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At least 901 records · Page 50

Next Generation X-Ray Optics: High-Resolution, Light-Weight, and Low-Cost

X-ray telescopes are essential to the future of x-ray astronomy. This paper describes a comprehensive program to advance the technology for x-ray telescopes well beyond the state of the art represented by the three currently operating missions: Chandra, XMM-Newton , and Suzaku . This program will address the three key issues in making an x-ray telescope: (I) angular resolution, (2) effective area per unit mass, and (3) cost per unit effective area. The objectives of this technology program are (1) in the near term, to enable Explorer-class x-ray missions and an IXO type mission, and (2) in the long term, to enable a flagship x-ray mission with sub-arcsecond angular resolution and multi-square-meter effective area, at an affordable cost. We pursue two approaches concurrently, emphasizing the first approach in the near term (2-5 years) and the second in the long term (4-10 years). The first approach is precision slumping of borosilicate glass sheets. By design and choice at the outset, this technique makes lightweight and low-cost mirrors. The development program will continue to improve angular resolution, to enable the production of 5-arcsecond x-ray telescopes, to support Explorer-class missions and one or more missions to supersede the original IXO mission. The second approach is precision polishing and light-weighting of single-crystal silicon mirrors. This approach benefits from two recent commercial developments: (1) the inexpensive and abundant availability of large blocks of mono crystalline silicon, and (2) revolutionary advances in deterministic, precision polishing of mirrors. By design and choice at the outset, this technique is capable of producing lightweight mirrors with sub-arcsecond angular resolution. The development program will increase the efficiency and reduce the cost of the polishing and the lightweighting processes, to enable the production of lightweight sub-arcsecond x-ray telescopes. Concurrent with the fabrication of lightweight mirror segments is the continued development and perfection of alignment and integration techniques, for incorporating individual mirror segments into a precision mirror assembly. Recently, we have been developing a technique called edge-bonding, which has achieved an accuracy to enable 10- arcsecond x-ray telescopes. Currently, we are investigating and improving the long-term alignment stability of so-bonded mirrors. Next, we shall refine this process to enable 5-arsecond x-ray telescopes. This technology development program includes all elements to demonstrate progress toward TRL-6: metrology; x-ray performance tests; coupled structural, thermal, and optical performance analysis, and environmental testing.

Zhang, William W.↗

Next Generation X-Ray Optics: High-Resolution, Light-Weight, and Low-Cost

X-ray telescopes are essential to the future of x-ray astronomy. In this talk I will describe a comprehensive program to advance the technology for x-ray telescopes well beyond the state of the art represented by the three currently operating missions: Chandra, XMM-Newton, and Suzaku. This program will address the three key issues in making an x-ray telescope: (1) angular resolution, (2) effective area per unit mass, and (3) cost per unit effective area. The objectives of this technology program are (1) in the near term, to enable Explorer-class x-ray missions and an IXO-type mission, and (2) in the long term, to enable a flagship x-ray mission with sub-arcsecond angular resolution and multi-square-meter effective area, at an affordable cost. We pursue two approaches concurrently, emphasizing the first approach in the near term (2-5 years) and the second in the long term (4-10 years). The first approach is precision slumping of borosilicate glass sheets. By design and choice at the outset, this technique makes lightweight and low-cost mirrors. The development program will continue to improve angular resolution, to enable the production of 5-arcsecond x-ray telescopes, to support Explorer-class missions and one or more missions to supersede the original IXO mission. The second approach is precision polishing and light-weighting of single-crystal silicon mirrors. This approach benefits from two recent commercial developments: (1) the inexpensive and abundant availability of large blocks of monocrystalline silicon, and (2) revolutionary advances in deterministic, precision polishing of mirrors. By design and choice at the outset, this technique is capable of producing lightweight mirrors with sub-arcsecond angular resolution. The development program will increase the efficiency and reduce the cost of the polishing and the light-weighting processes, to enable the production of lightweight sub-arcsecond x-ray telescopes. Concurrent with the fabrication of lightweight mirror segments is the continued development and perfection of alignment and integration techniques, for incorporating individual mirror segments into a precision mirror assembly. Recently, we have been developing a technique called edge-bonding, which has achieved an accuracy to enable 10-arcsecond x-ray telescopes. Currently, we are investigating and improving the long-term alignment stability of so-bonded mirrors. Next, we shall refine this process to enable 5-arsecond x-ray telescopes. This technology development program includes all elements to demonstrate progress toward TRL-6: metrology; x-ray performance tests; coupled structural, thermal, and optical performance analysis, and environmental testing.

