In situ examination of engineered local additives in cement paste via neutron based scattering techniques
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Kupwade-Patil, Kunal (ORCID:0000000271668257)↗
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A Measurement of the Neutron Electromagnetic Form Factor Ratio from a Rosenbluth Technique with Simultaneous Detection of Neutrons and Protons
The internal structure of protons and neutrons provides insight into both the dynamical behavior of the constitute quarks and gluons, and emergent properties of the nucleons (such as mass, spin, and electromagnetic distributions). Elastic electron-nucleon scattering can probe the elastic electromagnetic form factors of the nucleon. The electric and magnetic form factors, respectively, encode information about the internal charge and magnetization distributions within the nucleon. Precision data for these form factors, over a broad range of the four-momentum transfer squared, Q^2, can benchmark theoretical models describing the strong interaction of nuclear physics. The Super BigBite Spectrometer (SBS) program in Hall A at Jefferson Lab, is a series of high-precision experiments which seek to significantly extend the Q^2 reach of previous data for the nucleon electromagnetic form factors. The first two experiments of this program are known as G_M^n and the neutron Two Photon Exchange (nTPE) and the data were collected from October 2021 to February 2022. Both experiments were conducted with the simultaneous measurement of D(e,e'n) and D(e,e'p) reactions for quasi-elastic electron-deuteron scattering. The scattered electrons were detected in the BigBite Spectrometer, which features multiple large-acceptance Gas Electron Multiplier (GEM) detectors. The Super BigBite Spectrometer provided simultaneous detection of scattered nucleons, and utilized a large acceptance dipole magnet and Hadron Calorimeter (HCal). The G_M^n experiment provides precision measurements of the neutron magnetic form factor, via the ratio method, over a Q^2 range of 3.0 to 13.5 (GeV/c)2. From this data analysis, preliminary values for G_M^n/µ_n G_D are extracted. For Q^2=4.48 (GeV/c)2 we find G_M^n/µ_n G_D=0.9546±0.0132 and for Q^2=4.476 (GeV/c)2 we find G_M^n/µ_n G_D=0.9563±0.0110. These preliminary G_M^n/µ_n G_D values are more precise than existing world data in this Q^2 regime and are consistent with the most recent parameterization of the G_M^n/µ_n G_D world data. The nTPE experiment provides a first measurement of the neutron Rosenbluth Slope and seeks to quantify the two-photon exchange(TPE) contribution to elastic electron-neutron scattering at a fixed Q^2=4.5 (GeV/c)2 with two different beam energies and scattering angle values. For data of the proton form factor ratio, µ_p G_E^p/G_M^p, significant discrepancies exist between values obtained from Rosenbluth Separation and polarization transfer measurement, particularly at large Q^2, and TPE contributions are thought to resolve this discrepancy. The impacts of TPE contributions have not yet been experimentally established for the neutron. From the data analysis presented in this dissertation, a preliminary result for the neutron Rosenbluth Slope is found as S^n=(G_E^n )^2/t_n (G_M^n )^2=0.0916±0.0476 for Q^2=4.48 (GeV/c)2. This value of the neutron Rosenbluth Slope is consistent with the world data extrapolation and the absence of large TPE corrections.
