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At least 1,585 records · Page 88

High-reliability passivation of hydrogen-terminated diamond surface by atomic layer deposition of Al{sub 2}O{sub 3}

Although the two-dimensional hole gas (2DHG) of a hydrogen-terminated diamond surface provides a unique p-type conducting layer for high-performance transistors, the conductivity is highly sensitive to its environment. Therefore, the surface must be passivated to preserve the 2DHG, especially at high temperature. We passivated the surface at high temperature (450 °C) without the loss of C-H surface bonds by atomic layer deposition (ALD) and investigated the thermal reliability of the Al{sub 2}O{sub 3} film. As a result, C-H bonds were preserved, and the hole accumulation effect appeared after the Al{sub 2}O{sub 3} deposition by ALD with H{sub 2}O as an oxidant. The sheet resistivity and hole density were almost constant between room temperature and 500 °C by the passivation with thick Al{sub 2}O{sub 3} film thicker than 38 nm deposited by ALD at 450 °C. After the annealing at 550 °C in air The sheet resistivity and hole density were preserved. These results indicate the possibility of high-temperature application of the C-H surface diamond device in air. In the case of lower deposition temperatures, the sheet resistivity increased after air annealing, suggesting an insufficient protection capability of these films. Given the result of sheet resistivity after annealing, the increase in the sheet resistivity of these samples was not greatly significant. However, bubble like patterns were observed in the Al{sub 2}O{sub 3} films formed from 200 to 400 °C by air annealing at 550 °C for 1 h. On the other hand, the patterns were no longer observed at 450 °C deposition. Thus, this 450 °C deposition is the sole solution to enabling power device application, which requires high reliability at high temperatures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Demonstration and Concept of Operations for a Zero-Knowledge Protocol Passive Imaging Measurement for Arms Control

Here, we present an imaging system that employs zero-knowledge protocols to protect sensitive geometrical information, along with procedures to increase confidence in the result. The goal of this work is to enable the inclusion of warhead confirmation measurements in future arms control treaties. We present a demonstration of both true positive and true negative measurements that validate models and establish authenticating procedures toward meeting acceptance requirements for use in nuclear facilities. We use a two-dimensional time-encoded fast neutron imaging system with an anti-symmetric mask pattern; the fast neutron count values exceeding minimum or maximum thresholds indicate that two measured items are not identical. Laboratory measurements over twenty trials show that alarm rates for negative confirmation measurements are within uncertainties of model predictions. Positive confirmation measurements indicate that alarm rates are large enough to encourage treaty compliance.

Sweany, Melinda Dominique [Sandia National Laborat↗

Near-field interactions and nonuniversality in speckle patterns produced by a point source in a disordered medium

A point source in a disordered scattering medium generates a speckle pattern with nonuniversal features, giving rise to the so-called C{sub 0} correlation. We analyze theoretically the relationship between the C{sub 0} correlation and the statistical fluctuations of the local density of states, based on simple arguments of energy conservation. This derivation leads to a clear physical interpretation of the C{sub 0} correlation. Using exact numerical simulations, we show that C{sub 0} is essentially a correlation resulting from near-field interactions. These interactions are responsible for the nonuniversality of C{sub 0} that confers to this correlation a huge potential for sensing and imaging at the subwavelength scale in complex media.

74 ATOMIC AND MOLECULAR PHYSICS↗

Advanced Safeguards Technology Demonstration at Pacific Northwest National Laboratory

