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DOE OSTI2015

Simple expressions of the nuclear relaxation rate enhancement due to quadrupole nuclei in slowly tumbling molecules

For slowly tumbling entities or quasi-rigid lattices, we derive very simple analytical expressions of the quadrupole relaxation enhancement (QRE) of the longitudinal relaxation rate R{sub 1} of nuclear spins I due to their intramolecular magnetic dipolar coupling with quadrupole nuclei of arbitrary spins S ≥ 1. These expressions are obtained by using the adiabatic approximation for evaluating the time evolution operator of the quantum states of the quadrupole nuclei S. They are valid when the gyromagnetic ratio of the spin S is much smaller than that of the spin I. The theory predicts quadrupole resonant peaks in the dispersion curve of R{sub 1} vs magnetic field. The number, positions, relative intensities, Lorentzian shapes, and widths of these peaks are explained in terms of the following properties: the magnitude of the quadrupole Hamiltonian and the asymmetry parameter of the electric field gradient (EFG) acting on the spin S, the S-I inter-spin orientation with respect to the EFG principal axes, the rotational correlation time of the entity carrying the S–I pair, and/or the proper relaxation time of the spin S. The theory is first applied to protein amide protons undergoing dipolar coupling with fast-relaxing quadrupole {sup 14}N nuclei and mediating the QRE to the observed bulk water protons. The theoretical QRE agrees well with its experimental counterpart for various systems such as bovine pancreatic trypsin inhibitor and cartilages. The anomalous behaviour of the relaxation rate of protons in synthetic aluminium silicate imogolite nano-tubes due to the QRE of {sup 27}Al (S = 5/2) nuclei is also explained.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2018

Reconstruction of the remote dipole and quadrupole fields from the kinetic Sunyaev Zel’dovich and polarized Sunyaev Zel’dovich effects

The kinetic Sunyaev Zel’dovich (kSZ) and polarized Sunyaev Zel’dovich (pSZ) effects are temperature and polarization anisotropies induced by the scattering of cosmic microwave background (CMB) photons from structure in the post-reionization universe. In the case of the kSZ effect, small angular scale anisotropies in the optical depth are modulated by the CMB dipole field, i.e., the CMB dipole observed at each spacetime point, which is sourced by the primordial dipole and especially the local peculiar velocity. In the case of the pSZ effect, similar small-scale anisotropies are modulated by the CMB quadrupole field, which receives contributions from both scalar and tensor modes. Statistical anisotropies in the cross-correlations of CMB temperature and polarization with tracers of the inhomogeneous distribution of electrons provide a means of isolating and reconstructing the dipole and quadrupole fields. In this paper, we present a set of unbiased minimum variance quadratic estimators for the reconstruction of the dipole and quadrupole fields, and forecast the ability of future CMB experiments and large-scale structure surveys to perform this reconstruction. Furthermore, consistent with previous work, we find that a high fidelity reconstruction of the dipole and quadrupole fields over a variety of scales is indeed possible, and demonstrate the sensitivity of the pSZ effect to primordial tensor modes. Using a principle component analysis, we estimate how many independent modes could be accessed in such a reconstruction. We also comment on a few first applications of a detection of the dipole and quadrupole fields, including a reconstruction of the primordial contribution to our locally observed CMB dipole, a test of statistical homogeneity on large scales from the first modes of the quadrupole field, and a reconstruction technique for the primordial potential on the largest scales.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2015

Aharonov–Anandan quantum phases and Landau quantization associated with a magnetic quadrupole moment

