The suite of neutron powder diffractometers at Oak Ridge National Laboratory (ORNL) utilizes the distinct characteristics of the Spallation Neutron Source and High Flux Isotope Reactor to enable the measurements of powder samples over an unparalleled regime at a single laboratory. Full refinements over large Q ranges, total scattering methods, fast measurements under changing conditions, and a wide array of sample environments are available. This article provides a brief overview of each powder instrument at ORNL and details the complementarity across the suite. Future directions for the powder suite, including upgrades and new instruments, are also discussed.

Low dimensional quantum magnets are interesting because of the emerging collective behavior arising from strong quantum fluctuations. The one-dimensional (1D) S = 1/2 Heisenberg antiferromagnet is a paradigmatic example, whose low-energy excitations, known as spinons, carry fractional spin S = 1/2. These fractional modes can be reconfined by the application of a staggered magnetic field. Even though considerable progress has been made in the theoretical understanding of such magnets, experimental realizations of this low-dimensional physics are relatively rare. This is particularly true for rare-earth-based magnets because of the large effective spin anisotropy induced by the combination of strong spin–orbit coupling and crystal field splitting. Here, we demonstrate that the rare-earth perovskite YbAlO₃ provides a realization of a quantum spin S = 1/2 chain material exhibiting both quantum critical Tomonaga–Luttinger liquid behavior and spinon confinement–deconfinement transitions in different regions of magnetic field–temperature phase diagram.

The charge ordered structure of ions and vacancies characterizing rare-earth pyrochlore oxides serves as a model for the study of geometrically frustrated magnetism. The organization of magnetic ions into networks of corner-sharing tetrahedra gives rise to highly correlated magnetic phases with strong fluctuations, including spin liquids and spin ices. It is an open question how these ground states governed by local rules are affected by disorder. Here we demonstrate in the pyrochlore Tb₂Hf₂O₇, that the vicinity of the disordering transition towards a defective fluorite structure translates into a tunable density of anion Frenkel disorder while cations remain ordered. Quenched random crystal fields and disordered exchange interactions can therefore be introduced into otherwise perfect pyrochlore lattices of magnetic ions. We show that disorder can play a crucial role in preventing long-range magnetic order at low temperatures, and instead induces a strongly fluctuating Coulomb spin liquid with defect-induced frozen magnetic degrees of freedom.

We demonstrate the first live, autonomous control over neutron diffraction experiments by developing and deploying ANDiE: the autonomous neutron diffraction explorer. Neutron scattering is a unique and versatile characterization technique for probing the magnetic structure and behavior of materials. However, instruments at neutron scattering facilities in the world is limited, and instruments at such facilities are perennially oversubscribed. We demonstrate a significant reduction in experimental time required for neutron diffraction experiments by implementation of autonomous navigation of measurement parameter space through machine learning. Prior scientific knowledge and Bayesian active learning are used to dynamically steer the sequence of measurements. We show that ANDiE can experimentally determine the magnetic ordering transition of both MnO and Fe_1.09Te all while providing a fivefold enhancement in measurement efficiency. Furthermore, in a hypothesis testing post-processing step, ANDiE can determine transition behavior from a set of possible physical models. ANDiE's active learning approach is broadly applicable to a variety of neutron-based experiments and can open the door for neutron scattering as a tool of accelerated materials discovery.

An extraordinarily interesting series of metal–organic framework compounds are the isostructural microporous coordination polymers [M₂(dhtp)] (CPO-27–M, M–MOF-74 or M₂(dobdc)) in which a high concentration of coordinatively unsaturated metal sites results in high initial heats of adsorption for a variety of adsorbents. We present here a comparative study of hydrogen gas adsorption experiments on CPO-27–Cu and –Mn, which show significant differences in their hydrogen uptake behaviours which can be attributed to the difference in interaction between hydrogen and the respective metal cation incorporated in the framework structure. Inelastic neutron scattering and neutron diffraction experiments were carried out to gain additional insight into the adsorption processes leading to the difference in hydrogen uptake behaviour by the two compounds. On the basis of the experimental results the hydrogen uptake properties of CPO-27–Cu and –Mn are compared, and finally related to the properties of the other members of the CPO-27 series. It is found that CPO-27–Cu demonstrates the lowest isosteric heat of adsorption for H₂ of all the CPO-27–M materials reported to date, where M = Ni, Co, Mg, Zn, Mn, and Fe, whereas CPO-27–Mn demonstrates the second lowest. While all the previously reported CPO-27 materials show two steps in the adsorption isotherm and two distinct values corresponding to the first and second adsorption sites in the heats of adsorption, these are not observed for CPO-27–Cu. Consequently, the open metal site and the second adsorption site are energetically equivalent, and there is no preference for the hydrogen gas at the open metal centre.

The nascent suite of single-crystal neutron diffractometers at the Oak Ridge National Laboratory has no equal at any other neutron scattering facility worldwide and offers the potential to re-assert single-crystal diffraction using neutrons as a significant tool to study nuclear and magnetic structures of small unit cell crystals, nuclear structures of macromolecules, and diffuse scattering. Signature applications and features of single-crystal neutron diffraction are high resolution nuclear structure analysis, magnetic structure and spin density determinations, contrast variation (particularly D₂O/H₂O) for nuclear structural studies, lack of radiation damage when using crystals of biological molecules such as proteins, and the fidelity to measure nuclear and magnetic diffuse scattering with elastic discrimination.