Wave Vector Transfer Research Articles

Imaging and ferroelectric orientation mapping of photostriction in a single Bismuth Ferrite nanocrystal

The exploration of multiferroic materials and their interaction with light at the nanoscale presents a captivating frontier in materials science. Bismuth Ferrite (BiFeO3, BFO), a standout among these materials, exhibits room-temperature ferroelectric and antiferromagnetic behaviour and magnetoelectric coupling. Of particular interest is the phenomenon of photostriction, the light-induced deformation of crystal structures, which enhances the prospect for device functionality based on these materials. Understanding and harnessing multiferroic phenomena holds significant promise in various technological applications, from optoelectronics to energy storage. The orientation of the ferroelectric axis is an important design parameter for devices formed from multiferroic materials. Determining its orientation in the laboratory frame of reference usually requires knowing multiple wavevector transfer (Q-Vector) directions, which can be challenging to establish due to the need for extensive reciprocal-space searches. Our study demonstrates a method to identify the ferroelectric axis orientation using Bragg Coherent X-ray Diffraction Imaging (BCDI) measurements at a single Q-vector direction. This method involves applying photostriction-inducing laser illumination across various laser polarisations. Our findings reveal that photostriction primarily occurs as a surface phenomenon at the nanoscale. Moreover, a photo-induced crystal length change ranging from 30 to 60 nm was observed, consistent with earlier findings on bulk material.

Design of multi-shell nested fully annular quasi-ellipsoidal focusing mirrors for small-angle neutron scattering

The neutron flux is a crucial factor for neutron scattering measurements, especially for compact sources. Among various neutron optics, grazing-incidence focusing mirrors have been developed to give a significant increase in the neutron flux on a sample owing to their great potential for collecting neutrons in small-angle neutron scattering (SANS) instruments. Focusing mirrors with a supermirror coating can be nested to collect a neutron beam with large divergence. Nested conical integrated assembly technology is employed to manufacture nested focusing mirrors. This study describes the design of ten-shell nested fully annular quasi-ellipsoidal focusing mirrors with an m = 3 Ni/Ti supermirror coating to produce enough neutrons on a sample under the premise of satisfying the specified minimum wavevector transfer Q. For fully annular focusing mirrors, the neutron current received by a sample from the entire annular focusing neutron beam is more relevant. A ray-tracing method and current gain calculation are used to evaluate the performance of the designed mirrors. The ray-tracing result shows that the ideal resolution of quasi-ellipsoidal mirrors with four-segment conical approximation is 1.354 mm. As the source radius decreases from 20 mm, the neutron current with the designed focusing mirrors can be enhanced by a factor of 13 to over 100 compared with that without focusing mirrors in the same detected area. The effective collecting area is 186 cm2 when the source radius is the optimal 15 mm. An 83-fold current gain can be obtained for cold neutrons. The proposed mirrors can reach 90.7 and 87.3% of the maximum current of the corresponding optimal mirror structure when the source radii are 10 and 20 mm, respectively. The results demonstrate that the proposed mirrors are adaptable for instruments with changeable sources.

Performance of small- and wide-angle x-ray scattering beamline at Indus-2 synchrotron

A Small- and Wide-Angle X-ray Scattering (SWAXS) beamline (BL-18) is installed and commissioned at a 1.5 T bending magnet port (5°) of Indus-2 synchrotron at RRCAT, Indore, India. The ∼40-m-long beamline has tunable x-ray energy in the range of 5–20 keV by using a double crystal monochromator. A 1.5-m-long toroidal mirror is used to focus the x-ray beam at the detector position. The beamline is equipped with a 6-m-long movable detector stage to access different wave-vector transfer ranges. At present, an online image plate area detector and a linear position-sensitive gas detector are installed for Small-Angle X-ray Scattering (SAXS) and Wide-Angle X-ray Scattering (WAXS) measurements, respectively. The beamline is operational in simultaneous SAXS/WAXS mode to probe the mesoscopic as well as molecular level structure over a wide range of wave-vector transfer. The specification of the beamline and its performance are reported here. A few recent experimental results, as obtained from BL-18, are also described in brief.