The arising of geometric quantum phases in the wave function of a moving particle possessing a magnetic quadrupole moment is investigated. It is shown that an Aharonov–Anandan quantum phase (Aharonov and Anandan, 1987) can be obtained in the quantum dynamics of a moving particle with a magnetic quadrupole moment. In particular, it is obtained as an analogue of the scalar Aharonov–Bohm effect for a neutral particle (Anandan, 1989). Besides, by confining the quantum particle to a hard-wall confining potential, the dependence of the energy levels on the geometric quantum phase is discussed and, as a consequence, persistent currents can arise from this dependence. Finally, an analogue of the Landau quantization is discussed. -- Highlights: •Scalar Aharonov–Bohm effect for a particle possessing a magnetic quadrupole moment. •Aharonov–Anandan quantum phase for a particle with a magnetic quadrupole moment. •Dependence of the energy levels on the Aharonov–Anandan quantum phase. •Landau quantization associated with a particle possessing a magnetic quadrupole moment.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2018

Rapid Quadrupole-Time-of-Flight Mass Spectrometry Method Quantifies Oxygen-Rich Lignin Compound in Complex Mixtures

Complex mixture analysis is a costly and time-consuming task facing researchers with foci as varied as food science and fuel analysis. When faced with the task of quantifying oxygen-rich bio-oil molecules in a complex diesel mixture, we asked whether complex mixtures could be qualitatively and quantitatively analyzed on a single mass spectrometer with mid-range resolving power without the use of lengthy separations. To answer this question, we developed and evaluated a quantitation method that eliminated chromatography steps and expanded the use of quadrupole-time-of-flight mass spectrometry from primarily qualitative to quantitative as well. To account for mixture complexity, the method employed an ionization dopant, targeted tandem mass spectrometry, and an internal standard. This combination of three techniques achieved reliable quantitation of oxygen-rich eugenol in diesel from 300 to 2500 ng/mL with sufficient linearity (R{sup 2} = 0.97 ± 0.01) and excellent accuracy (percent error = 0% ± 5). To understand the limitations of the method, it was compared to quantitation attained on a triple quadrupole mass spectrometer, the gold standard for quantitation. The triple quadrupole quantified eugenol from 50 to 2500 ng/mL with stronger linearity (R{sup 2} = 0.996 ± 0.003) than the quadrupole-time-of-flight and comparable accuracy (percent error = 4% ± 5). This demonstrates that a quadrupole-time-of-flight can be used for not only qualitative analysis but also targeted quantitation of oxygen-rich lignin molecules in complex mixtures without extensive sample preparation. The rapid and cost-effective method presented here offers new possibilities for bio-oil research, including: (1) allowing for bio-oil studies that demand repetitive analysis as process parameters are changed and (2) making this research accessible to more laboratories. .

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

Single Quadrupole Multiple Fragment Ion Monitoring Quantitative Mass Spectrometry

Single quadrupole mass spectrometry (MS) with enhanced in-source multiple fragment ion monitoring was designed to perform high sensitivity quantitative mass analyses. Enhanced in-source fragmentation amplifies fragmentation from traditional soft electrospray ionization producing fragment ions that have been found to be identical to those generated in tandem MS. We have combined enhanced in-source fragmentation data with criteria established by the European Union Commission Directive 2002/657/EC for electron ionization single quadrupole quantitative analysis to perform quantitative analyses. These experiments were performed on multiple types of complex samples that included a mixture of 50 standards, as well as cell and plasma extracts. The dynamic range for these quantitative analyses was comparable to triple quadrupole multiple reaction monitoring (MRM) analyses at up to 5 orders of magnitude with the cell and plasma extracts showing similar matrix effects across both platforms. Amino acid and fatty acid measurements performed from certified NIST 1950 plasma with isotopically labeled standards demonstrated accuracy in the range of 91–110% for the amino acids, 76–129% for the fatty acids, and good precision (coefficient of variation <10%). To enhance specificity, a newly developed correlated ion monitoring algorithm was designed to facilitate these analyses. This algorithm autonomously processes, aligns, filters, and compiles multiple ions within one chromatogram enabling both precursor and in-source fragment ions to be correlated within a single chromatogram, also enabling the detection of coeluting species based on precursor and fragment ion ratios. Single quadrupole instrumentation can provide MRM level quantitative performance by monitoring/correlating precursor and fragment ions facilitating high sensitivity analysis on existing single quadrupole instrumentation that are generally inexpensive, easy to operate, and technically less complex.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2014

