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At least 1,297 records · Page 72

Improved Self-Assembly of P3HT with Pyrene-Functionalized Methacrylates

A block copolymer with discotic liquid crystalline behavior was synthesized using Grignard metathesis polymerization (GRIM) and initiators for continuous activator regeneration atom transfer radical polymerization (ICAR-ATRP). A novel discotic liquid crystalline mesogen, 6-(pyren-1-yloxy)hexyl methacrylate (PyMA), comprises a block that is attached to regioregular poly(3- hexylthiophene) (rr-P 3 HT) generated by GRIM and subjected to end-group modification. Due to the continuous regeneration of Cu + in the reaction mixture in ICAR-ATRP compared to conventional methods, the synthesis was successfully performed with less catalyst. The purity and yield of the final product are increased by eliminating rigorous post-synthesis purification. Stacked pyrene units have contributed to the enhanced long-range π-π interactions and aligning of the P 3 HT block as observed in thin-film X-ray diffraction (XRD). Furthermore, field-effect mobilities in the order of 10 -2 cm 2 V -1 s -1 in bottom-gate, top-contact organic field-effect transistors (OFETs) suggest an enhancement in charge transport due to the discotic electron-rich pyrene units that help mitigate the insulating effect of the methacrylate backbone. The formation of uniform microdomains of P 3 HT-bpoly(PyMA) observed with tapping mode atomic force microscopy (TMAFM) on the channel regions of OFETs indicates the unique packing of the block copolymer in comparison to pristine P 3 HT. Thermotropic properties of the novel discotic mesogen in the presence and absence of P3HT were observed with both the poly(3-hexylthiophene)-b-poly(6-(pyren-1-yloxy)hexyl methacrylate) (P3HT-b-poly(PyMA)) block copolymer and poly(6-(pyren-1-yloxy)hexyl methacrylate) (poly(PyMA)) homopolymer using polarized optical microscopy (POM) and differential scanning calorimetry (DSC).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

One- and two-qubit gate infidelities due to motional errors in trapped ions and electrons

In this work, we derive analytic formulas that determine the effect of error mechanisms on one- and two-qubit gates in trapped ions and electrons. First, we analyze and derive expressions for the effect of driving field inhomogeneities on one-qubit gate fidelities. Second, we derive expressions for two-qubit gate errors, including static motional frequency shifts, trap anharmonicities, field inhomogeneities, heating, and motional dephasing. We show that, for small errors, each of our expressions for infidelity converges to its respective numerical simulation; this shows that our formulas are sufficient for determining error budgets for high-fidelity gates, obviating numerical simulations in future projects. All of the derivations are general to any internal qubit state, and any mixed state of the ion crystal's motion that is diagonal in the Fock state basis. Our treatment of static motional frequency shifts, trap anharmonicities, heating, and motional dephasing apply to both laser-based and laser-free gates, while our treatment of field inhomogeneities applies to laser-free systems.

74 ATOMIC AND MOLECULAR PHYSICS↗

Indistinguishable photons from an artificial atom in silicon photonics

Silicon is the ideal material for building electronic and photonic circuits at scale. Integrated photonic quantum technologies in silicon offer a promising path to scaling by leveraging advanced semiconductor manufacturing and integration capabilities. However, the lack of deterministic quantum light sources and strong photon-photon interactions in silicon poses a challenge to scalability. In this work, we demonstrate an indistinguishable photon source in silicon photonics based on an artificial atom. We show that a G center in a silicon waveguide can generate high-purity telecom-band single photons. We perform high-resolution spectroscopy and time-delayed two-photon interference to demonstrate the indistinguishability of single photons emitted from a G center in a silicon waveguide. Our results show that artificial atoms in silicon photonics can source single photons suitable for photonic quantum networks and processors.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Molecular and solid-state topological polaritons induced by population imbalance

Abstract Strong coupling between electronic excitations in materials and photon modes results in the formation of polaritons, which display larger nonlinearities than their photonic counterparts due to their material component. We theoretically investigate how to optically control the topological properties of molecular and solid-state exciton–polariton systems by exploiting one such nonlinearity: saturation of electronic transitions. We demonstrate modification of the Berry curvature of three different materials when placed within a Fabry–Perot cavity and pumped with circularly polarized light, illustrating the broad applicability of our scheme. Importantly, while optical pumping leads to nonzero Chern invariants, unidirectional edge states do not emerge in our system as the bulk-boundary correspondence is not applicable. This work demonstrates a versatile approach to control topological properties of novel optoelectronic materials.

