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At least 505 records · Page 28

Absorption and scattering limits of silicon nitride integrated photonics in the visible spectrum

Visible-light photonic integrated circuits (PICs) promise scalability for technologies such as quantum information, biosensing, and scanning displays, yet extending large-scale silicon photonics to shorter wavelengths has been challenging due to the higher losses. Silicon nitride (SiN) has stood out as the leading platform for visible photonics, but the propagation losses strongly depend on the film’s deposition and fabrication processes. Current loss measurement techniques cannot accurately distinguish between absorption and surface scattering, making it difficult to identify the dominant loss source and reach the platform’s fundamental limit. Here we demonstrate an ultra-low loss, high-confinement SiN platform that approaches the limits of absorption and scattering across the visible spectrum. Leveraging the sensitivity of microresonators to loss, we probe and discriminate each loss contribution with unparalleled sensitivity, and derive their fundamental limits and scaling laws as a function of wavelength, film properties and waveguide parameters. Through the design of the waveguide cross-section, we show how to approach the absorption limit of the platform, and demonstrate the lowest propagation losses in high-confinement SiN to date across the visible spectrum. We envision that our techniques for loss characterization and minimization will contribute to the development of large-scale, dense PICs that redefine the loss limits of integrated platforms across the electromagnetic spectrum.

Corato-Zanarella, Mateus (ORCID:0000000327318046)↗

Plasmon Dynamics Driven by Aggregation of Tris(2,2′-bipyridine)ruthenium(II)-Functionalized Gold Nanoparticles Probed by XANES and Transient Absorption Spectroscopy

Energy conversion dynamics is critical for advancing next-generation photovoltaics, optoelectronics, and light-harvesting technologies. Noble metal plasmonic nanoparticles play a pivotal role as nanoscale electromagnetic confinement structures, driving photon-induced chemical reactions. In this study, we explore the effects of [Ru(bpy) 3 ] 2+ functionalization and aggregation on citrate-capped gold nanoparticles (AuNPs) of 40 and 100 nm diameters, focusing on molecule-plasmon interactions and their influence on electronic and energy dissipation properties. X-ray absorption near-edge spectroscopy (XANES) revealed that [Ru(bpy) 3 ] 2+ functionalization induces controlled aggregation without altering the oxidation state of gold. A more pronounced white-line intensity is observed in 40 nm AuNPs, consistent with greater s–p–d hybridization and a higher density of surface states, likely influenced by both nanoparticle size and aggregation. Transient absorption (TA) spectroscopy highlights faster electron–phonon relaxation dynamics in aggregated 40 nm nanoparticles, which is attributed to increased electron delocalization and more efficient coupling to the phonon bath. In contrast, 100 nm nanoparticles exhibit minimal changes due to a lower degree of aggregation. Interestingly, we observe that enhanced electron–phonon coupling in aggregated nanoparticles coincides with a slowing of electron–electron scattering. These observations suggest a competitive interplay between the two relaxation pathways, where enhanced energy transfer to the lattice in aggregated systems can suppress electronic thermalization. In conclusion, these findings underscore the critical role of nanoparticle size, aggregation, and molecule–surface interactions in modulating plasmonic dynamics and excited-state lifetimes and further provide valuable insights into designing tailored plasmonic systems with transformative potential for sensing, catalysis, and energy conversion.

36 MATERIALS SCIENCE↗

Suppressing parametric instabilities in direct-drive inertial-confinement-fusion plasmas using broadband laser light

It has long been recognized that broadband laser light has the potential to control parametric instabilities in inertial-confinement-fusion (ICF) plasmas. Here, we use results from laser-plasma-interaction simulations to estimate the bandwidth requirements for mitigating the three predominant classes of instabilities in direct-drive ICF implosions: cross-beam energy transfer (CBET), two-plasmon decay (TPD), and stimulated Raman scattering (SRS). We find that for frequency-tripled, Nd:glass laser light, a bandwidth of 8.5 THz can significantly increase laser absorption by suppressing CBET, while ∼13 THz is needed to mitigate absolute TPD and SRS on an ignition-scale platform. None of the glass lasers used in contemporary ICF experiments, however, possess a bandwidth greater than 1 THz and reaching larger values requires the use of an auxiliary broadening technique such as optical parametric amplification or stimulated-rotational-Raman scattering. An arguably superior approach is the adoption of an argon-fluoride (ArF) laser as an ICF driver. Besides having a broad bandwidth of ∼10 THz, the ArF laser also possesses the shortest wavelength (193 nm) that can scale to the high energy/power required for ICF—a feature that helps to mitigate parametric instabilities even further. We show that these native properties of ArF laser light are sufficient to eliminate nearly all CBET scattering in a direct-drive target and also raise absolute TPD and SRS thresholds well above those for broadband glass lasers. The effective control of parametric instabilities with broad bandwidth is potentially a “game changer” in ICF because it would enable higher laser intensities and ablation pressures in future target designs.

