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DOE OSTI2023

Lattice Mie resonances and emissivity enhancement in mid-infrared iron pyrite metasurfaces

High-refractive-index antennas with characteristic dimensions comparable to wavelength have a remarkable ability to support pronounces electric and magnetic dipole resonances. Furthermore, periodic arrangements of such resonant antennas result in narrow and strong lattice resonances facilitated by the lattice. We design iron pyrite antennas operating in the mid-infrared spectral range due to the material’s low-energy bandgap and high refractive index. We utilize Kirchhoff’s law, stating that emissivity and absorptance are equal to each other in equilibrium, and we apply it to improve the thermal properties of the iron pyrite metasurface. Through the excitation of collective resonances and manipulation of the antenna lattice’s period, we demonstrate our capacity to control emissivity peaks. These peaks stem from the resonant excitation of electric and magnetic dipoles within proximity to the Rayleigh anomalies. In the lattice of truncated-cone antennas, we observe Rabi splitting of electric and magnetic dipole lattice resonances originating from the antennas’ broken symmetry. We demonstrate that the truncated-cone antenna lattices support strong out-of-plane magnetic dipole lattice resonances at oblique incidence. We show that the truncated-cone antennas, as opposed to disks or cones, facilitate a particularly strong resonance and bound state in the continuum at the normal incidence. Our work demonstrates the effective manipulation of emissivity peaks in iron pyrite metasurfaces through controlled lattice resonances and antenna design, offering promising avenues for mid-infrared spectral engineering.

Islam, Md Sakibul↗

DOE OSTI2021

Group-velocity-dispersion engineering of tantala integrated photonics

Designing integrated photonics, especially to leverage Kerr-nonlinear optics, requires accurate and precise knowledge of the refractive index across the visible to infrared spectral ranges. Tantala ( T a 2 O 5 ) is an emerging material platform for integrated photonics and nanophotonics that offers broadband ultralow loss, moderately high nonlinearity, and advantages for scalable and heterogeneous integration. We present refractive index measurements on a thin film of tantala, and we explore the efficacy of this data for group-velocity-dispersion (GVD) engineering with waveguide and ring-resonator devices. In particular, the observed spectral extent of supercontinuum generation in fabricated waveguides and the wavelength dependence of free spectral range (FSR) in optical resonators provide a sensitive test of our integrated photonics design process. Our work opens up new design possibilities with tantala, including with octave-spanning soliton microcombs.

Black, Jennifer A.↗

DOE OSTI2023

Influence of defects on the femtosecond laser damage resistance of multilayer dielectric gratings

Multilayer dielectric (MLD) gratings with high diffraction efficiency and a high laser-induced damage (LID) threshold for pulse compressors are key to scaling the peak and average power of chirped pulse amplification lasers. However, surface defects introduced by manufacturing, storage, and handling processes can reduce the LID resistance of MLD gratings and impact the laser output. The underlying mechanisms of such defect-initiated LID remain unclear, especially in the femtosecond regime. In this Letter, we model dynamic processes in interactions of a 20-fs near-infrared (NIR) laser pulse and a MLD grating design in the presence of cylindrically symmetrical nodules and particle contaminants and cracks at the surface. Utilizing a dynamic model based on a 2D finite difference in time domain (FDTD) field solver coupled with photoionization, electron collision, and refractive index modification, we study the simulation results for the damage site distribution initiated by defects of various types and sizes and its impact on the LID threshold of the grating design.

Zhang, Simin (ORCID:0000000174948230)↗

DOE OSTI2020

Adiabatic frequency shifting in epsilon-near-zero materials: the role of group velocity

The conversion of a photon’s frequency has long been a key application area of nonlinear optics. It has been discussed how a slow temporal variation of a material’s refractive index can lead to the adiabatic frequency shift (AFS) of a pulse spectrum. Such a rigid spectral change has relevant technological implications, for example, in ultrafast signal processing. Here, we investigate the AFS process in epsilon-near-zero (ENZ) materials and show that the frequency shift can be achieved in a shorter length if operating in the vicinity of R e { ε <#comment/> r } = 0 . We also predict that, if the refractive index is induced by an intense optical pulse, the frequency shift is more efficient for a pump at the ENZ wavelength. Remarkably, we show that these effects are a consequence of the slow propagation speed of pulses at the ENZ wavelength. Our theoretical predictions are validated by experiments obtained for the AFS of optical pulses incident upon aluminum zinc oxide thin films at ENZ. Our results indicate that transparent metal oxides operating near the ENZ point are good candidates for future frequency conversion schemes.