The International Atomic Energy Agency (IAEA) has established international safeguards standards for fissionable material at spent fuel reprocessing plants to ensure that significant quantities of weapons-grade nuclear material are not diverted over a specified time frame. Currently, methods to verify that the facilities are operating under adequate safeguard-declared conditions require time consuming sampling and expensive, destructive analysis. The time delay between sampling and subsequent analysis provides a potential opportunity to divert the material out of the appropriate chemical stream. One way to avoid this problem is to use process monitoring equipment that is capable of on-line and in near-real time monitoring of the flowsheet radiochemical streams to rapidly identify deviations from normal operating conditions. Three integrated systems for flowsheet monitoring are currently being developed at PNNL including: 1) Multi-Isotope Process Monitor (MIP), 2) a spectroscopy-based monitor utilizing UV-Vis-NIR (Ultra Violet-Visible-Near Infrared) and Raman spectrometers, and 3) Electrochemically Modulated Separations (EMS). MIP uses gamma spectroscopy and pattern recognition software to identify off-normal conditions in process streams. The UV-Vis-NIR and Raman spectroscopic monitoring continuously measures chemical compositions of the process streams including actinide metal ions (U, Pu, Np), selected fission products, and major cold flowsheet chemicals. EMS provides an on-line means for pre-separating and preconcentrating elements of interest out of complex matrices prior to detection via non-destructive assay by gamma spectroscopy or destructive analysis with mass spectrometry. PNNL previously reported some of its initial modeling work as proof of principle. Here we will provide a general overview of the technologies and the ongoing demonstrations that utilize actual spent fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Entanglement rearrangement in self-consistent nuclear structure calculations

Background: Entanglement plays a central role in a diverse array of increasingly important research areas, including quantum computation, simulation, measurement, sensing, and communication. Extensive suites of investigations have been performed to better understand entanglement in atomic and molecular quantum many-body systems, while the exploration of entanglement in the structure of nuclei and their reactions is presently in its infancy. Purpose: The goal of this work is to begin investigating the entanglement properties of nuclei from first-principles nuclear many-body calculations. We attempt to identify common features and emergent structures of entanglement that could ultimately lead to new and natural many-body schemes. With an eye toward quantum accelerators in future hybrid-supercomputers, criteria for partitioning nuclear many-body calculations into quantum and classical components may provide advantages in future large-scale computations. Along the way we look for explanations of the relative success of phenomenological models such as the nuclear shell model, and for better ways to match to low-energy nuclear effective field theories and lattice QCD calculations to nuclear many-body techniques that are based upon entanglement. Method: We explore the entanglement between single-particle states in 4 He and 6 He. The patterns of entanglement emerging from different single-particle bases are compared, and possible links with the convergence of observables are explored, in particular, ground-state energies. The nuclear wave functions are obtained by performing active-space no-core configuration-interaction calculations using a two-body nucleon-nucleon interaction derived from chiral effective field theory. Entanglement measures within single-particle bases exhibiting different degrees of complexity are determined, in particular, harmonic oscillator (HO), Hartree-Fock (HF), natural (NAT) and variational natural (VNAT) bases. Specifically, single-orbital entanglement entropy, two-orbital mutual information, and negativity are studied. Results: The entanglement structures in 4 He and 6 He are found to be more localized within NAT and VNAT bases than within a HO basis for the optimal HO parameters we have worked with. In particular a core-valence structure clearly emerges from the full no-core calculation of 6 He. Here, the two-nucleon mutual information shows that the VNAT basis, which typically exhibits good convergence properties, effectively decouples the active and inactive spaces. Conclusions: Measures of one- and two-nucleon entanglement are found to be useful in analyzing the structure of nuclear wave functions, in particular the efficacy of basis states, and may provide useful metrics toward developing more efficient schemes for ab initio computations of the structure and reactions of nuclei, and quantum many-body systems more generally.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Development of a wide bandwidth heterodyne dispersion interferometer for electron density measurement of atmospheric pressure plasmas

One of the challenges of electron density measurements of an atmospheric pressure plasma (APP) with a laser interferometer is the significant and unwanted phase shift caused by changes in the neutral gas density. These unwanted phase shifts can be mitigated and plasma density measured using an interferometer architecture called a dispersion interferometer (DI). A DI is composed of two nonlinear orientation patterned GaAs crystals for frequency doubling and measures the phase shift induced by a plasma in the interference signal between two second-harmonic beams. Measurement of plasma dynamics or a short plasma pulse in less than a millisecond is enabled with heterodyne detection in a DI using an acousto-optic cell with a frequency of 40 MHz. This heterodyne DI (HDI) is targeted to measure APPs in an electron density range of 10 20 –10 24 m −3 . Finally, the HDI achieves a line-integrated density resolution of 2 × 10 15 m −2 (a phase resolution of 0.005°) with a time constant of 1 μs using ensemble averaging techniques.