Zhang, William W.↗

Surface chemical trapping of optical cycling centers

Quantum information processors based on trapped atoms utilize laser-induced optical cycling transitions for state preparation and measurement. These transitions consist of an electronic excitation from the ground to an excited state and a decay back to the initial ground state, associated with a photon emission. While this technique has been used primarily with atoms, it has also recently been shown to work for some divalent metal hydroxides ( e.g. SrOH) and alkoxides ( e.g. SrOCH 3 ). Additionally, this extension to molecules is possible because these molecules feature nearly isolated, atomic-like ground and first-excited electronic states centered on the radical metal atom. We theoretically investigate the extension of this idea to a larger scale by growing the alkyl group, R, beyond the initial methyl group, CH 3 , while preserving the isolated and highly vertical character of the electronic excitation on the radical metal atom, M. Theory suggests that in the limit as the size of the ligand carbon chain increases, it can be considered a functionalized diamond (or cubic boron nitride) surface. Several requirements must be observed for the cycling centers to function when bound to the surface. First, the surface must have a significant band gap that fully encapsulates both the ground and excited states of the cycling center. Second, while the surface lattice imposes strict limits on the achievable spacing between the SrO– groups, at high coverage, SrO– centers can interact, and show geometric changes and/or electronic state mixing. We show that the coverage of the diamond surface with SrO– cycling centers needs to be significantly sub-monolayer for the functionality of the cycling center to be preserved. Having the lattice-imposed spatial control of SrO– placements will allow nanometer-scale proximity between qubits and will eliminate the need for atom traps for localized cycling emitters. Our results also imply that a functionalization could be done on a scanning microscope tip for local quantum sensing or on photonic structures for optically-mediated quantum information processing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Multi-scale time-resolved electron diffraction: A case study in moiré materials

Ultrafast-optical-pump — structural-probe measurements, including ultrafast electron and x-ray scattering, provide direct experimental access to the fundamental timescales of atomic motion, and are thus foundational techniques for studying matter out of equilibrium. High-performance detectors are needed in scattering experiments to obtain maximum scientific value from every probe particle. Here we deploy a hybrid pixel array direct electron detector to perform ultrafast electron diffraction experiments on a WSe 2 /MoSe 2 2D heterobilayer, resolving the weak features of diffuse scattering and moiré superlattice structure without saturating the zero order peak. Enabled by the detector’s high frame rate, we show that a chopping technique provides diffraction difference images with signal-to-noise at the shot noise limit. Finally, we demonstrate that a fast detector frame rate coupled with a high repetition rate probe can provide continuous time resolution from femtoseconds to seconds, enabling us to perform a scanning ultrafast electron diffraction experiment that maps thermal transport in WSe 2 /MoSe 2 and resolves distinct diffusion mechanisms in space and time.

36 MATERIALS SCIENCE↗

Data-Driven Mapping of the Cesium Cadmium Bromide Phase Space Utilizing a Soft-Chemistry Approach

Soft-chemistry techniques provide a versatile approach to synthesizing inorganic materials under mild conditions, enabling access to compositions and structures that are challenging to achieve through traditional thermodynamically driven solid-state methods. However, these solution-based routes often result in phase competition, requiring precise control over reaction conditions to achieve selective product formation. While one-variable-at-a-time (OVAT) approaches have traditionally been used for phase selection, data-driven strategies are emerging as more efficient methods for navigating complex synthetic spaces. Ternary metal halides, such as cesium cadmium bromides (Cs–Cd–Br), are of growing interest due to their potential in wide and ultrawide band gap applications. Unlike the well-studied cesium lead halide phases, the compositional diversity and solution-based synthesis of ternary Cs–Cd–Br phases remain largely unexplored. This study systematically investigates the synthetic phase space of the Cs–Cd–Br system by constructing a data-driven phase map. Using a common set of precursors and a standardized experimental procedure, we successfully synthesize all four known Cs–Cd–Br phases—CsCdBr 3 , Cs 2 CdBr 4 , Cs 3 CdBr 5 , and Cs 7 Cd 3 Br 13 —each exhibiting distinct structures, morphologies, and optical properties. Our findings highlight the potential of soft-chemistry methods for expanding the library of ternary metal halides and provide key insights into the thermodynamic and kinetic factors governing phase formation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Toward Quantum Confinement in Graphitic Carbon Nitride-Based Polymeric Monolayers