Ab initio quantum approach to electron-hole exchange for semiconductors hosting Wannier excitons

We propose a quantum approach to ``electron-hole exchange,'' better named electron-hole pair exchange, that makes use of the second quantization formalism to describe the problem in terms of Bloch-state electron operators. This approach renders transparent the fact that such singular effect comes from interband Coulomb processes. We first show that, due to the sign change when turning from valence-electron destruction operator to hole creation operator, the interband Coulomb interaction only acts on spin-singlet electron-hole pairs, just like the interband electron-photon interaction, thereby making these spin-singlet pairs optically bright. We then show that, when written in terms of reciprocal lattice vectors ${\mathbf{G}}_{m}$, the singularity of the interband Coulomb scattering in the small wave-vector transfer limit entirely comes from the ${\mathbf{G}}_{m}=\mathbf{0}$ term, which renders its singular behavior easy to calculate. Comparison with the usual real-space formulation in which the singularity appears through a sum of ``long-range processes'' over all ${\mathbf{R}}_{\ensuremath{\ell}}\ensuremath{\ne}\mathbf{0}$ lattice vectors once more proves that periodic systems are easier to handle in terms of reciprocal vectors ${\mathbf{G}}_{m}$ than in terms of lattice vectors ${\mathbf{R}}_{\ensuremath{\ell}}$. Well-accepted consequences of the electron-hole exchange on excitons and polaritons are reconsidered and refuted for different major reasons.

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 1Hz. 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.

M-STAR: Magnetism second target advanced reflectometer at the Spallation Neutron Source.

M-STAR is a next generation polarized neutron reflectometer with advanced capabilities. A new focusing guide concept is optimized for samples with dimensions down to a millimeter range. A proposed hybrid pulse-skipping chopper will enable experiments at constant geometry at one incident angle in a broad range of wavevector transfer Q up to 0.3A-1 for specular, off-specular, and GISANS measurements. M-STAR will empower nanoscience and spintronics studies routinely on small samples (∼2 × 2mm2) and of atomic-scale thickness using versatile experimental conditions of magnetic and/or electric fields, light, and temperature applied in situ to novel complex device-like nanosystems with multiple buried interfaces. M-STAR will enable improved grazing incidence diffraction measurements, as a surface-sensitive depth-resolved probe of, e.g., the out-of-plane component of atomic magnetic moments in ferromagnetic, antiferromagnetic, and more complex structures as well as in-plane atomic-scale structures inaccessible with contemporary diffractometry and reflectometry. New horizons will be opened by the development of an option to probe near-surface dynamics with inelastic grazing incidence scattering in the time-of-flight mode. These novel options in combination with ideally matched parameters of the second target station will place M-STAR in the world's leading position for high resolution polarized reflectometry.

Microscopic collective dynamics in liquid neon-deuterium mixtures: Inelastic neutron scattering and quantum simulations.

In this paper a combined neutron scattering and quantum simulation study of the collective dynamics in liquid Ne-D_{2} mixtures, at a temperature of T=30K and in the wave-vector transfer range 4 nm^{-1}<q<51nm^{-1}, is presented. Two D_{2} concentrations are investigated, one close to 25% molar and the other close to 50% molar, together with pure Ne. The dynamic structure factor for the centers of mass of the two molecular species is extracted from the neutron scattering data and subsequently compared with that obtained from three different quantum simulation methods, such as ring polymer molecular dynamics and two slightly different versions of the Feynman-Kleinert approach. A general agreement is found, even though some discrepancies both among simulations, and between simulations and experimental data, can be observed. In order to clarify the physical meaning of the present spectroscopic results, an analysis of the longitudinal current spectral maxima is carried out showing the peculiarities of the D_{2} center-of-mass dynamics in these mixtures. A comparison with the centroid molecular dynamics results obtained for the D_{2} center-of-mass self-dynamics in the same liquid mixtures is finally proposed.

Unravelling the structural hierarchy in microemulsion droplet templated dendritic fibrous nano silica

Microemulsion-templated dendritic fibrous nanosilica (DFNS) has attracted considerable attention owing to their unique accessible pore structure and high-surface-area but their complex structural hierarchy is still intriguing. In this work, a correlative quantification of the hierarchical structure of such nanospheres has been presented based upon three complementary techniques; small-angle scattering, gas sorption, and electron microscopy. Analysis of scattering data over a wide range of wave-vector transfer using polydisperse Teubner Strey model reveals three distinct levels of correlated bicontinuous morphology and the pore-size distribution from N2 gas sorption resembles well with the results obtained from scattering analysis. The formation mechanism of such hierarchical pore morphology in these nanospheres is elucidated and it is observed that a relative variation in periodicity, sheet thickness, and their correlation significantly affects the specific surface area and pore structure, which is strongly influenced by hydrolysis rate and reaction time.