Wertz, Ezekiel [Thomas Jefferson National Accelera↗
Optically multiplexed neutron time-of-flight technique for inertial confinement fusion
Neutron time-of-flight (nTOF) detectors are crucial in diagnosing the performance of inertial confinement fusion (ICF) experiments, which implode targets of deuterium–tritium fuel to achieve thermonuclear conditions. These detectors utilize the fusion neutron energy spectrum to extract key measurements, including the hotspot ion temperature and fuel areal density. Previous work [Danly et al., Rev. Sci. Instrum. 94, 043502 (2023)] has demonstrated adding 1D spatial resolution to an nTOF-like detector using a neutron aperture and streak camera to measure the ion temperature profile of an ICF implosion. By contrast, the study presented herein explores modifying the 1D detector to use a fast photomultiplier tube (PMT) to validate the design of a 2D spatially resolved instrument based on reconstruction from 1D profiles. The modification would collect time-of-flight traces from separate scintillators in an imaging array with one PMT using optical fibers of varying lengths to time-multiplex the signals. This technique has been demonstrated in ride-along experiments on the OMEGA laser with 20 fiber-coupled scintillator channels connected to a Photek PMT210. Results provide constraints on the fiber lengths and PMT gating requirements to promote pulse fidelity throughout all channels. Calibration of the detector to fixed nTOFs can provide a preliminary estimate of the instrument response function (IRF), although measurement of the IRF is currently under way. These results suggest that nTOF signals can potentially be time-multiplexed with fibers so long as the design is strategic to mitigate signal-to-noise reduction, modal dispersion, and charge build-up in the PMT, which has implications beyond ion temperature imaging.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Modulation of intensity emerging from zero effort (MIEZE) with extended Fourier time at large scattering angle
Modulation of Intensity Emerging from Zero Effort (MIEZE) is a neutron resonant spin echo technique that allows one to measure time correlation scattering functions in materials by implementing radio-frequency (RF) intensity modulation at the sample and the detector. The technique avoids neutron spin manipulation between the sample and the detector and, thus, could find applications in cases where the sample depolarizes the neutron beam. However, the finite sample size creates a variance in the path length between the locations where scattering and detection happen, which limits the contrast in intensity modulation that one can detect, in particular, toward long correlation times or large scattering angles. We propose a modification to the MIEZE setup that will enable one to extend those detection limits to longer times and larger angles. Furthermore, we use Monte Carlo simulations of a neutron scattering beamline to show that by tilting the RF flippers in the primary spectrometer with respect to the beam direction, one can shape the wave front of the intensity modulation at the sample to compensate for the path variance from the sample and the detector. The simulation results indicate that this change enables one to operate a MIEZE instrument at much increased RF frequencies, thus improving the effective energy resolution of the technique. For the MIEZE instrument simulated, it shows that for an incident beam with the maximum divergence of 0.33°, the maximum Fourier time can be increased by a factor of 3.
47 OTHER INSTRUMENTATION↗
Development and evaluation of a list mode neutron coincidence collar for spatial response measurements of fresh fuel assemblies
A traditional safeguards neutron coincidence counting system, the Neutron Coincidence Collar, has been modified to incorporate individual preamplifiers on each of its 18 3He tubes in active interrogation mode. When used with list mode data acquisition (LMDA) and analysis, a signal from each 3He tube can be recorded and analyzed to allow a spatial response measurement to be performed on an item based on count rate and 3He tube location within the system. The ultimate goal of this project is to demonstrate the capabilities of a list mode response matrix for the nondestructive assay of fresh nuclear fuel assemblies. To enable partial defect detection of fuel pin locations and absences within an assembly, the project aims to extend well-established correlated neutron analysis techniques on a preexisting Neutron Coincidence Collar by extracting a greater number of useful signatures from the system than are currently generated. LMDA, combined with the addition of multiple preamplifiers, facilitates this capability by increasing the number of simultaneous signals that can be measured; this allows an in-depth analysis of neutron coincidence events to determine a fissioning item’s location based on the measured doubles count rate in various channel logic coincidence combinations. All of this can be done from a single measurement pulse train in offline analysis, which is the major benefit provided by LMDA. Through various stages of development and testing, a Mirion Technologies model JCC-71 Neutron Coincidence Collar has been successfully retrofit with modern electronics designed in-house at Oak Ridge National Laboratory, matching preexisting JAB-01 electronics performance, while maintaining the original system footprint. This paper presents these various stages of development and experimental evaluation of the proof of concept system.
