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.

On the structure and dynamics of water associated with single-supported zwitterionic and anionic membranes.

We have used high-resolution quasielastic neutron scattering (QENS) to investigate the dynamics of water molecules (time scale of motion ∼10-11-10-9 s) in proximity to single-supported bilayers of the zwitterioniclipid DMPC (1,2-dimyristoyl-sn-glycero-3-phosphorylcholine) and the anionic lipid DMPG (1,2-dimyristoyl-sn-glycero-3-phosphoglycerol) in the temperature range 160-295 K. For both membranes, the temperature dependence of the intensity of neutronsscattered elastically and incoherently from these samples indicates a series of freezing/melting transitions of the membrane-associated water, which have not been observed in previous studies of multilayer membranes. We interpret these successive phase transitions as evidence of different types of water that are common to the two membranes and which are defined by their local environment: bulk-like water located furthest from the membrane and two types of confined water in closer proximity to the lipids. Specifically, we propose a water type termed "confined 2" located within and just above the lipid head groups of the membrane and confined 1 water that lies between the bulk-like and confined 2 water. Confined 1 water is only present at temperatures below the freezing point of bulk-like water. We then go on to determine the temperature dependence of the translational diffusion coefficient of the water associated with single-supported DMPG membranes containing two different amounts of water as we have previously done for DMPC. To our knowledge, there have been no previous studies comparing the dynamics of water in proximity to zwitterionic and anionic membranes. Our analysis of the water dynamics of the DMPG and DMPC membranes supports the classification of water types that we have inferred from their freezing/melting behavior. However, just as we observe large differences in the freezing/melting behavior between these model membranes for the same water type, our measurements demonstrate variation between these membranes in the dynamics of their associated water over a wide temperature range. In particular, there are differences in the diffusive motion of water closest to the lipid head groups. Previously, QENS spectra of the DMPC membranes have revealed the motion of water bound to the lipid head groups. For the DMPG membrane, we have found some evidence of such bound water molecules; but the signal is too weak for a quantitative analysis. However, we observe confined 2 water in the DMPG membrane to undergo slow translational diffusion in the head group region, which was unobserved for DMPC. The weak temperature dependence of its translational diffusion coefficient allows extrapolation to physiological temperatures for comparison with molecular dynamics simulations.

Conceptual moderator studies for the Spallation Neutron Source short-pulse second target station.

Candidate moderator configurations for a short-pulse second target station (STS) at the Oak Ridge National Laboratory Spallation Neutron Source (SNS) have been identified using a global optimizer framework built around the MCNPX particle transport code. Neutron brightness metrics were selected as the figure-of-merit. We assumed that STS would use one out of six proton pulses produced by an SNS accelerator upgraded to operate at 1.3 GeV proton energy, 2.8 MW power and 60 Hz repetition rate. The simulations indicate that the peak brightness can be increased by a factor of 5 and 2.5 on a per proton pulse basis compared to the SNS first target station for both coupled and decoupled para-hydrogen moderators, respectively. Additional increases by factors of 3 and 2 were demonstrated for coupled and decoupled moderators, respectively, by reducing the area of neutron emission from 100 × 100 mm(2) to 20 × 20 mm(2). This increase in brightness has the potential to translate to an increase of beam intensity at the instruments' sample positions even though the total neutron emission of the smaller moderator is less than that of the larger. This is especially true for instruments with small samples (beam dimensions). The increased fluxes in the STS moderators come at accelerated poison and de-coupler burnout and higher radiation-induced material damage rates per unit power, which overall translate into lower moderator lifetimes. A first effort was undertaken to group decoupled moderators into a cluster collectively positioning them at the peak neutron production zone in the target and having a three-port neutron emission scheme that complements that of a cylindrical coupled moderator.

A new apparatus design for high temperature (up to 950°C) quasi-elastic neutron scattering in a controlled gaseous environment.

A design for a sample cell system suitable for high temperature Quasi-Elastic Neutron Scattering (QENS) experiments is presented. The apparatus was developed at the Spallation Neutron Source in Oak Ridge National Lab where it is currently in use. The design provides a special sample cell environment under controlled humid or dry gas flow over a wide range of temperature up to 950 °C. Using such a cell, chemical, dynamical, and physical changes can be studied in situ under various operating conditions. While the cell combined with portable automated gas environment system is especially useful for in situ studies of microscopic dynamics under operational conditions that are similar to those of solid oxide fuel cells, it can additionally be used to study a wide variety of materials, such as high temperature proton conductors. The cell can also be used in many different neutron experiments when a suitable sample holder material is selected. The sample cell system has recently been used to reveal fast dynamic processes in quasi-elastic neutron scattering experiments, which standard probes (such as electrochemical impedance spectroscopy) could not detect. In this work, we outline the design of the sample cell system and present results demonstrating its abilities in high temperature QENS experiments.

A time-of-flight backscattering spectrometer at the Spallation Neutron Source, BASIS.

