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All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Materials Data on Y(SiOs)2 by Materials Project

Y(OsSi)2 crystallizes in the tetragonal I4/mmm space group. The structure is three-dimensional. Y3+ is bonded in a 8-coordinate geometry to eight equivalent Os+1.50- atoms. All Y–Os bond lengths are 3.19 Å. Os+1.50- is bonded in a 4-coordinate geometry to four equivalent Y3+ and four equivalent Si atoms. All Os–Si bond lengths are 2.40 Å. Si is bonded in a 5-coordinate geometry to four equivalent Os+1.50- and one Si atom. The Si–Si bond length is 2.49 Å.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Photonic integration of Er 3+ :Y 2 SiO 5 with thin-film lithium niobate by flip chip bonding

Rare earth ions are known as promising candidates for building quantum light-matter interface. However, tunable photonic cavity access to rare earth ions in their desired host crystal remains challenging. Here, we demonstrate the integration of erbium doped yttrium orthosilicate (Er 3+ :Y 2 SiO 5 ) with thin-film lithium niobate photonic circuit by plasma-activated direct flip chip bonding. Resonant coupling to erbium ions is realized by on-chip electro-optically tuned high Q lithium niobate micro-ring resonators. Fluorescence and absorption of erbium ions at 1536.48 nm are measured in the waveguides, while the collective ion-cavity cooperativity with micro-ring resonators is assessed to be 0.36. This work presents a versatile scheme for future rare earth ion integrated quantum devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Thermal properties of field-assisted-sintered SiCN–Y 2 O 3 composites

Polymer-derived amorphous SiCN has excellent high-temperature stability and properties. To reduce the shrinkage during pyrolysis and to improve the high-temperature oxidation resistance, Y 2 O 3 was added as a filler. In this study, polymer-derived SiCN–Y 2 O 3 composites were fabricated by mixing a polymeric precursor of SiCN with Y 2 O 3 submicron powders in different ratios. The mixtures were cross-linked and pyrolyzed in argon. SiCN–Y 2 O 3 composites were processed using field-assisted sintering technology at 1350°C for 5 min under vacuum. Dense SiCN–Y 2 O 3 composite pellets were successfully made with relative density higher than 98% and homogeneous microstructure. Due to low temperature and short time of the heat-treatment, the grain growth of Y 2 O 3 was substantially inhibited. The Y 2 O 3 grain size was ~1 μm after sintering. The composites’ heat capacity, thermal diffusivity, and thermal expansion coefficients were characterized as a function of temperature. The thermal conductivity of the composites ceramics decreased as the amount of amorphous SiCN increased and the coefficient of thermal expansion (CTE) of the composites increased with Y 2 O 3 content. However, the thermal conductivity and CTE did not follow the rule of mixture. This is likely due to the partial oxidation of SiCN and the resultant impurity phases such as Y 2 SiO 5 , Y 2 Si 2 O 7 , and Y 4.67 (SiO 4 ) 3 O.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Structure of diopside, enstatite, and magnesium aluminosilicate glasses: A joint approach using neutron and x-ray diffraction and solid-state NMR

Neutron diffraction with magnesium isotope substitution, high energy x-ray diffraction, and 29 Si, 27 Al, and 25 Mg solid-state nuclear magnetic resonance (NMR) spectroscopy were used to measure the structure of glassy diopside (CaMgSi 2 O 6 ), enstatite (MgSiO 3 ), and four (MgO) x (Al 2 O 3 ) y (SiO 2 ) 1–x–y glasses, with x = 0.375 or 0.25 along the 50 mol. % silica tie-line (1 – x – y = 0.5) or with x = 0.3 or 0.2 along the 60 mol. % silica tie-line (1 – x – y = 0.6). The bound coherent neutron scattering length of the isotope 25 Mg was remeasured, and the value of 3.720(12) fm was obtained from a Rietveld refinement of the powder diffraction patterns measured for crystalline 25 MgO. The diffraction results for the glasses show a broad asymmetric distribution of Mg–O nearest-neighbors with a coordination number of 4.40(4) and 4.46(4) for the diopside and enstatite glasses, respectively. As magnesia is replaced by alumina along a tie-line with 50 or 60 mol. % silica, the Mg–O coordination number increases with the weighted bond distance as less Mg 2+ ions adopt a network-modifying role and more of these ions adopt a predominantly charge-compensating role. 25 Mg magic angle spinning (MAS) NMR results could not resolve the different coordination environments of Mg 2+ under the employed field strength (14.1 T) and spinning rate (20 kHz). The results emphasize the power of neutron diffraction with isotope substitution to provide unambiguous site-specific information on the coordination environment of magnesium in disordered materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Mapping the structural trends in zinc aluminosilicate glasses

