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At least 109 records · Page 6

Shape evolution of neutron-rich 106,108,110 Mo isotopes in the triaxial degree of freedom

Background: Neutron-rich nuclei with mass number between 100 and 110 attract much attention, since several kinds of shapes, such as spherical, prolate, oblate, and triaxial shapes, are predicted. In particular, for neutron-rich Mo isotopes, different models predict different magnitudes and rigidity of triaxial deformation. Previous interpretations of experimental results based solely on low-lying $2^+_2$ states are insufficient to distinguish between the rigid triaxial shape, $\gamma$ vibration, or $\gamma$-soft rotor. Purpose: The shape evolution of 106 Mo, 108 Mo, and 110 Mo is investigated through their $2^+_1$-state lifetimes, decay-branching ratios of the $2^+_2$ state, and energies of the low-lying collective excited states with $K^π = 0^+, 2^+$, and $4^+$. Method: $\beta$-delayed $\gamma$-ray spectroscopy was employed for neutron-rich Nb and Zr isotopes produced at the RIKEN RI Beam Factory to populate excited states in 106 Mo, 108 Mo, and 110 Mo. The EUroball-RIKEN Cluster Array was used for high-resolution $\gamma$-ray detection and lifetimes of the $2^+_1$ states were determined using the UK fast-timing array of LaBr 3 (Ce) detectors. Results: New $\gamma$-ray transitions and levels are reported, including newly assigned $0^+_2$ states in 108,110 Mo. Quadrupole deformations were obtained for 106,108,110 Mo from their $2^+_1$ energies and lifetimes. The $\beta$-delayed neutron-emission probabilities of 108 Nb and 110 Nb were determined by examining the $\gamma$ rays of their respective daughter decays. Conclusions: In this work, the even-odd energy staggering in the $2^+_2$ band was compared with typical patterns of the $\gamma$-vibrational band, rigid triaxial rotor, and $\gamma$-soft rotor. The very small even-odd staggering of 106 Mo, 108 Mo, and 110 Mo favors a $\gamma$-vibrational band assignment. The kinematic moment of inertia for the $2^+_2$ band showed a trend similar to the ground-state band, which is as expected for the $\gamma$-vibrational band. Beyond-mean-field calculations employing the constrained Hartree-Fock-Bogoliubov and local quasiparticle-random-phase approximation method using the SLy5 + T interaction reproduced the ground and $2^+_2$ bands in 106 Mo and 108 Mo. The collective wave functions are consistent with the interpretation of the $2^+_2$ band as the $\gamma$-vibrational band of the prolate shape. However, the staggering pattern observed in 110 Mo differs from the one suggested in the calculations which predict a $\gamma$-soft rotor. There was no experimental indication of the oblate shape or the $\gamma$-soft rotor predicted in these Mo isotopes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Mean-field equation for phase-modulated optical parametric oscillator

The widely established techniques for the generation of ultrashort optical pulses rely on passive mode locking of lasers, with the output pulse duration and emission spectrum determined by the intrinsic lifetime of laser transition in the gain medium. Due to the instantaneous nature of nonlinear gain, optical parametric oscillators (OPOs) are capable of generating optical radiation in all timescales from continuous-wave (cw) to ultrashort femtosecond regime, if driven by laser pump sources in the corresponding time domain. In the ultrashort timescale, operation of OPOs conventionally relies on mode-locked pump lasers, with the concomitant disadvantages of large footprint and high cost. At the same time, the lack of gain storage mandates the use of synchronous pumping, resulting in increased complexity. In this paper, we present the concept of phase-modulated OPO driven by cw pump laser. The approach overcomes the traditional drawbacks of ultrafast OPOs, enabling femtosecond pulse generation without the need for synchronous pumping, resulting in a simplified, compact, and cost-effective architecture using cw input pump lasers. We derive a mean-field equation for a degenerate χ ( 2 ) OPO driven by a cw laser with intracavity electro-optic modulator (EOM), and also including dispersion compensation. The equation predicts the formation of stable femtosecond pulses ( < 200 fs ) , in both normal and anomalous dispersion regimes, with a controllable repetition rate determined by the frequency of the EOM. The remarkable functionality of the proposed scheme paves the way for the development of an alternative class of widely tunable coherent femtosecond light sources in both bulk and integrated format based on χ ( 2 ) OPOs using cw pump lasers. Published by the American Physical Society 2024