raphitic carbon nitride (g-C 3 N 4 ) has garnered much attention due to its potential as an efficient metal-free photocatalyst. This study examines the evolution of properties in zero-dimensional quantum dots up to sizable clusters that mimic extended g-C 3 N 4 monolayers. We employ density functional theory to investigate systematically the structural, electronic, and optical properties of the g-C 3 N 4 -based melamine and heptazine building blocks using a “bottom-up” construction of polymeric monolayers. The results from our computations indicate that the melamine- and heptazine-based polymeric g-C 3 N 4 systems must be reduced to at least 2.74 and 4.00 nm, respectively, to observe an increase of its optical gap with a size reduction. The present study also examines the nature of the electronic transitions exhibited by g-C 3 N 4 -based monolayers through full natural transition orbital and density of state analyses. Furthermore, the most promising sites for water splitting and subsequent chemical doping studies are identified, which generally correspond to the nitrogen and carbon atoms, respectively.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

All-polymer organic solar cells with nano-to-micron hierarchical morphology and large light receiving angle

Distributed photovoltaics in living environment harvest the sunlight in different incident angles throughout the day. The development of planer solar cells with large light-receiving angle can reduce the requirements in installation form factor and is therefore urgently required. Here, thin film organic photovoltaics with nano-sized phase separation integrated in micro-sized surface topology is demonstrated as an ideal solution to proposed applications. All-polymer solar cells, by means of a newly developed sequential processing, show large magnitude hierarchical morphology with facilitated exciton-to-carrier conversion. The nano fibrilar donor-acceptor network and micron-scale optical field trapping structure in combination contributes to an efficiency of 19.06% (certified 18.59%), which is the highest value to date for all-polymer solar cells. Furthermore, the micron-sized surface topology also contributes to a large light-receiving angle. A 30% improvement of power gain is achieved for the hierarchical morphology comparing to the flat-morphology devices. These inspiring results show that all-polymer solar cell with hierarchical features are particularly suitable for the commercial applications of distributed photovoltaics due to its low installation requirement.

14 SOLAR ENERGY↗

Single-photon emission from two-dimensional perovskites channeled through low-energy edge states

Two-dimensional perovskites, an emerging family of van der Waals materials with an innate quantum-well structure, exhibit remarkable optical characteristics and compositional tunability. However, their potential as a source for quantum emitters remains unexplored. Here, we investigate low-energy edge states unique to two-dimensional perovskites using comprehensive photoluminescence imaging and spectroscopy, to further leverage them towards uncovering quantum emitters. In contrast to above-bandgap excitation, spatially localized single-photon emitters are realized through sub-bandgap energy excitation at the edges in exfoliated single crystals. Specifically, the sub-bandgap excitation facilitates efficient access to deeply confined states within the bandgap, as charge carriers can channel through low-energy edge states while inhibiting competing processes. Furthermore, we demonstrate single-photon emitters from artificially created edges via strain as well as from two-dimensional perovskites with different quantum-well thicknesses. Our findings provide promising opportunities in the development of two-dimensional quantum emitters, where two-dimensional perovskites may provide added functionalities with versatility in material design, fabrication, and scalability.

