Cinematic reflectometry using QIKR, the quite intense kinetics reflectometer.

The Quite Intense Kinetics Reflectometer (QIKR) will be a general-purpose, horizontal-sample-surface neutron reflectometer. Reflectometers measure the proportion of an incident probe beam reflected from a surface as a function of wavevector (momentum) transfer to infer the distribution and composition of matter near an interface. The unique scattering properties of neutrons make this technique especially useful in the study of soft matter, biomaterials, and materials used in energy storage. Exploiting the increased brilliance of the Spallation Neutron Source Second Target Station, QIKR will collect specular and off-specular reflectivity data faster than the best existing such machines. It will often be possible to collect complete specular reflectivity curves using a single instrument setting, enabling "cinematic" operation, wherein the user turns on the instrument and "films" the sample. Samples in time-dependent environments (e.g., temperature, electrochemical, or undergoing chemical alteration) will be observed in real time, in favorable cases with frame rates as fast as 1 Hz. Cinematic data acquisition promises to make time-dependent measurements routine, with time resolution specified during post-experiment data analysis. This capability will be deployed to observe such processes as in situ polymer diffusion, battery electrode charge-discharge cycles, hysteresis loops, and membrane protein insertion into lipid layers.

CHESS: The future direct geometry spectrometer at the second target station.

CHESS, chopper spectrometer examining small samples, is a planned direct geometry neutron chopper spectrometer designed to detect and analyze weak signals intrinsic to small cross sections (e.g., small mass, small magnetic moments, or neutron absorbing materials) in powders, liquids, and crystals. CHESS is optimized to enable transformative investigations of quantum materials, spin liquids, thermoelectrics, battery materials, and liquids. The broad dynamic range of the instrument is also well suited to study relaxation processes and excitations in soft and biological matter. The 15 Hz repetition rate of the Second Target Station at the Spallation Neutron Source enables the use of multiple incident energies within a single source pulse, greatly expanding the information gained in a single measurement. Furthermore, the high flux grants an enhanced capability for polarization analysis. This enables the separation of nuclear from magnetic scattering or coherent from incoherent scattering in hydrogenous materials over a large range of energy and momentum transfer. This paper presents optimizations and technical solutions to address the key requirements envisioned in the science case and the anticipated uses of this instrument.

A concept of a broadband inverted geometry spectrometer for the Second Target Station at the Spallation Neutron Source.

BWAVES is an acronym for Broadband Wide-Angle VElocity Selector spectrometer, indicating that a novel WAVES (Wide-Angle VElocity Selector) device will be used to select the velocity/wavelength of the detected neutrons after they are scattered by the sample. We describe a conceptual design of BWAVES, a time-of-flight broadband inverted-geometry neutron spectrometer for the Second Target Station at the Spallation Neutron Source operated by Oak Ridge National Laboratory. Being the first inverted geometry spectrometer where the energy of the detected neutrons can be chosen by a WAVES device mechanically, irrespective of the limitations imposed by the crystal analyzers or filters, BWAVES will feature a uniquely broad, continuous dynamic range of measurable energy transfers, spanning 4.5 decades. This will enable measurements of both vibrational and relaxational excitations within the same, continuous scattering spectra. Novel approaches that are necessary for the implementation of a WAVES device at the BWAVES spectrometer will result in a spectrometer with the design and characteristics much different from those displayed by the neutron spectrometers in existence today.

Extended anharmonic collapse of phonon dispersions in SnS and SnSe.

The lattice dynamics and high-temperature structural transition in SnS and SnSe are investigated via inelastic neutron scattering, high-resolution Raman spectroscopy and anharmonic first-principles simulations. We uncover a spectacular, extreme softening and reconstruction of an entire manifold of low-energy acoustic and optic branches across a structural transition, reflecting strong directionality in bonding strength and anharmonicity. Further, our results solve a prior controversy by revealing the soft-mode mechanism of the phase transition that impacts thermal transport and thermoelectric efficiency. Our simulations of anharmonic phonon renormalization go beyond low-order perturbation theory and capture these striking effects, showing that the large phonon shifts directly affect the thermal conductivity by altering both the phonon scattering phase space and the group velocities. These results provide a detailed microscopic understanding of phase stability and thermal transport in technologically important materials, providing further insights on ways to control phonon propagation in thermoelectrics, photovoltaics, and other materials requiring thermal management.

Nuclear quantum effect with pure anharmonicity and the anomalous thermal expansion of silicon.

Despite the widespread use of silicon in modern technology, its peculiar thermal expansion is not well understood. Adapting harmonic phonons to the specific volume at temperature, the quasiharmonic approximation, has become accepted for simulating the thermal expansion, but has given ambiguous interpretations for microscopic mechanisms. To test atomistic mechanisms, we performed inelastic neutron scattering experiments from 100 K to 1,500 K on a single crystal of silicon to measure the changes in phonon frequencies. Our state-of-the-art ab initio calculations, which fully account for phonon anharmonicity and nuclear quantum effects, reproduced the measured shifts of individual phonons with temperature, whereas quasiharmonic shifts were mostly of the wrong sign. Surprisingly, the accepted quasiharmonic model was found to predict the thermal expansion owing to a large cancellation of contributions from individual phonons.

Design and operating characteristic of a vacuum furnace for time-of-flight inelastic neutron scattering measurements.

We present the design and operating characteristics of a vacuum furnace used for inelastic neutron scattering experiments on a time-of-flight chopper spectrometer. The device is an actively water cooled radiant heating furnace capable of performing experiments up to 1873 K. Inelastic neutron scattering studies performed with this furnace include studies of phonon dynamics and metallic liquids. We describe the design, control, characterization, and limitations of the equipment. Further, we provide comparisons of the neutron performance of our device with commercially available options. Finally we consider upgrade paths to improve performance and reliability.

Design and operation of the wide angular-range chopper spectrometer ARCS at the Spallation Neutron Source.

The wide angular-range chopper spectrometer ARCS at the Spallation Neutron Source (SNS) is optimized to provide a high neutron flux at the sample position with a large solid angle of detector coverage. The instrument incorporates modern neutron instrumentation, such as an elliptically focused neutron guide, high speed magnetic bearing choppers, and a massive array of (3)He linear position sensitive detectors. Novel features of the spectrometer include the use of a large gate valve between the sample and detector vacuum chambers and the placement of the detectors within the vacuum, both of which provide a window-free final flight path to minimize background scattering while allowing rapid changing of the sample and sample environment equipment. ARCS views the SNS decoupled ambient temperature water moderator, using neutrons with incident energy typically in the range from 15 to 1500 meV. This range, coupled with the large detector coverage, allows a wide variety of studies of excitations in condensed matter, such as lattice dynamics and magnetism, in both powder and single-crystal samples. Comparisons of early results to both analytical and Monte Carlo simulation of the instrument performance demonstrate that the instrument is operating as expected and its neutronic performance is understood. ARCS is currently in the SNS user program and continues to improve its scientific productivity by incorporating new instrumentation to increase the range of science covered and improve its effectiveness in data collection.

Phonon density of states of LaFeAsO(1-x)Fx.

We have studied the phonon density of states (PDOS) in LaFeAsO(1-x)Fx with inelastic neutron scattering methods. The PDOS of the parent compound (x=0) is very similar to the PDOS of samples optimally doped with fluorine to achieve the maximum Tc (x approximately 0.1). Good agreement is found between the experimental PDOS and first-principles calculations with the exception of a small difference in Fe mode frequencies. The PDOS reported here is not consistent with conventional electron-phonon mediated superconductivity.