Moore, Angela S.↗
Nature of Reactive Hydrogen for Ammonia Synthesis over a Ru/C12A7 Electride Catalyst
Recently, there have been renewed interests in exploring new catalysts for ammonia synthesis under mild conditions. Electride-based catalysts are among the emerging ones. Ruthenium particles supported on an electride composed of a mixture of calcium and aluminum oxides (C12A7) have attracted great attention for ammonia synthesis due to their facile ability in activating N2 under ambient pressure. However, the exact nature of the reactive hydrogen species and the role of electride support still remain elusive for this catalytic system. Here, we report for the first time that the surface-adsorbed hydrogen, rather than the hydride encaged in the C12A7 electride, plays a major role in ammonia synthesis over the Ru/C12A7 electride catalyst with the aid of in situ neutron scattering techniques. Combining in situ neutron diffraction, inelastic neutron spectroscopy, density functional theory (DFT) calculation, and temperature-programmed reactions, the results provide direct evidence for not only the presence of encaged hydrides during ammonia synthesis but also the strong thermal and chemical stability of the hydride species in the Ru/C12A7 electride. Steady state isotopic transient kinetic analysis (SSITKA) of ammonia synthesis showed that the coverage of reactive intermediates increased significantly when the Ru particles were promoted by the electride form (coverage up to 84%) of the C12A7 support rather than the oxide form (coverage up to 15%). Such a drastic change in the intermediate coverage on the Ru surface is attributed to the positive role of electride support where the H2 poisoning effect is absent during ammonia synthesis over Ru. The finding of this work has significant implications for understanding catalysis by electride-based materials for ammonia synthesis and hydrogenation reactions in general.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Development of a portable high-T c spherical neutron polarimetry device at the Oak Ridge National Laboratory
Spherical neutron polarimetry is a powerful polarized neutron scattering technique used to determine complex magnetic structures which are only partly accessible by other methods. This technique measures the full neutron polarization change upon scattering from a sample by fully decoupling the incoming and outgoing neutron polarization with a zero-field chamber placed at the sample position. Recent advancements and testing are presented for a new spherical neutron polarimetry device utilizing high-T c superconducting YBCO films, PHiTPAD, at the High Flux Isotope Reactor at Oak Ridge National Laboratory. Furthermore, we introduce a conceptual design that utilizes wavelength-independent adiabatic transitions to adapt spherical neutron polarimetry for use with pulsed neutron sources, thereby expanding its potential applications in neutron scattering research.
47 OTHER INSTRUMENTATION↗
Neutron Tagging From Neutrino Interactions in DUNE-ND 2x2 Prototype
The Deep Underground Neutrino Experiment (DUNE) is a long-baseline neutrino oscillation experiment that aims to measure whether CP is violated in the leptonic sector (if violated, how much) and unambiguously determine the neutrino mass ordering. DUNE consists of near and far detectors that rely on liquid argon time projection chamber (LArTPC) technology to observe neutrino interactions. The near detector (ND) will be placed in Fermilab, near the neutrino source, while the far detector (FD) will be deployed in Sanford Lab, 1.5 km deep underground, which is 1300 km away from the source. LArTPCs provide excellent particle identification and calorimetry; however, detecting neutrons is challenging, as they do not leave direct ionization signals in LArTPCs. Neutrons can carry away up to 25% of the neutrino energy, introducing a significant uncertainty in DUNE measurements. The DUNE near detector (ND) features a novel modular LArTPC with pixelated charge readout, which enhances event recons truction. The modular design enables precise correlation between ionization signals and light signals in a high-rate environment, improving the identification of delayed energy depositions from neutrons in neutrino interactions. We introduce a neutron tagging technique using the 2x2 Demonstrator, a small-scale prototype of the DUNE ND LArTPC. The analysis utilizes Monte Carlo simulations and deep-learning techniques to identify neutron-induced energy depositions and reconstruct low-energy activity.
Kufatty, Georgette [Florida State U.]↗
Chapter 10.02 - Neutron Scattering Studies of Materials for Hydrogen Storage
Hydrogen storage presents a significant barrier to the widespread adaptation of hydrogen as an energy source in mobile and stationary applications. The development of new candidate hydrogen storage materials is therefore an outstanding goal in the field of inorganic chemistry. Neutron scattering techniques - including diffraction, inelastic, and quasielastic scattering - are integral in investigating these materials. Here, we review some of the key studies of candidate hydrogen storage materials which have employed neutron scattering techniques. We begin with a brief discussion of hydrogen's current position in the global energy landscape. Next, we provide a brief description of the theory and practical aspects of the neutron scattering techniques germane to the study of hydrogen storage. Then we enumerate the neutron scattering studies of candidate hydrogen storage materials, including metal hydrides, chemical hydrides, and porous compounds. We focus on the studies which helped develop our understanding of hydrogen storage by revealing the underlying fundamental physics and chemistry of hydrogen sorption in these systems. Finally, we provide an outlook to the future of hydrogen storage research.