Materials for optics↗

Ultrafast vibrational control of organohalide perovskite optoelectronic devices using vibrationally promoted electronic resonance

Vibrational control (VC) of photochemistry through the optical stimulation of structural dynamics is a nascent concept only recently demonstrated for model molecules in solution. Extending VC to state-of-the-art materials may lead to new applications and improved performance for optoelectronic devices. Metal halide perovskites are promising targets for VC due to their mechanical softness and the rich array of vibrational motions of both their inorganic and organic sublattices. Here, we demonstrate the ultrafast VC of FAPbBr 3 perovskite solar cells via intramolecular vibrations of the formamidinium cation using spectroscopic techniques based on vibrationally promoted electronic resonance. The observed short (~300 fs) time window of VC highlights the fast dynamics of coupling between the cation and inorganic sublattice. First-principles modelling reveals that this coupling is mediated by hydrogen bonds that modulate both lead halide lattice and electronic states. Cation dynamics modulating this coupling may suppress non-radiative recombination in perovskites, leading to photovoltaics with reduced voltage losses.

36 MATERIALS SCIENCE↗

Prediction of BiS2-type pnictogen dichalcogenide monolayers for optoelectronics

Abstract In this work, we introduce a 2D materials family with chemical formula MX 2 (M={As, Sb, Bi} and X={S, Se, Te}) having a rectangular 2D lattice. This materials family has been predicted by systematic ab-initio structure search calculations in two dimensions. Using density-functional theory and many-body perturbation theory, we study the structural, vibrational, electronic, optical, and excitonic properties of the predicted MX 2 family. Our calculations reveal that the predicted SbX 2 and BiX 2 monolayers are stable while the AsX 2 layers exhibit an in-plane ferroelectric instability. All materials display strong excitonic effects and good optical absorption within the infrared-to-visible range. Hence, these monolayers can harvest solar energy and serve in optoelectronics applications. Furthermore, our results indicate that exfoliation of the predicted MX 2 monolayers from their bulk counterparts is experimentally viable.

Materials Science↗

Crystal engineering of heterocyclic arylene(ethynylene) oligomers through programmed aromatic stacking

Conjugated oligomers and polymers consisting of aromatic heterocycles are examples of next-generation organic electronic materials. However, control and optimization of the self-assembly of these materials in the solid-state, which is a crucial parameter for high efficiency performance, remains an unsolved challenge in materials development. In this work, we provide valuable insight into aromatic stacking interactions between fluorinated arene rings (ArF) and heterocycles with different electronic character (Het), and elaborate on the prospect of using these interactions to control the solid-state configurations of three-ring phenyleneethynylene oligomers (PEs). Oligomers possessing heterocycles typically thought of as electron-rich (ER) show blue-shifted optical spectra in the solid-state, while those incorporating heterocycles typically thought of us electron deficient (ED) show red-shifted solid-state optical spectra. Crystal structures show ArF-Het stacking interactions between the fluorinated side-chains and ER units, which twist the backbone out of planarity and prevent chromophore aggregation. Further, the interactions are absent in ED oligomers, highlighting cofacial incompatibility between ArF rings and ED units. A combination of TD-DFT computations and novel heterocycle descriptors reinforce our assignment of the oligomers as ED or ER, while exhaustive conformer analysis shows ArF-Het stacking interactions are a significant contributor to compound stability. Overall, this work describes the importance of heterocycle electronics in conformational control in the solid state, understanding of which can be a valuable asset in the development of novel optoelectronic materials.

36 MATERIALS SCIENCE↗

Bandgap engineering of SrZrS 3 chalcogenide perovskite via substitutional doping for photovoltaic applications: a first-principles DFT study