74 ATOMIC AND MOLECULAR PHYSICS↗

High Thermoelectric Performance in the New Cubic Semiconductor AgSnSbSe 3 by High-Entropy Engineering

We investigate the structural and physical properties of the AgSn m SbSe m+2 system with m = 1-20 (i.e., SnSe matrix and ~5-50% AgSbSe 2 ) from atomic, nano, and macro length scales. We find the 50:50 composition, with m = 1 (i.e., AgSnSbSe 3 ), forms a stable cation-disordered cubic rock-salt p-type semiconductor with a special multi-peak electronic valence band structure. AgSnSbSe 3 has an intrinsically low lattice thermal conductivity of ~0.47 W m -1 K -1 at 673 K owing to the synergy of cation disorder, phonon anharmonicity, low phonon velocity, and low-frequency optical modes. Furthermore, Te alloying on Se sites creates a quinary high-entropy NaCl-type solid solution AgSnSbSe 3-x Te x with randomly disordered cations and anions. The extra point defects and lattice dislocations lead to glass-like lattice thermal conductivities of ~0.32 W m -1 K -1 at 723 K and higher hole carrier concentration than AgSnSbSe 3 . Concurrently, the Te alloying promotes greater convergence of the multiple valence band maxima in AgSnSbSe 1.5 Te 1.5 , the composition with the highest configurational entropy. Facilitated by these favorable modifications, we achieve a high average power factor of ~9.54 μW cm -1 K -2 (400-773 K), a peak thermoelectric figure of merit ZT of 1.14 at 723 K, and a high average ZT of ~1.0 over a wide temperature range of 400-773 K in AgSnSbSe 1.5 Te 1.5 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Implementing an electronic sideband offset lock for isotope shift spectroscopy in radium

We demonstrate laser frequency stabilization with at least 6 GHz of offset tunability using an in-phase/quadrature (IQ) modulator to generate electronic sidebands (ESB) on a titanium sapphire laser at 714 nm and we apply this technique to perform isotope shift spectroscopy of 226 Ra and 225 Ra. By locking the laser to a single resonance of a high finesse optical cavity and adjusting the lock offset, we determine the frequency difference between the magneto-optical trap (MOT) transitions in the two isotopes to be 2630.0 ± 0.3 MHz, a factor of 29 more precise than the previously available data. Using the known value of the hyperfine splitting of the 3 P 1 level, we calculate the isotope shift for the 1 S 0 to 3 P 1 transition to be 2267.0 ± 2.2 MHz, a factor of 8 more precise than the best available value. Our technique could be applied to countless other atomic systems to provide unprecedented precision in isotope shift spectroscopy and other relative frequency comparisons.

47 OTHER INSTRUMENTATION↗

Anharmonic Eigenvectors and Acoustic Phonon Disappearance in Quantum Paraelectric SrTiO 3

Pronounced anomalies in the SrTiO 3 dynamical structure factor, S(Q,E), including the disappearance of acoustic phonon branches at low temperatures, were uncovered with inelastic neutron scattering (INS) and simulations. The striking effect reflects anharmonic couplings between acoustic and optic phonons and the incipient ferroelectric instability near the quantum critical point. It is rationalized using a first-principles renormalized anharmonic phonon approach, pointing to nonlinear Ti-O hybridization causing unusual changes in real-space phonon eigenvectors, frequencies, group velocities, and scattering phase space. Lastly, our method is general and establishes how T dependences beyond the harmonic regime, assessed by INS mapping of large reciprocal-space volumes, provide real-space insights into anharmonic atomic dynamics near phase transitions.

36 MATERIALS SCIENCE↗

Controlled molecule injector for cold, dense, and pure molecular beams at the European x-ray free-electron laser

A permanently available molecular-beam injection setup for controlled molecules (COMO) was installed and commissioned at the small quantum systems (SQS) instrument at the European x-ray free-electron laser (EuXFEL). A b-type electrostatic deflector allows for pure state-, size-, and isomer-selected samples of polar molecules and clusters. The source provides a rotationally cold (T ≈ 1 K) and dense (ρ ≈ 10 8 cm −3 ) molecular beam with pulse durations up to 100 µs generated by a new version of the Even-Lavie valve. Here, a performance overview of the COMO setup is presented along with characterization experiments performed both with an optical laser at the Center for Free-Electron-Laser Science and with x rays at EuXFEL under burst-mode operation. COMO was designed to be attached to different instruments at the EuXFEL, in particular, the SQS and single particles, clusters, and biomolecules (SPB) instruments. This advanced controlled-molecules injection setup enables x-ray free-electron laser studies using highly defined samples with soft and hard x-ray FEL radiation for applications ranging from atomic, molecular, and cluster physics to elementary processes in chemistry and biology.

