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DOE OSTI2024

Advances in Molecular Beam Epitaxy Growth of Ultra-Wide Bandgap Ga2O3 Based Alloys

Gallium oxide (Ga2O3) is an emerging ultra-wide bandgap semiconductor material that has attracted attention for its potential to outperform existing SiC and GaN based devices operating at high breakdown voltages and high temperature. Isovalent alloying of In and Al in Ga2O3 provides the ability to engineer bandgap energy and strain of the material. Alloying with Al increases the bandgap energy and the theoretically achievable Baliga's figure of merit, a key measure of a material's ultimate performance limits for high power switching devices. Alloying with In introduces compressive strain and can be used to counteract the tensile strain of Al incorporation. The resulting (AlxGa1-x-yIny)2O3 alloy can be lattice-matched to commercially available Ga2O3 wafers and has a tunable bandgap energy greater than that of Ga2O3, 4.76 eV. Such lattice-matched material can be grown arbitrarily thick without the detrimental effects of elastic strain and relaxation, making it suitable for high voltage diodes and transistors. However, efforts to synthesize isovalent alloys are complicated by their tendency to phase separate into corundum Al2O3 or bixbyite In2O3. Literature reports of the quaternary (AlxGa1-x-yIny)2O3 are limited to <1% unintentional indium incorporation in In-catalyzed (AlxGa1-x)2O3. The primary limitation to quaternary growth is the limited incorporation of indium at elevated growth temperatures. This limited incorporation is due to both the volatility of indium oxide and Al and Ga cation exchange reactions which replace indium in In2O3. We report on the development of a novel high-throughput molecular beam epitaxy (MBE) technique to screen the growth conditions for the ternary alloy (InyGa1-y)2O3, and the application of these findings to the first successful synthesis of phase pure monoclinic (AlxGa1-x-yIny)2O3 by MBE. By leveraging the unique sub-oxide chemistry of Ga2O3 and in-situ monitoring of crystal properties by reflection high-energy electron diffraction (RHEED), a cyclical growth and etch-back method is developed and applied to rapidly characterize the (InyGa1-y)2O3 growth space. This cyclical method provides approximately 10x increase in experimental throughput and up to 46x improvement in Ga2O3 substrate utilization. Appropriate growth conditions for monoclinic (InyGa1- y)2O3 are identified by machine learning analysis of RHEED patterns and targeted growths are characterized ex-situ to confirm improved In incorporation. These growth conditions are then combined with established (AlxGa1-x)2O3 growth conditions to grow quaternary (AlxGa1-x-yIny)2O3 with Al mole fractions ranging from 1.4% - 24.4% and In mole fractions ranging from 3.1% to 15.5%. The chemical and optical properties of the alloys are investigated by XRD, XPS, and spectroscopic ellipsometry. A lattice-matched (AlxGa1-x-yIny)2O3 alloy is examined by 4D-STEM and the chemical and physical uniformity of Al and In incorporation are discussed.

alloy↗

NASA NTRS1987

Velocimetry with refractive index matching for complex flow configurations, phase 1

The feasibility of obtaining detailed velocity field measurements in large Reynolds number flow of the Space Shuttle Main Engine (SSME) main injector bowl was demonstrated using laser velocimetry and the developed refractive-index-matching technique. An experimental system to provide appropriate flow rates and temperature control of refractive-index-matching fluid was designed and tested. Test results are presented to establish the feasibility of obtaining accurate velocity measurements that map the entire field including the flow through the LOX post bundles: sample mean velocity, turbulence intensity, and spectral results are presented. The results indicate that a suitable fluid and control system is feasible for the representation of complex rocket-engine configurations and that measurements of velocity characteristics can be obtained without the optical access restrictions normally associated with laser velocimetry. The refractive-index-matching technique considered needs to be further developed and extended to represent other rocket-engine flows where current methods either cannot measure with adequate accuracy or they fail.