Strontium zirconium sulfide (SrZrS 3 ) has garnered significant attention for photovoltaic (PV) applications due to its excellent optoelectronic properties, high chemical and moisture stability, and non-toxicity. However, the bandgaps of both the α- and β-phases lie outside the optimum ranges for both single-junction solar cells (SJSCs) and tandem solar cells (TSCs), thereby limiting their applications in PV technologies. In this study, we employed hybrid density functional theory to engineer the band gaps of α- and β-SrZrS 3 through substitutional doping. We considered three dopants (Hf, Sn, and Ti) at the Zr site of SrZrS 3 with varying doping concentrations and investigated their effects on the structural, electronic, and optical properties of the materials. We found that Sn and Ti doping effectively lowers the band gaps of both α- and β-SrZrS 3 , whereas Hf doping increases them. For x values up to 0.25, the band gaps of the α-SrZr 1−x Sn x S 3 and α-SrZr 1−x Ti x S 3 are within the optimum range for SJSCs, and those of β-SrZr 1−x Sn x S 3 and β-SrZr 1−x Ti x S 3 lie within the optimum range for Si/perovskite as well as perovskite/perovskite TSCs. The three dopants exhibited significant effects on the optical properties of both α- and β-SrZrS 3 , including the absorption coefficient, energy-loss functions, reflectivity, and refractivity spectra. Thermodynamic stability analysis revealed that for both phases, SrZr 1−x Hf x S 3 can be synthesized via exothermic processes, whereas the formation of SrZr 1−x Ti x S 3 and SrZr1−xSn x S 3 is endothermic and hence, not thermodynamically favorable. Further analysis showed that SrZr 1−x Ti x S 3 in both α- and β-phases are stable under thermodynamic equilibrium conditions, whereas SrZr 1−x Sn x S 3 is prone to dissociation into ternary phases (SrZrS 3 and SrSnS 3 ), especially at higher doping concentrations. These results show that Ti doping is effective in tuning the band gaps of α- and β-SrZrS 3 toward the optimal values for PV applications.

14 SOLAR ENERGY↗

Hybridization and deconfinement in colloidal quantum dot molecules

The structural, electronic, and optical properties of CdSe/CdS core–shell colloidal quantum dot molecules, a new class of coupled quantum dot dimers, are explored using atomistic approaches. Unlike the case of dimers grown by molecular beam epitaxy, simulated strain profile maps of free-standing colloidal dimers show negligible additional strain resulting from the attachment. Further, the electronic properties of the relaxed dimers are described within a semiempirical pseudopotential model combined with the Bethe–Salpeter equation within the static screening approximation to account for electron–hole correlations. The interplay of strain, hybridization (tunneling splitting), quantum confinement, and electron–hole binding energies on the optical properties is analyzed and discussed. The effects of the dimensions of the neck connecting the two quantum dot building blocks, as well as the shell thickness, are studied.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Quantum efficiency enhancement in simulated nanostructured negative electron affinity GaAs photocathodes

We report nanostructured negative electron affinity GaAs photocathodes for a polarized electron source are studied using finite difference time domain optical simulation. The structures studied are nanosquare columns, truncated nanocones, and truncated nanopyramids. Mie-type resonances in the 700–800 nm waveband, suitable for generation of polarized electrons, are identified. At resonance wavelengths, the nanostructures can absorb up to 99% of the incident light. For nanosquare columns and truncated nanocones, the maximum quantum efficiency (QE) at 780 nm obtained from simulation is 27%, whereas for simulated nanopyramids, the QE is ~21%. The high photocathode quantum efficiency is due to the shift of Mie resonance toward the longer wavelength, leading to increased light absorption. The field profile distribution shows the excitation of dipole and quadrupole modes within the nanostructures at resonant frequencies. This leads to enhanced photoabsorption and photoelectron generation closer to emission surfaces than for a flat photocathode. The enhanced photoabsorption and reduced electron transport distance for the nanostructured photocathode enhance its QE compared to that for the flat surface wafer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Direct time-domain determination of electron-phonon coupling strengths in chromium

In this work, we report the results of an ultrafast, direct structural measurement of optically pumped phonons in a Cr thin film using ultrashort x-ray pulses from a free-electron laser. In addition to measuring and confirming the known long-wavelength dispersion relation of Cr along a particular acoustic branch, we are able to determine the relative phase of the phonons as they are generated. The Cr sample exhibits two generation mechanisms for the phonons: the releasing of a preexisting charge density wave at higher frequencies, and the creation of an acoustic strain pulse via laser heating that dominates at lower frequencies. Furthermore, for the latter mechanism, we are able to measure the frequency dependence of the time required to generate the phonons. To explain the observed magnitude and slope of the delays, we perform first-principles simulations in the framework of density functional perturbation theory and ab initio molecular dynamics to fit anharmonic phonon models. In conclusion, these results show that the wave-vector dependence of the electron-phonon coupling is the driving mechanism behind the delay times: Phase-space limitation leads to higher times near the zone center. The absolute magnitudes of the delay times measured are found to be much shorter than the equilibrium electron-phonon coupling times we compute, indicating that the coupling strength is greatly enhanced when the electronic system is out of equilibrium with the lattice, as has been seen in bismuth and other systems.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Dephasingless Laser Wakefield Acceleration