atmospheric pressure plasma↗

From phase decomposition to evaporation: A multi-modal evaluation of thermally degraded model lightweight high-entropy alloy

Lightweight high-entropy alloys (LHEAs) have the potential to replace conventional lightweight materials due to their superior mechanical properties and thermal stability. However, the thermal degradation pattern of LHEAs from phase decomposition to evaporation is not clear. We develop a new Al-based dual phase (FCC + HCP) LHEA—AlTi 0.45 CuZn, and further investigate its thermal degradation behavior for potential high-temperature structural applications. Using multimodal advanced characterization techniques such as differential scanning calorimetry/thermogravimetric analysis, scanning/transmission electron microscopy, and synchrotron X-ray diffraction/pair distribution function (XRD/PDF), a sequence of thermal degradation events beyond the thermal phase stability limit—between 250 and 360 °C—is observed. These include phase decomposition at ~360 °C, Zn evaporation at ~750 °C, and LHEA melting at 880 °C which results in ~25% cumulative weight loss. The formation of Al-Ti phase off the AlTi 0.45 CuZn matrix is due to the largest negative mixing enthalpy for Al-Ti than other binary pairs. Similarly, Zn evaporation from AlTi 0.45 CuZn LHEA is due to its faster evaporation rate than other constituent elements. The high-resolution synchrotron XRD and PDF results support the aforementioned observations; in addition, they reveal local atomic arrangements, local strain, and sluggish grain growth in the LHEA. Among other LHEAs of close density range (5.55 ≤ ρ ≤ 5.85 g/cc), the investigated LHEA exhibits outstanding nano-indentation hardness values due to the coupled grain size effect and HCP phase strengthening of the FCC matrix. As the search for LHEAs for lightweight applications grows, this study shows the potential use of AlTi 0.45 CuZn LHEA for structural applications even at elevated temperatures.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Area-Selective Atomic Layer Deposition of Metal Oxides on Noble Metals through Catalytic Oxygen Activation

Area-selective atomic layer deposition (ALD) is envisioned to play a key role in next-generation semiconductor processing and can also provide new opportunities in the field of catalysis. In this work, we developed an approach for the area-selective deposition of metal oxides on noble metals. Using O 2 gas as co-reactant, area-selective ALD has been achieved by relying on the catalytic dissociation of the oxygen molecules on the noble metal surface, while no deposition takes place on inert surfaces that do not dissociate oxygen (i.e., SiO 2 , Al2O 3 , Au). The process is demonstrated for selective deposition of iron oxide and nickel oxide on platinum and iridium substrates. Characterization by in situ spectroscopic ellipsometry, transmission electron microscopy, scanning Auger electron spectroscopy, and X-ray photoelectron spectroscopy confirms a very high degree of selectivity, with a constant ALD growth rate on the catalytic metal substrates and no deposition on inert substrates, even after 300 ALD cycles. We demonstrate the area-selective ALD approach on planar and patterned substrates and use it to prepare Pt/Fe 2 O 3 core/shell nanoparticles. Finally, the approach is proposed to be extendable beyond the materials presented here, specifically to other metal oxide ALD processes for which the precursor requires a strong oxidizing agent for growth.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Unusual flaring activity in the blazar PKS 1424-418 during 2008-2011

Context. Blazars are a subset of active galactic nuclei (AGN) with jets that are oriented along our line of sight. Variability and spectral energy distribution (SED) studies are crucial tools for understanding the physical processes responsible for observed AGN emission. Aims. We report peculiar behaviour in the bright γ-ray blazar PKS 1424-418 and use its strong variability to reveal information about the particle acceleration and interactions in the jet. Methods. Correlation analysis of the extensive optical coverage by the ATOM telescope and nearly continuous γ-ray coverage by the Fermi Large Area Telescope is combined with broadband, time-dependent modeling of the SED incorporating supplemental information from radio and X-ray observations of this blazar. Results. We analyse in detail four bright phases at optical-GeV energies. These flares of PKS 1424-418 show high correlation between these energy ranges, with the exception of one large optical flare that coincides with relatively low γ-ray activity. Although the optical/ γ-ray behaviour of PKS 1424-418 shows variety, the multiwavelength modeling indicates that these differences can largely be explained by changes in the flux and energy spectrum of the electrons in the jet that are radiating. We find that for all flares the SED is adequately represented by a leptonic model that includes inverse Compton emission from external radiation fields with similar parameters. Conclusions. Detailed studies of individual blazars like PKS 1424-418 during periods of enhanced activity in different wavebands are helping us identify underlying patterns in the physical parameters in this class of AGN.