Thompson, B. E.↗

NASA NTRS2015

Investigation of Unsteady Tip Clearance Flow in a Low-Speed One and Half Stage Axial Compressor with LES And PIV

The primary focus of this paper is to investigate how a rotor's unsteady tip clearance flow structure changes in a low speed one and half stage axial compressor when the rotor tip gap size is increased from 0.5 mm (0.49% of rotor tip blade chord, 2% of blade span) to 2.4 mm (2.34% chord, 4% span) at the design condition are investigated. The changes in unsteady tip clearance flow with the 0.62 % tip gap as the flow rate is reduced to near stall condition are also investigated. A Large Eddy Simulation (LES) is applied to calculate the unsteady flow field at these three flow conditions. Detailed Stereoscopic PIV (SPIV) measurements of the current flow fields were also performed at the Johns Hopkins University in a refractive index-matched test facility which renders the compressor blades and casing optically transparent. With this setup, the unsteady velocity field in the entire flow domain, including the flow inside the tip gap, can be measured. Unsteady tip clearance flow fields from LES are compared with the PIV measurements and both LES and PIV results are used to study changes in tip clearance flow structures. The current study shows that the tip clearance vortex is not a single structure as traditionally perceived. The tip clearance vortex is formed by multiple interlaced vorticities. Therefore, the tip clearance vortex is inherently unsteady. The multiple interlaced vortices never roll up to form a single structure. When phased-averaged, the tip clearance vortex appears as a single structure. When flow rate is reduced with the same tip gap, the tip clearance vortex rolls further upstream and the tip clearance vortex moves further radially inward and away from the suction side of the blade. When the tip gap size is increased at the design flow condition, the overall tip clearance vortex becomes stronger and it stays closer to the blade suction side and the vortex core extends all the way to the exit of the blade passage. Measured and calculated unsteady flow fields inside the tip gap agree fairly well. Instantaneous velocity vectors inside the tip gap from both the PIV and LES do show flow separation and reattachment at the entrance of tip gap as some earlier studies suggested. This area at the entrance of tip gap flow (the pressure side of the blade) is confined very close to the rotor tip section. With a small tip gap (0.5mm), the gap flow looks like a simple two-dimensional channel flow with larger velocity near the casing for both flow rates. A small area with a sharp velocity gradient is observed just above the rotor tip. This strong shear layer is turned radially inward when it collides with the incoming flow and forms the core structure of the tip clearance vortex. When tip gap size is increased to 2.4 mm at the design operation, the radial profile of the tip gap flow changes drastically. With the large tip gap, the gap flow looks like a two-dimensional channel flow only near the casing. Near the rotor top section, a bigger region with very large shear and reversed flow is observed.

compressor↗

NASA NTRS2015

Investigation of Unsteady Tip Clearance Flow in a Low-Speed One and Half Stage Axial Compressor with LES And PIV

unsteady↗

DOE OSTI2025

Transferable dispersion-aware machine learning interatomic potentials for multilayer transition metal dichalcogenide heterostructures

Stacking atomically thin transition metal dichalcogenides (TMDs) into heterostructures enables exploration of exotic quantum phases, particularly through twist-angle-controlled moiré superlattices. These structures exhibit novel electronic and optical behaviors driven by atomic-scale structural reconstruction. However, studying such systems with DFT is computationally demanding due to their large unit cells and van der Waals (vdW) interactions between layers. To address this, we develop a transferable neural network potential (NNP) that includes long-range vdW corrections up to 12Å with minimal overhead. Trained on vdW-corrected DFT data for Mo- and W-based TMDs with S, Se, and Te, the NNP accurately models monolayers, bilayers, heterostructures, and their interaction with h-BN substrates. It reproduces equilibrium structures, energy landscapes, phonon dispersions, and matches experimental atomic reconstructions in twisted WS2 and MoS2/WSe2 systems. We demonstrate that our NNP achieves DFT-level accuracy and high computational efficiency, enabling large-scale simulations of TMD-based moiré superlattices both with and without substrates.