Sanchez, A. D. (ORCID:0000000327630339)↗

Multimodal Imaging of Autofluorescent Sites Reveals Varied Chemical Speciation in SSZ-13 Crystals

Here, a multimodal imaging study of chabazite is used to show the distribution of and discriminate between different emissive deposits arising as a result of the detemplation process. 3D confocal imaging, fluorescence lifetime imaging, spectral imaging, and Raman mapping are used to show three different types of emissive behaviours each characterised by different spatial distributions, trends in lifetime, spectral signals, and Raman signatures. A notable difference is seen in the morphology of agglomerated surface deposits and larger subsurface deposits, which experience lifetime augmentation due to spatial confinement. The distribution of organic residue throughout the crystal volume is comparable to XRF mapping that shows Si enrichment on the outer edges and higher Al content through the centre, demonstrating that a fluorescence-based technique can also be used to indirectly comment on the compositional chemistry of the inorganic framework.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Reconciliation of asynchronous satellite-based $\mathrm{NO_2}$ and $\mathrm{XCO_2}$ enhancements with mesoscale modeling over two urban landscapes

Fossil fuel carbon dioxide (CO 2ff ), the main driver of global warming and climate change, is often co-emitted with nitrogen oxides (NO x ) and precursors to ground-level ozone from anthropogenic sources like power plants or vehicles. In urban and suburban areas, satellite-based NO 2 can be used as a proxy to track the emissions of CO 2ff . Because of NO 2 ’s shorter lifetime, urban NO 2 plumes are more distinguishable from backgrounds and more sensitive to variations in emissions. However, the combination of these two gases is limited by the asynchrony among NO 2 and CO 2 monitoring satellites. We used CO 2ff simulated by the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) model to reconcile the tropospheric NO 2 vertical column density (VCD) from the Tropospheric Monitoring Instrument (TROPOMI) and column-averaged dry-air mole fractions of carbon dioxide enhancements (ΔXCO 2 ) from Orbiting Carbon Observatory 3 (OCO-3) Snapshot Area Maps (SAMs) over a multicity area, Washington D.C.-Baltimore (DC-Balt), and a basin city, Mexico City. NO 2 /CO 2ff ratios over DC-Balt are smaller than Mexico City, indicative of stricter emission restrictions, a more combustion-efficient vehicle fleet, and higher combustion efficiency due to lower altitude in DC-Balt. For single-track cases, the spatial correlations between NO 2 and ΔXCO 2 over Mexico City are stronger than DC-Balt because the NO 2 and CO 2 are mostly trapped in the valley of Mexico City, while DC-Balt is severely affected by distant sources (i.e., US East Coast cities). Using multi-track averaging, spatial correlation coefficients increase with the number of days used for averaging. The correlations reached a maximum when averaging >12 continuous images for DC-Balt and > 10 continuous images for Mexico City. This finding indicates that multi-track averaging using modeled CO 2ff as a proxy is helpful to filter the noise in single-track images, to cancel the interference from distant sources, and to magnify correlations between NO 2 and CO 2ff . Mexico City showed stronger spatial correlations but weaker temporal correlations than DC-Balt due to biomass burning hot spots and large transport errors caused by the trapping effects of the surrounding mountains. Tracking the 20-day moving average of CO 2ff emissions using TROPOMI NO 2 seems technically feasible, considering the relationship between correlation coefficients and the number of available satellite images.