The structure of zinc aluminosilicate glasses with the composition (ZnO) x (Al 2 O 3 ) y (SiO 2 ) 1-x-y , where 0 ≤ x < 1, 0 ≤ y < 1, and x + y < 1, was investigated over a wide composition range by combining neutron and high-energy x-ray diffraction with 27 Al magic angle spinning nuclear magnetic resonance spectroscopy. The results were interpreted using an analytical model for the composition-dependent structure in which the zinc ions do not act as network formers. Four-coordinated aluminum atoms were found to be in the majority for all the investigated glasses, with five-coordinated aluminum atoms as the main minority species. Mean Al–O bond distances of 1.764(5) and 1.855(5) Å were obtained for the four- and five-coordinated aluminum atoms, respectively. The coordination environment of zinc was not observed to be invariant. Instead, it is dependent on whether zinc plays a predominantly network-modifying or charge-compensating role and, therefore, varies systematically with the glass composition. The Zn–O coordination number and bond distance were found to be 4.36(9) and 2.00(1) Å, respectively, for the network-modifying role vs 5.96(10) and 2.08(1) Å, respectively, for the charge-compensating role. The more open coordination environment of the charge-compensator is related to an enhanced probability of zinc finding bridging oxygen atoms as nearest-neighbors, reflecting a change in the connectivity of the glass network comprising four-coordinated silicon and aluminum atoms as the alumina content is increased.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Visible emission spectra of thermographic phosphors under x-ray excitation

Thermographic phosphors have been employed for temperature sensing in challenging environments, such as on surfaces or within solid samples exposed to dynamic heating, because of the high temporal and spatial resolution that can be achieved using this approach. Typically, UV light sources are employed to induce temperature-sensitive spectral responses from the phosphors. However, it would be beneficial to explore x-rays as an alternate excitation source to facilitate simultaneous x-ray imaging of material deformation and temperature of heated samples and to reduce UV absorption within solid samples being investigated. Here, the phosphors BaMgAl 10 O 17 :Eu (BAM), Y 2 SiO 5 :Ce, YAG:Dy, La 2 O 2 S:Eu, ZnGa 2 O 4 :Mn, Mg 3 F 2 GeO 4 :Mn, Gd 2 O 2 S:Tb, and ZnO were excited using incident synchrotron x-ray radiation. These materials were chosen to include conventional thermographic phosphors as well as x-ray scintillators (with crossover between these two categories). X-ray-induced thermographic behavior was explored through the measurement of visible spectral response with varying temperature. The incident x-rays were observed to excite the same electronic energy level transitions in these phosphors as UV excitation. Similar shifts in the spectral response of BAM, Y 2 SiO 5 :Ce, YAG:Dy, La 2 O 2 S:Eu, ZnGa 2 O 4 :Mn, Mg 3 F 2 GeO 4 :Mn, and Gd 2 O 2 S:Tb were observed when compared to their response to UV excitation found in literature. Some phosphors were observed to thermally quench in the temperature ranges tested here, while the response from others did not rise above background noise levels. This may be attributed to the increased probability of non-radiative energy release from these phosphors due to the high energy of the incident x-rays. These results indicate that x-rays can serve as a viable excitation source for phosphor thermometry.

42 ENGINEERING↗
DOE OSTI2020

Tape casting and characterizations of MgO ceramics

Herein we report a high density MgO ceramic substrate produced by the tape casting technology. The tape casting formulation and process produced a uniform tape free of cracking. Y 2 O 3 and SiO 2 were used as the sintering aid for the pressureless sintering of the green tape. X-ray diffraction phase identification indicates that MgO is the main phase, while both Y 2 O 3 and SiO 2 sintering aids react with MgO to form MgY 4 Si 3 O 13 as the second phase. Liquid phase sintering occurs in the temperature range from 1030°C to ~1500°C, which is confirmed by the simultaneous Thermal Gravitation Analysis/ Differential Scanning Calorimeter (TGA/DSC) and the percent linear shrinkage and densification. A 96.5% theoretical density was achieved by presureless sintering at 1650°C for 2 hours, which was further increased to a fully dense structure using hotisostatic- pressing(HIP) at 1650°C and 207 MPa in argon. Scanning electron microscopy (SEM) and energy dispersive(EDS) spectroscopic analysis on the HIP’ed sample show that MgY 4 Si 3 O 13 is located at the MgO grain boundary and the sample has a fully dense structure. The refractive indices and extinction coefficient were measured on the HIP’ed sample along with thermal properties and dielectric properties. Thermal diffusivity and heat capacity were measured to calculate the thermal conductivity.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Supported Platinum Nanoparticles Catalyzed Carbon–Carbon Bond Cleavage of Polyolefins: Role of the Oxide Support Acidity