We describe the design and current performance of the backscattering silicon spectrometer (BASIS), a time-of-flight backscattering spectrometer built at the spallation neutron source (SNS) of the Oak Ridge National Laboratory (ORNL). BASIS is the first silicon-based backscattering spectrometer installed at a spallation neutron source. In addition to high intensity, it offers a high-energy resolution of about 3.5 µeV and a large and variable energy transfer range. These ensure an excellent overlap with the dynamic ranges accessible at other inelastic spectrometers at the SNS.

Structure and phase transitions of monolayers of intermediate-length n-alkanes on graphite studied by neutron diffraction and molecular dynamics simulation.

We present evidence from neutron diffraction measurements and molecular dynamics (MD) simulations of three different monolayer phases of the intermediate-length alkanes tetracosane (n-C(24)H(50) denoted as C24) and dotriacontane (n-C(32)H(66) denoted as C32) adsorbed on a graphite basal-plane surface. Our measurements indicate that the two monolayer films differ principally in the transition temperatures between phases. At the lowest temperatures, both C24 and C32 form a crystalline monolayer phase with a rectangular-centered (RC) structure. The two sublattices of the RC structure each consists of parallel rows of molecules in their all-trans conformation aligned with their long axis parallel to the surface and forming so-called lamellas of width approximately equal to the all-trans length of the molecule. The RC structure is uniaxially commensurate with the graphite surface in its [110] direction such that the distance between molecular rows in a lamella is 4.26 A=sqrt[3a(g)], where a(g)=2.46 A is the lattice constant of the graphite basal plane. Molecules in adjacent rows of a lamella alternate in orientation between the carbon skeletal plane being parallel and perpendicular to the graphite surface. Upon heating, the crystalline monolayers transform to a "smectic" phase in which the inter-row spacing within a lamella expands by approximately 10% and the molecules are predominantly oriented with the carbon skeletal plane parallel to the graphite surface. In the smectic phase, the MD simulations show evidence of broadening of the lamella boundaries as a result of molecules diffusing parallel to their long axis. At still higher temperatures, they indicate that the introduction of gauche defects into the alkane chains drives a melting transition to a monolayer fluid phase as reported previously.

Observation of fractional Stokes-Einstein behavior in the simplest hydrogen-bonded liquid.

Quasielastic neutron scattering has been used to investigate the single-particle dynamics of hydrogen fluoride across its entire liquid range at ambient pressure. For T>230 K, translational diffusion obeys the celebrated Stokes-Einstein relation, in agreement with nuclear magnetic resonance studies. At lower temperatures, we find significant deviations from the above behavior in the form of a power law with exponent xi=-0.71+/-0.05. More striking than the above is a complete breakdown of the Debye-Stokes-Einstein relation for rotational diffusion. Our findings provide the first experimental verification of fractional Stokes-Einstein behavior in a hydrogen-bonded liquid, in agreement with recent computer simulations [S. R. Becker, Phys. Rev. Lett. 97, 055901 (2006)10.1103/PhysRevLett.97.055901].

Quasi-elastic neutron scattering study of dimethyl-sulfoxide-water mixtures: probing molecular mobility in a nonideal solution.

The translational and rotational motions of water and dimethyl sulfoxide, [DMSO, (CH(3))(2)SO] have been investigated using quasi-elastic neutron scattering. Water-DMSO mixtures at five DMSO mole fractions, chi(DMSO), ranging from 0 to 0.75, were measured. Hydrogen-deuterium substitution was used to extract independently the water proton dynamics (d-DMSO-H(2)O), the DMSO methyl proton dynamics (h-DMSO-D(2)O) and to obtain background corrections (d-DMSO-D(2)O). The translational diffusion of water slows down significantly compared to bulk water at all chi(DMSO)>0. The rotational time constant for water exhibits a maximum at chi(DMSO)=0.33 that corresponds to the observed maximum of the viscosity of the mixture. Data for DMSO can be analyzed in terms of a relatively slow tumbling of the molecule about its center-of-mass in conjunction with random translational diffusion. The rotational time constant for this motion exhibits some dependence on chi(DMSO), while the translational diffusion constant shows no clear variation for chi(DMSO)>0. The results presented reinforce the idea that due to the stronger associative nature of DMSO, DMSO-water aggregates are formed over the whole composition range, disturbing the tetrahedral natural arrangement of the water molecules. As a consequence adding DMSO to water causes a drastic slowing down of the dynamics of the water molecule, and vice versa.

Intramolecular diffusive motion in alkane monolayers studied by high-resolution quasielastic neutron scattering and molecular dynamics simulations.

Molecular dynamics simulations of a tetracosane (n-C24H50) monolayer adsorbed on a graphite basal-plane surface show that there are diffusive motions associated with the creation and annihilation of gauche defects occurring on a time scale of approximately 0.1-4 ns. We present evidence that these relatively slow motions are observable by high-energy-resolution quasielastic neutron scattering (QNS) thus demonstrating QNS as a technique, complementary to nuclear magnetic resonance, for studying conformational dynamics on a nanosecond time scale in molecular monolayers.