chemical hydrides↗
Preliminary RAM-RODD results for the MUSiC subcritical configurations
The Measurement of Uranium Subcritical and Critical (MUSiC) was performed at the DOE’s National Criticality Experiments Research Center (NCERC) located in the Nevada National Security Site (NNSS). The measurement utilized the Rocky Flats shells to perform benchmark measurements of similar highly enriched uranium (HEU) systems that span a wide range of reactivities. The Rocky Flats (RF) shells are 93.16% U-235 enriched metal hemishells that can be stacked concentrically. Ten configurations were measured with effective multiplication factors spanning between deeply subcritical (~ 0.64) through delayed critical. Details of the measured configurations are listed in Table 1. This unique set of measurements with its large span of reactivies is being used to determine the range over which neutron noise techniques such as Feynman variance-to-mean, Rossi-alpha, and pulsed neutron source techniques can be accurately employed for a bare HEU system. The results of the measurements will be published as a benchmark in The International Criticality Safety Benchmark Evaluation Project (ICSBEP) Handbook. The results will support the growing amount of subcritical benchmark data, such as the SCRaP measurements, that is available to the community. The measurements were performed using several different detector systems for the purposes of cross-validation and obtaining detector independent results. Four detector systems were deployed, three by the NCERC team and one from the University of Michigan. The detector systems included a Neutron Multiplicity Array Detector (NoMAD) system (similar to the MC-15), four small volume 0.635 cm (Ø) × 7.59 cm 3 He detectors (ideal for measuring prompt neutron decay constants due to their fast recovery speed), the Rossi Alpha Measurements – Rapid Organic (n, γ) Discrimination Detector (RAM-RODD), and the Organic Scintillator Array (OSCAR). RAM-RODD is an array of eight 5.08 cm (Ø) × 5.08 cm EJ-309 organic scintillator detectors. OSCAR is a University of Michigan system and is an array of twelve 5.08 cm (Ø) × 5.08 cm stilbene detectors. Details of measurements performed with OSCAR will be discussed in a separate talk. The focus of this work is preliminary results obtained by RAM-RODD for the 8 subcritical configurations. Additional details on the measurements and on the setup and deployment of RAM-RODD will be discussed. Preliminary neutron noise analysis results including Rossi-alpha and Feynman-alpha will also be presented.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Characterization of a collimated neutron imager for low-rate fast neutron imaging
Spatial localization of special nuclear materials (SNM) via their neutron signatures amidst background requires knowledge of the background neutron environment or a means of separating a source from background based on low amounts of information. This requirement has created the need for characterizing the spatial distribution of the cosmogenic neutron background. Neutron scatter cameras have been developed and optimized for rapid detection of high activity sources, but have low imaging efficiency, making it difficult to use them to characterize low rate diffuse sources, such as the neutron background. The Low Intensity Neutron Imaging System (LINIS) is a collimated neutron imager that has been designed and optimized for imaging diffuse cosmogenic neutron background in the energy range of 0.5–15 MeV. LINIS operates using 16 liquid scintillation detectors shielded by ultra-high molecular weight polyethylene cylindrical collimators in a staggered orientation and rotates to 7 discrete positions, giving it roughly 2π sensitivity. Finally, LINIS has been characterized using (α, n) and fission neutron sources using two imaging techniques for neutron source localization, simple backprojection and Maximum Likelihood Expectation Maximization.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Scintillator-based Timepix3 detector for neutron spin-echo techniques using intensity modulation
A scintillator-based Timepix3 (TPX3) detector was developed to resolve the high-frequency modulation of a neutron beam in both spatial and temporal domains, as required for neutron spin-echo experiments. In this system, light from a scintillator is manipulated with an optical lens and is intensified using an image intensifier, making it detectable with the TPX3 chip. Two different scintillators, namely, 6 LiF:ZnS(Ag) and 6 LiI:Eu, were investigated to achieve the high resolution needed for spin-echo modulated small-angle neutron scattering (SEMSANS) and modulation of intensity with zero effort (MIEZE). The methodology for conducting event-mode analysis is described, including the optimization of clustering parameters for both scintillators. The detector with both scintillators was characterized with respect to detection efficiency, spatial resolution, count rate, uniformity, and γ-sensitivity. The 6 LiF:ZnS(Ag) scintillator-based detector achieved a spatial resolution of 200 μm and a count rate capability of 1.1 × 10 5 cps, while the 6 LiI:Eu scintillator-based detector demonstrated a spatial resolution of 250 μm and a count rate capability exceeding 2.9 × 10 5 cps. Furthermore, high-frequency intensity modulations in both spatial and temporal domains were successfully observed, confirming the suitability of this detector for SEMSANS and MIEZE techniques, respectively.
