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At least 1,675 records · Page 93

Probing the Mechanism of Cadmium Sulfide Cluster Nucleation and Growth via Sequential Infiltration Synthesis

Few-atom metal chalcogenide clusters may be realized through the sequential infiltration of metal–organic precursors in polymer films. However, the underlying nucleation and growth mechanisms that allow for cluster synthesis with near atomic-scale precision are not fully resolved. The kinetics of the sequential infiltration synthesis (SIS) method that control the nucleation and growth mechanisms of primarily Cd 4 S 4 -core clusters within a poly­(4-vinylpyridine) (P4VP) matrix are probed with in situ UV–visible absorbance spectroscopy. Density functional theory (DFT) calculations that allow simulation of the optical properties of cluster fragments further reveal the thermodynamics that guide cluster growth within the P4VP matrix. Here, we conclude that a reactive capture mechanism for cluster nucleation and growth is dominant, although transient dimethyl cadmium adduction to the polymer backbone may contribute to cluster nucleation under shorter metal–organic purge process conditions. Grazing incidence X-ray diffraction (GI-XRD) and X-ray absorption spectroscopy (XAS) analyses further corroborate the cluster size and atom connectivity throughout the stepwise synthesis.

Jayaweera, Nuwanthaka P. [Argonne National Laborat↗

Electron-hole symmetry in quasiparticle spectral weight of cuprates observed via infrared and photoemission spectroscopy

Here we performed an optical spectroscopy study of single crystals of Pr 0.85 LaCe 0.15 CuO 4–δ (PLCCO) to revisit the electron-hole asymmetry, which has been understood as a fundamental property of cuprates. Four differently annealed samples—as-grown, reduced, optimally oxygenated, and overoxygenated samples—were prepared, which have superconducting transition temperatures T c = 0, 15, 24, and 18 K, respectively. We observed that the low-energy quasiparticle spectral weights of all the PLCCO samples are significantly small in comparison with those of other electron-doped cuprate families. Instead, they are rather close to those of their hole-doped counterpart La 2–x Sr x CuO 4 . Accordingly, estimated effective carrier numbers N eff per Cu atom of superconducting samples are also very small, despite their relatively high critical temperatures. A complementary photoemission study reveals that the low-energy quasiparticle spectral weight of PLCCO is much smaller than that of Nd 1.85 Ce 0.15 CuO 4–δ , consistent with the optical results. Our observations demonstrate that PLCCO provides the electron-hole symmetry in the quasiparticle spectral weight and highlight the importance of Cu 3d–O 2p hybridization to understand the low-energy spectral weight transfer in doped cuprates.

36 MATERIALS SCIENCE↗

Robust and ultrafast state preparation by ramping artificial gauge potentials

Abstract The implementation of static artificial magnetic fields in ultracold atomic systems has become a powerful tool, e.g. for simulating quantum-Hall physics with charge-neutral atoms. Taking an interacting bosonic flux ladder as a minimal model, we investigate protocols for adiabatic state preparation via magnetic flux ramps. Considering the fact that it is actually the artificial vector potential (in the form of Peierls phases) that can be experimentally engineered in optical lattices, rather than the magnetic field, we find that the time required for adiabatic state preparation dramatically depends on which pattern of Peierls phases is used. This can be understood intuitively by noting that different patterns of time-dependent Peierls phases that all give rise to the same magnetic field ramp, generally lead to different artificial electric fields during the ramp. As an intriguing result, we find that an optimal choice allows for preparing the ground state almost instantaneously in the non-interacting system, which can be related to the concept of counterdiabatic driving. Remarkably, we find extremely short preparation times also in the strongly-interacting regime. Our findings open new possibilities for robust state preparation in atomic quantum simulators.