materials for energy and catalysis↗

NASA NTRS2012

NASA Tech Briefs, July 2012

Topics covered include: Instrument Suite for Vertical Characterization of the Ionosphere-Thermosphere System; Terahertz Radiation Heterodyne Detector Using Two-Dimensional Electron Gas in a GaN Heterostructure; Pattern Recognition Algorithm for High-Sensitivity Odorant Detection in Unknown Environments; Determining Performance Acceptability of Electrochemical Oxygen Sensors; Versatile Controller for Infrared Lamp and Heater Arrays; High-Speed Scanning Interferometer Using CMOS Image Sensor and FPGA Based on Multifrequency Phase-Tracking Detection; Ultra-Low-Power MEMS Selective Gas Sensors; Compact Receiver Front Ends for Submillimeter-Wave Applications; Dynamically Reconfigurable Systolic Array Accelerator; Blocking Losses With a Photon Counter; Motion-Capture-Enabled Software for Gestural Control of 3D Mod; Orbit Software Suite; CoNNeCT Baseband Processor Module Boot Code SoftWare (BCSW); Trajectory Software With Upper Atmosphere Model; ALSSAT Version 6.0; Employing a Grinding Technology to Assess the Microbial Density for Encapsulated Organisms; Demonstration of Minimally Machined Honeycomb Silicon Carbide Mirrors; Polyimide Aerogel Thin Films; Nanoengineered Thermal Materials Based on Carbon Nanotube Array Composites; Composite Laminate With Coefficient of Thermal Expansion Matching D263 Glass; Robust Tensioned Kevlar Suspension Design; Focal Plane Alignment Utilizing Optical CMM; Purifying, Separating, and Concentrating Cells From a Sample Low in Biomass; Virtual Ultrasound Guidance for Inexperienced Operators; Beat-to-Beat Blood Pressure Monitor; Non-Contact Conductivity Measurement for Automated Sample Processing Systems; An MSK Radar Waveform; Telescope Alignment From Sparsely Sampled Wavefront Measurements Over Pupil Subapertures; Method to Remove Particulate Matter from Dusty Gases at Low Pressures; Terahertz Quantum Cascade Laser With Efficient Coupling and Beam Profile; Measurement Via Optical Near-Nulling and Subaperture Stitching; 885-nm Pumped Ceramic Nd:YAG Master Oscillator Power Amplifier Laser System; Airborne Hyperspectral Imaging System; Heat Shield Employing Cured Thermal Protection Material Blocks Bonded in a Large-Cell Honeycomb Matrix; and Asymmetric Supercapacitor for Long-Duration Power Storage.

Source record↗

NASA NTRSDate not supplied

Comparing Low-Cost Sensors with Ground-Based and Airborne In-Situ and Column Observations of NO2 and HCHO during the FRAPPE Field Campaign in Colorado, USA

Even in the presence of more reliable air quality tools, low-cost sensors have the benefit of recording data on highly localized spatial and temporal scales, allowing for multiple measurements within a single satellite pixel and on pixel boundaries. However, they are less accurate than their regulatory-grade counterparts, requiring regular co-locations with accepted instruments to ensure their validity. Thus, the addition of low-cost sensors to a field campaign – where reference-grade air quality instruments are abundant – not only provides ample opportunities for low-cost sensor co-location and calibration, but also allows the low-cost instruments to be used for sub-pixel validation, covering more surface area than the regulatory instruments alone with a network of sensors. During the summer of 2014, our low-cost sensor network was deployed during the Front Range Air Pollution and Photochemistry Experiment (FRAPPÉ) campaign conducted to sample the composition of air at and above ground level in northeastern Colorado, USA. The low-cost sensor platform included a suite of gas-phase sensors, notably NO2 and two generalized volatile organic compound (VOC) sensors, which were leveraged together to quantify speciated hydrocarbons such as formaldehyde. These key pollutants were chosen for their impacts on human health and climate change, as well as their inclusion on the TEMPO satellite launching this year. Airborne campaign measurements included slant column optical observations of formaldehyde (HCHO), nitrogen dioxide (NO2), and ozone (O3). Myriad additional in-situ instruments described chemical composition up to approximately 5 km above surface level. Ground-based instrumentation included both stationary and mobile regulatory-grade instruments, which were used for sensor calibration. Machine learning techniques such as artificial neural networks (ANNs) were used to match the low-cost signals to that of the reference-grade instruments. Here, we compare calibrated low-cost sensor data collected at ground level in a variety of locations along Colorado’s Front Range to various data sources from the FRAPPÉ campaign to better understand how well airborne and regulatory ground-based measurements can be extrapolated to other locations. Further, as the slant column measurements act as satellite simulators, we explore how low-cost instruments can be used for satellite validation purposes. Comparisons among these different data types also have important implications in data fusion.

Kristen Okorn↗

NASA NTRS1999

Melt Growth of a Nonlinear Optical Crystal Triethylphosphine Sulfide using Modified Bridgman-Stockbarger Technique

Bulk single crystals of triethylphosphine sulfide (C2H5)3P(S), a potential nonlinear optical organic material has been grown from melt using Bridgman- Stockbarger method. Commercially available material triethylphosphine sulfide procured from Johnson Matthey was purified by physical vapor transport using low pressure sublimaton (about 30 mTorr). Modified Bridgman-Stockbarger technique is characterized by the smallest possible quantity of product in the melt for a short period of time. The temperature gradient was chosen to be about 10 C/cm and the ampoule was lowering rate was chosen to be 0.2-0.3 mm/h. For various growth conditions, several single crystal of triethylphosphine sulfide have been grown with sizes 10X10X15mm(exp 3). The second harmonic generation (SHG) efficiency was measured and has been found to be comparable to phase matched potassium dihydrogen phosphate crystals. Further characterization of the grown single crystals is in progress and the results will be presented at the symposium.