36 MATERIALS SCIENCE↗

DOE OSTI2024

2D material platform for overcoming the amplitude–phase tradeoff in ring resonators

Compact and high-speed electro-optic phase modulators play a vital role in various large-scale applications including optical computing, quantum and neural networks, and optical communication links. Conventional electro-refractive phase modulators such as silicon (Si), III-V and graphene on Si suffer from a fundamental tradeoff between device length and optical loss that limits their scaling capabilities. High-finesse ring resonators have been traditionally used as compact intensity modulators, but their use for phase modulation has been limited due to the high insertion loss associated with the phase shift. Here, we show that high-finesse resonators can achieve a strong phase shift with low insertion loss by simultaneous modulation of the real and imaginary parts of the refractive index, to the same extent, i.e., Δ n Δ k ∼1. To implement this strategy, we demonstrate an active hybrid platform that combines a low-loss SiN ring resonator with 2D materials such as graphene and transition metal dichalcogenide [tungsten disulphide (WSe 2 )], which induces a strong change in the imaginary and real parts of the index. Our platform consisting of a 25 µm long Gr-Al 2 O 3 -WSe 2 capacitor embedded on a SiN ring of 50 µm radius (∼8% ring coverage) achieves a continuous phase shift of (0.46±0.05) π radians with an insertion loss (IL) of 3.18±0.20 dB and a transmission modulation (Δ T Ring ) of 1.72±0.15dB at a probe wavelength ( λ p ) of 1646.18 nm. We find that our Gr-Al 2 O 3 -WSe 2 capacitor exhibits a phase modulation efficiency ( V π 2 ⋅ L ) of 0.530±0.016V⋅cm and can support an electro-optic bandwidth of 14.9±0.1GHz. We further show that our platform can achieve a phase shift of π radians with an IL of 5 dB and a minimum Δ T of 0.046 dB. We demonstrate the broadband nature of the binary phase response, by measuring a phase shift of (1.00±0.10) π radians, with an IL of 5.20±0.31dB and a minimal Δ T Ring of 0.015±0.006dB for resonances spanning from 1564 to 1650 nm. This SiN–2D hybrid platform provides the design for compact and high-speed reconfigurable circuits with graphene and transition metal dichalcogenide (TMD) monolayers that can enable large-scale photonic systems.

Datta, Ipshita (ORCID:0000000318842882)↗

DOE OSTI2024

Low loss fiber-coupled volumetric interconnects fabricated via direct laser writing

Photonic integrated circuits (PICs) are vital for high-speed data transmission. However, optical routing is limited in PICs composed of only one or a few stacked planes. Further, coupling losses must be low in deployed systems. Previously, we developed the subsurface controllable refractive index via beam exposure (SCRIBE) technique to write accurate 3D gradient refractive index (GRIN) profiles within a mesoporous silica scaffold. Here, we apply SCRIBE to fabricate low loss, broadband, polarization insensitive, fiber-coupled, single-mode volumetric interconnects that include waveguides traversing arbitrary 3D paths. By seamlessly integrating mode-matching subsurface lenses and GRIN waveguide tapers, calibrating for positional writing errors, implementing multipass exposure, automating alignment, and switching to antireflection coated fibers, we reduced the insertion loss for a fiber-PIC-fiber interconnect from 50 to 2.14 dB, or 1.47 dB, excluding the fiber array’s loss. Further, we establish an upper bound of 0.45 dB loss per coupler. We report quality factors of 27,000 and 77,000 and bending losses of 6 and 3 dB/cm for 15 and 30 µm radii microrings, respectively. We also demonstrate Bézier escalators, polarization-rotating and polarization-splitting interconnects, and a seven-channel 25 µm pitch volumetric interconnect. The SCRIBE platform presents a clear path toward realizing 3D PICs with unique functionality.