Design of large aperture superferric quadrupole magnets for an in-flight fragment separator

Superferric quadrupole magnets to be used for in-flight fragment separator have been designed. A quadrupole magnet triplet for beam focusing is placed in a cryostat together with superconducting correction coils. To maximize acceptance of rare isotope beams produced by projectile fragmentation, it is essential to use large-aperture quadrupole magnets. The pole tip radius is 17 cm in the current design, and we tried to enlarge the aperture with 3D analysis on magnetic fields. In the front end of the separator, where a target and beam dump are located, we plan to use two sets of quadrupole triplets made of high-Tc superconductor (HTS) operating at 20-50 K considering high radiation heat load. The HTS magnet will use warm iron poles. Both low-Tc and high-Tc superconductors are acquired for test winding, and two kinds of dewar and cryostat are under construction to perform the coil and magnet tests. The magnetic design of superferric quadrupole is mainly discussed.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2016

{sup 1}H NMR relaxometry and quadrupole relaxation enhancement as a sensitive probe of dynamical properties of solids—[C(NH{sub 2}){sub 3}]{sub 3}Bi{sub 2}I{sub 9} as an example

{sup 1}H nuclear magnetic resonance relaxometry has been applied to reveal information on dynamics and structure of Gu{sub 3}Bi{sub 2}I{sub 9} ([Gu = C(NH{sub 2}){sub 3}] denotes guanidinium cation). The data have been analyzed in terms of a theory of quadrupole relaxation enhancement, which has been extended here by including effects associated with quadrupole ({sup 14}N) spin relaxation caused by a fast fluctuating component of the electric field gradient tensor. Two motional processes have been identified: a slow one occurring on a timescale of about 8 × 10{sup −6} s which has turned out to be (almost) temperature independent, and a fast process in the range of 10{sup −9} s. From the {sup 1}H-{sup 14}N relaxation contribution (that shows “quadrupole peaks”) the quadrupole parameters, which are a fingerprint of the arrangement of the anionic network, have been determined. It has been demonstrated that the magnitude of the quadrupole coupling considerably changes with temperature and the changes are not caused by phase transitions. At the same time, it has been shown that there is no evidence of abrupt changes in the cationic dynamics and the anionic substructure upon the phase transitions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Observation of a dipole-bound excited state in 4-ethynylphenoxide and comparison with the quadrupole-bound excited state in the isoelectronic 4-cyanophenoxide

Negative ions do not possess Rydberg states, but can have Rydberg-like nonvalence excited states near the electron detachment threshold, including dipole-bound states (DBSs) and quadrupole-bound states (QBSs). While DBSs have been studied extensively, quadrupole-bound excited states have been more rarely observed. 4-cyanophenoxide (4CP – ) was the first anion observed to possess a quadrupole-bound exited state 20 cm-1 below its detachment threshold. Here we report the observation of a DBS in the isoelectronic 4-ethynylphenoxide anion (4EP – ), providing a rare opportunity to compare the behaviors of a dipole-bound and a quadrupole-bound excited state in a pair of very similar anions. Photodetachment spectroscopy (PDS) of cryogenically-cooled 4EP – reveals a DBS 76 cm -1 below its detachment threshold. Photoelectron spectroscopy (PES) at 266 nm shows that the electronic structure of 4EP – and 4CP – are nearly identical. The observed vibrational features in both the PDS and PES, as well as autodetachment from the nonvalence excited states, are also found to be similar for both anions. However, resonant two-photon detachment (R2PD) from the bound vibrational ground state is observed to be very different for the DBS in 4EP – and the QBS in 4CP – . The R2PD spectra reveal that decays take place from both the DBS and QBS to the respective anion ground electronic states within the 5 ns detachment laser pulse due to internal conversion followed by intramolecular vibrational redistribution (IVR), but the decay mechanisms appear to be very different. In the R2PD spectrum of 4EP – , we observe strong threshold electron signals, which are due to detachment, by the second photon, of highly rotationally excited anions resulted from the decay of the DBS. On the other hand, in the R2PD spectrum of 4CP – we observe well-resolved vibrational peaks due to the three lowest-frequency vibrational modes of 4CP – , which are populated from the decay of the QBS. Here, the different behaviors of the R2PD spectra suggest unexpected differences between the relaxation mechanisms of the dipole-bound and quadrupole-bound excited states.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Understanding the Quadrupole Mass Filter and Testing a High-Resolution QMS RGA for ITER