Laser wakefield accelerators (LWFAs) produce significantly high gradients enabling compact accelerators and radiation sources, but face design limitations, such as dephasing, occurring when trapped electrons outrun the accelerating phase of the wakefield. In this report we combine spherical aberration with a novel cylindrically symmetric echelon optic to spatiotemporally structure an ultra-short, high-intensity laser pulse that can overcome dephasing by propagating at any velocity over any distance. The ponderomotive force of the spatiotemporally shaped pulse can drive a wakefield with a phase velocity equal to the speed of light in vacuum, preventing trapped electrons from outrunning the wake. Simulations in the linear regime and scaling laws in the bubble regime illustrate that this dephasingless LWFA can accelerate electrons to high energies in much shorter distances than a traditional LWFA—a single 4.5 m stage can accelerate electrons to TeV energies without the need for guiding structures.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Cosmological Constraints from Combining Photometric Galaxy Surveys and Gravitational Wave Observatories

Spatial variations in survey properties due to selection effects generate substantial systematic errors in large-scale structure measurements in optical galaxy surveys on very large scales. On such scales, the statistical sensitivity of optical surveys is also limited by their finite sky coverage. By contrast, gravitational wave (GW) sources appear to be relatively free of these issues, provided the angular sensitivity of GW experiments can be accurately characterized. We quantify the expected cosmological information gain from combining the forecast LSST 3$\times$2pt analysis (combination of three 2-point correlations of galaxy density and weak lensing shear fields) with the large-scale auto-correlation of GW sources from proposed next-generation GW experiments. We find that in $\Lambda$CDM and $w$CDM models, there is no significant improvement in cosmological constraints from combining GW with LSST 3$\times$2pt over LSST alone, due to the large shot noise for the former; however, this combination does enable a $\sim6\%$ constraint on the linear galaxy bias of GW sources. More interestingly, the optical-GW data combination provides tight constraints on models with primordial non-Gaussianity (PNG), due to the predicted scale-dependent bias in PNG models on large scales. Assuming that the largest angular scales that LSST will probe are comparable to those in Stage III surveys ($\ell_{\rm min}\sim50$), the inclusion of next-generation GW measurements could improve constraints on the PNG parameter $f_{\rm NL}$ by up to a factor of $\simeq6.6$ compared to LSST alone, yielding $\sigma(f_{\rm NL})=8.5$. These results assume the expected capability of a network of Einstein Telescope-like GW observatories, with a detection rate of $10^6$ events/year. We investigate the sensitivity of our results to different assumptions about future GW detectors as well as different LSST analysis choices.

79 ASTRONOMY AND ASTROPHYSICS↗

Atmospheric Pressure Plasma Deposition of TiO2: A Review

Atmospheric pressure plasma (APP) deposition techniques are useful today because of their simplicity and their time and cost savings, particularly for growth of oxide films. Among the oxide materials, titanium dioxide (TiO2) has a wide range of applications in electronics, solar cells, and photocatalysis, which has made it an extremely popular research topic for decades. Here, we provide an overview of non-thermal APP deposition techniques for TiO2 thin film, some historical background, and some very recent findings and developments. First, we define non-thermal plasma, and then we describe the advantages of APP deposition. In addition, we explain the importance of TiO2 and then describe briefly the three deposition techniques used to date. We also compare the structural, electronic, and optical properties of TiO2 films deposited by different APP methods. Lastly, we examine the status of current research related to the effects of such deposition parameters as plasma power, feed gas, bias voltage, gas flow rate, and substrate temperature on the deposition rate, crystal phase, and other film properties. The examples given cover the most common APP deposition techniques for TiO2 growth to understand their advantages for specific applications. In addition, we discuss the important challenges that APP deposition is facing in this rapidly growing field.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