Optics↗

DOE OSTI2021

High-temperature stable FBGs fabricated by a point-by-point femtosecond laser inscription for multi-parameter sensing

A high-temperature resistant fiber Bragg grating (FBG) with pronounced cladding modes is fabricated using a simple, fast, and flexible point-by-point femtosecond laser inscription. Cladding modes of different orders exhibit various sensitivities to changes in refractive index of the surrounding medium and temperature, while the Bragg wavelength is only dependent on the ambient temperature. By combining the resonance of cladding modes and the Bragg resonance, measurement of variations of temperature and surrounding refractive index can be achieved. Survivability of the cladding modes and the core mode in the fabricated FBG at elevated temperatures up to 1000°C is demonstrated.

Zhu, Chen (ORCID:0000000232567330)↗

DOE OSTI2022

Temporal and spatial tuning of optical constants in praseodymium doped ceria by electrochemical means

Abstract Temporal and spatial tuning of the refractive index of optical thin films is desired for flat optics applications. The redistribution of mobile ions in mixed ionic-electronic conductors (MIEC) has been demonstrated to serve as a viable means for achieving optical tuning down to the nanoscale. Here we studied the dynamic range of the optical tuning achievable in the refractive index, in the MIEC oxide – Pr x Ce 1− x O 2− δ (PCO), for x = 0.1, 0.2 and 0.4, at 500 °C, by in-situ spectrophotometry. Significant increases in the modulation of both the imaginary and real optical constants in the visible and the adjacent spectra were obtained for increased doping levels. Device employing an electrochemical titration method was implemented to modulate the oxygen concentration, and thereby the optical transmission of PCO. Incorporation of a patterned top electrode allowed for the demonstration of spatial control of PCO thin film properties by in-situ video imaging of the optical switching process. The electrochemically induced optical state is shown to remain non-volatile upon quenching the device to room temperature under applied bias.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Single‐photon emitters in PECVD‐grown silicon nitride films: from material growth to photophysical properties

Abstract Silicon nitride (SiN) is a key material for quantum photonics due to its wide transparency window, high refractive index, low optical losses, and semiconductor foundry compatibility. We study the formation of single‐photon emitters in SiN films grown by plasma‐enhanced chemical vapor deposition (PECVD), exploring their photophysical properties and dependence on growth conditions. Emitters were observed across the entire range of nitrogen‐to‐silicon precursor ratios, from silicon‐rich to nitrogen‐rich conditions, enabled by the low background fluorescence. We demonstrate single‐photon emitters in SiN films with a higher refractive index (1.8–1.9) compared to our previous reports (∼1.7). Notably, nitrogen‐rich, thinner films yield particularly bright emitters with shorter emission lifetimes, likely due to more efficient annealing. Silicon‐rich SiN films exhibit red‐shifted emission, suggesting that composition may provide a mechanism for wavelength tuning. These findings establish the feasibility of emitters formation in foundry standard PECVD tools, advancing the scalability and lab‐to‐fab transition of SiN‐based quantum photonic technologies.

Materials Science↗

DOE OSTI2020

Development and Validation of Physics-Based Sub-Models of High-Pressure Supercritical Fuel Injection at Diesel Conditions Insert