Wang, Botao (ORCID:0000000282202452)↗

SI IV Resonance Line Emission during Solar Flares: Non-LTE, Non-equilibrium, Radiation Transfer Simulations

The Interface Region Imaging Spectrograph routinely observes the Si IV resonance lines. When analyzing quiescent observations of these lines, it has typically been assumed that they form under optically thin conditions. This is likely valid for the quiescent Sun, but this assumption has also been applied to the more extreme flaring scenario. We used 36 electron-beam-driven radiation hydrodynamic solar flare simulations, computed using the RADYN code, to probe the validity of this assumption. Using these simulated atmospheres, we solved the radiation transfer equations to obtain the non-LTE, nonequilibrium populations, line profiles, and opacities for a model silicon atom, including charge exchange processes. This was achieved using the "minority species" version of RADYN. The inclusion of charge exchange resulted in a substantial fraction of Si IV at cooler temperatures than those predicted by ionization equilibrium. All simulations with an injected energy flux F> 5 x 10(exp 10) erg cm(exp -2) s(exp -1) resulted in optical depth effects on the Si IV emission, with differences in both intensity and line shape compared to the optically thin calculation. Weaker flares (down to F ~ 10(exp 9) erg cm(exp -2) s(exp -1)) also resulted in Si IV emission forming under optically thick conditions, depending on the other beam parameters. When opacity was significant, the atmospheres generally had column masses in excess of 5 x 10-6 g cm-2 over the temperature range 40-100 kK, and the Si IV formation temperatures were between 30 and 60 kK. We urge caution when analyzing Si IV flare observations, or when computing synthetic emission without performing a full radiation transfer calculation.

Kerr, Graham S.↗

Analysis of laser-induced modification of collagen structure using nonlinear optical microscopy

Nonlinear optical microscopy is used to monitor changes in the collagen structure of patellar ligament after IR laser heating up to a temperature of 60 °C. Pre-denaturation modification of the tissue matrix exhibits specific properties and consists in splitting of initially parallel fibre bundles into array of divergent fibres. Image processing employing Fast Fourier transform analysis is used for characterising images of the fibre structure and determining the collagen orientation index. An increase in manifestation of laser-induced disordering with an increase in IR laser radiation power from 0.3 to 2 W is accompanied by a decrease in the collagen orientation index. The specific disorganisation of the collagen tissue structure during laser heating is supposed to be due to fast speed and local action of the laser heating, which leads to mechanical distortions of the structural elements of tissue matrix. (paper)

36 MATERIALS SCIENCE↗

X-Ray, EUV, UV and Optical Emissivities of Astrophysical Plasmas

This grant primarily covered the development of the thermal X-ray emission model code called APEC, which is meant to replace the Raymond and Smith (1977) code. The new code contains far more spectral lines and a great deal of updated atomic data. The code is now available (http://hea-www.harvard.edu/APEC), though new atomic data is still being added, particularly at longer wavelengths. While initial development of the code was funded by this grant, current work is carried on by N. Brickhouse, R. Smith and D. Liedahl under separate funding. Over the last five years, the grant has provided salary support for N. Brickhouse, R. Smith, a summer student (L. McAllister), an SAO predoctoral fellow (A. Vasquez), and visits by T. Kallman, D. Liedahl, P. Ghavamian, J.M. Laming, J. Li, P. Okeke, and M. Martos. In addition to the code development, the grant supported investigations into X-ray and UV spectral diagnostics as applied to shock waves in the ISM, accreting black holes and white dwarfs, and stellar coronae. Many of these efforts are continuing. Closely related work on the shock waves and coronal mass ejections in the solar corona has grown out of the efforts supported by the grant.

Raymond, John C.↗

Dipole-Dipole Frequency Shifts in Multilevel Atoms

Dipole-dipole interactions lead to frequency shifts that are expected to limit the performance of next-generation atomic clocks. In this work, we compute dipolar frequency shifts accounting for the intrinsic atomic multilevel structure in standard Ramsey spectroscopy. When interrogating the transitions featuring the smallest Clebsch-Gordan coefficients, we find that a simplified two-level treatment becomes inappropriate, even in the presence of large Zeeman shifts. Further, for these cases, we show a net suppression of dipolar frequency shifts and the emergence of dominant nonclassical effects for experimentally relevant parameters. Our findings are pertinent to current generations of optical lattice and optical tweezer clocks, opening a way to further increase their current accuracy, and thus their potential to probe fundamental and many-body physics.