47 OTHER INSTRUMENTATION↗
Aberration corrected RF flipper for high resolution neutron spectroscopy
Project Summary Company: Adelphi Technology, Inc. Title: Aberration-corrected High Frequency RF Flipper for High-Resolution Neutron Spectroscopy PI: Dr. Jay Theodore Cremer Topic: C55-11 Enhancement of Scattering Instrumentation Technology Used at Pulsed and Continuous Sources Subtopic: d. Other Statement of the problem or situation that is being addressed. The quest to understand heterogeneous and hierarchical materials is gathering momentum, as described in a 2015 report by the Basic Energy Sciences Advisory Committee on Challenges at the Frontiers of Matter and Energy. For the past 40 years a technique called neutron spin echo (NSE) has been used to probe molecular motions in such non-crystalline materials over time scales from 10’s of picoseconds to 100’s of nanoseconds. The method has provided unique information about the dynamics of soft heterogeneous materials, including confirmation of the de Gennes model of polymer reptation and quantitative measurement of bending constants of biologically relevant lipid membranes. However, scientists continue to clamor for even higher resolution than NSE can provide. Biomaterials, polymers, glasses, and artificially nanostructured materials all manifest slow molecular motions because of weak or competing interactions between subunits and are amenable to study with neutrons, provided sufficiently long dynamical correlation times can be achieved. All these materials have important applications to advanced technologies so understanding them is key to technological progress. General statement of how this problem is being addressed. We will address the need for high-resolution neutron spectroscopy by using a technique called Neutron Resonance Spin Echo (NRSE). While similar to NSE in many respects, this method has the potential to exceed the NSE capabilities, if 2 technical hurdles can be overcome. The major impediments to successful high-resolution NRSE are the availability of two technologies: a very high frequency, efficient, radiofrequency (rf) flipper for neutrons and a method to correct certain magnetic aberrations. Based on previous STTR support and follow-on research we have developed a suitable rf flipper and we have invented a method to correct the magnetic aberrations. Both technologies need refinement to make them suitable for implementation at a neutron source such as the Oak Ridge National Laboratory nuclear reactor. In this proposal we seek to perfect the two technologies and to combine them into a single, operationally convenient device. Commercial Applications and Other Benefits In view of the increasing demand for the unique scientific information that high resolution neutron spectroscopy can provide, we expect several major instrumentation upgrades at both U.S. and foreign neutron centers will require make use of the NRSE method over the coming decade, creating a market for the devices we will design. These components will enhance scientists’ abilities to probe the time dependence of density fluctuations in a wide range of hierarchical and heterogeneous materials many of which are vital to existing and future technologies. Key Words – Polarized Neutrons, Neutron Spin Echo, Neutron Scattering, advanced materials. Summary for Members of Congress Neutron beams are a powerful materials-science probe that provide unique information about the structure of matter. The proposed devices will accelerate scientific discoveries required to achieve national goals for new technological materials.
36 MATERIALS SCIENCE↗
Neutron Total Scattering Analysis of Materials for the Nuclear Fuel Cycle
Here, this paper reviews recent experimental efforts at the University of Tennessee and Oak Ridge National Laboratory to comprehensively characterize the structural details of materials relevant for the nuclear fuel cycle by employing advanced neutron scattering techniques. For the study of nuclear ceramics, neutron scattering offers distinct advantages over traditional laboratory or synchrotron X-ray diffraction, including enhanced sensitivity to elements with a low atomic mass, such as oxygen, nitrogen, and carbon. The key to these efforts is the recent advancement in the neutron scattering infrastructure at the high-flux diffractometers at the Spallation Neutron Source. The high neutron flux at these instruments enables neutron total scattering, a nondestructive bulk technique that simultaneously captures both short-range structural effects through pair distribution function analysis and long-range order through diffraction pattern analysis. This approach is particularly important for a comprehensive description of defective, disordered, or amorphous nuclear materials. The case studies presented here include analyses of the local defect structure in hyperstoichiometric uranium oxides and short-range order of ion-irradiated ceramics. This advanced analytical methodology will improve our understanding of the behavior of materials in extreme environments and contribute to the development of more resilient nuclear materials.