54 ENVIRONMENTAL SCIENCES↗

Sensitive Response of Atmospheric Oxidative Capacity to the Uncertainty in the Emissions of Nitric Oxide (NO) From Soils in Amazonia

Abstract Soils are a major source of nitrogen oxides, which in the atmosphere help govern its oxidative capacity. Thus the response of soil nitric oxide (NO) emissions to forcings such as warming or forest loss has a meaningful impact on global atmospheric chemistry. We find that the soil emission rate of NO in Amazonia from a common inventory is biased low by at least an order of magnitude in comparison to tower‐based observations. Accounting for this regional bias decreases the modeled global methane lifetime by 1.4%–2.6%. In comparison, a fully deforested Amazonia, representing a 37% decrease in global emissions of isoprene, decreases methane lifetime by at most 4.6%, highlighting the sensitive response of oxidation rates to changes in emissions of NO compared to those of terpenes. Our results demonstrate that improving our understanding of soil NO emissions will yield a more accurate representation of atmospheric oxidative capacity.

Geology↗

Multimodal Imaging of Autofluorescent Sites Reveals Varied Chemical Speciation in SSZ-13 Crystals

In this report a multimodal imaging study of chabazite is used to analyse emissive deposits. A notable difference is seen in the morphology of agglomerated surface deposits and larger subsurface deposits. Comparison of the distribution of organic residue throughout the crystal volume and XRF mapping is demonstrating that a fluorescence-based technique can also be used to indirectly comment on the compositional chemistry of the inorganic framework. A multimodal imaging study of chabazite is used to show the distribution of and discriminate between different emissive deposits arising as a result of the detemplation process. Confocal imaging, 3D fluorescence lifetime imaging, 3D multispectral fluorescence imaging, and Raman mapping are used to show three different types of emissive behaviours each characterised by different spatial distributions, trends in lifetime, spectral signals, and Raman signatures. A notable difference is seen in the morphology of agglomerated surface deposits and larger subsurface deposits, which experience lifetime augmentation due to spatial confinement. The distribution of organic residue throughout the crystal volume is comparable to XRF mapping that shows Si enrichment on the outer edges and higher Al content through the centre, demonstrating that a fluorescence-based technique can also be used to indirectly comment on the compositional chemistry of the inorganic framework.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Benefits and risks of lead halide perovskite photovoltaics

Photovoltaics (PV) do not emit anything during operation, but, over their life-cycle, emissions are generated from the use of fossil-fuels in the extraction and production of materials and in the manufacturing and installation of PV components and systems. Nonetheless, these emissions are always very small compared to those from conventional combustion-based generators of electricity. The case for CO2 emissions has been well documented; over their lifetime, they range from 10 g CO2-eq / kWh for CdTe PV system installed in high-irradiation (2300 kWh/(m2-yr) locations to 80 g CO2-eq / kWh for Chinese single-crystalline silicon PV systems installed in low-irradiation (1000 kWh/(m2-yr) locations,1 compared to ~1000 g CO2-eq/kWh for electricity from coal. However, in the case of the rapidly emerging lead halide perovskite PV (LHP-PV) technology, concerns are raised regarding the potential of emissions of lead from the life-cycles of LHP-PV, including at their end of life. This warranted an evaluation of lead emissions from PV and comparisons with emissions in other power generation life-cycles.

Perovskites, PV, Lead, Risks↗

High Carrier Lifetimes in Epitaxial Germanium-Tin/Al(In)As Heterostructures with Variable Tin Compositions

Group IV-based germanium-tin (Ge1-ySny) compositional materials have recently shown great promise for infrared detection, light emission and ultra-low power transistors. High carrier lifetimes are desirable for enhancing the detection limit and efficiency of photodetectors, low threshold current density in lasers, and low tunneling barrier height by lowering defects and dislocations at the heterointerface of a source and a channel. Here, carrier lifetimes in epitaxial germanium (Ge) and variable tin (Sn) compositional Ge1-ySny materials were experimentally determined on GaAs substrates using the contactless microwave photoconductive decay (u-PCD) technique at an excitation wavelength of 1500 nm. Sharp (2 x 2) reflection high energy electron diffraction patterns and low surface roughness were observed from the surface of the Ge0.97Sn0.03 epilayer. X-ray rocking curves from Ge0.97Sn0.03 and Ge0.94Sn0.06 layers demonstrated the pseudomorphic and lattice-matched growth on AlAs and In0.12Al0.88As buffers, respectively, further substantiated by reciprocal space maps and abrupt heterointerfaces evident from the presence of Pendellosung oscillations. High effective carrier lifetimes of 150 ns to 450 ns were measured for Ge1-ySny epilayers as a function of Sn composition, surface roughness, growth temperature, and layer thickness. The observed increase in the carrier lifetime with an increasing Ge layer thickness and a reducing surface roughness, by incorporating Sn, were explained. The enhancement of the carrier lifetime with an increasing Sn concentration was achieved by controlling the defects with lattice-matched Ge0.94Sn0.06/In0.12Al0.88As heterointerfaces or the pseudomorphic growth of Ge0.94Sn0.06 on GaAs. Therefore, our monolithic integration of variable Sn alloy compositional Ge1-ySny materials with high carrier lifetimes opens avenues to realize electronic and optoelectronic devices.