74 ATOMIC AND MOLECULAR PHYSICS↗

Selective Antisite Defect Formation in WS 2 Monolayers via Reactive Growth on Dilute W-Au Alloy Substrates

Defects are ubiquitous in 2D materials and can affect the structure and properties of the materials and also introduce new functionalities. Methods to adjust the structure and density of defects during bottom-up synthesis are required to control the growth of 2D materials with tailored optical and electronic properties. In this study, the authors present an Au-assisted chemical vapor deposition approach to selectively form S W and S2 W antisite defects, whereby one or two sulfur atoms substitute for a tungsten atom in WS 2 monolayers. Guided by first-principles calculations, they describe a new method that can maintain tungsten-poor growth conditions relative to sulfur via the low solubility of W atoms in a gold/W alloy, thereby significantly reducing the formation energy of the antisite defects during the growth of WS 2 . The atomic structure and composition of the antisite defects are unambiguously identified by Z-contrast scanning transmission electron microscopy and electron energy-loss spectroscopy, and their total concentration is statistically determined, with levels up to ≈5.0%. Furthermore, scanning tunneling microscopy/spectroscopy measurements and first-principles calculations also verified these antisite defects and revealed the localized defect states in the bandgap of WS 2 monolayers. This bottom-up synthesis method to form antisite defects should apply in the synthesis of other 2D materials.

2D materials↗

Theoretical investigation of charge transfer between the NV – center in diamond and substitutional N and P

The nitrogen-vacancy (NV) lattice defect in diamond, consisting of an N substitutional atom and an adjacent C vacancy, is commonly observed in two charge states, negative (NV – ) and neutral (NV 0 ). The NV – defect exhibits spin state-dependent fluorescence and is, therefore, amenable to optical methods for spin-state readout, while the NV 0 is not. Hence, the NV – defect is much more useful for quantum sensing and quantum information processing. However, only NV 0 electroluminescence has been observed, even from centers showing NV – in photoluminescence. In the present work, we use first-principles electronic structure calculations to determine adiabatic charge transition levels for the conversion of NV – to NV 0 in the presence of substitutional N or P impurities, which provide the charge of the NV center. Here, we find that the adiabatic charge transition levels in the presence of such impurities lie at energies close to or lower than the zero-phonon line of the NV – center and that these energies only decrease as the concentration of N donors increases. This work, therefore, elucidates the absence of observed electroluminescence from the NV – and proposes a path toward observation of the phenomenon.

36 MATERIALS SCIENCE↗

Second-harmonic generation in zinc blende crystals under combined action of femtosecond optical and strong terahertz fields

The influence of a short intense (with an electric field strength up to 250 kV cm{sup −1}) terahertz (THz) pulse on the generation of second harmonic (SH) of Ti : sapphire laser radiation in crystals of zinc blende type (InAs and GaAs), characterised by nonzero bulk quadratic susceptibility, is investigated. It is experimentally shown for InAs(100) that, in the case of s-polarised first and second harmonics, an application of s-polarised THz field changes significantly the SH signal. The THz field-induced azimuthal dependence of the SH signal is in good agreement with the results of theoretical calculation within a phenomenological approach. The dependence of the SH signal on the delay time between the optical and THz pulses is investigated. This dependence for the GaAs crystal repeats the envelope of the THz pulse intensity, whereas in the case of InAs crystal there is a significant discrepancy, caused by the nonlinear dynamics of strong THz field in InAs. (nonlinear optical phenomena)

36 MATERIALS SCIENCE↗

BaGa{sub 2}GeS{sub 6} and BaGa{sub 2}GeSe{sub 6} crystals for nonlinear optical frequency conversion