Neutron scattering↗
Variance reduction techniques for Monte Carlo neutron noise simulations
The small fluctuations of the neutron flux caused by small perturbations of the macroscopic cross-sections take the name of neutron noise. Advanced Monte Carlo methods have been recently proposed in order to solve the neutron noise equations in the frequency domain, which allows establishing reference solutions to validate faster but approximate deterministic solvers. Due to the presence of particles carrying two statistical weights (for the real and imaginary components of the noise field), both of which may be positive or negative, Monte-Carlo simulations of neutron noise pose distinct challenges in terms of variance reduction. In this work we investigate two variance-reduction techniques, namely branchless collisions and weight cancellation, and probe their effectiveness for a benchmark con- figuration concerning the noise field induced by a pin with oscillating cross sections in a fuel assembly.
22 GENERAL STUDIES OF NUCLEAR REACTORS↗
Different agglomeration properties of PC 61 BM and PC 71 BM in photovoltaic inks – a spin-echo SANS study
Fullerene derivatives are used in a wide range of applications including as electron acceptors in solution-processable organic photovoltaics. We report agglomeration of fullerene derivatives in optically opaque solutions of PC 61 BM and PC 71 BM, with concentrations ranging from 30 mg mL -1 up to 90 mg mL -1 , in different solvents with relevance to organic photovoltaics, using a novel neutron scattering technique, Spin-Echo Small Angle Neutron Scattering (SESANS). From SESANS, agglomerates with correlation lengths larger than 1 μm are found in some PC 61 BM solutions, in contrast no agglomerates are seen in PC 71 BM solutions. These results clearly show that PC 71 BM is fundamentally more soluble than PC 61 BM in the solvents commonly used in photovoltaic inks and corroborating similar observations previously achieved using other experimental techniques. Computer models are presented to study the energetics of solution and agglomeration of both species, ascribing the difference to a kinetic effect probably related to the larger anisotropy of PC 71 BM. Also, this work showcases the power of SESANS to probe agglomerates of fullerene derivatives in completely opaque solutions for agglomerates of the order of one to several microns.
36 MATERIALS SCIENCE↗
Active Neutron Multiplicity Counting of Kilogram Quantities of Highly Enriched Uranium [Slides]
LANL seeks to analyze neutron noise techniques for large HEU assemblies, specifically neutron multiplicity counting (NMC). NMC provides the activity and quantity of fissionable and fissile material, which is useful in safeguards and criticality safety.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Biomembrane Structure and Material Properties Studied With Neutron Scattering
Cell membranes and their associated structures are dynamical supramolecular structures where different physiological processes take place. Detailed knowledge of their static and dynamic structures is therefore needed, to better understand membrane biology. The structure–function relationship is a basic tenet in biology and has been pursued using a range of different experimental approaches. In this review, we will discuss one approach, namely the use of neutron scattering techniques as applied, primarily, to model membrane systems composed of lipid bilayers. An advantage of neutron scattering, compared to other scattering techniques, is the differential sensitivity of neutrons to isotopes of hydrogen and, as a result, the relative ease of altering sample contrast by substituting protium for deuterium. This property makes neutrons an ideal probe for the study of hydrogen-rich materials, such as biomembranes. In this review article, we describe isotopic labeling studies of model and viable membranes, and discuss novel applications of neutron contrast variation in order to gain unique insights into the structure, dynamics, and molecular interactions of biological membranes. We specifically focus on how small-angle neutron scattering data is modeled using different contrast data and molecular dynamics simulations. We also briefly discuss neutron reflectometry and present a few recent advances that have taken place in neutron spin echo spectroscopy studies and the unique membrane mechanical data that can be derived from them, primarily due to new models used to fit the data.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