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DOE OSTI2025

Characterizing the surface compositions of supported bimetallic PtSn clusters: Effects of cluster-support interactions and surface adsorbates

PtSn bimetallic clusters on TiO2(110) and highly oriented pyrolytic graphite (HOPG) surfaces have been characterized by scanning tunneling microscopy, low energy ion scattering (LEIS), Xray photoelectron spectroscopy, and temperature programmed desorption (TPD); density functional theory (DFT) calculations have also been performed to better understand adsorption of CO and D2 on the PtSn surfaces. On TiO2 at coverages of 2 ML of Pt and 2 ML of Sn, exclusively bimetallic clusters are formed for both orders of deposition because clusters of the first metal completely cover the surface such that all atoms of the second metal are incorporated into the existing clusters. In contrast, on HOPG, the high mobility and weak cluster-support interactions on HOPG result in much larger 2 ML monometallic clusters (~30 Å high) that do not completely cover the surface, and deposition of the second metal produces larger clusters as well as smaller ones. Despite the difference in cluster morphologies for the different orders of deposition and supports, the LEIS experiments demonstrate that in all cases, the PtSn clusters are rich in Sn at the surface, as expected based on the lower surface free energy for Sn compared to Pt. Furthermore, the +0.2 eV shift in the Sn(3d5/2) binding energy observed on all surfaces in the presence of Pt is consistent with PtSn alloy formation. Deposition of 2 ML of Sn on TiO2 produces two-dimensional clusters with oxidation of Sn and reduction of titania at the clustersupport interface, but addition of Pt to the Sn clusters causes Sn to diffuse away from this interface, leaving Sn in the metallic state. TPD experiments on 2 ML Pt/TiO2 with increasing coverages of Sn show that the number of adsorption sites for D2 sharply decreases to nearly zero at 0.5 ML, while CO adsorption decreases to zero only at much higher Sn coverages of 2 ML. DFT studies for Sn modified Pt surfaces and bulk structures demonstrate that for CO adsorption at low Sn coverages (<0.25 ML), the strong Pt-CO interactions induce diffusion of Pt to the cluster surface and the formation of a bulk Pt3Sn alloy, whereas D2 adsorption does not lead to interactions with the Pt surface that are strong enough to induce alloy formation. A single Sn adatom prevents D2 adsorption on four neighboring Pt atoms via site-blocking and the donation of electron density to Pt.

Li, Fangliang↗

NASA NTRS1993

Measuring rapid ocean tidal earth orientation variations with very long baseline interferometry

Ocean tidal effects on universal time and polar motion (UTPM) are investigated at four nearly diurnal (K(sub 1), P(sub 1), O(sub 1), and Q(sub 1)) and four nearly semidiurnal (K(sub 2), S(sub 2), M(sub 2), and N(sub 2)) frequencies by analyzing very long baseline interferometry (VLBI) data extending from 1978 to 1992. We discuss limitations of comparisons between experiment and theory for the retograde nearly diurnal polar motion components due to their degeneracy with prograde components of the nutation model. Estimating amplitudes of contributions to the modeled VLBI observables at these eight frequencies produces a statistically highly significant improvement of 7 mm to the residuals of a fit to the observed delays. Use of such an improved UTPM model also reduces the 14-30 mm scatter of baseline lengths about a time-linear model of tectonic motion by 3-14 mm, also withhigh significance levels. A total of 28 UTPM ocean tidal amplitudes can be unambiguously estimated from the data, with resulting UTI and PM magnitudes as large as 21 micro secs and 270 microarc seconds and formal uncertainties of the order of 0.3 micro secs and 5 microarc secs for UTI and PM, respectively. Empirically determined UTPM amplitudes and phases are com1pared to values calculated theoretically by Gross from Seiler's global ocean tide model. The discrepancy between theory and experiment is larger by a factor of 3 for UTI amplitudes (9 micro secs) than for prograde PM amplitudes (42 microarc secs). The 14-year VLBI data span strongly attenuates the influence of mismodeled effects on estimated UTPM amplitudes and phases that are not coherent with the eight frequencies of interest. Magnitudes of coherent and quasi-coherent systematic errors are quantified by means of internal consistency tests. We conclude that coherent systematic effects are many times larger than the formal uncertainties and can be as large as 4 micro secs for UTI and 60 microarc secs for polar motion. On the basis of such ealistic error estimates, 22 of the 31 fitted UTPM ocean tidal amplitudes differ from zero by more than 2 sigma.