We analyse the functional capabilities of new crystals, BaGa{sub 2}GeS{sub 6} (BGGS) and BaGa{sub 2}GeSe{sub 6} (BGGSe), which are used for nonlinear optical frequency conversion in their transparency range. The wavelengths at which maximum conversion efficiencies can be obtained and the tuning range for difference-frequency generation are found. It is shown that there are wavelength combinations at which the effective nonlinearity coefficient varies only slightly in a wide frequency band. (nonlinear optical phenomena)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

First-principles electron-phonon interactions and polarons in the parent cuprate La 2 CuO 4

Understanding electronic interactions in high-temperature superconductors is an outstanding challenge. In the widely studied cuprate materials, experimental evidence points to strong electron-phonon ( e -ph) coupling and broad photoemission spectra. Yet, the microscopic origin of this behavior is not fully understood. Here, we study e -ph interactions and polarons in a prototypical parent (undoped) cuprate, La 2 CuO 4 (LCO), by means of first-principles calculations. Leveraging parameter-free Hubbard-corrected density functional theory, we obtain a ground state with the band gap and Cu magnetic moment in nearly exact agreement with experiments. This enables a quantitative characterization of e -ph interactions. Our calculations reveal two classes of longitudinal optical (LO) phonons with strong e -ph coupling to hole states. These modes consist of bond stretching and bond bending in the Cu-O plane as well as vibrations of apical O atoms. The hole spectral functions, obtained with a cumulant method that can capture strong e -ph coupling, exhibit broad quasiparticle peaks with a small spectral weight ( Z ≈ 0.25 ) and pronounced LO-phonon sidebands characteristic of polaron effects. Our calculations predict features observed in photoemission spectra, including a 40-meV peak in the e -ph coupling distribution function not explained by existing models. These results show that the universal strong e -ph coupling found experimentally in doped lanthanum cuprates is also present in the parent compound, and elucidate its microscopic origin. Published by the American Physical Society 2025

Chang, Benjamin K. (ORCID:0000000313049324)↗

Ultra-high Q alumina optical microresonators in the UV and blue bands

UV and visible photonics enable applications ranging from spectroscopic sensing to communication and quantum information processing. Photonics structures in these wavelength regimes, however, tend to experience higher loss than their IR counterpart. Particularly in the near-UV band, on-chip optical microresonators have not yet achieved a quality factor beyond 1 million. Here, we report ultra-low-loss photonic waveguides and resonators patterned from alumina thin films prepared by a highly scalable atomic layer deposition process. We demonstrate ultra high Q factor of 1.5×10 6 at 390 nm, a record value at UV bands, and 1.9×10 6 at 488.5 nm.

He, Chengxing (ORCID:0000000347166078)↗

In-situ mid-circuit qubit measurement and reset in a single-species trapped-ion quantum computing system

We implement in-situ mid-circuit measurement and reset (MCMR) operations on a trapped-ion quantum computing system by using metastable qubit states in $^{171}\textrm{Yb}^+$ ions. We introduce and compare two methods for isolating data qubits from measured qubits: one shelves the data qubit into the metastable state and the other drives the measured qubit to the metastable state without disturbing the other qubits. We experimentally demonstrate both methods on a crystal of two $^{171}\textrm{Yb}^+$ ions using both the $S_{1/2}$ ground state hyperfine clock qubit and the $S_{1/2}$-$D_{3/2}$ optical qubit. These MCMR methods result in errors on the data qubit of about $2\%$ without degrading the measurement fidelity. With straightforward reductions in laser noise, these errors can be suppressed to less than $0.1\%$. The demonstrated method allows MCMR to be performed in a single-species ion chain without shuttling or additional qubit-addressing optics, greatly simplifying the architecture.