A common type of residual gas analyzer is the quadrupole mass spectrometer. One of the main components within this instrument is a mass filter known as the quadrupole. It is responsible for the selective throughput of the ionized gas particles - by ascending mass number - prior to ion impacts on the analyzer (or detector) surface from which the ion current signal is generated for processing. However, the quadrupole is not fully described in relation to the electric field characteristics and the function as an ion mass separator. This paper describes the basic origins of the electrical design, the intricate assembly criteria, and performance of the quadrupole within the spectrometer. A specialized quadrupole mass spectrometer is part of a configuration for a diagnostic gas analyzer system planned for ITER, a fusion research machine. It has a verified capability, essential as a diagnostic criterion for this reactor project, to successfully deconvolute the mass signals of Helium-4 and deuterium (reactor fuel exhaust gases, separated by only 0.026 atomic mass units), down to a relative three-percent concentration of the former gas. The associated preliminary testing, performed at the Oak Ridge National Laboratory, is also addressed. Finally, one of the key parameters used to express gas concentration, the relative sensitivity factor, will be explained, including an evaluation of dependency on other variables.

Marcus, Chris [ORNL] (ORCID:0000000190139636)↗

NASA NTRS1993

Dipole and quadrupole tests of the isotropy of gamma-ray burst locations

Dipole and quadrupole tests of the isotropy of locations on the sphere are discussed. The statistics (cos theta), the dipole moment to the Galactic center, and mean (sin-squared b - 1/3), the quadrupole moment about the Galactic plane, can be used to search for significant anisotropies in galactic coordinates. Such coordinate-system-based tests are the most powerful tests of dipole and quadrupole anisotropies in the particular coordinate system. Two statistics which have not been previously applied to gamma-ray burst data are described. The Rayleigh-Watson statistic measures the size of the dipole moment of the locations and the Bingham statistic measures the deviation of the eigenvalues of a quadrupole-like matrix from the values expected for isotropy. Tests based upon these two statistics search for dipole and quadrupole moments in spherical location data in a coordinate-system-independent, and thus model-independent, manner. They can detect an anisotropy in any direction and yield an analytic statistical significance to any detected anisotropy. The statistical tests are demonstrated herein using a variety of data sets.

Briggs, Michael S.↗

NASA NTRS2000

Miniature micromachined quadrupole mass spectrometer array and method of making the same

The present invention provides a quadrupole mass spectrometer and an ion filter for use in the quadrupole mass spectrometer. The ion filter includes a thin patterned layer including a two-dimensional array of poles forming one or more quadrupoles. The patterned layer design permits the use of very short poles and with a very dense spacing of the poles, so that the ion filter may be made very small. Also provided is a method for making the ion filter and the quadrupole mass spectrometer. The method involves forming the patterned layer of the ion filter in such a way that as the poles of the patterned layer are formed, they have the relative positioning and alignment for use in a final quadrupole mass spectrometer device.