Bates, J. W. (ORCID:0000000188087240)↗

Hydrophilic, light active coating for membranes

A porous membrane provides enhanced filtration of pollutants and particles by coating the membrane with conformal thin films of doped titanium dioxide via atomic layer deposition or, alternatively, sequential infiltration synthesis. The membrane can either be organic or inorganic, and the doping of the membrane, usually with nitrogen, is an important feature that shifts the optical absorption of the TiO2 from the UV range into the visible-light range. This enables the use of lower energy light, including sunlight, to activate the photocatalytic function of the film. The coating described in the present invention is compatible with virtually any porous membrane and allows for precise tuning of the pore size with molecular precision. The present invention presents a new coating process and chemical structure that provides catalytic activity, strongly enhanced by light, to both mitigate fouling and break down various organic pollutants in the process stream.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Efficient light harvesting and photon sensing via engineered cooperative effects

Abstract Efficient devices for light harvesting and photon sensing are fundamental building blocks of basic energy science and many essential technologies. Recent efforts have turned to biomimicry to design the next generation of light-capturing devices, partially fueled by an appreciation of the fantastic efficiency of the initial stages of natural photosynthetic systems at capturing photons. In such systems extended excitonic states are thought to play a fundamental functional role, inducing cooperative coherent effects, such as superabsorption of light and supertransfer of photoexcitations. Inspired by this observation, we design an artificial light-harvesting and photodetection device that maximally harnesses cooperative effects to enhance efficiency. The design relies on separating absorption and transfer processes (energetically and spatially) in order to overcome the fundamental obstacle to exploiting cooperative effects to enhance light capture: the enhanced emission processes that accompany superabsorption. This engineered separation of processes greatly improves the efficiency and the scalability of the system.

42 ENGINEERING↗

Direct Evidence of Visible Light-Induced Homolysis in Chlorobis(2,9-dimethyl-1,10-phenanthroline)copper(II)

Developments in the field of photoredox catalysis that leveraged the long-lived excited states of Ir(III) and Ru(II) photosensitizers to enable radical coupling processes paved the way for explorations of synthetic transformations that would otherwise remain unrealized. While first row transition metal photocatalysts have not been as extensively investigated, valuable synthetic transformations covering broad scopes of olefin functionalization have been recently reported featuring photoactivated chlorobis(phenanthroline) Cu(II) complexes. In this study, the photochemical processes underpinning the catalytic activity of [Cu(dmp) 2 Cl]Cl (dmp = 2,9-dimethyl-1,10-phenanthroline) were studied. The combined results from static spectroscopic measurements and conventional photochemistry, ultrafast transient absorption, and electron paramagnetic resonance spin trapping experiments strongly support blue light (λ ex = 427 or 470 nm)-induced Cu–Cl homolytic bond cleavage in [Cu(dmp) 2 Cl] + occurring in <100 fs. On the basis of electronic structure calculations, this bond-breaking photochemistry corresponds to the Cl → Cu(II) ligand-to-metal charge transfer transition, unmasking a Cu(I) species [Cu(dmp) 2 ] + and a Cl atom, thereby serving as a departure point for both Cu(I)- or Cu(II)-based photoredox transformations. No net photochemistry was observed through direct excitation of the ligand-field transitions in the red (λ ex = 785 or 800 nm), and all combined experiments indicated no evidence of Cu–Cl bond cleavage under these conditions. As a result, the underlying visible light-induced homolysis of a metal–ligand bond yielding a one-electron-reduced photosensitizer and a radical species may form the basis for novel transformations initiated by photoinduced homolysis featuring in situ-formed metal–substrate adducts utilizing first row transition metal complexes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Short pulsewidth high repetition rate nanosecond transient absorption spectrometer