The project sought to develop and validate accurate, physics-based, numerical submodels and implement them in computational fluid dynamics (CFD) software codes to enable accurate predictions of diesel sprays at pressures higher than the current systems. The combined experimental-computational effort has four main objectives: (1) acquire spatially and temporally resolved scalar measurements of fuel-oxidizer mixing in the near field of the fuel jet, (2) develop software modules to calculate thermo-physical properties of diesel surrogates and their mixtures with oxidizer of interest in real-gas operating regime, (3) integrate the real-fluid model into a commercial and an open-source CFD code to simulate fuel-air mixing in high-pressure diesel sprays, and (4) assess the robustness, accuracy, and uncertainty of the integrated CFD solvers in computing diesel sprays. Project accomplishments are consistent with the original goals of the project. Although we acquired spatially and temporally resolved scalar measurements, they were limited to refractive index difference and not to thermodynamic properties such as temperature and equivalence ratio. However, we successfully developed the theoretical background needed to acquire such measurements at diesel conditions and demonstrated the capability of the RSD for scalar measurements in a canonical turbulent jet flow replicating features of the diesel jet. Additional work will be needed to implement these procedures at high-pressure, high-temperature engine-like conditions of the CPFR. Mainly, we did not anticipate the need to find the liquid boundary and its statistical features or the state relationships between refractive index and thermodynamic properties, assuming the widely known Dale-Gladstone equation would suffice. Still, efforts devoted to these tasks were essential to fulfil the goals of the project and serves as the foundation on which many of the conclusions and key contributions of this project are based. Further assessment and application of the developed CFD codes is recommended to fully realize the benefits of this research.

33 ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2021

Plasma Photonics: Manipulating Light Using Plasmas (Full Technical Final Report)

In this LDRD, we made significant advances on multiple fronts on the investigation and design of plasma-based optical structures to manipulate light at extreme intensities. We have unveiled new fundamental properties of laser-plasma interaction that were leveraged to introduce transformative applications. We first investigated new ways to generate high-amplitude plasma-based optical structures, based on the auto-resonance mechanism in order to produce refractive structures in plasmas. New insights into the interaction of such plasma structures with light waves allowed us to propose new methods for polarization manipulation and control for high-intensity lasers in the nonlinear regime, i.e. allowing the manipulation of an intense laser via its interaction with a less intense “control” laser beam in plasmas. Another application that we demonstrated experimentally is the capability to manipulate the velocity of light waves in plasmas by tailoring its refractive index; we reported the first demonstration of “slow light” and supra-luminal light propagation in plasmas. We also developed a new technological concept that would allow the probing of the type of plasma structures investigated in such applications, using high-bandwidth laser probing [Ludwig Phys. Plasmas 2019]. Finally, first steps were taken towards the demonstration of a plasma-based amplifier and compressor for the National Ignition Facility, in order to achieve powers equal of greater than those delivered by the Advanced Radiographic Capability (ARC). This technique uses a plasma-based grating acting like a compressor and amplifier, which could potentially compress and amplify an 88 ps, 56 J beam from the National Ignition Facility to <10 ps and hundreds of J.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

A novel approach to characterize the full spectrum and radiative properties of aerosols

Organic aerosols play a significant role in the absorption and radiative budget of the atmosphere, but current modeling approaches do not adequately capture the photo-chemical and oxidative bleaching that occurs during their lifetimes. Most climate models inaccurately assume constant optical properties of these particles, therefore leading to errors in their predictions. In this study we present an approach to better parameterize the optical properties of atmospheric aerosols, including brown carbon (BrC). Using thin-film spectrometry, the full spectrum of reflectivity and emissivity was used to calculate the complex refractive index for multiple species of organic aerosols. This is in contrast to previous techniques which only probe single wavelengths. Since BrC is a complex molecular mixture, we initially focused on single species absorption using four molecular surrogates. Dye-doped polyacrylic-acid thin-films were prepared on glass slides and compared to an aerosolized collection method. Verification of the collection method will open the door to characterizing the complex refractive index of smoke and ambient aerosol.