Supported platinum nanoparticle catalysts are known to convert polyolefins to high-quality liquid hydrocarbons using hydrogen under relatively mild conditions. To date, few studies using platinum grafted onto various metal oxide (M x O y ) supports have been undertaken to understand the role of the acidity of the oxide support in the carbon-carbon bond cleavage of polyethylene under consistent catalytic conditions. Specifically, two Pt/M x O y catalysts (M x O y = SrTiO 3 and SiO 2 -Al 2 O 3 ; Al = 3.0 wt %, target Pt loading 2 wt % Pt similar to 1.5 nm), under identical catalytic polyethylene hydrogenolysis conditions (T = 300 degree celsius, P(H 2 ) = 170 psi, t = 24 h; M w = similar to 3,800 g/mol, M n = similar to 1,100 g/mol, D = 3.45, N branch/100C = 1.0), yielded a narrow distribution of hydrocarbons with molecular weights in the range of lubricants (M w = < 600 g/mol; M n < 400 g/mol; D = 1.5). While Pt/SrTiO 3 formed saturated hydrocarbons with negligible branching, Pt/SiO 2 -Al 2 O 3 formed partially unsaturated hydrocarbons (<1 mol % alkenes and similar to 4 mol % alkyl aromatics) with increased branch density (N branch/100C = 5.5). Further investigations suggest evidence for a competitive hydrocracking mechanism occurring alongside hydrogenolysis, stemming from the increased acidity of Pt/SiO 2 -Al 2 O 3 compared to Pt/SrTiO 3 . Additionally, the products of these polymer deconstruction reactions were found to be independent of the polyethylene feedstock, allowing the potential to upcycle polyethylenes with various properties into a value-added product.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Nanoscopic Plugs Block Hydrogen Crossover in Submicron Thick Proton-Conducting SiO 2 Membranes for Water Electrolysis

Zero-gap electrolyzers based on submicron thick proton-conducting oxide membranes (POMs) represent a promising approach to increasing the efficiency of H 2 production from water electrolysis while moving away from conventional perfluorosulfonic acid (PFSA) membranes. A critical barrier to the commercialization of such electrolyzers is that the ultrathin nature of POMs, which is necessary to achieve low cell resistance, makes them more susceptible to defects that can lead to unacceptably high rates of H 2 crossover. Herein, we demonstrate an approach to mitigate this problem through selective deposition of carbon-containing silicon oxide (SiO x C y ) “nanoplugs” into the defects of submicron thick SiO 2 membranes using a facile electrochemically mediated deposition process. Selective deposition of nanoplugs within the defects was verified by multiple characterization techniques, while scanning electrochemical microscopy (SECM) was used to confirm selective plugging of H 2 -crossover hotspots associated with defects at identical locations. Thanks to the use of nanoplugs, the H 2 permeance of 250 nm thick SiO 2 membranes was reduced by 5 to 6 orders of magnitude compared to the unmodified atomic layer deposition (ALD) SiO 2 membranes while having negligible impact on the ionic resistance of the membrane. These plug-modified membranes also enabled safe and stable operation of a zero-gap full cell electrolysis cell, in contrast to cells lacking nanoplugs that produced anode effluent streams having H 2 concentrations near or exceeding the lower flammability limit (LFL) of H 2 . Furthermore, beyond water electrolysis, this defect-sealing strategy has the potential to be broadly implemented in other applications, such as fuel cells and flow batteries, offering a versatile solution to mitigate crossover-related performance losses.