Atomic Physics (physics.atom-ph)↗

A static model of chromospheric heating in solar flares

The response of the solar chromosphere to flare processes, namely nonthermal electrons, thermal conduction, and coronal pressure, is modeled. Finite difference methods employing linearization and iteration are used in obtaining simultaneous solutions to the equations of steady-state energy balance, hydrostatic equilibrium, radiative transfer, and atomic statistical equilibrium. The atmospheric response is assumed to be confined to one dimension by a strong vertical magnetic field. A solution is obtained to the radiative transfer equation for the most important optically thick transitions of hydrogen, magnesium, and calcium. The theoretical atmospheres discussed here are seen as elucidating the role of various physical processes in establishing the structure of flare chromospheres. At low coronal pressures, conduction is found to be more important than nonthermal electrons in establishing the position of the transition region. Only thermal conduction can adequately account for the chromospheric evaporation in compact flares. Of the mechanisms considered, only nonthermal electrons bring about significant heating below the flare transition region.

Ricchiazzi, P. J.↗

The impact of LDEF results on the space application of metal matrix composites

Over 200 graphite/aluminum and graphite/magnesium composites were flown on the leading and trailing edges of LDEF on the Advanced Composites Experiment. The performance of these composites was evaluated by performing scanning electron microscopy and x-ray photoelectron spectroscopy of exposed surfaces, optical microscopy of cross sections, and on-orbit and postflight thermal expansion measurements. Graphite/aluminum and graphite/magnesium were found to be superior to graphite/polymer matrix composites in that they are inherently resistant to atomic oxygen and are less susceptible to thermal cycling induced microcracking. The surface foils on graphite/aluminum and graphite/magnesium protect the graphite fibers from atomic oxygen and from impact damage from small micrometeoroid or space debris particles. However, the surface foils were found to be susceptible to thermal fatigue cracking arising from contamination embrittlement, surface oxidation, or stress risers. Thus, the experiment reinforced requirements for carefully protecting these composites from prelaunch oxidation or corrosion, avoiding spacecraft contamination, and designing composite structures to minimize stress concentrations. On-orbit strain measurements demonstrated the importance of through-thickness thermal conductivity in composites to minimize thermal distortions arising from thermal gradients. Because of the high thermal conductivity of aluminum, thermal distortions were greatly reduced in the LDEF thermal environment for graphite/aluminum as compared to graphite/magnesium and graphite/polymer composites. The thermal expansion behavior of graphite/aluminum and graphite/magnesium was stabilized by on-orbit thermal cycling in the same manner as observed in laboratory tests.

Steckel, Gary L.↗

Cold Flow Testing for Liquid Propellant Rocket Injector Scaling and Throttling

Scaling and throttling of combustion devices are important capabilities to demonstrate in development of liquid rocket engines for NASA's Space Exploration Mission. Scaling provides the ability to design new injectors and injection elements with predictable performance on the basis of test experience with existing injectors and elements, and could be a key aspect of future development programs. Throttling is the reduction of thrust with fixed designs and is a critical requirement in lunar and other planetary landing missions. A task in the Constellation University Institutes Program (CUIP) has been designed to evaluate spray characteristics when liquid propellant rocket engine injectors are scaled and throttled. The specific objectives of the present study are to characterize injection and primary atomization using cold flow simulations of the reacting sprays. These simulations can provide relevant information because the injection and primary atomization are believed to be the spray processes least affected by the propellant reaction. Cold flow studies also provide acceptable test conditions for a university environment. Three geometric scales - 1/4- scale, 1/2-scale, and full-scale - of two different injector element types - swirl coaxial and shear coaxial - will be designed, fabricated, and tested. A literature review is currently being conducted to revisit and compile the previous scaling documentation. Because it is simple to perform, throttling will also be examined in the present work by measuring primary atomization characteristics as the mass flow rate and pressure drop of the six injector element concepts are reduced, with corresponding changes in chamber backpressure. Simulants will include water and gaseous nitrogen, and an optically accessible chamber will be used for visual and laser-based diagnostics. The chamber will include curtain flow capability to repress recirculation, and additional gas injection to provide independent control of the backpressure. This paper provides a short review of the appropriate literature, as well as descriptions of plans for experimental hardware, test chamber instrumentation, diagnostics, and testing.

Kenny, Jeremy R.↗