A high-sensitivity nanosecond to millisecond transient absorption spectrometer for measurements of miniscule signals under low excitation intensities includes an excitation source generating a >100 Hz, <5 ns pulsewidth excitation pulse for exciting a light absorbing sample, a probe light source for generating a high photon flux probe light beam producing an average irradiance greater than 1 μW m-2 nm-1 for measuring the transient absorption spectrum of the sample before and after excitation by the excitation source, a DC-coupled detector capable of measuring light for enabling synchronous measurement of both the transmission of the probe light beam and the change in transmission of the probe light beam between a signal with the excitation pulse present and a signal in the absence of the excitation pulse, and a digital oscilloscope with a trigger rearm time capable of collecting every trigger event at frequencies including 1MHz, for enabling sequential noise subtraction protocols.

Rimshaw, Adam↗

Submicron Thickness Characterization of Poly-Si Thin Films on Textured Surfaces by X-Ray Diffraction for Minimizing Parasitic Absorption in Poly-Si/SiO2 Passivating Contact Cells

Poly-Si/SiO2 passivating contacts have shown great potential for industry-relevant next-generation solar cells. Previous work has demonstrated an improved Jsc from dry reactive ion etching in an SF6 environment, using front metal grids as a self-aligned mask. Here, we show an effective method to measure the front poly-Si thickness on an alkaline textured surface using X-ray diffraction. The calculated thicknesses are compared with cross-section SEM analysis and Quokka simulation. We show that by thinning the front poly-Si from 200 nm to 60 nm, Jsc increases by 2.4 mA/cm2, leading to an absolute efficiency gain of 1.73%. Finally, we discuss possible reasons for the premature loss of passivation before the removal of all poly-Si.

41 EE - Solar Energy Technologies Office (EE-4S)↗

Autonomous light management system for a window and method of controlling light transmission

An autonomous light management system for a window includes an electrochromic film stack comprising an electrochromic layer on a first transparent electrode, an ion storage layer on a second transparent electrode, and an electrolyte sandwiched between the ion storage and electrochromic layers. The electrochromic film stack exhibits a transmissive state or an absorptive state depending on charging or discharging of the electrochromic layer. The light management system further comprises an array of power units disposed on a front surface of the electrochromic film stack, where each power unit comprises at least one solar microcell. Collectively, the solar microcells cover an area no greater than about 6% of a total area of the front surface. The array of power units is configured to control the charging and discharging of the electrochromic layer, thereby manipulating light transmission through the electrochromic film stack.

Yoder, Mikayla A.↗

Measurement of anti- 3 He nuclei absorption in matter and impact on their propagation in the Galaxy

In our Galaxy, light antinuclei composed of antiprotons and antineutrons can be produced through high-energy cosmic-ray collisions with the interstellar medium or could also originate from the annihilation of dark-matter particles that have not yet been discovered. On Earth, the only way to produce and study antinuclei with high precision is to create them at high-energy particle accelerators. Although the properties of elementary antiparticles have been studied in detail, the knowledge of the interaction of light antinuclei with matter is limited. We determine the disappearance probability of 3 $\overline{He}$ when it encounters matter particles and annihilates or disintegrates within the ALICE detector at the Large Hadron Collider. We extract the inelastic interaction cross section, which is then used as an input to the calculations of the transparency of our Galaxy to the propagation of 3 $\overline{He}$ stemming from dark-matter annihilation and cosmic-ray interactions within the interstellar medium. For a specific dark-matter profile, we estimate a transparency of about 50%, whereas it varies with increasing 3 $\overline{He}$ momentum from 25% to 90% for cosmic-ray sources. The results indicate that 3 $\overline{He}$ nuclei can travel long distances in the Galaxy, and can be used to study cosmic-ray interactions and dark-matter annihilation.

79 ASTRONOMY AND ASTROPHYSICS↗

Trends in relativistic laser–matter interaction: the promises of structured light

Time and space envelope, frequency and wavelength distributions, polarization, and phase are quantities that define the properties of laser light. Controlling them opens up strategies for manipulating the properties of atoms in various media. At relativistic intensity, matter is rapidly transformed into a plasma state, which is modifying the laser’s propagation, its absorption enabling the generation of intense magnetic and electric fields. In this context, structured light presents exciting, promising, and challenging opportunities for research. This review article aims to explain the concepts of structured light, their applications to real experiments at relativistic intensities, practical considerations, and some scientific perspectives.