Curry, K.↗

DOE OSTI2025

Shock-induced bubble jets: a dual perspective of bubble collapse and interfacial instability theory

Interactions between shock waves and gas bubbles in a liquid can lead to bubble collapse and high-speed liquid jet formation, relevant to biomedical applications such as shock wave lithotripsy and targeted drug delivery. This study reveals a complex interplay between acceleration-induced instabilities that drive jet formation and radial accelerations causing overall bubble collapse under shock wave pressure. Using high-speed synchrotron X-ray phase contrast imaging, the dynamics of micrometre-sized air bubbles interacting with laser-induced underwater shock waves are visualised. These images offer full optical access to phase discontinuities along the X-ray path, including jet formation, its propagation inside the bubble, and penetration through the distal side. Jet formation from laser-induced shock waves is suggested to be an acceleration-driven process. A model predicting jet speed based on the perturbation growth rate of a single-mode Richtmyer–Meshkov instability shows good agreement with experimental data, despite uncertainties in the jet-driving mechanisms. The jet initially follows a linear growth phase, transitioning into a nonlinear regime as it evolves. To capture this transition, a heuristic model bridging the linear and nonlinear growth phases is introduced, also approximating jet shape as a single-mode instability, again matching experimental observations. Upon piercing the distal bubble surface, jets can entrain gas and form a toroidal secondary bubble. Linear scaling laws are identified for the pinch-off time and volume of the ejected bubble relative to the jet’s Weber number, characterising the balance of inertia and surface tension. At low speeds, jets destabilise due to capillary effects, resulting in ligament pinch-off.

Drops and Bubbles: Bubble dynamics↗

NASA NTRS2001

Mid-infrared trace gas detection using continuous-wave difference frequency generation in periodically poled RbTiOAsO4

A tunable mid-infrared continuous-wave (cw) spectroscopic source in the 3.4-4.5 micrometers region is reported, based on difference frequency generation (DFG) in a quasi-phase-matched periodically poled RbTiOAsO4 (PPRTA) crystal. DFG power levels of 10 microW were generated at approximately 4 micrometers in a 20-mm long PPRTA crystal by mixing two cw single-frequency Ti:Al2O3 lasers operating near 713 nm and 871 nm, respectively, using a laser pump power of 300 mW. A quasi-phase-matched infrared wavelength-tuning bandwidth (FWHM) of ~ 12 cm-1 and a temperature tuning rate of 1.02 cm-1/degree C were achieved. Experimental details regarding the feasibility of trace gas detection based on absorption spectroscopy of CO2 in ambient air using this DFG radiation source are also described.

NASA Discipline Life Sciences Technologies↗

NASA NTRS1999

A Frequency Transfer and Cleanup System for Ultra-High Stability at Both Long and Short Times for the Cassini Ka-Band Experiment

New radio science experiments, including a gravitational wave search and several atmospheric occultation studies, are planned for the Cassini Ka-band experiment. These experiments are made possible by reduced solar-induced phase fluctuations at the high-frequency (32 GHZ) of the radio link between the earth and the spacecraft. In order to match the improved link performance, a significant upgrade is under way to improve the frequency stability capabilities of NASA's Deep Space Network (DSN). Significant improvements are being undertaken in many areas, including antenna vibration and (wet) tropospheric calibration, in addition to frequency generation and distribution. We describe here the design and development of a system to provide a reference signal with the highest possible frequency stability for both long-term, short-term, and phase noise, at an antenna (DSS 25) that is remote from the frequency standards room at SPC-10 at the Goldstone site. The new technologies were developed in order to meet the very tight requirements. They are: 1) a Stabilized Fiber-Optic Distribution Assembly (SFODA) that includes active compensation of thermal variations to transfer long-term stability over 16 km of ordinary fiber-optic cable, and 2) a Compensated Sapphire Oscillator (CSO) that provides short-term performance in a cryocooled sapphire oscillator with ultra-high short-term stability and low phase noise.