carrier lifetimes↗

Dynamical Unification of Tidal Disruption Events

The ~100 tidal disruption events (TDEs) observed so far exhibit a wide range of emission properties both at peak and over their lifetimes. Some TDEs radiate predominantly at X-ray energies, while others radiate chiefly at UV and optical wavelengths. While the peak luminosities across TDEs show distinct properties, the evolutionary behavior can also vary between TDEs with similar peak emission properties. In particular, for optical TDEs, while their UV and optical emissions decline somewhat following the fallback pattern, some events can greatly rebrighten in X-rays at late time. In this Letter, we conduct three-dimensional general relativistic radiation magnetohydrodynamics simulations of TDE accretion disks at varying accretion rates in the regime of super-Eddington accretion. We make use of Monte Carlo radiative transfer simulations to calculate the reprocessed spectra at various inclinations and at different evolutionary stages. We confirm the unified model proposed by Dai et al., which predicts that the observed emission largely depends on the viewing angle of the observer with respect to the disk orientation. Furthermore, we find that disks with higher accretion rates have elevated wind and disk densities, which increases the reprocessing of the high-energy radiation and thus generally augments the optical-to-X-ray flux ratio along a particular viewing angle. This implies that at later times, as the accretion level declines, we expect that more X-rays will leak out along intermediate viewing angles. Such dynamical model for TDEs can provide a natural explanation for the diversity in the emission properties observed in TDEs at peak and along their temporal evolution.

79 ASTRONOMY AND ASTROPHYSICS↗

Uranyl fluorescence in acidic solution: quenching effects by tetramethylammonium (TMA + )

The quenching of uranyl luminescence by various cation species was studied in aqueous media at low pH. Solutions with different nitrate salts, held at constant uranyl nitrate, nitric acid, and ion concentration, were tested to examine the quenching effects of the cations from the nitrate salts. Alkali metal (Li + , Na + , Rb + ) and quaternary ammonium cations (NH 4 + ), (CH 3 ) 4 N + (TMA + ), (C 2 H 5 ) 4 N + (TEA + ) were investigated. Solutions containing TMA + reduced the lifetime of uranyl fluorescence significantly more than the other cations. Uranyl emission spectra also showed that TMA + increased the complex formation between uranyl and nitrate ions. Fluorescence decay lifetime measurements for most solutions yielded values between 1.4–1.9 μs at 20 °C, while 1.8 M TMA + reduced the lifetime of uranyl fluorescence to 0.6 μs. Decay rate versus concentration data (Stern–Volmer plots) indicated a dynamic quenching process with increasing fluorescence decay rates at higher cation concentrations for Li + , TMA + , and TEA + . The temperature dependencies of the decay rates and the kinetics in D 2 O were also examined.

Persinger, Thomas D. [Argonne National Laboratory ↗

Perform Life Cycle Energy and GHG Emission Analysis, Select Candidate Refrigerant(s), Developing Heat Pump by Using Low-GWP Refrigerants and 5 mm Diameter Tubes

