Lin-Shu Du
Stanford University
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Featured researches published by Lin-Shu Du.
Journal of Non-crystalline Solids | 2003
Lin-Shu Du; Jonathan F. Stebbins
In several series of lithium, sodium, and potassium borosilicate glasses whose compositions traverse known regions of liquid–liquid phase separation, we have applied triple-quantum magic-angle spinning (3QMAS) 11B and 17O NMR to obtain high-resolution information about short-range structure and connections among various network structural units, and their variation with composition and thermal history. Oxygen-17 3QMAS spectra reveal changes in connectivities between silicate and BO3 ([3]B) and BO4 ([4]B) units, by quantifying populations of bridging oxygens such as B–O–B, Si–O–B and Si–O–Si, and of non-bridging oxygens. [3]B–O–Si and [4]B–O–Si as well as [3]B–O–[3]B and [4]B–O–[3]B linkages can be distinguished. 11B MAS and 3QMAS at a magnetic field of 14.1 T allow proportions of several borate units to be determined, including [3]B in boroxol ring and non-ring sites and [4]B with 3 versus 4 Si neighbors. By combining the 11B and 17O NMR results, detailed information on Si/B mixing in sodium borosilicates can be derived, showing, for example, that [4]B and non-ring [3]B tend to mix with silicate units, while ring [3]B is mainly connected to borate groups. In a preliminary study of the effects of varying alkali cation, potassium-containing glasses are similar to those in the sodium borosilicate system, but a lithium borosilicate seems to exhibit considerably greater chemical heterogeneity. In annealing experiments that converted an optically clear to obviously phase-separated glasses, the ratio of [3]B to [4]B does not change significantly, but part of the non-ring [3]B converts to ring [3]B as the degree of unmixing increases.
American Mineralogist | 2002
Jonathan F. Stebbins; Lin-Shu Du
Abstract Despite the importance of the chloride ion in magmas and the fluids that separate from them, very little is known about atomic-scale structural environments for Cl- in silicate glasses. We present here the first solid-state 35Cl NMR data for Cl in silicate and aluminosilicate glasses, made possible by the availability of very high (14.1 to 18.8 Tesla) magnetic fields. We find that 35Cl has a wide range in chemical shifts that correlate well with cation-Cl distance and thus contain considerable structural information. In general, Cl is coordinated primarily by network-modifying alkali or alkaline earth cations, and we see no evidence for Al-Cl bonding.
American Mineralogist | 2002
Philip S. Neuhoff; Scott Kroeker; Lin-Shu Du; Thráinn Fridriksson; Jonathan F. Stebbins
Abstract Disordering of Si and Al in natrolite, scolecite, mesolite, and gonnardite was investigated with 29Si and 27Al magic angle spinning nuclear magnetic resonance (MAS NMR) spectroscopy. The results indicate that with the exception of one sample of natrolite (from San Benito County, California), the natrolite, mesolite, and scolecite samples studied all exhibit small degrees (<10% Al occupancy of Si sites) of Si-Al disorder. The spectra for these samples are consistent with Al avoidance. Gonnardite is confirmed to have extensive Si-Al disorder, with only slight preferential Si occupation of the T1 site. Fits of 29Si MAS NMR spectra and mathematical relations based on Al avoidance were used to calculate Si and Al occupancies across the tetrahedral sites in these minerals. Configurational entropies arising from Si-Al disorder in natrolite, mesolite, and scolecite can add an addition 1-2% [up to 11 J/(mol·K)] to the total entropies of these phases at 298.15 K, whereas it may add as much as 7% to that of gonnardite [up to 27.7 J/(mol·K)]. These results also concur with previous observations of a gap in Si-Al disordering between orthorhombic and tetragonal natrolite samples and suggest that the state of disorder in natrolite is a function of temperature. The 29Si MAS NMR spectrum of gonnardite is consistent with a disordered natrolite framework structure, and not an intergrowth of thomsonite and natrolite structural domains.