58 GEOSCIENCES↗

DOE OSTI2022

Aero-Optics of Hypersonic Turbulent Boundary Layers

Aero-optics refers to optical distortions due to index-of-refraction gradients that are induced by aerodynamic density gradients. At hypersonic flow conditions, the bulk velocity is many times the speed of sound and density gradients may originate from shock waves, compressible turbulent structures, acoustic waves, thermal variations, etc. Due to the combination of these factors, aero-optic distortions are expected to differ from those common to sub-sonic and lower super-sonic speeds. This report summarizes the results from a 2019-2022 Laboratory Directed Research and Development (LDRD) project led by Sandia National Laboratories in collaboration with the University of Notre Dame, New Mexico State University, and the Georgia Institute of Technology. Efforts extended experimental and simulation methodologies for the study of turbulent hypersonic boundary layers. Notable experimental advancements include development of spectral de-aliasing techniques for highspeed wavefront measurements, a Spatially Selective Wavefront Sensor (SSWFS) technique, new experimental data at Mach 8 and 14, a Quadrature Fringe Imaging Interferometer (QFII) technique for time-resolved index-of-refraction measures, and application of QFII to shock-heated air. At the same time, model advancements include aero-optic analysis of several Direct Numerical Simulation (DNS) datasets from Mach 0.5 to 14 and development of wall-modeled Large Eddy Simulation (LES) techniques for aero-optic predictions. At Mach 8 measured and predicted root mean square Optical Path Differences agree within confidence bounds but are higher than semi-empirical trends extrapolated from lower Mach conditions. Overall, results show that aero-optic effects in the hypersonic flow regime are not simple extensions from prior knowledge at lower speeds and instead reflect the added complexity of compressible hypersonic flow physics.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Reducing module soiling with scalable and robust photocatalytic coatings

The air-glass interface at the front of a photovoltaic (PV) module reflects approximately 4% of incident light, decreasing the potential power output of the module by the same amount. Today’s modules reduce this loss by adding a low-refractive-index (1.25-1.30) SiO2 coating to the sunward side of the module glass; this antireflection coating recovers approximately 3% of the 4% light that would otherwise be lost. While such antireflection coatings work very well on clean, new modules, they do not inhibit soiling—the accumulation of soilants such as dust, pollen, soot, or other foreign material—on the module glass, and soilants reflect and scatter incident light. An improved coating would serve provide not only an antireflection effect, but also an anti-soiling effect. The goal of this project was to develop such a coating and provide a path for it to be manufactured in the U.S. The project successfully designed and fabricated coatings that provided >3% transmittance gain compared to bare glass (matching the performance of commercial antireflection coatings) and displayed anti-soiling behavior in standard laboratory soiling effects. This was achieved by using a Swift Coat proprietary coating deposition technique, aerosol impact-driven assembly (AIDA), to control the porosity and thus refractive index of coatings of photocatalytic materials—such as TiO2—that would otherwise increase (instead of decrease) reflection. These combined antireflection/anti-soiling coatings passed PV industry standard module reliability tests as well as coating-specific abrasion tests, showing that they have the durability needed for decades in the field. Swift Coat scaled the AIDA hardware and deposition process to make mini-modules that were monitored for nearly two years during field tests administered by a third party, as well as demonstrated scaling to the widths of full-sized modules. The fielded mini-modules outperformed reference modules (with commercial antireflection coatings) in two locations, providing a 1% absolute average performance boost and larger increases during periods of heavier soiling. Swift Coat’s cost analysis indicated a coating manufacturing cost below the sales price of today’s antireflection coatings. More than five module manufacturers sampled and assessed the coatings, and three provided letters of support. The coating developed in this project increases the energy output of PV modules, thereby decreasing the cost per kilowatt-hour of solar energy generated. Cheaper solar electricity benefits the public by accelerating the transition to a stable, affordable, carbon-free energy economy. In addition, for select applications in which PV modules are highly visible—such as on residential rooftops—the coating provides an aesthetic benefit because it stays cleaner than today’s modules. Finally, Swift Coat and its prospective customers are U.S. companies, and successful commercialization of this technology will provide U.S. jobs and a secure solar supply chain.