Calhoun, M. D.↗

NASA NTRSDate not supplied

Ice-Over-Water Cloud Properties in an Artificial Neural Network Approach

Clouds are a crucial component of the atmospheric energy system, particularly the radiative balance within, above, and below the troposphere. The vertical distribution of cloud mass and phase determines layer heating rates, the loss of radiation to space, and the amount of radiative heating at the surface. Thus, it is important to know how clouds are distributed both vertically and horizontally at all times of day. Satellite remote sensing is the only approach available to monitor clouds day and night around the globe. In this paper several artificial neural network (ANN) algorithms, employing several Aqua MODIS infrared channels, profiles of relative humidity and temperature from GMAO numerical weather analyses, and the retrieved total cloud visible optical depth, are trained to detect multilayer ice-over-water cloud systems and to retrieve some of their properties as identified by a year of 2008 Aqua MODIS data matched with CloudSat and CALIPSO (CC) cloud profiles. The CC lidar and radar profiles provide the vertical structure that serves as output truth for the multilayer algorithm. The neural networks were trained using one year (2008) of cloud top height data from the CC dataset, with correlation around 0.94 (0.95) and MAE as low as 0.82 (0.81) km for nonpolar regions during the day (night). Applying the trained ANN to independent year 2009 MODIS data resulted in a combined ML and single layer hit rate of 86.4% (85.1%) for nonpolar regions during the day (night). Since the ANN is trained using near-nadir MODIS pixels, infrared radiance corrections were developed as a function of view zenith angle from MODIS and applied to off-nadir pixels when processing MODIS swath data. The multilayer amount derived with the ANN is relatively invariant with increasing view zenith angle compared to the multilayer amount without the corrections.

MODIS↗

DOE OSTI2024

Epitaxial (Al x Ga 1-x-y In y ) 2 O 3 Alloys Lattice Matched to Monoclinic Ga 2 O 3 Substrates

We have epitaxially stabilized a series of monoclinic (Al x Ga 1-x-y In y ) 2 O 3 alloys by careful choice of molecular beam epitaxy growth conditions, which balance alloy growth with suboxide desorption. The films are pseudomorphic to (010) β-Ga 2 O 3 substrates at thicknesses up to 150 nm with compositions ranging from (Al 0.01 Ga 0.83 In 0.16 ) 2 O 3 to (Al 0.24 Ga 0.75 In 0.03 ) 2 O 3 . The absorption edge shifts from approximately 4.62-5.14 eV with coincidently increasing Al and decreasing In mole fractions. J-V measurements reveal an increase in resistivity over four orders of magnitude with a maximum value of 4.2 x 10 5 Ω-cm for (Al 0.17 Ga 0.76 In 0.07 ) 2 O 3 , which has nearly identical lattice parameters (both in-plane and out-of-plane) to the underlying β-Ga 2 O 3 . Scanning transmission electron microscopy of this sample reveals a mostly uniform and single crystalline film, though we identify areas of non-uniform In incorporation and some γ-phase inclusions. This work demonstrates the feasibility of thick layers lattice-matched to β-Ga 2 O 3 with increased bandgap compared to phase-separation limited (Al,Ga) 2 O 3 . These alloys can enable higher bandgap epitaxial dielectrics and high sheet charge density transistors by increasing the conduction band offset with respect to β-Ga 2 O 3 .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2022

Orbiting Laser Configuration and Sky Coverage: Coherent Reference for Breakthrough Starshot Ground-based Laser Array

We present the concept of using an orbiting laser as a coherent optical reference to phase a several kilometer diameter array of ground-based lasers designed to accelerate interstellar nano-spacecraft to 20% light-speed using laser propulsion. We investigate the geometrical and temporal constraints for the initial case of the target star Proxima b in the Alpha Centauri system using a laser ground site in the southern hemisphere. Based on these constraints, we detail requirements for the mission architecture for an orbiting laser to be used as an optical reference. We then present two orbits that can meet all given requirements and represent a range of engagement times and days between engagements. We also present a range of orbits with periods from 3 to 4 days and engagement times from 660 to 800 s. If desired, the orbit can be matched to the sidereal day, so each orbit period, the beacon can align with the ground station and the same target star without maneuvers. A discussion of the tradeoff between the Earth-based site latitude, time on engagement, and days between engagements is presented.

