They manage this by presuming contradictory premises: that a specific linear combination of four angles involved in their proposed parallel experiments on two pairs of electrons equals both π and 0 at the same time. Ignoring this while presuming the contradictory implications of these two conditions, they introduce the contradiction themselves. The notation they use in their “derivation” is not sufficiently ornate to represent the entanglement in the double electron spin pair problem they design, confounding their error. The situation they propose actually motivates only an understanding of the full array of symmetries involved in their problem. In tandem with the error now recognised in the supposed defiance of Bell’s inequality by quantum probabilities, my reassessment of their work should motivate a reevaluation of the current consensus outlook regarding the principle of local realism and the proposition of hidden variables.

Numerical Precision Effects on GPU Simulation of Massive Spatial Data, Based on the Modified Planar Rotator Model

The present research builds on a recently proposed spatial prediction method for discretized two-dimensional data, based on a suitably modified planar rotator (MPR) spin model from statistical physics. This approach maps the measured data onto interacting spins and, exploiting spatial correlations between them, which are similar to those present in geostatistical data, predicts the data at unmeasured locations. Due to the shortrange nature of the spin pair interactions in the MPR model, parallel implementation of the prediction algorithm on graphical processing units (GPUs) is a natural way of increasing its efficiency. In this work we study the effects of reduced computing precision as well as GPU-based hardware intrinsic functions on the speedup and accuracy of the MPR-based prediction and explore which aspects of the simulation can potentially benefit the most from the reduced precision. It is found that, particularly for massive data sets, a thoughtful precision setting of the GPU implementation can significantly increase the computational efficiency, while incurring little to no degradation in the prediction accuracy.

Generating and sustaining long-lived spin states in 15N,15N′-azobenzene

Long-Lived spin States (LLSs) hold a great promise for sustaining non-thermal spin order and investigating various slow processes by Nuclear Magnetic Resonance (NMR) spectroscopy. Of special interest for such application are molecules containing nearly equivalent magnetic nuclei, which possess LLSs even at high magnetic fields. In this work, we report an LLS in trans-15N,15N′-azobenzene. The singlet state of the 15N spin pair exhibits a long-lived character. We solve the challenging problem of generating and detecting this LLS and further increase the LLS population by converting the much higher magnetization of protons into the 15N singlet spin order. As far as the longevity of this spin order is concerned, various schemes have been tested for sustaining the LLS. Lifetimes of 17 minutes have been achieved at 16.4 T, a value about 250 times longer than the longitudinal relaxation time of 15N in this magnetic field. We believe that such extended relaxation times, along with the photochromic properties of azobenzene, which changes conformation upon light irradiation and can be hyperpolarized by using parahydrogen, are promising for designing new experiments with photo-switchable long-lived hyperpolarization.