ALD SiO2↗
DOE OSTI2024

Mechanism and Kinetics of Ethanol–Acetaldehyde Conversion to 1,3-Butadiene over Isolated Lewis Acid La Sites in Silanol Nests in Dealuminated Beta Zeolite

Biomass-derived ethanol (EtOH) and acetaldehyde (AcH) conversion to 1,3-butadiene (1,3-BD) is an alternative process for 1,3-BD production. The present investigation reports the preparation and characterization of isolated La sites introduced into the silanol nests in DeAlBEA as well as detailed studies of the mechanism and kinetics for the conversion of an EtOH-AcH mixture to 1,3-BD. La sites supported on DeAlBEA are found to be present as (≡SiO) 2 La-OH groups that are H-bonded with adjacent Si-OH groups, possessing high C-C coupling activity and stability, superior to state-of-the-art Y-DeAlBEA. La sites supported on silica (La-SiO 2 ) with a similar chemical structure but no H-bonding interaction with Si-OH groups were prepared for comparison. Lewis acid La sites promote AcH aldol condensation, and the activity of such sites is nearly identical for both La-DeAlBEA and La-SiO 2 . Further, the rate of C 4 product formation increases by a factor of 4.8 upon addition of EtOH to the feed of AcH over La-DeAlBEA, whereas that over La/SiO 2 remains unchanged. Investigation of the mechanism and kinetics of AcH aldol condensation and EtOH-AcH conversion to 1,3-BD revealed two C-C bond forming pathways-AcH aldol condensation by Lewis acid La sites and direct coupling of EtOH-AcH over H-bonded (≡SiO) 2 La-OH···HO-Si≡ sites. This study provides important information about the role of the local environment of isolated Lewis acid sites and their effects on the direct coupling of EtOH and AcH to form 1,3-BD.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Intrinsic chemical reactivity of solid-electrolyte interphase components in silicon–lithium alloy anode batteries probed by FTIR spectroscopy

Herein we report the solid reaction products from the chemical reaction of aprotic battery electrolyte and three purported components of the Si-based anode SEI : SiO 2 nanoparticles (NPs), lithium silicate (Li x SiO y ) powders, and Si NPs. We use FTIR and classical molecular dynamics/density functional perturbation theory to assess the solid products remaining with these model materials after exposure to electrolyte. The absence of electrochemical bias provides a view of the chemical speciation resulting from early-stage chemical reactivity during battery assembly as well as under open circuit storage conditions. We believe these species represent the initial stages of SEI growth and predict they likely drive subsequent chemical and electrochemical reactions by controlling molecular interactons at the Si active material interface. We find that nominally equivalent materials react differently even before any electrochemistry is performed (e.g., acidic SiO 2 dissolves whereas alkaline SiO 2 is relatively robust), and derive new understanding of the chemical species that could and could not form stable SEI components in Si-based anodes. These results can be used to inform how to passivate Si anode surfaces and potentially generate an artificially engineered SEI that would be stable and enable next-generation battery anodes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Impact of non‐framework cation mixing on the structure and crystallization behavior of model high‐level waste glasses

Abstract Spinel crystallization is known to be detrimental to the operation of Joule heated ceramic melters during the vitrification of iron‐rich high‐level nuclear wastes (HLW) into borosilicate glasses. The literature on this subject focuses on tackling the problem by developing empirical constraints to design compositions, which limit the fraction of spinels formed in the melter or by developing empirical models to predict the settling behavior of spinels in the melter as a function of the glass composition. While these empirical models can predict the behavior of most of the compositions, they are not failsafe as there are always some compositions, whose behavior is beyond the predictive ability of these models. This can lead to undesirable situations during the vitrification of the nuclear waste, and therefore an in‐depth investigation of the chemo‐structural descriptors controlling the crystallization behavior in these glasses is warranted. Accordingly, the present study aims to understand the impact of non‐framework cation mixing (i.e., Li + /Na + and Ca 2+ /Na + ) on the structure (through Raman spectroscopy and Mössbauer spectroscopy) and crystallization behavior (through XRD, SEM‐EDS, and vibrating sample magnetometry) of iron‐rich model HLW glasses in the system: (mol.%) x M y O–(25− x ) Na 2 O–9.12 B 2 O 3 –6.4 Al 2 O 3 –51.25 SiO 2 –7.22 Fe 2 O 3 –0.38 MnO–0.08 Cr 2 O 3 –0.55NiO (M y O = Li 2 O or CaO).