Buson, S.↗

Development of nanodiamond foils for H- stripping to Support the Spallation Neutron Source (SNS) using hot filament chemical vapor deposition

Thin diamond foils are needed in many particle accelerator experiments regarding nuclear and atomic physics, as well as in some interdisciplinary research. Particularly, nanodiamond texture is attractive for this purpose as it possesses a unique combination of diamond properties such as high thermal conductivity, mechanical strength and high radiation hardness; therefore, it is a potential material for energetic ion beam stripper foils. At the ORNL Spallation Neutron Source (SNS), the installed set of foils must be able to survive a nominal five-month operation period, without the need for unscheduled costly shutdowns and repairs. Thus, a small foil about the size of a postage stamp is critical to the operation of SNS and similar sources in U.S. laboratories and around the world. We are investigating nanocrystalline, polycrystalline and their admixture films fabricated using a hot filament chemical vapor deposition (HFCVD) system for H- stripping to support the SNS at Oak Ridge National Laboratory. Here we discuss optimization of process variables such as substrate temperature, process gas ratio of H2/Ar/CH4, substrate to filament distance, filament temperature, carburization conditions, and filament geometry to achieve high purity diamond foils on patterned silicon substrates with manageable intrinsic and thermal stresses so that they can be released as free standing foils without curling. An in situ laser reflectance interferometry tool (LRI) is used for monitoring the growth characteristics of the diamond thin film materials. The optimization process has yielded free standing foils with no pinholes. The sp3/sp2 bonds are controlled to optimize electrical resistivity to reduce the possibility of surface charging of the foils. The integrated LRI and HFCVD process provides real time information on the growth of films and can quickly illustrate growth features and control film thickness. The results are discussed in the light of development of nanodiamond foils that will be able to withstand a few MW proton beam and hopefully will be able to be used after possible future upgrades to the SNS to greater than a 3MW beam.

Vispute, R D↗

Effects of growth temperatures on the structural and optoelectronic properties of sputtered zinc sulfide thin films for solar cell applications

The role of various substrate temperatures on the structural and optoelectronic properties of sputtered zinc sulfide (ZnS) thin films has been investigated in this work. The study of prepared film characterization has been done by XRD, AFM, UV–Vis spectrometry and Hall-effect measurement analysis. XRD patterns of the room temperature grown films reveal an amorphous nature, while the films deposited at 100 °C, 200 °C. 300 °C and 400 °C are found to be polycrystalline having the (111) preferential orientation. The optical bandgap values are found in the range of 3.18–3.61 eV depending on the substrate temperatures. The bulk and surface carrier densities are found in the order of 10{sup 12} cm{sup −3} and 10{sup 7} cm{sup −3}, respectively. The growth temperatures are also observed to have a significant effect on the electrical characteristic of the deposited films.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Low-temperature, site selective graphitization of SiC via ion implantation and pulsed laser annealing

A technique is presented to selectively graphitize regions of SiC by ion implantation and pulsed laser annealing (PLA). Nanoscale features are patterned over large areas by multi-ion beam lithography and subsequently converted to few-layer graphene via PLA in air. Graphitization occurs only where ions have been implanted and without elevating the temperature of the surrounding substrate. Samples were characterized using Raman spectroscopy, ion scattering/channeling, SEM, and AFM, from which the degree of graphitization was determined to vary with implantation species, damage and dose, laser fluence, and pulsing. Contrasting growth regimes and graphitization mechanisms during PLA are discussed.