He, Lanhai↗

Optimizing qubit control pulses for state preparation

In the burgeoning field of quantum computing, the precise design and optimization of quantum pulses are essential for enhancing qubit operation fidelity. This study focuses on refining the pulse engineering techniques for superconducting qubits, employing a detailed analysis of square and Gaussian pulse envelopes under various approximation schemes. We evaluated the effects of coherent errors induced by naive pulse designs. Furthermore, we identified the sources of these errors in the Hamiltonian model’s approximation level. We mitigated these errors through adjustments to the external driving frequency and pulse durations, thus implementing a pulse scheme with stroboscopic error reduction. Our results demonstrate that these refined pulse strategies improve performance and reduce coherent errors. Moreover, the techniques developed herein are applicable across different quantum architectures, such as ion-trap, atomic, and photonic systems.

Chirp modulation↗

Density of molten oxides measured in an aero-acoustic levitator

Knowing the thermophysical properties of high-temperature melts can aid the design of melt processes and validate atomic structural models, such as those used in studying glass formation. Property measurements on such melts are challenging, however, due to container-related contamination and heterogeneous nucleation. Containerless processing techniques that employ levitation can be used to avoid these obstacles. In that context, we demonstrate here the application of silhouette imaging to measure the density of molten oxides in an aero-acoustic levitation instrument (AAL). The AAL combines gas jet levitation with actively controlled acoustic positioning to enable full optical access to samples ca. 2–4 mm in diameter, which are laser beam heated and melted. The cross sections of molten drops are imaged using a monochromatic light source and narrowband-filtered camera. Melt volume is calculated from the cross sections and used to find density at several temperatures ranging 1530–1920 K, including up to 350 K of supercooling. We report densities for CaAl 2 O 4 , Ca 12 Al 14 O 33 , CaSiO 3 , their Fe 2 O 3 -bearing analogs, and 83TiO 2 -17RE 2 O 3 (RE = La or Nd). These provide important benchmarks of the capabilities, measurement uncertainties, and future outlook for this technique.

36 MATERIALS SCIENCE↗

Atomic dynamics in 𝑀⁢Cr⁢𝑋 2 (𝑀=Ag, Cu; 𝑋 = S, Se) across magnetic and superionic transitions

Here, a systematic study of atomic dynamics and thermal properties of the family of layered chalcogenide compounds 𝑀⁢Cr⁢𝑋 2 (𝑀= Ag, Cu; 𝑋 = S, Se) was performed, including neutron and x-ray scattering, thermal characterization, and first-principles simulations. In all compounds, we observe a breakdown of specific phonon modes across the superionic phase transition, for phonons whose eigenvectors exhibit large contributions of mobile ions. In particular, the nondispersive portions of transverse acoustic (TA) branches at short-wavelengths and the low-energy optical phonons with large contributions from Ag + or Cu + become severely damped in the superionic phase. However, well-defined quasiparticles persist in the superionic state for long-wavelength TA phonons. In the case of AgCrS 2 , the coupling of lattice dynamics with its antiferromagnetic transition was also investigated. The magnetic ordering couples with the monoclinic–rhombohedral structural transition, and the Cr 3+ spin arrangement strongly affects the phonon dispersions. We qualitatively reproduce the magnetic and nuclear components of the INS measurement for antiferromagnetic AgCrS 2 by combining models of spin-waves and spin-polarized first-principles phonon simulations. Quasielastic magnetic fluctuations persist in the paramagnetic phase up to high temperature, but are clearly distinguished from the nuclear component through their momentum dependence. Finally, we report measurements of the thermal properties of the selenide compounds and find good agreement with our DFT simulations.

36 MATERIALS SCIENCE↗

Anisotropic band structure of TiS 3 nanoribbon revealed by polarized photocurrent spectroscopy

A re-discovered member of the layered material family, Titanium Trisulfide (TiS 3 ), has attracted intense research interest recently for the possibility of realizing an exciton insulator in the monolayer limit. However, due to their quasi-one-dimensional nature, thin TiS 3 flakes are typically in the form of nanoribbons that are challenging to characterize by optical absorption spectra, due to their small cross section. Here, we employ a sensitive photocurrent spectroscopy technique to probe the absorption of a thin TiS 3 nanoribbon in a field-effect transistor configuration. We have found a significant modification of the band structure of the thin TiS 3 nanoribbon, compared to its bulk counterpart. In addition, the polarization-dependent photocurrent spectra of thin TiS 3 nanoribbons exhibit greatly enhanced anisotropy compared to that of a thick TiS 3 device. The atomically thin TiS 3 flake, thus, not only provides an exciting platform for investigating many-body physics but also enables anisotropic quantum optoelectronics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Absolute electron density fluctuation reconstruction for two-dimensional hydrogen beam emission spectroscopy