47 OTHER INSTRUMENTATION↗

Photophysical properties of zero-dimensional perovskites studied by PBE0 and GW+BSE methods

Due to the exceptional photophysical properties and great potential applications in solid state lighting, zero-dimensional halide perovskites with broadband emitting have recently attracted much attention. In this work, to reveal the origin of the broadband absorption and emission spectra of 0D (C 4 N 2 H 14 Br) 4 SnBr x I 6-x (x = 3), the ground state and exciton dynamics properties have been studied by hybrid PBE0 functional and the GW+BSE method. Different self-trapped excitons (STEs) are obtained, and their emission energies by PBE0 are consistent well with experimental data. By considering the vibrational broadening of emission, our calculated full width at half maximum of emission accords well with the experiment. The absorption of free exciton and STEs is also calculated by considering the quasiparticle and excitonic effect. Our results show that these light-induced trapped states can be observed by experiments, as confirmed in other similar systems by the femtosecond transient absorption spectra.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Transition Metal Dichalcogenides: Making Atomic‐Level Magnetism Tunable with Light at Room Temperature

Abstract The capacity to manipulate magnetization in 2D dilute magnetic semiconductors (2D‐DMSs) using light, specifically in magnetically doped transition metal dichalcogenide (TMD) monolayers ( M ‐doped TX 2 , where M = V, Fe, and Cr; T = W, Mo; X = S, Se, and Te), may lead to innovative applications in spintronics, spin‐caloritronics, valleytronics, and quantum computation. This Perspective paper explores the mediation of magnetization by light under ambient conditions in 2D‐TMD DMSs and heterostructures. By combining magneto‐LC resonance (MLCR) experiments with density functional theory (DFT) calculations, we show that the magnetization can be enhanced using light in V‐doped TMD monolayers (e.g., V‐WS 2 , V‐WSe 2 ). This phenomenon is attributed to excess holes in the conduction and valence bands, and carriers trapped in magnetic doping states, mediating the magnetization of the semiconducting layer. In 2D‐TMD heterostructures (VSe 2 /WS 2 , VSe 2 /MoS 2 ), the significance of proximity, charge‐transfer, and confinement effects in amplifying light‐mediated magnetism is demonstrated. We attributed this to photon absorption at the TMD layer that generates electron–hole pairs mediating the magnetization of the heterostructure. These findings will encourage further research in the field of 2D magnetism and establish a novel design of 2D‐TMDs and heterostructures with optically tunable magnetic functionalities, paving the way for next‐generation magneto‐optic nanodevices.

36 MATERIALS SCIENCE↗

The Effect of Physically Based Ice Radiative Processes on Greenland Ice Sheet Albedo and Surface Mass Balance in E3SM

Abstract A significant portion of surface melt on the Greenland Ice Sheet (GrIS) is due to dark ice regions in the ablation zone, where solar absorption is influenced by the physical properties of the ice, light absorbing constituents (LACs), and the overlying crustal surface or melt ponds. Earth system models (ESMs) typically prescribe the albedo of ice surfaces as a constant value in the visible and near‐infrared spectral regions. This work advances ESM ice radiative transfer modeling by (a) incorporating a physically based radiative transfer model (SNow, ICe and Aerosol Radiation model Adding‐Doubling Version 4; SNICAR‐ADv4) into the Energy Exascale Earth System Model (E3SM), (b) determining spatially and temporally varying bare ice physical properties over the GrIS ablation zone from satellite observations to inform SNICAR‐ADv4, and (c) assessing the impacts on simulated GrIS albedo and surface mass balance associated with modeling of more realistic bare ice albedo. GrIS‐wide bare ice albedo in E3SMv2 is overestimated by ∼4% in the visible and ∼7% in the near‐infrared wavelengths compared to the Moderate Resolution Imaging Spectroradiometer. Our bare ice physical property retrieval method found that LACs, ice crustal surfaces, and melt ponds reduce visible albedo by 30% in the bare ice region of the GrIS ablation zone. The realistic bare ice albedo reduces surface mass balance by ∼145 Gt, or 0.4 mm of sea‐level equivalent between 2000 and 2021 compared to the default E3SM. This work highlights the importance of simulating bare ice albedo accurately and realistically to improve our ability to quantify changes in the GrIS surface mass and radiative energy budgets.