36 MATERIALS SCIENCE↗

Charge-distribution effect of imaging molecular structure by high-order above-threshold ionization

Using a triatomic molecular model, we show that the interference pattern in the high-order above-threshold ionization (HATI) spectrum depends dramatically on the charge distribution of the molecular ion. Therefore the charge distribution can be considered a crucial factor for imaging a molecular geometric structure. Based on this study, a general destructive interference formula for each above-threshold ionization channel is obtained for a polyatomic molecule concerning the positions and charge values of each nuclei. Comparisons are made for the HATI spectra of CO{sub 2}, O{sub 2}, NO{sub 2}, and N{sub 2}. These results may shed light on imaging complex molecular structure by the HATI spectrum.

74 ATOMIC AND MOLECULAR PHYSICS↗

Momentum vector correlations in three-particle fragmentation of triatomic hydrogen

The correlation pattern in the center of mass motion of the three fragments from dissociation of well-defined Rydberg states of H{sub 3} and D{sub 3} is studied. Dissociation of the molecules is induced by an external electric field. Through a comparison with results obtained in radiative cascading we can show that the correlation pattern is that of the short-lived 2s {sup 2}A{sub 1}{sup '} electronic state, of which a tiny amplitude is admixed by the external electric field. A comparison of our results with the predictions by M. Lehner and M. Jungen [J. Phys. B 42, 065101 (2009)] and U. Galster [Phys. Rev. A 81, 032517 (2010)] for predissociation of the 2s {sup 2}A{sub 1}{sup '} state is made. We show that the experimental vector correlation maps are direct images of the spatial symmetry of the product of the vibrational wave function and spatial dependence of the nonadiabatic coupling operator.

74 ATOMIC AND MOLECULAR PHYSICS↗

A model of the effects of heavy ion radiation on human tissue

In heavy ion radiotherapy and space travel humans are exposed to energetic heavy ions (C, Si, Fe and others). This type of irradiation often produces more severe biological effects per unit dose than more common X-rays. A new Monte Carlo model generates a physical space with the complex geometry of human tissue or a cell culture based model of tissue, which is affected by the passage of ionizing radiation. For irradiation, the model relies on a physical code for the ion track structure; for tissues, cellular maps are derived from two- or three-dimensional confocal microscopy images using image segmentation algorithm, which defines cells as pixilated volumes. The model is used to study tissue-specific statistics of direct ion hits and the remote ion action on cells. As an application of the technique, we considered the spatial pattern of apoptotic cells after heavy ion irradiation. The pattern of apoptosis is modeled as a stochastic process, which is defined by the action cross section taken from available experimental data. To characterize the degree of apoptosis, an autocorrelation function that describes the spatial correlation of apoptotic cells is introduced. The values of the autocorrelation function demonstrate the effect of the directionality of the radiation track on the spatial arrangements of inactivated cells in tissue. This effect is intrinsic only to high linear-energy-transfer radiation.

59 BASIC BIOLOGICAL SCIENCES↗

Local twin domains and tip-voltage-induced domain switching of monoclinic M C phase in Pb ( M g 1 / 3 N b 2 / 3 ) O 3 - 0.34 PbTi O 3 single crystal revealed by piezoresponse force microscopy

Here, the monoclinic (M) phases in high-performance relaxor-based ferroelectric single crystals have been recognized to be a vital structural factor for the outstanding piezoelectric property. However, due to the complexity of the structure in M phases, the understanding about it is still limited. In this paper, the local twin domains and tip-voltage-induced domain switching of the M C phase in Pb(Mg 1/3 Nb 2/3 )O 3 - 0.34PbTiO 3 (PMN-0.34PT) single crystal have been intensively investigated by piezoresponse force microscopy (PFM). By theoretically analyzing the experimental patterns of domain walls on the (001) C face, the specific M C twin domains in the initial annealed state of a selected area have been clarified, and the polarization orientation of the M C phase in this sample is determined to be at an angle of 29 degrees to the < 001 > C directions. In addition, based on the evolution of domains and the motion of domain walls under the step-increased PFM tip dc voltage (V dc ), the switching process and features of different types of M C domain variants are visually revealed

74 ATOMIC AND MOLECULAR PHYSICS↗

Nanodiamond Foils for H- Stripping to Support the Spallation Neutron Source (SNS) and Related Applications