Chutjian, Ara↗

NASA NTRS2000

Miniature micromachined quadrupole mass spectrometer array and method of making the same

The present invention provides a quadrupole mass spectrometer and an ion filter, or pole array, for use in the quadrupole mass spectrometer. The ion filter includes a thin patterned layer including a two-dimensional array of poles forming one or more quadrupoles. The patterned layer design permits the use of very short poles and with a very dense spacing of the poles, so that the ion filter may be made very small. Also provided is a method for making the ion filter and the quadrupole mass spectrometer. The method involves forming the patterned layer of the ion filter in such a way that as the poles of the patterned layer are formed, they have the relative positioning and alignment for use in a final quadrupole mass spectrometer device.

Chutjian, Ara↗

NASA NTRS2001

Miniature micromachined quadrupole mass spectrometer array and method of making the same

Chutjian, Ara↗

NASA NTRS2001

Miniature micromachined quadrupole mass spectrometer array and method of making the same

Chutjian, Ara↗

NASA NTRS2001

Miniature micromachined quadrupole mass spectrometer array and method of making the same

The present invention provides a quadrupole mass spectrometer and an ion filter for use in the quadrupole mass spectrometer. The ion filter includes a thin patterned layer including a two-dimensional array of poles forming one or more quadrupoles. The patterned layer design permits the use of very short poles and with a very dense spacing of the poles, so that the ion filter may be made very small. Also provided is a method for making the ion filter and the quadrupole mass spectrometer. The method involves forming the patterned layer of the ion filter in such a way that as the poles of the patterned layer are formed, they have the relative positioning and aligrnent for use in a final quadrupole mass spectrometer device.

Chutjian, Ara↗

NASA NTRS2002

Miniature micromachined quadrupole mass spectrometer array and method of making the same

Chutjian, Ara↗

NASA NTRS2011

Higher Order Parametric Excitation Modes for Spaceborne Quadrupole Mass Spectrometers

This paper describes a technique to significantly improve upon the mass peak shape and mass resolution of spaceborne quadrupole mass spectrometers (QMSs) through higher order auxiliary excitation of the quadrupole field. Using a novel multiresonant tank circuit, additional frequency components can be used to drive modulating voltages on the quadrupole rods in a practical manner, suitable for both improved commercial applications and spaceflight instruments. Auxiliary excitation at frequencies near twice that of the fundamental quadrupole RF frequency provides the advantages of previously studied parametric excitation techniques, but with the added benefit of increased sensed excitation amplitude dynamic range and the ability to operate voltage scan lines through the center of upper stability islands. Using a field programmable gate array, the amplitudes and frequencies of all QMS signals are digitally generated and managed, providing a robust and stable voltage control system. These techniques are experimentally verified through an interface with a commercial Pfeiffer QMG422 quadrupole rod system.When operating through the center of a stability island formed from higher order auxiliary excitation, approximately 50% and 400% improvements in 1% mass resolution and peak stability were measured, respectively, when compared with traditional QMS operation. Although tested with a circular rod system, the presented techniques have the potential to improve the performance of both circular and hyperbolic rod geometry QMS sensors.

Gershman, D. J.↗

DOE OSTI2014

Nonuniform radiation damage in permanent magnet quadrupoles

We present data that indicate nonuniform magnetization loss due to radiation damage in neodymium-iron-boron Halbach-style permanent magnet quadrupoles. The proton radiography (pRad) facility at Los Alamos uses permanent-magnet quadrupoles for magnifying lenses, and a system recently commissioned at GSI-Darmsdadt uses permanent magnets for its primary lenses. Large fluences of spallation neutrons can be produced in close proximity to these magnets when the proton beam is, intentionally or unintentionally, directed into the tungsten beam collimators; imaging experiments at LANL’s pRad have shown image degradation with these magnetic lenses at proton beam doses lower than those expected to cause damage through radiation-induced reduction of the quadrupole strength alone. We have observed preferential degradation in portions of the permanent magnet quadrupole where the field intensity is highest, resulting in increased high-order multipole components.

36 MATERIALS SCIENCE↗