58 GEOSCIENCES↗

Time-resolved 3D imaging of two-phase fluid flow inside a steel fuel injector using synchrotron X-ray tomography

The multiphase flow inside a diesel injection nozzle is imaged using synchrotron X-rays from the Advanced Photon Source at Argonne National Laboratory. Through acquisitions performed at several viewing angles and subsequent tomographic reconstruction, in-situ 3D visualization is achieved for the first time inside a steel injector at engine-like operating conditions. The morphology of the internal flow reveals strong flow separation and vapor-filled cavities (cavitation), the degree of which correlates with the nozzle's asymmetric inlet corner profile. Micron-scale surface features, which are artifacts of manufacturing, are shown to influence the morphology of the resulting liquid-gas interface. The data obtained at 0.1 ms time resolution exposes transient flow features and the flow development timescales are shown to be correlated with in-situ imaging of the fuel injector's hydraulically-actuated valve (needle). As more than 98.5% of the X-ray photon flux is attenuated within the steel injector body itself, we are posed with a unique challenge for imaging the flow within. Time-resolved imaging under these low-light conditions is achieved by exploiting both the refractive and absorptive properties of X-ray photons. The data-processing strategy converted these images with a signal-to-noise ratio of similar to 10 into a meaningful dataset for understanding internal flow and cavitation in a nozzle of diameter 200 mu m enclosed within 1-2 millimeters of steel.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Visualizing plasmons and ultrafast kinetic instabilities in laser-driven solids using X-ray scattering

Ultra-intense lasers that ionize atoms and accelerate electrons in solids to near the speed of light can lead to kinetic instabilities that alter the laser absorption and subsequent electron transport, isochoric heating, and ion acceleration. These instabilities can be difficult to characterize, but X-ray scattering at keV photon energies allows for their visualization with femtosecond temporal resolution on the few nanometer mesoscale. Here, we perform such experiment on laser-driven flat silicon membranes that shows the development of structure with a dominant scale of 60 nm in the plane of the laser axis and laser polarization, and 95 nm in the vertical direction with a growth rate faster than 0.1 fs -1 . Combining the XFEL experiments with simulations provides a complete picture of the structural evolution of ultra-fast laser-induced plasma density development, indicating the excitation of plasmons and a filamentation instability. Particle-in-cell simulations confirm that these signals are due to an oblique two-stream filamentation instability. These findings provide new insight into ultra-fast instability and heating processes in solids under extreme conditions at the nanometer level with possible implications for laser particle acceleration, inertial confinement fusion, and laboratory astrophysics.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Double photoionization of atomic oxygen: Feshbach resonances in the two-electron continuum

In this work, we describe a joint experimental and theoretical investigation on oxygen double photoionization—the emission of two electrons from atomic oxygen following single photon absorption. High-resolution experimental measurements were performed at the Advanced Light Source, revealing sharp resonance structure superimposed on the more familiar Wannier-like, nearly-linear background. These resonance features are attributed to ionization-plus-excitation Feshbach resonances embedded in the double ionization continuum, doubly-excited states that lie above the double-ionization threshold. Such features are absent in the double photoionization cross section of He, or other quasi-two-electron systems, for which the doubly-ionized atomic core remains inert. For a corresponding theoretical analysis, the R-matrix with pseudostates (RMPS) method was invoked by calculating final-state, two-electron resonances-plus-continua wavefunctions and corresponding single-photon absorption cross sections. Overall agreement is found in the direct, background double photoionization cross section. However, the RMPS method, using a small basis due to practical computational limitations, was unable to reproduce quantitatively the smooth background or the sharper resonance features observed in the measurements, showing instead large-scale oscillations about the experimental background, and characteristic pseudoresonance jitter, associated with an insufficient convergence of the pseudostate representation to the true two-electron infinite series of Feshbach resonances embedded in the two-electron continuum. The prominent resonance structure observed highlights the need to consider multiple excitation processes in atoms more complex than He or quasi-two-electron systems.

74 ATOMIC AND MOLECULAR PHYSICS↗