Thin diamond foils are needed in many particle accelerator experiments regarding nuclear and atomic physics, as well as in some interdisciplinary research. Particularly, nanodiamond texture is attractive for this purpose as it possesses a unique combination of diamond properties such as high thermal conductivity, mechanical strength and high radiation hardness; therefore, it is a potential material for energetic ion beam stripper foils. At the ORNL Spallation Neutron Source (SNS), the installed set of foils must be able to survive a nominal five-month operation period, without the need for unscheduled costly shutdowns and repairs. Thus, a single nanodiamond foil about the size of a postage stamp is critical to the entire operation of SNS and similar sources in U.S. laboratories and around the world. We are investigating nanocrystalline, polycrystalline and their admixture films fabricated using a hot filament chemical vapor deposition (HFCVD) system for H- stripping to support the SNS at Oak Ridge National Laboratory. Here we discuss optimization of process variables such as substrate temperature, process gas ratio of H2/Ar/CH4, substrate to filament distance, filament temperature, carburization conditions, and filament geometry to achieve high purity diamond foils on patterned silicon substrates with manageable intrinsic and thermal stresses so that they can be released as free standing foils without curling. An in situ laser reflectance interferometry tool (LRI) is used for monitoring the growth characteristics of the diamond thin film materials. The optimization process has yielded free standing foils with no pinholes. The sp3/sp2 bonds are controlled to optimize electrical resistivity to reduce the possibility of surface charging of the foils. The integrated LRI and HFCVD process provides real time information on the growth of films and can quickly illustrate growth features and control over film thickness. The results are discussed in the light of development of nanodiamond foils that will be able to withstand a few MW proton beam and hopefully will be able to be used after possible future upgrades to the SNS to greater than a 3MW beam.

Vispute, R D↗

Mechanism of CO 2 Hydrogenation on Pd/Al 2 O 3 Catalysts: Kinetics and Transient DRIFTS-MS Studies

The hydrogenation of CO 2 was investigated over a wide range of reaction conditions, using two Pd/γ-Al 2 O 3 catalysts with different Pd loadings (5% and 0.5%) and dispersions (~11% and ~100%, respectively). Turnover rates for CO and CH 4 formation were both higher over 5% Pd/Al 2 O 3 with a larger average Pd particle size than those over 0.5% Pd/Al 2 O 3 with a smaller average particle size. The selectivity to methane (22-40%) on 5% Pd/Al 2 O 3 was higher by a factor of 2-3 than that on 0.5% Pd/Al 2 O 3 . The drastically different rate expressions and apparent energies of activation for CO and CH 4 formation lead us to conclude that reverse water gas shift and CO 2 methanation do not share the same rate-limiting step on Pd, and that the two pathways are probably catalyzed at different surface sites. Measured reaction orders in CO 2 and H 2 pressures were similar over the two catalysts, suggesting that the reaction mechanism for each pathway does not change with particle size. In accordance, the DRIFTS results reveal that the prevalent surface species and their evolution patterns are comparable on the two catalysts during transient and steady-state experiments, switching feed gases among CO 2 , H 2 and CO 2 +H 2 . The DRIFTS and MS results also demonstrate that no direct dissociation of CO 2 takes place over the two catalysts, and that CO 2 has to first react with surface hydroxyls on the oxide support. The thus-formed bicarbonates react with dissociatively adsorbed hydrogen on Pd particles to produce adsorbed formate species (bifunctional catalyst: CO 2 activation on the oxide support, and H 2 dissociation on the metal particles). Formates near the Pd particles (most likely at the metal/oxide interface) can react rapidly with adsorbed H to produce CO, which then adsorbs on the metallic Pd particles. Two types of Pd sites are identified: one has a weak interaction with CO, which easily desorbs into gas phase at reaction temperatures, while the other interacts more strongly with CO, which is mainly in multi-bound forms and remains stable in He flow at high temperatures, but is reactive towards adsorbed H atoms on Pd leading eventually to CH 4 formation. 5% Pd/Al 2 O 3 contains a larger fraction of terrace sites favorable for forming these more stable CO species than 0.5% Pd/Al 2 O 3 . Consequently, we propose that the difference in the formation rate and selectivity to CH 4 on different Pd particle sizes stems from the different concentrations of the reactive intermediate for the methanation pathway on the Pd surface. JS gratefully acknowledges the financial support of this work by the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