Collective particle dynamics of molten NaCl by inelastic x-ray scattering

An inelastic x-ray scattering experiment has been performed on molten NaCl over wide wave vector and energy transfer ranges. Data of high statistical quality are analyzed using a memory function approach within a generalized Langevin equation. The approach with two relaxation times for the memory function provides a very good data description over the whole wave vector range beyond the hydrodynamic regime. A slow thermal and a fast structural relaxation process in the memory function completely define the density fluctuations in molten NaCl and evidences the thermal-viscoelastic model as the minimal description for collective particle dynamics in molten alkali halides. The obtained excitation frequencies demonstrate a large positive dispersion effect, which can be related to the viscoelastic reaction of the molten salt. A transition from the viscoelastic to a hydrodynamic response of the molten salt at small wave vectors is observed. In the hydrodynamic regime the resulting thermal diffusivity agrees well with values obtained through light scattering. The modeling indicates some deficiencies at small wave vectors and large energy transfers and the spectra of the current correlation function evidences additional intensity at high frequency. The frequency of these additional modes approach a non-zero value at zero wave vector and indicates a non-acoustic character of these excitations. The frequency center of this additional inelastic intensity coincides with optic-type modes in molten NaCl predicted by simulations.

Terahertz collective dynamics of DNA as affected by hydration and counterions

Local and propagating vibrations occurring in DNA in the terahertz domain are essential for processes at the basis of cellular metabolism. Here we report the results of a study on the B-DNA terahertz dynamics where we combined high-resolution inelastic x-ray experiments and incoherent inelastic neutron scattering. By using two different high-hydration conditions we could study the effect of packing interactions between double helices, while by selecting Na and Cs counterions we could inspect how the mass loading affects the DNA low-frequency modes. The pattern of coherent excitation energies is well represented in terms of two branches, an acoustic-like one, with an associated propagation velocity of 3000 ± 100 m/s, and the other almost dispersionless at ~2 meV. This picture is also supported by the vibrational density of states projected on the hydrogen atoms. The acoustic-like mode is assigned to DNA excitations, despite its intriguing similarity with the analogous acoustic mode of bulk water at low wave-vector transfers. We also provide evidence for the intrahelical optic-like character of the low-energy mode, that we ascribe to large scale relative motions of DNA sub-domains.

Accurate background correction in neutron reflectometry studies of soft condensed matter films in contact with fluid reservoirs.

Neutron reflectometry (NR) is a powerful method for looking at the structures of multilayered thin films, including biomolecules on surfaces, particularly proteins at lipid interfaces. The spatial resolution of the film structure obtained through an NR experiment is limited by the maximum wavevector transfer at which the reflectivity can be measured. This maximum is in turn determined primarily by the scattering background, e.g. from incoherent scattering from a liquid reservoir or inelastic scattering from cell materials. Thus, reduction of scattering background is an important part of improving the spatial resolution attainable in NR measurements. Here, the background field generated by scattering from a thin liquid reservoir on a monochromatic reflectometer is measured and calculated. It is shown that background subtraction utilizing the entire background field improves data modeling and reduces experimental uncertainties associated with localized background subtraction.

Polarized inelastic neutron scattering of nonreciprocal spin waves in MnSi

We report spin-polarized inelastic neutron scattering of the dynamical structure factor of the conical magnetic helix in the cubic chiral magnet MnSi. We find that the spectral weight of spin-flip scattering processes is concentrated on single branches for wavevector transfer parallel to the helix axis as inferred from well-defined peaks in the neutron spectra. In contrast, for wavevector transfers perpendicular to the helix the spectral weight is distributed among different branches of the magnon band structure as reflected in broader features of the spectra. Taking into account the effects of instrumental resolution, our experimental results are in excellent quantitative agreement with parameter-free theoretical predictions. Whereas the dispersion of the spin waves in MnSi appears to be approximately reciprocal at low energies and small applied fields, the associated spin-resolved spectral weight displays a pronounced non-reciprocity that implies a distinct non-reciprocal response in the limit of vanishing uniform magnetization at zero magnetic field.