American Mineralogist | 2007
Kimberly E. Kelsey; Jonathan F. Stebbins; Lin-Shu Du; Ben Hankins
Abstract The 17O NMR spectra of glasses quenched from melts at high pressure are often difficult to interpret due to overlapping peaks and lack of crystalline model compounds. High-pressure aluminosilicate glasses often contain significant amounts of [5]Al and [6]Al, thus these high-pressure glasses must contain oxygen bonded to high-coordinated aluminum. The 17O NMR parameters for the minerals jadeite, pyrope, grossular, and mullite are presented to assist interpretation of glass spectra and to help test quantum chemical calculations. The 17O NMR parameters for jadeite and grossular support previous peak assignments of oxygen bonded to Si and high-coordinated Al in high-pressure glasses as well as quantum chemical calculations. The oxygen tricluster in mullite is very similar to the previously observed tricluster in grossite (CaAl4O7) and suspected triclusters in glasses. We also present 27Al NMR spectra for pyrope, grossular, and mullite.
American Mineralogist | 2006
Jonathan F. Stebbins; Lin-Shu Du; Kimberly E. Kelsey; Hiroshi Kojitani; Masaki Akaogi; Shigeaki Ono
Abstract Aluminum is an important minor constituent of a number of high-pressure mantle silicates in which it substitutes for octahedrally coordinated silicon. In several cases, its solid solution may be linked to the presence of oxygen vacancies; in others, to charge balance with H+. Here we present new data from high-resolution, high-field (18.8 Tesla) 27Al NMR of aluminous stishovite and of a non-stoichiometric perovskite with nominal composition MgSi0.95Al0.05O2.975. For the stishovite, we characterize the local structure of the symmetrical, octahedral site for Al. These results, combined with 27Al{1H} REDOR NMR, are consistent with hypothesized H+ charge balance, although the presence of a significant fraction of randomly distributed oxygen vacancies could remain undetected. As in a recent previous study of a related perovskite composition, the observed ratio of Al at symmetrical octahedral B sites to that of Al at large, central A sites is about 2:1, indicating the presence of oxygen vacancies to account for charge neutrality in this phase. Such vacancies are not preferentially associated with the Al octahedra, however, suggesting a random distribution in the structure.
Archive | 2009
Corey W. Liu; Viktor Y. Alekseyev; Jeffrey R. Allwardt; Alexander J. Bankovich; Barbara J. Cade-Menun; Ronald W. Davis; Lin-Shu Du; K. Christopher Garcia; Daniel Herschlag; Chaitan Khosla; Daniel A. Kraut; Qing Li; Brian Null; Joseph D. Puglisi; Paul A. Sigala; Jonathan F. Stebbins; Luca Varani
The discovery of the physical phenomenon of Nuclear Magnetic Resonance (NMR) in 1946 gave rise to the spectroscopic technique that has become a remarkably versatile research tool. One could oversimplify NMR spectros-copy by categorizing it into the two broad applications of structure eluci-dation of molecules (associated with chemistry and biology) and imaging (associated with medicine). But, this certainly does not do NMR spectros-copy justice in demonstrating its general acceptance and utilization across the sciences. This manuscript is not an effort to present an exhaustive, or even partial review of NMR spectroscopy applications, but rather to pro-vide a glimpse at the wide-ranging uses of NMR spectroscopy found within the confines of a single magnetic resonance research facility, the Stanford Magnetic Resonance Laboratory. Included here are summaries of projects involving protein structure determination, mapping of intermolecular inter-actions, exploring fundamental biological mechanisms, following compound cycling in the environmental, analysis of synthetic solid compounds, and microimaging of a model organism.
Journal of Non-crystalline Solids | 2005
Lin-Shu Du; Jonathan F. Stebbins
Geochimica et Cosmochimica Acta | 2004
Travis O. Sandland; Lin-Shu Du; Jonathan F. Stebbins; James D. Webster
Journal of Non-crystalline Solids | 2004
Lin-Shu Du; Jeffrey R. Allwardt; B. Schmidt; Jonathan F. Stebbins
Journal of Non-crystalline Solids | 2004
T. J. Kiczenski; Lin-Shu Du; Jonathan F. Stebbins