Sovers, O. J.↗

DOE OSTI2025

Equilibrium Fe isotope fractionation between olivine, pyroxene, spinel and MORB glass: Implications for mantle partial melting to generate MORBs

Primitive mid-ocean ridge basalts (MORBs) exhibit Fe isotopic compositions heavier than the upper mantle by +0.074 ± 0.028 ‰ for δ 56 Fe. The processes responsible for this isotopic difference remain unclear. Modeling of Fe isotope fractionation during mantle partial melting requires reliable equilibrium Fe isotope fractionation factors between minerals and melts, for which consistent data are still lacking. Here, in this study, we used Nuclear Resonant Inelastic X-ray Scattering (NRIXS) technique to measure Fe force constants for a MORB glass (ALV 519-4-1) and natural mantle minerals (olivine, orthopyroxene, clinopyroxene, and spinel) to determine the equilibrium Fe isotope fractionation factors between them. The force constants determined in this study, in increasing order, are 167 ± 26 N/m for spinel, 175 ± 17 N/m for olivine, 176 ± 20 N/m for MORB glass, 205 ± 26 N/m for clinopyroxene, and 219 ± 36 N/m for orthopyroxene. We evaluated the previously proposed mechanisms for the heavy Fe isotopic composition of MORBs, including (i) mantle partial melting, (ii) mantle lithological heterogeneity, with pyroxenite in the source, (iii) mantle metasomatism by low-degree melts, and (iv) fractional crystallization of olivine from melts. For (i), we used the pMELTS program to simulate adiabatic decompression melting of mantle peridotites, and calculated Fe isotope fractionation based on Fe 3+ –Fe 2+ equilibrium-controlled fractionation, where Fe 3+ forms stronger bonds and is more incompatible than Fe 2+ . At 10 wt% peridotite melting, corresponding to MORB generation, only +0.03 ‰ Fe isotope fractionation between the melt and the original bulk composition (Δ 56 Fe = δ 56 Fe melt - δ 56 Fe 0 ) was produced, insufficient to account for the observed MORB-upper mantle difference. For (ii), melting of pyroxenites yields smaller Fe isotope fractionation than melting of peridotites, making it unlikely the cause for the MORB-upper mantle isotopic difference. For (iii), both the Fe 3+ /ΣFe ratio and the δ 56 Fe of melts increase with the degree of partial melting, indicating that low-degree melts are not isotopically heavy enough to significantly alter the isotopic composition of lithospheric mantle through metasomatism. For (iv), equilibrium isotope fractionation between olivine and melt is near zero. These results suggest that equilibrium Fe isotope fractionation alone cannot explain the MORB isotopic signature, highlighting the potential role of kinetic isotope fractionation. Using a diffusion model, we calculated kinetic Fe and Mg isotope fractionations associated with (iv) olivine crystallization from a melt, and found that the predicted Fe and Mg isotope fractionations were inconsistent with observations in MORBs. Qualitatively, two processes could have induced kinetic Fe isotope fractionation during MORB generation: (a) Fe-Mg interdiffusion between melt and solid during melt migration and (b) reactive melt-rock interactions during melt focusing. However, a quantitative understanding of their role in modifying the melt isotopic composition remains limited and requires further investigation.

Fe isotopes↗

NASA NTRS2001

Water Ice and Life's Roots in Space

Nearly three decades ago as Voyager 2 spacecraft raced out of the Solar System. NASA engineers turned its camera arm around (at the request of the American astronomer Carl Sagan) to take a parting snapshot of Earth. Earth's image was a single pale blue pixel, its color caused by the Rayleigh scattering of sunlight in the water of our oceans. Earth is a water planet, and this is the color of life. No matter how far we travel on our planet, no matter how high or deep, if we find liquid water, we find some form of life that manages to survive there. And yet there is a cruel irony. Water in its solid crystalline form is hostile to life. Organisms can roost in geysers, wallow in brine and gulp down acid, but they cowered from ice. The rigid ordering of water molecules in ice crystals expels impurities and tears organic tissue beyond repair. In fact, about the only good thing you can say about ice is that it gets out of the way: Its low density ensures that it floats and leaves the water dwelling creatures in peace. Recent discoveries have caused us to rethink this basic premise. New lines of evidence both observational and experimental - suggest that prebiotic organic compounds are not only comfortable in, but in fact had their origin in a peculiar form of solid water ice that is ubiquitous in interstellar space, but completely absent from Earth. Only recently have we been able to create even submicroscopic quantities of this ice in terrestrial laboratories, yet it constitutes the most abundant form of water in the universe. Interstellar ice is a far cry from the ice we are so familiar with on Earth. This interstellar ice has no crystalline structure, and despite the fact that its temperature is a scant few degrees above absolute zero (where all molecular motion ceases), it is highly reactive and can flow like water when exposed to radiation. It is in fact this ice's similarity to liquid water that allows it to participate in the creation of the very first organic compounds.