Neutron visualization of inhomogeneous buried interfaces in thin films

When designing some functions in thin film systems, one of the key concepts is the structure of the constituent layers and interfaces. In an actual system, the layers and interfaces are often inhomogeneous in different scales, from hundreds of microns to several nanometers, causing differences in properties, despite very similar average structures. In this case, the choice of the observation point is critical to clarify the problem. Another critical aspect is the identification of these points by surveying the entire inhomogeneous thin film system. This article presents a description of a novel promising solution that is suitable for nondestructive visualization of inhomogeneous buried layers and interfaces in thin films. Such observations have been impossible until now. In this investigation, a unique extension of neutron reflectometry is proposed. While conventional neutron reflectivity just gives average depth-profiling of the scattering length density of layered thin films, the present method provides full picture of the inhomogeneity. In general, achieving a high spatial-resolving power for neutron scattering is not straightforward because the neutron counts become fairly limited at the sample or the detector position when the beam size is reduced. As a result, XY scanning of a sample with a small neutron beam is fairly difficult because of the required long measurement time. To address these issues, new concepts have been introduced for neutron reflectivity. The proposed method uses a wide beam instead of reducing the beam size. In addition, it measures the projection reflection profile instead of the total integrated intensity. These profiles are collected at a set of different in-plane angles. Similar to computed tomography, it is possible to obtain the specimen’s two-dimensional (2D) neutron reflectivity distribution as one image. Because the spatial resolution is limited by the detection method, a Hadamard coded mask is employed to measure the reflection projection with only 50% loss of the primary neutron intensity. When the time-of-flight (ToF) mode is used for the neutron experiment, one can obtain many images as a function of ToF, i.e., the wavevector transfer. Such series of images can be displayed as a video. This indicates that the neutron reflectivity profiles of local points can be retrieved from the above video images. This paper presents the first report on the development of neutron reflectivity with imaging capability, and the analysis of local points in inhomogeneous layered thin-films without utilizing a small neutron beam. In the present work, the feasibility of the proposed method with approximately 1 mm spatial resolution was examined. In addition, further improvements of the approach are discussed. It is anticipated that this technique will facilitate new opportunities in the study of buried function interfaces.

Inconsistency between linearized Thomas–Fermi approximation and electron-ionized impurity scattering rate in the first Born approximation

We show that by computing the electron-impurity scattering rate at the first order via Fermi’s golden rule, and assuming that the localized impurity potential is of Yukawa form, one obtains a wave vector transfer distribution which is inconsistent with the finite temperature linearized Thomas–Fermi approximation for n-type semiconductors. Our previous findings show that this is not the case for the carrier nondegenerate dynamics, because the average wave vector transferred being in general negligible in this regime. Moreover, we examine the behavior of the electron-impurity differential cross-sections in the first Born approximation for relevant values of the wave vector transfer. We find that in the majority of collisions, the scattering probabilities differ at the most by 1% from the estimates computed by means of the impurity potential at random phase approximation level.

Gamma background characterization on VESUVIO: before and after the moderator upgrade

The VESUVIO spectrometer at the ISIS pulsed neutron and muon source is a unique instrument which makes use of eV neutrons and inverted geometry, allowing deep inelastic neutron scattering experiments with high values of energy and wavevector transfers. The neutron detection techniques on the VESUVIO forward-scattering detector banks is based on (n,γ) conversion, therefore neutrons are indirectly detected and the signals produced by scattered neutrons, accordingly the photons, is recorded using gamma scintillators. The use of γ-sensitive detectors make γ-background one of the main limiting factors affecting the data quality and instrument sensitivity on VESUVIO. This work aims to assess how the sample-independent gamma background has changed after the recent upgrades to the water moderator viewed by the instrument, which resulted in a twofold increase of the thermal neutron flux. Here we show that the gamma background is mainly influenced by the thermal neutron flux and that the recent upgrade results in a fivefold increase in the gamma background in the photon energy range 300 keV-3 MeV. We point out the possibility of providing a thermal-neutron filter along the incident beam in order to suppress this background source.

MultiFLEXX - The new multi-analyzer at the cold triple-axis spectrometer FLEXX

The first experimental characterization of a multiple energy analysis wide angle backend for a cold triple-axis spectrometer is reported. The multi-analyzer module MultiFLEXX employs 155 detection channels which simultaneously probe an extensive range in wavevector and energy transfer. Successful mapping of magnetic excitations in MnF2 and Ho demonstrate order of magnitude gains in data collection efficiency using this novel type backend. MultiFLEXX is competitive to standard triple-axis spectroscopy in terms of energy resolution and signal-to-noise ratio. A minority of the detector channels is affected by spurious signals inherent to this multiplexing concept. The characteristic signature of these spurious signals easily allows for their discrimination. The instrument concept focuses on detection efficiency in the horizontal scattering plane which makes it an ideal technique for fast mapping and parametric studies including extreme sample environment.