Balasubramanya, Nikhila↗
DOE OSTI2025

Supported Organoiridium-Pincer Catalysts for the Nonoxidative Dehydrogenation of High-Density Polyethylene

The iridium-pincer complex {p-OP( t Bu) 2 -C 6 H 2 -2,6-OP( t Bu) 2 ] 2 }Ir(C 2 H 4 ) ( P [Ir]) has been reported as a stable and active catalyst toward alkane dehydrogenation in homogeneous and supported heterogeneous systems. Dehydrogenation has been shown as a practical method toward functional polyolefins, with dehydrogenated high-density polyethylene (deHDPE) demonstrated as a valuable synthon for upcycling, as orthogonal C-H strategies are key to end-of-life upcycling. The heterogenization of P [Ir] on oxides (SiO 2 , Al 2 O 3 , and TiO 2 ; P [Ir]/E y O x ) yields a mixture of organometallic Ir-fragments whose catalytic nonoxidative dehydrogenation activity is modulated by the binding modes of the active metal on the surface. The binding mode was elucidated by a combination of solid-state NMR and XAFS analyses and supported by DFT calculations. Surface binding through the ligand enables active organoiridium that catalyzes internal olefination of deHDPE up to 1.23 mol % at 200 °C under dynamic vacuum. Alternatively, when the organoiridium is bonded though the metal center (Ir-O SiO ), catalyst activity is negligible. Furthermore, the catalytic activity of P [Ir]/SiO 2 showed comparable reactivity with the homogeneous analogue under the same catalytic conditions, and the heterogenized catalyst can be reused up to three cycles. In conclusion, this work highlights the importance of understanding how organometallic precursors react with hydroxylated metal oxide surfaces to establish structure-property relationships.

Hunt, Samuel B. [Argonne National Laboratory (ANL)↗
DOE OSTI2025

Comparative Study of Vinylene Carbonate and Lithium Difluoro(oxalate)borate Additives in a SiO x /Graphite Anode Lithium-Ion Battery in the Presence of Fluoroethylene Carbonate

The SiO x /graphite composite is recognized as a promising anode material for lithium-ion batteries (LIBs), owing to the high theoretical capacity of SiO x combined with the excellent stability of graphite. However, the inherent disadvantage of volume expansion in silicon-based anodes places significant challenges on the solid electrolyte interphase (SEI) and severely degrades the electrochemical performance. Rational formulation of electrolyte, including its additives, is crucial in accommodating and optimizing the composition of the SEI and enhancing the cell performance. In this work, we present a comparative study of vinylene carbonate (VC) and lithium difluoro(oxalate)borate (LiDFOB) additives combined with fluoroethylene carbonate (FEC) in the electrolyte for SiO x /graphite∥LiNi 1–x–y–z Co x Mn y Al z O 2 full cells. VC outperformed LiDFOB as an additive, delivering higher capacity cycling, higher Coulombic efficiency, and better cycle stability up to 400 cycles. XPS and impedance analyses reveal that LiDFOB contributed to SEI/CEI with both a lower proportion of LiF and a higher proportion of poly(VC), which tended to produce higher cell impedance. XRD and XANES further indicated that using the LiDFOB additive, the NCMA cycled to a shallower degree than that of the VC additive. Although the VC additive maintained a higher capacity up to 400 cycles, microstrain and SEM analyses show a higher strained NCMA along with clear evidence of cracking over the surface of the NCMA particle in VC-based electrolyte but not in LiDFOB. In conclusion, this suggests that the negative influence of LiDFOB at the anode (inferior SEI) supersedes the negative impact of both a cracked NCMA and a deeper cycled NCMA and SiO x -based anode.

36 MATERIALS SCIENCE↗
DOE OSTI2021

A refined design concept for sulfur-tolerant Pd catalyst supported on zeolite by shape-selective exclusion and hydrogen spillover for hydrogenation of aromatics