Reducing environmental impacts from the energy conversion systems has been an important research topic due to recent severe global climate changes. In residential buildings, the space heating and cooling are main energy consumers, which are relying on vapor compression based heat pumps. To mitigate the environmental impacts of residential systems, the heat pumps using low-GWP refrigerants and 5mm-tube heat exchangers are proposed to replace the conventional 9 mm or 7 mm tube heat exchangers. This research uses a simulation-based design method to optimize the refrigerant circuitries of a 5-ton low-GWP refrigerant heat pumps whose indoor and outdoor heat exchangers adopt 5 mm tubes. Heat pump systems using four commercially available low-GWP refrigerants (R454A, R454C, ARM20A and ARM20B) are optimized and compared with the baseline R410A system. The results indicate that directly replacing 9 mm tubes into 5mm tubes in the baseline systems induces heat pump performance degradation; by optimizing the 5 mm tube heat pumps with added tube rows, the system refrigerant charge is reduced up to 33% compared with the baseline; the optimized low-GWP 5 mm tube heat pumps offer the same or higher performance under both cooling and heating mode; that under cooling mode, the EER improvement is up to 10.7% and under heating mode the COP improvement is up to 3.4%; and a smart flow control device to maintain counter-flow circuitry pattern on both operating modes can improve the heating performance of 5 mm tube optimized system by up to 3.0%. In an effort to better understand the environmental impacts of these systems, life cycle climate performance (LCCP) evaluation method is used to assess the baseline and optimized systems. LCCP considers the direct and indirect emissions of the system over the course of its lifetime from manufacturing to disposal. Our analyses indicate that the optimized systems using 5mm tubes and low-GWP refrigerants can reduce life-cycle CO 2 emission significantly. And improving system efficiency is the most effective way to reduce the emission of low-GWP refrigerant systems. This report shows that using 5 mm diameter tubes in heat exchangers is a feasible approach to develop heat pumps with low-GWP refrigerants. Using the proposed design approach can yield higher system efficiency with lower environmental impact.

42 ENGINEERING↗

Comparing Pr 3+ and Nd 3+ for deactivating the Er 3+ : 4 I 13/2 level in lanthanum titanate glass

Erbium lanthanum titanate glasses were prepared by levitation melting for the spectroscopic study of ways to promote the mid-infrared fluorescence. Two series of heavily erbium doped glasses (15 wt%) were prepared with the addition of either Pr 3+ or Nd 3+ in amounts relative to Er 3+ of 0.05, 0.1, and 0.2. Both ions quench the lower Er 3+ laser level with the Pr 3+ doing so more rapidly. Although high co-dopant concentrations result in higher energy transfer, as clearly evidenced in upconversion and downconversion fluorescence measurements, the mid-infrared lifetime also suffers a reduction and, therefore, a balance must be struck in the co-dopant concentration. Lifetime and spectral measurements indicate that, at a fixed relative co-dopant amount, Pr 3+ is more effective than Nd 3+ at removing the bottleneck of the Er 3+ 4 I 13/2 level. Moreover, consideration of the lifetimes alongside the absorption data of the individual ions indicates that despite the large absorption cross-section of Nd 3+ at 808 nm, the concentration needed to yield more absorbed power than utilizing direct 976 nm excitation of Er 3+ results in unfavorable lifetimes of the mid-infrared transition. In the end, Pr 3+ prevails as the superior co-dopant in terms of the effects on fluorescence lifetimes as well as potential laser system design considerations. In a unique self-doping approach, a reducing melt atmosphere of Ar instead of O 2 creates a small fraction of Ti 3+ . In 5Er 2 O 3 -12La 2 O 3 -83TiO 2 glass, the presence of Ti 3+ quenches the 4 I 13/2 emission about 2.6 times more than the 4 I 11/2 when lifetimes are compared to an O 2 melt environment. As an additional means of increasing the mid-infrared emission, the effect of temperature on the mid- and near- infrared lifetimes of a lightly doped lanthanum titanate composition is investigated between 77-300 K. The mid-infrared lifetime increases by ∼30% while the near-infrared lifetime increases by ∼10%, which suggests in addition to co-doping, active cooling of the gain media will further enhance performance.