Characterisation of the incident beam and current diffraction capabilities on the VESUVIO spectrometer

The VESUVIO spectrometer at the ISIS pulsed neutron and muon source is a unique instrument amongst those available at neutron facilities. This is the only inverted-geometry neutron spectrometer accessing values of energy and wavevector transfer above tens of eV and , respectively, and where deep inelastic neutron scattering experiments are routinely performed. As such, the procedure at the base of the technique has been previously described in an article published by this journal (Mayers and Reiter 2012 Meas. Sci. Technol. 23 045902). The instrument has recently witnessed an upsurge of interest due to a new trend to accommodate, within a single experiment, neutron diffraction and transmission measurements in addition to deep inelastic neutron scattering. This work presents a broader description of the instrument following these recent developments. In particular, we assess the absolute intensity and two-dimensional profile of the incident neutron beam and the capabilities of the backscattering diffraction banks. All results are discussed in the light of recent changes to the moderator viewed by the instrument. We find that VESUVIO has to be considered a high-resolution diffractometer as much as other diffractometers at ISIS, with a resolution as high as in backscattering. Also, we describe the extension of the wavelength range of the instrument to include lower neutron energies for diffraction measurements, an upgrade that could be readily applied to other neutron instruments as well.

Probing ultrafast changes of spin and charge density profiles with resonant XUV magnetic reflectivity at the free-electron laser FERMI.

We report the results of resonant magnetic XUV reflectivity experiments performed at the XUV free-electron laser FERMI. Circularly polarized XUV light with the photon energy tuned to the Fe M2,3 edge is used to measure resonant magnetic reflectivities and the corresponding Q-resolved asymmetry of a Permalloy/Ta/Permalloy trilayer film. The asymmetry exhibits ultrafast changes on 240 fs time scales upon pumping with ultrashort IR laser pulses. Depending on the value of the wavevector transfer Qz, we observe both decreasing and increasing values of the asymmetry parameter, which is attributed to ultrafast changes in the vertical spin and charge density profiles of the trilayer film.

Spin-analyzed SANS for soft matter applications

The small angle neutron scattering (SANS) of nearly Q-independent nuclear spin-incoherent scattering from hydrogen present in most soft matter and biology samples may raise an issue in structure determination in certain soft matter applications. This is true at high wave vector transfer Q where coherent scattering is much weaker than the nearly Q-independent spin-incoherent scattering background. Polarization analysis is capable of separating coherent scattering from spin-incoherent scattering, hence potentially removing the nearly Q-independent background. Here we demonstrate SANS polarization analysis in conjunction with the time-of-flight technique for separation of coherent and nuclear spin-incoherent scattering for a sample of silver behenate back-filled with light water. We describe a complete procedure for SANS polarization analysis for separating coherent from incoherent scattering for soft matter samples that show inelastic scattering. Polarization efficiency correction and subsequent separation of the coherent and incoherent scattering have been done with and without a time-of-flight technique for direct comparisons. In addition, we have accounted for the effect of multiple scattering from light water to determine the contribution of nuclear spin-incoherent scattering in both the spin flip channel and non-spin flip channel when performing SANS polarization analysis. We discuss the possible gain in the signal-to-noise ratio for the measured coherent scattering signal using polarization analysis with the time-of-flight technique compared with routine unpolarized SANS measurements.

Interface-sensitive imaging by an image reconstruction aided X-ray reflectivity technique.

Recently, the authors have succeeded in realizing X-ray reflectivity imaging of heterogeneous ultrathin films at specific wavevector transfers by applying a wide parallel beam and an area detector. By combining in-plane angle and grazing-incidence angle scans, it is possible to reconstruct a series of interface-sensitive X-ray reflectivity images at different grazing-incidence angles (proportional to wavevector transfers). The physical meaning of a reconstructed X-ray reflectivity image at a specific wavevector transfer is the two-dimensional reflectivity distribution of the sample. In this manner, it is possible to retrieve the micro-X-ray reflectivity (where the pixel size is on the microscale) profiles at different local positions on the sample.