Scrape-off layer (SOL) and edge plasma turbulence significantly contribute to the radial particle and heat transport, lowering the plasma confinement and increasing the heat load on the plasma facing components. SOL turbulence is predominantly intermittent, which manifests in the occurrence of isolated density filaments or blobs. Filaments propagate radially outward toward plasma facing components, limiting their lifetime by erosion and sputtering. To characterize this phenomenon in detail, few diagnostic techniques are available. Beam emission spectroscopy is a diagnostic capable of measuring plasma turbulence in both SOL and edge plasmas. Due to the finite lifetime of the excitation states during the beam–plasma interaction and the misalignment between the optics and the magnetic field, spatial smearing is introduced in the measurement. In this paper, a novel method is introduced to overcome this hindering effect by inverting the fluctuation response matrix on an optimally smoothed signal. We show that this method is fast and provides significantly more accurate absolute density fluctuation reconstruction than the direct inversion technique. Here, the presented method is usable for all types of beam emission diagnostics where the spatial resolution is higher than the combined smearing of the atomic physics and the observation.

47 OTHER INSTRUMENTATION↗

A Molecular Gas Ring Hidden in the Sombrero Galaxy

We present Herschel, ALMA, and MUSE observations of the molecular ring of Messier 104, also known as the Sombrero galaxy. These previously unpublished archival data shed new light on the content of the interstellar medium of M104. In particular, molecular hydrogen measured by CO emission and dust measured by far-infrared light are uniformly distributed along the ring. The ionized gas revealed by Hα and [C II] emission is distributed in knots along the ring. Despite being classified as an SAa galaxy, M104 displays features typical of early-type galaxies. We therefore compared its [C II] and dust emission to a sample of early-type galaxies observed with Herschel and SOFIA. The [C II]/FIR ratio of M104 is much lower than that of typical star-forming galaxies and is instead much more similar to that of early-type galaxies. By classifying regions using optical emission line diagnostics, we also find that regions classified as H II lie closer to star-forming galaxies in the [C II]/FIR diagram than those classified as low-ionization emission regions. The good match between [C II] and Hα emission, in conjunction with the lack of correlation between CO emission and star formation, suggests that there is very limited active star formation along the ring and that most of the [C II] emission is from ionized and neutral atomic gas rather than molecular gas. From the total intensity of the CO line, we estimate a molecular hydrogen mass of 0.9 × 10 9 M ⊙ , a value intermediate between those of early-type galaxies and the content of the molecular ring of our galaxy.

79 ASTRONOMY AND ASTROPHYSICS↗

Generation and detection of 50 GHz surface acoustic waves by extreme ultraviolet pulses

In this work, we use femtosecond extreme ultraviolet pulses derived from a free electron laser to excite and probe surface acoustic waves (SAWs) on the (001) surface of single crystal SrTiO 3 . SAWs are generated by a pair of 39.9 nm pulses crossed at the sample with the crossing angle defining the SAW wavelength at 84 nm. Detection of SAWs is performed via diffraction of a time-delayed 13.3 nm probe pulse by SAW-induced surface ripples. Despite the low reflectivity of the sample in the extreme ultraviolet range, the reflection mode detection is found to be efficient because of an increase in the diffraction efficiency for shorter wavelengths. We describe a methodology for extracting the SAW attenuation in the presence of a thermal grating, which is based on measuring the decay of oscillations at twice the SAW frequency. The proposed approach can be used to study ultrahigh frequency SAWs in a broad range of materials and will bridge the wave vector gap in surface phonon spectroscopy between Brillouin scattering and He atom scattering.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Intermediate-Term Thermal Aging Effect Evaluation for Grade 92 and 316L at The LWR Relevant Temperature