Materials Science↗

Point and extended defects in heteroepitaxial 𝛽−G⁡a 2 ⁢O 3 films

G⁡a 2 ⁢O 3 is emerging as an excellent potential semiconductor for high power and optoelectronic devices. However, the successful development of G⁡a 2⁢ O 3 in a wide range of applications requires a full understanding of the role and nature of its point and extended defects. Here, in this work, high quality epitaxial G⁡a 2 ⁢O 3 films were grown on sapphire substrates by metal-organic chemical vapor deposition and fully characterized in terms of structural, optical, and electrical properties. Then defects in the films were investigated by a combination of depth-resolved Doppler broadening and lifetime of positron annihilation spectroscopies and thermally stimulated emission (TSE). Positron annihilation techniques can provide information about the nature and concentration of defects in the films, while TSE reveals the energy level of defects in the bandgap. Despite very good structural properties, the films exhibit short positron diffusion length, which is an indication of high defect density and long positron lifetime, a sign for the formation of Ga vacancy related defects and large vacancy clusters. These defects act as deep and shallow traps for charge carriers as revealed from TSE, which explains the reason behind the difficulty of developing conductive G⁡a 2 ⁢O 3 films on non-native substrates. Positron lifetime measurements also show nonuniform distribution of vacancy clusters throughout the film depth. Further, the work investigates the modification of defect nature and properties through thermal treatment in various environments. It demonstrates the sensitivity of G⁡a 2 ⁢O 3 microstructures to the growth and thermal treatment environments and the significant effect of modifying defect structure on the bandgap and optical and electrical properties of G⁡a 2 ⁢O 3 .

defects↗

Kinetic control of phase evolution and defect-mediated recombination in AACVD-grown copper antimony sulphide thin films

Copper antimony sulphide (CAS) is a multinary chalcogenide semiconductor in which small deviations from stoichiometry can drive phase competition and strong defect-mediated modulation of optoelectronic properties. However, the systematic roles of copper precursor fraction and deposition time in governing phase evolution, off-stoichiometry, and recombination dynamics in aerosol-assisted chemical vapour deposition (AACVD)-grown undoped CAS thin films remain insufficiently understood. In this work, undoped CAS thin films were deposited by AACVD using Cu(dedtc)2 and Sb(dedtc)3 single-source precursors at 550 °C and a carrier gas flow rate of 150 sccm, while the Cu(dedtc)2 mole fraction (x = 0.15 – 0.55) and deposition time (1 – 2 hours) were systematically varied to probe how growth kinetics influence phase composition, microstructure, and defect-mediated optical properties without post-deposition annealing or extrinsic doping. Increasing copper precursor content drives phase evolution toward tetrahedrite-dominant CAS films at intermediate Cu(dedtc)2 mole fractions, with the film deposited at x = 0.35 exhibiting the strongest tetrahedrite character within the parameter space examined. The films are also copper-rich, antimony-poor, and sulphur-deficient, consistent with off-stoichiometric growth and intrinsic defect formation, plausibly including copper interstitials, Cu-on-Sb antisites, and sulphur vacancies. These growth-dependent compositional deviations are accompanied by tunable indirect optical bandgaps of approximately 1.60 – 2.18 eV and weak visible photoluminescence governed by defect-mediated recombination. Time-resolved photoluminescence reveals bi-exponential decay behaviour with lifetimes of approximately 0.1 – 3.6 ns, with emission dominated by slower donor–acceptor pair recombination and a smaller contribution from faster trap-assisted pathways. Collectively, these results establish an explicit kinetic process–structure–defect–property relationship for AACVD-grown CAS thin films and provide a growth–structure–property framework relevant to future optimization of CAS-based optoelectronic and energy materials.

36 MATERIALS SCIENCE↗

Sub-2 Kelvin Characterization of Nitrogen-Vacancy Centers in Silicon Carbide Nanopillars

The development of efficient quantum communication technologies depends on the innovation in multiple layers of its implementation, a challenge we address from the fundamental properties of the physical system at the nanoscale to the instrumentation level at the macroscale. We select a promising near-infrared quantum emitter, the nitrogen-vacancy (NV) center in 4H-SiC, and integrate it, at an ensemble level, with nanopillar structures that enhance photon collection efficiency into an objective lens. Moreover, changes in collection efficiency in pillars compared to bulk can serve as indicators of color center orientation in the lattice. To characterize NV center properties at the unprecedented sub-2 K temperatures, we incorporate compatible superconducting nanowire single photon detectors inside the chamber of an optical cryostat and create the ICECAP, the Integrated Cryogenic system for Emission, Collection And Photon detection. ICECAP measurements show no significant line-width broadening of NV ensemble emission and up to 14-fold enhancement in collected emission. With additional filtering, we measure emitter lifetimes of NV centers in a basal ( hk ) and axial ( kk ) orientation, unveiling their cryogenic values of 2.2 and 2.8 ns.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Exploiting heat transfer to achieve efficient photoelectrochemical CO 2 reduction under light concentration