14 SOLAR ENERGY↗

DOE OSTI2025

Extinction of Laser Light Due to Arctic Haze Final Campaign Report

Recent changes in emission patterns may have altered the historical stability of light attenuation strengths within the Arctic and, more specifically, the polar dome. While there have been decades of past and ongoing research on how atmospheric constituents, such as aerosols, affect light absorption, the bulk of this work is focused on the visible region. In recent years, there has been renewed interest in understanding laser light propagation at wavelengths such as 1 and 2 µm in this area. There is a need to evaluate how specific environmental parameters affect the propagation of light in this wavelength region, in particular: the extinction, scattering, and absorption coefficients, and how they relate to particle concentration; cn 2 and refractive index variations. Seasonally dependent variations in particle concentrations and compositions introduce different absorption and scattering characteristics that, in conjunction with varying temperatures, index-of-refraction variations, and wind, can result in laser beam focus and irradiance degradation. Understanding the fundamental influence of these parameters with respect to the propagation of light across a wide spectral band could lead to new insights about the minimal required datastreams required to provide accurate light propagation forecasting.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Systematic study of radioluminescence and light propagation effects in scintillating nanoguide materials

Nanoguide optical waveguides are thermally processed materials based on polymers that have different refractive indices. Scintillating versions of these materials have been under development since 2019 and feature PMMA as the low refractive index constituent and Organic Glass Scintillator-polymer blends as the high index component. Characterization efforts to date have focused on the functional characteristics of nanoguide pertaining to its envisioned use in high-resolution transmission radiography applications.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Explosive Soot Challenge (Final Report)

This project assembled a broad ensemble of modeling and experimentation tools to study the morphological and optical properties of detonation soots in explosive fireballs. A gram-scale hemispherical high explosive was studied in a low-pressure controlled environment using in-situ experimentation with diffusely illuminated visible absorption spectroscopy, particle sizing through light scattering techniques, and post-test collections with subsequent morphological analysis. Hydrocode modeling was performed to replicate the detonation flow observations, and subsequent aerosol kinetics models provided particle size distributions and extinction coefficients from the hydrocode results. Experimentally observed soot morphologies agreed with expectation from the literature - a bimodal distribution was found, brought upon by the particles growing to a size where their inertia and fluid wakes are non-negligible. The aerosol kinetics model did not replicate the observed bimodal size distribution for lack of a coagulation kernel to represent the behavior. To recover particulate optical properties, a spectrally resolved absorption spectroscopy method termed Spectral diffuse back-illuminated extinction imaging (SBI-EI) was developed and implemented on two explosive types. Inverting the absorption spectra using a Kramers-Kronig consistent method yielded the complex index of refraction for the soots produced by the explosives. This method resulted in an unrealistic index of refraction for one of the two explosives, and this is suspected to be due to the model neglecting scattering brought upon by the large particle sizes observed. In addition to the core work, three additional studies were performed in parallel. These investigated the impact of scattering on diffuse absorption spectroscopy, studied how soots oxidate and sublimate in a well-controlled shock tube, and laid the theoretical groundwork for a new collision kernel to replicate the bimodal size distribution from the observations. Summaries of these efforts are included at the end of this report.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

DOE OSTI2026

How Do You Hear a Quantum Computer Whisper?

Quantum transduction is the process of upconverting microwave quantum signals into optical signals to develop quantum networks through optical fibers outside the dilution refrigerator, enabling connections between quantum technologies on the quantum internet. In this project, upconversion is achieved by directing an optical laser and the microwave quantum signal into an electro-optic bulk crystal. The crystal is housed within a Superconducting Radio Frequency (SRF) cavity designed to maximize the overlap between the microwave field and the crystal volume. In the presence of microwaves, the refractive index of the crystal changes through the Pockels effect. This change in refractive index modifies the propagation of the optical field within the crystal, allowing the quantum information carried by the microwave field to be transferred to the optical field. This study focuses on coupling laser light from suspended waveguide chips into the whispering-gallery modes (WGMs) of the crystal to enable transduction. The coupling efficiency between the optical field in the suspended waveguide and the WGM depends on the position of the laser spot on the crystal. To address this challenge, a feedback-based algorithm is being developed to fine-tune the waveguide position so that the optical signal is coupled efficiently into the crystal. After passing through the crystal, the optical signal is detected by a photodiode connected to an oscilloscope. The algorithm evaluates the coupling quality and iteratively adjusts the waveguide position to maximize coupling efficiency. The expected outcome is an automated waveguide alignment method that improves optical coupling and enables more efficient microwave-to-optical quantum transduction.

Karanastasis, Mihael [Fermilab]↗