Sulfur poisoning of noble metal catalysts has been a major challenge for decades. This work demonstrates the superior sulfur tolerance of a hybrid zeolite-supported Pd catalyst for hydrogenation of tetralin containing benzothiophene. The hybrid catalyst consists of Pd supported on a large-pore acidic zeolite Y (Pd/HY) and a small-pore zeolite A without (Pd/HA) or with surface metal passivation by chemical vapor deposition of SiO 2 (SiO 2 -Pd/HA) and with potassium ion exchange (SiO 2 -Pd/KA). Pd/HY is very active for tetralin hydrogenation but quickly deactivates after exposure to benzothiophene at high concentration of 100 ppm sulfur. The SiO 2 -coated Pd/HA shows no activity for tetralin hydrogenation, but continues to activate H 2 and serve as a source of hydrogen spillover from Pd/HA since these metal sites are protected from thiophenic sulfur due to size-selective exclusion. Adding K ion-exchanged and SiO 2 -coated catalyst SiO 2 -Pd/KA to Pd/HY is even more effective for enhancing sulfur tolerance, both for tetralin hydrogenation and for isomerization of cis-decalin to trans-decalin in the presence of benzothiophene. The turnover frequencies (TOF) of all the catalysts are similar at the exposed sulfur/Pd atomic ratio of around 0.5. With further increase in sulfur/Pd ratio, rapid decline in TOF was observed on Pd/HY, but SiO 2 -Pd/KA + Pd/HY hybrid catalyst shows a significantly higher TOF than that over Pd/HY, even though SiO 2 -Pd/KA or SiO 2 -Pd/HA alone shows no TOF for tetralin hydrogenation. Even after high-dose poisoning at 400 ppm sulfur, the SiO 2 -Pd/KA + Pd/HY hybrid recovered activity more quickly than SiO 2 -Pd/HA + Pd/HY, while the latter in turn is much better than Pd/HY alone. These results point to the higher activity for hydrogen spillover from SiO 2 -Pd/KA where Pd metal sites are protected from not only thiophenic sulfur but also inorganic sulfur H 2 S by shape-selective exclusion. The present work further establishes the validity of shape-selective exclusion and hydrogen spillover in the design concept proposed for a sulfur-tolerant bimodal acidic zeolite-supported metal catalyst for hydrogenation of naphthalene [C.S. Song, Chemtech, 29 (1999) 26–30], and refines the design concept further for limiting the size of small pore in hybrid catalysts to~3 Å for restricting access of H 2 S but allowing entrance of H 2 . Further, this refined design concept is applicable to other supported monometallic and bimetallic catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Creating Brønsted acidity at the SiO 2 -Nb 2 O 5 interface

Catalytically active acid sites associated with the silica-niobia interface were probed with a series of overcoated SiO 2 on Nb 2 O 5 (SiO 2 /Nb 2 O 5 ) mixed oxide materials prepared by deposition of tetraethyl orthosilicate onto niobic acid (Nb 2 O 5 nH 2 O) or calcined niobia (Nb 2 O 5 ). NH 3 TPD and pyridine DRIFTS studies indicated that the speciation of acid sites in the materials evolved as a function of SiO 2 loading, impacting the quantity and stability of Brønsted sites. Catalyst activity was highly dependent on SiO 2 loading in the liquid phase hydroalkoxylation of dihydropyran with n-octanol. At SiO 2 surface densities corresponding to approximately 1 Si per 2 surface Nb, the activity of these catalysts passed through a maximum approximately 20 times higher than the activity of calcined Nb 2 O 5 . We found that apparent reaction barriers measured over the most active SiO 2 /Nb 2 O 5 catalysts were 10 kJ/mol lower than those measured over niobic acid, suggesting that the OH features unique to the SiO 2 -Nb 2 O 5 interface were slightly more reactive than those on niobic acid.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Epitaxial Er-doped Y 2 O 3 on silicon for quantum coherent devices

Rare-earth ions have incomplete 4f shells and possess narrow optical intra-4f transitions due to shielding from electrons in the 5s and 5p orbitals, making them good candidates for solid-state optical quantum memory. The emission of Er 3+ in the telecom C-band (1530 nm – 1565 nm) makes it especially attractive for this application. In order to build practical, scalable devices, the REI needs to be embedded in a non-interacting host material, preferably one that can be integrated with silicon. In this paper, we show that Er 3+ can be isovalently incorporated into epitaxial Y 2 O 3 thin films on Si (111). We report on the synthesis of epitaxial, single-crystalline Er:Y 2 O 3 on Si with a narrow inhomogeneous linewidth in the photoluminescence spectra, 5.1 GHz (<100 mK) and an optical excited state lifetime of 8.1 ms. The choice of Y 2 O 3 was driven by its low nuclear spin and small lattice mismatch with Si. Using photoluminescence (PL) and electron paramagnetic resonance, we show that Er 3+ substitutes for Y in the crystal lattice. The role of interfacial SiO x , diffusion of silicon into the film, and the effect of buffer layers on inhomogeneous PL linewidth are examined. We also find that the linewidth decreased monotonically with film thickness but surprisingly exhibits no correlation with the film crystalline quality as measured by the x-ray rocking curve scans suggesting other factors at play that limit the inhomogeneous broadening in Y 2 O 3 films.

36 MATERIALS SCIENCE↗