Photoelectrochemical (PEC) conversion of carbon dioxide into valuable chemicals and fuels represents a promising path towards combating anthropogenic CO 2 emissions. However, the limited conversion efficiencies, operation lifetimes and CO 2 utilization efficiencies of PEC devices currently prohibit their application beyond the laboratory scale. Here, a wireless device converting CO 2 and water into carbon monoxide and hydrogen at a peak solar conversion efficiency exceeding 16% under an illumination intensity of 5 suns is demonstrated. A CO/H 2 product ratio between 10–20 is measured during a 17 h stability test. Fluctuations in device performance are rigorously analyzed via deconvolution of electrochemical and photoabsorber contributions. Furthermore, it is demonstrated that beneficial heat dissipation is enabled by wireless integration of the photoabsorber and electrocatalyst components, accounting for roughly 10% of the achieved conversion efficiency, an achievement unattainable with physically separated photoabsorber and electrolyzer components.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Quantification of trace iodine using laser-induced breakdown spectroscopy for real-time monitoring of nuclear off-gas streams

This study evaluated the potential of laser-induced breakdown spectroscopy (LIBS) for real-time monitoring of trace gas-phase iodine, which is an element of high significance in nuclear applications due to its long radioactive half-life (as iodine-129), volatility, and biological impact. In anticipation of iodine evolving into off-gas systems in molten salt reactor and nuclear fuel recycling applications, this research aimed to assess LIBS performance in flowing argon and helium matrices; optimize measurement parameters using a multichannel spectrometer; and perform calibrations to assess predictive capabilities and limits of detection (LODs). Experimental results successfully measured gas-phase iodine in flowing argon and helium; however, trace iodine was not detected in air. Optimal delay times were determined to be 10 µs for argon and 1 µs for helium, which are consistent with the expected shorter plasma lifetime in helium relative to argon. An emission line survey was provided with the 206.16, 804.37, 902.24, and 905.83 nm peaks, which were identified as the strongest emission peaks. Calibration models were successfully built in both helium and argon, achieving LODs down to 3 ppm in helium and 5 ppm in argon. The iodine emission at 905.83 nm emerged as the most robust for calibration and was subsequently applied to a time series dataset in argon. The predictive trace confirmed the feasibility of employing LIBS for continuous, online quantification of trace iodine in flowing gas systems.

Andrews, Hunter B. [Oak Ridge National Laboratory ↗

Erbium quantum memory platform with long optical coherence via back-end-of-line deposition on foundry-fabricated photonics

Realizing scalable quantum interconnects necessitates the integration of solid-state quantum memories with foundry photonics processes. While prior photonic integration efforts have relied upon specialized, laboratory-scale fabrication techniques, this work demonstrates the monolithic integration of a quantum memory platform with low-loss foundry photonic circuits via back-end-of-line deposition. We deposited thin films of titanium dioxide (Ti⁢O 2 ) doped with erbium (Er) onto silicon nitride nanophotonic waveguides and studied Er optical coherence at subkelvin temperatures with photon echo techniques. Furthermore, we suppressed optical dephasing through ex-situ oxygen annealing and optimized measurement conditions, which yielded an optical coherence time of 64 μ⁢s (a 5-kHz homogeneous linewidth) and slow spectral diffusion of 27 kHz over 4 ms, results that are comparable to state-of-the-art Er nanophotonic devices. Combined with second-long electron spin lifetimes and demonstrated electrical control of Er emission, our findings establish Er:Ti⁢O 2 on foundry photonics as a manufacturable platform for ensemble and single-ion quantum memories.

Electro-optic effects↗