Breakthrough Starshot; interstellar spacecraft; co↗

DOE OSTI2025

Production, quality assurance and quality control of the SiPM Tiles for the DarkSide-20k Time Projection Chamber

The DarkSide-20k dark matter direct detection experiment will employ a 21 m 2 silicon photomultiplier (SiPM) array, instrumenting a dual-phase 50 tonnes liquid argon Time Projection Chamber (TPC). SiPMs are arranged into modular photosensors called Tiles, each integrating 24 SiPMs onto a printed circuit board (PCB) that provides signal amplification, power distribution, and a single-ended output for simplified readout. Tiles are further grouped into Photo-Detector Units (PDUs). This paper details the production of the Tiles and the Quality Assurance and Quality Control (QA-QC) protocol established to ensure their performance and uniformity. The production and QA-QC of the Tiles are carried out at Nuova Officina Assergi (NOA), an ISO-6 clean room facility at LNGS. This process includes wafer-level cryogenic characterisation, precision die attaching, wire bonding, and extensive electrical and optical validation of each Tile. The overall production yield exceeds 83.5%, matching the requirements of the DarkSide-20k production plan. These results validate the robustness of the Tile design and its suitability for operation in a cryogenic environment.

Acerbi, F. [Fondazione Bruno Kessler]↗

NASA NTRS1991

Optical phase-locked loop (OPLL) for free-space laser communications with heterodyne detection

Several advantages of coherent free-space optical communications are outlined. Theoretical analysis is formulated for an OPLL disturbed by shot noise, modulation noise, and frequency noise consisting of a white component, a 1/f component, and a 1/f-squared component. Each of the noise components is characterized by its associated power spectral density. It is shown that the effect of modulation depends only on the ratio of loop bandwidth and data rate, and is negligible for an OPLL with loop bandwidth smaller than one fourth the data rate. Total phase error variance as a function of loop bandwidth is displayed for several values of carrier signal to noise ratio. Optimal loop bandwidth is also calculated as a function of carrier signal to noise ratio. An OPLL experiment is performed, where it is shown that the measured phase error variance closely matches the theoretical predictions.

Win, Moe Z.↗

NASA NTRS1992

Electro-optic resonant phase modulator

An electro-optic resonant cavity is used to achieve phase modulation with lower driving voltages. Laser damage thresholds are inherently higher than with previously used integrated optics due to the utilization of bulk optics. Phase modulation is achieved at higher speeds with lower driving voltages than previously obtained with non-resonant electro-optic phase modulators. The instant scheme uses a data locking dither approach as opposed to the conventional sinusoidal locking schemes. In accordance with a disclosed embodiment, a resonant cavity modulator has been designed to operate at a data rate in excess of 100 megabits per sec. By carefully choosing the cavity finesse and its dimension, it is possible to control the pulse switching time to within 4 nano-sec. and to limit the required switching voltage to within 10 V. This cavity locking scheme can be applied by using only the random data sequence, and without the need of dithering of the cavity. Compared to waveguide modulators, the resonant cavity has a comparable modulating voltage requirement. Because of its bulk geometry, the resonant cavity modulator has the potential of accommodating higher throughput power. Mode matching into the bulk device is easier and typically can be achieved with higher efficiency. An additional control loop is incorporated into the modulator to maintain the cavity on resonance.

Chen, Chien-Chung↗

DOE OSTI2026

Quantum Theory of Surface Lattice Resonances

The collective interactions of nanoparticles arranged in periodic structures give rise to high‐ in‐plane diffractive modes known as surface lattice resonances. Although these resonances and their broader implications have been extensively studied within the framework of classical electrodynamics and linear response theory, a quantum optical theory capable of describing the dynamics of these structures, especially in the presence of material nonlinearities beyond ad hoc few‐mode approximations, is largely missing. To this end, we consider a lattice of metallic nanoparticles coupled to the electromagnetic field and derive the quantum input–output relations within the electric dipole approximation. As applications, we analyze coupling between the nanoparticle array and external quantum emitters, and show how the formalism extends to molecular optomechanics, where the high ‐factors of SLRs enable coupling to collective vibrational modes. We further consider arrays composed of saturable excitonic emitters, demonstrating how emitter nonlinearities can be used to switch the SLR condition between electronic transitions. Using a perturbative approach that accounts for population dynamics, we show how these effects can be probed in pump–probe experiments and give rise to nonlinear phase‐matching phenomena. Our work provides a microscopic framework for modeling SLRs interacting with quantum emitters without phenomenological descriptions of the electromagnetic environment.

molecular optomechanics↗