Blake, David↗

DOE OSTI2023

Anisotropic magnetism and electronic structure of trigonal EuAl 2 Ge 2 single crystals

Understanding the interplay between magnetic and electronic degrees of freedom is of profound recent interest in different Eu-based magnetic topological materials. Here, we studied the magnetic and electronic properties of the layered Zintl-phase compound EuAl 2 Ge 2 crystallizing in the trigonal CaAl 2 Si 2 -type structure. We report zero-field neutron diffraction, temperature T - and magnetic-field H-dependent magnetic susceptibility χ(T, H), isothermal magnetization M(T, H), heat capacity C p (T, H), and electrical resistivity ρ(T, H) measurements, together with T-dependent angle-resolved photoemission spectroscopy (ARPES) measurements complemented with first-principle calculations. EuAl 2 Ge 2 undergoes second-order A-type antiferromagnetic (AFM) ordering below T N = 27.5(5) K, with the Eu moments (Eu 2+ , S = 7/2) aligned ferromagnetically in the ab plane while these layers are stacked antiferromagnetically along the c axis. The critical fields at which all moments become parallel to the field are 37.5(5) and 52.5(5) kOe for H ∥ ab and H ∥ c, respectively. The H = 0 magnetic structure consists of trigonal AFM domains associated with ab-plane magnetic anisotropy and a field-induced reorientation of the Eu spins in the domains is also evident at T = 2 K below the critical field H c1 = 2.5(1) kOe. The ρ(T) measurements reveal metallic behavior transforming into a slight resistivity increase on cooling towards T N . A pronounced loss of spin-disorder scattering is observed below T N . The ARPES results show that EuAl 2 Ge 2 is metallic both above and below T N , and the Fermi surface is anisotropic with two hole pockets at the zone center and one small electron pocket at each M point. In the AFM phase, we directly observe folded bands in ARPES due to the doubling of the magnetic unit cell along the c axis with an enhancement of quasiparticle weight due to the complex change in the coupling between the magnetic moments and itinerant electrons on cooling below T N . The observed electronic structure is well reproduced by first-principle calculations, which also predict the presence of nontrivial electronic states near the Fermi level in the AFM phase with Z 2 topological numbers 1;(000)

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS1998

Studies of Long Period Variability in Neutron Star HMXB Systems

The purpose of this effort was to investigate the long term, quasi-periodic variability of the X-ray emission from the accreting X-ray pulsars LMC X-4 and SMC X-1. These high mass X-ray binary (HMXB) sources are known to vary in a nearly periodic fashion with cycle lengths of about 30 and 60 days respectively. The prevailing model for such behavior is that it is due to the precession of a tilted accretion disk around the neutron star which is the source of the X-ray emission. As the disk precesses, it periodically obscures the emitting region, resulting in reduced flux as observed at the Earth. The obscuration is not strictly periodic, as the disk precession period changes as the total mass and size of the disk change through variable accretion processes. This model is well established for the long-period variability in the X-ray pulsar Her X-1. With this work, my collaborators and I sought to test whether this model works for LMC X-4 and SMC X-1. Observations with the pointed instruments on the Rossi X-ray Timing Explorer (RXTE) were carried out in order to observe changes in the X-ray spectrum and total flux which were correlated with the long period cycles in these objects. One of the main predictions of the precessing disk model is that the periods of low emission are caused not by changes in the central source, but by increased absorption of that flux as seen at the Earth. Such behavior would be observed in the X-ray spectrum as a relative lack of low energy X-rays (which are more easily absorbed) as compared to high energy X-rays. This is what was observed for SMC X-1, landing strong support to the precessing disk model for this system. For LMC X-1, however, the absorption was consistent with zero at the time of minimum flux. The entire spectrum appeared to be equally reduced. This is not supporting evidence for the model. However, it also does not rule out a precessing disk. If at the time of minimum flux, the intervening disk is so thick that no flux, even high energy X-rays, can penetrate, and if there is material above the disk which can scatter X-rays, then a small scattered spectrum will be seen which is indistinguishable from the unobscured source flux. This is quite possibly the case in LMC X-1.

Heindl, William A.↗