Life extension of the existing nuclear reactors imposes accumulated damages, such as higher fluences and longer period of corrosion, to structural materials, which would result in significant challenges to the traditional reactor materials such as type 304 and 316 stainless steels. Advanced alloys with superior radiation resistance will increase safety margins, design flexibility, and economics for not only the life extension of the existing fleet but also new builds with advanced reactor designs. The Electric Power Research Institute (EPRI) teamed up with Department of Energy (DOE) on the Advanced Radiation Resistant Materials (ARRM) program, aiming to develop and test degradation resistant alloys from current commercial alloy specifications by 2021 to a new advanced alloy with superior degradation resistance in light water reactor (LWR)-relevant environments by 2024. Based on a comprehensive microstructure and property screening performed in Phase-1 of the ARRM program, a total of five alloys, together with 316L and X-750 as references, were down-selected for Phase-2 neutron irradiation studies. Because thermal aging could exert a synergistic effect on neutron irradiation due to the low neutron damage rate on the order of 10 –7 displacements per atom per second (dpa/s), Grade 92 (one of the five down-selected alloys) and two heats of 316L were selected in this task to study the effect of aging at 350°C for 12.5–12.7 kh on microstructure and mechanical properties. The aging time is approximately corresponding to 5 dpa neutron irradiation, which can be served as a reference for the 5-dpa-irradiated samples of the alloys to help understand the independent neutron damage influence on microstructure and mechanical properties. Optical microscopy and scanning electron microscopy were used for microstructural characterization. Hardness, tensile, Charpy impact toughness, and fracture toughness in the ductile regime of the aged samples were examined. The aging of Grade 92 led to the formation of many Laves phase in sizes of ~100–200 nm and resulted in some reduction in hardness and yield/ultimate tensile strength with some increases in uniform and total plastic elongations, which may have helped the enhancement of Charpy impact toughness, e.g., ~4 J increase in upper-shelf energy and 20.5°C reduction in ductile-brittle transition temperature compared with the unaged condition. The fracture toughness of the aged Grade 92 showed decent toughness of ~303 MPa√m (K Jq ) with ~87 tearing modulus at 22°C, which reduced to ~241 MPa√m (~20% reduction) with ~75 tearing modulus at 300°C. The two heats of 316L are differentiated by their amounts of δ-ferrite, i.e., ~1 vol% in heat T1103 and ~4 vol% in heat N5B8. The two heats of 316L were subjected to 15% cold work (CW) as this condition is often used in nuclear reactors to help trapping radiation-induced defects and thus postpone the steady state swelling stage. The aging did not result in any noticeable microstructure changes, except for possible segregations at grain boundaries that need to be further investigated. The aging resulted in slight reduction in hardness of 316L-T1103 and slight increase in hardness of 316L-N5B8, which is consistent with their tensile testing results. The 15%CW might have introduced some inhomogeneity, resulting in large standard deviations in hardness, which were reduced after the aging. The aged 316L followed the same trend as the unaged condition for the strength and elongation results from the tensile testing. Minimum elongations appeared within ~300–600°C, above which the elongations seem to increase. Unlike the negligible or minor changes in microstructure, hardness and tensile results of the two heats of 316L, their fracture toughness showed noticeable difference. The aged 316L-T1103 showed good toughness of ~350 MPa√m with ~80 tearing modulus at 22°C, which reduced to ~271 MPa√m (~23% reduction) with ~83 tearing modulus at 300°C. In contrast, the aged 316L-N5B8 showed lower toughness of ~244 MPa√m with ~53 tearing modulus at 22°C, which reduced to ~180 MPa√m (~26% reduction) with ~31 tearing modulus at 300°C. The preliminary results indicate that the presence of high volume of δ-ferrite would noticeable impair fracture toughness although it may not influence hardness and tensile properties.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Symmetric carbon tetramers forming spin qubits in hexagonal boron nitride

Abstract Point defect quantum bits in semiconductors have the potential to revolutionize sensing at atomic scales. Currently, vacancy-related defects are at the forefront of high spatial resolution and low-dimensional sensing. On the other hand, it is expected that impurity-related defect structures may give rise to new features that could further advance quantum sensing in low dimensions. Here, we study the symmetric carbon tetramer clusters in hexagonal boron nitride and propose them as spin qubits for sensing. We utilize periodic-DFT and quantum chemistry approaches to reliably and accurately predict the electronic, optical, and spin properties of the studied defect. We show that the nitrogen-centered symmetric carbon tetramer gives rise to spin state-dependent optical signals with strain-sensitive intersystem crossing rates. Furthermore, the weak hyperfine coupling of the defect to their spin environments results in a reduced electron spin resonance linewidth that can enhance sensitivity.

Chemistry↗

Modulating effect of evanescent waves on thin film growth

Atomic-scale smooth thin films are keys to successful integration and proper function of many multilayer-structured devices. However, the intrinsic islandlike growth mode prevents human beings from realizing such ultrasmooth films of many important functional materials. To solve this problem, we propose a negative entropy-infusing method that employs evanescent waves to enhance the downward interlayer diffusion of adatoms and thus transform the islandlike growth mode to the layer-by-layer growth mode. In this work, the formulas of the optical force and the lowered diffusion barrier were derived, and the application of this theory on a simplified example demonstrates significantly improved surface morphologies through numerical simulations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