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DOE OSTI2026

Bound Exciton Complexes in Near-Infrared Emitting Quantum Shells

Near-infrared (NIR) light sources based on colloidal semiconductor nanocrystals (NCs) represent a scalable, low-cost alternative to epitaxial semiconductor platforms. However, their performance remains hindered by rapid Auger recombination, a problem that is particularly pronounced in narrow-bandgap materials. Here, we report on CdS/HgS/CdS and CdS/HgCdSe/ ZnS quantum shells (QSs), a class of spherical quantum wells specifically engineered for a suppression of nonradiative Auger processes. Fabricated QSs exhibit tunable NIR emission with photoluminescence quantum yields reaching ∼60% below 1000 nm and up to 30% near 1300 nm. Optical gain and stimulated emission were observed in CdS/HgS/CdS QSs. In contrast, CdS/HgCdSe/ZnS QSs displayed a photoinduced absorption in lieu of optical gain despite demonstrating a comparatively stronger Auger suppression. Transient absorption spectroscopy revealed that this phenomenon arises from the formation of bound multiexciton complexes that induce long-lived sub-bandgap multiexciton states. The observation of such bound excitonic clusters at room temperature offers a pathway toward nonlinear NIR photonic phenomena, including biexciton−exciton cascade emission, optical modulation, and singleexciton gain.

Auger recombination↗

NASA NTRS1996

The Effect of Gravity Axis Orientation on the Growth of Phthalocyanine Thin Films

Experimentally, many of the functions of electrical circuits have been demonstrated using optical circuits and, in theory, all of these functions may be accomplished using optical devices made of nonlinear optical materials. Actual construction of nonlinear optical devices is one of the most active areas in all optical research being done at this time. Physical vapor transport (PVT) is a promising technique for production of thin films of a variety of organic and inorganic materials. Film optical quality, orientation of microcrystals, and thickness depends critically on type of material, pressure of buffer gas and temperature of deposition. An important but understudied influence on film characteristics is the effect of gravity-driven buoyancy. Frazier, Hung, Paley, Penn and Long have recently reported mathematical modelling of the vapor deposition process and tested the predictions of the model on the thickness of films grown by PVT of 6-(2-methyl-4-nitroanilino)-2,4-hexadiyn-l-ol (DAMNA). In an historic experiment, Debe, et. al. offered definitive proof that copper phthalocyanine films grown in a low gravity environment are denser and more ordered than those grown at 1 g. This work seeks to determine the influence on film quality of gravity driven buoyancy in the low pressure PVT film growth of metal-free phthalocyanine.

Pearson, Earl F.↗

NASA NTRS1989

Simulation and analysis of an intermediate frequency (IF) distribution system with applications for Space Station

Simulation and analysis results are described for a wideband fiber optic intermediate frequency distribution channel for a frequency division multiple access (FDMA) system where antenna equipment is remotely located from the signal processing equipment. The fiber optic distribution channel accommodates multiple signals received from a single antenna with differing power levels. Performance parameters addressed are intermodulation degradations, laser noise, and adjacent channel interference, as they impact the overall system design. Simulation results showed that the laser diode modulation level can be allowed to reach 100 percent without considerable degradation. The laser noise must be controlled as to provide a noise floor of less than -90 dBW/Hz. The fiber optic link increases the degradation due to power imbalance yet diminishes the effects of the transmit amplifier nonlinearity. Overall, optimal operation conditions can be found to yield a degradation level of about .1 dB caused by the fiber optic link.

Costello, Thomas A.↗

NASA NTRS2008

WGM Resonators for Terahertz-to-Optical Frequency Conversion

Progress has been made toward solving some practical problems in the implementation of terahertz-to-optical frequency converters utilizing whispering-gallery-mode (WGM) resonators. Such frequency converters are expected to be essential parts of non-cryogenic terahertz- radiation receivers that are, variously, under development or contemplated for a variety of applications in airborne and spaceborne instrumentation for astronomical and military uses. In most respects, the basic principles of terahertz-to-optical frequency conversion in WGM resonators are the same as those of microwave (sub-terahertz)-to-optical frequency conversion in WGM resonators, various aspects of which were discussed in the three preceeding articles. To recapitulate: In a receiver following this approach, a preamplified incoming microwave signal (in the present case, a terahertz signal) is up-converted to an optical signal by a technique that exploits the nonlinearity of the electromagnetic response of a whispering-gallery-mode (WGM) resonator made of LiNbO3 or another suitable electro-optical material. Upconversion takes place by three-wave mixing in the resonator. To ensure the required interaction among the optical and terahertz signals, the WGM resonator must be designed and fabricated to function as an electro-optical modulator while simultaneously exhibiting (1) resonance at the required microwave and optical operating frequencies and (2) phase matching among the microwave and optical signals circulating in the resonator. Downstream of the WGM resonator, the up-converted signal is processed photonically by use of a tunable optical filter or local oscillator and is then detected. The practical problems addressed in the present development effort are the following: Satisfaction of the optical and terahertz resonance-frequency requirement is a straightforward matter, inasmuch as the optical and terahertz spectra can be measured. However, satisfaction of the phase-matching requirement is more difficult. The approach followed in the present development is to perform computer simulations of the microwave and optical signals circulating in the resonator to test for phase matching. To enable excitation of the terahertz WGM resonator mode, it is also necessary to ensure phase matching between that mode and the incoming terahertz radiation. In the present development, the incoming signal is coupled into the WGM resonator via a tapered waveguide in the form of a fused silica rod. The phase-matching requirement is satisfied at one point along the taper; the rod is positioned with this point in proximity to the WGM resonator. To maximize the conversion efficiency, it is necessary to maximize the spatial overlap among the terahertz and optical modes in the WGM resonator. In the absence of a special design effort to address this issue, there would be little such overlap because, as a consequence of a large difference between wavelengths, the optical and terahertz modes would be concentrated at different depths from the rim of a WGM resonator. In the present development, overlap is ensured by constructing the WGM resonator as a ring (see figure) so thin that the optical and terahertz modes are effectively forced to overlap.

Strekalov,Dmitry↗

DOE OSTI2020

Machine-Learning Enabled Evaluation of Probability of Piping Degradation In Secondary Systems of Nuclear Power Plants

The transition to condition-based, risk-informed automated maintenance will contribute to a significant reduction of operations and maintenance costs that account for the majority of nuclear power generation costs. Furthermore, of the operations and maintenance costs in U.S. plants, approximately 80% are labor costs. To address the issue of rising operating costs and economic viability, technologies used to perform online monitoring of piping and other secondary system structural components in commercial nuclear power plants (NPPs) are under evaluation. These online monitoring systems have the potential to identify when a more detailed inspection is needed using real time measurements, rather than at a pre-determined inspection interval thus reducing the maintenance cost. This paper describes distributed high-temperature stable fiber sensors fabricated in optical fibers through a roll-to-roll laser direct writing process using femtosecond lasers. Using phase-sensitive optical time domain reflectometry, distributed acoustic and vibration sensors can be developed and deployed to critical components and systems in NPPs to perform active measurements with spatial resolution down to 0.5-meter throughout the piping systems. Complex acoustic and vibration signatures harnessed by distributed sensors are registered and analyzed by artificial intelligence algorithms for degradation detection and flaw identification. Piping elbows with machined-in flaws were instrumented with fiber sensors. High-spatial-resolution data were used to develop and validate machine learning algorithms, including both linear and nonlinear regression, and classification. Additionally, classification and sensor analysis were also performed for data analysis. The paper concludes with recommendations and future work on applications of machine learning enabled high-resolution fiber sensors for piping degradation monitoring in current or future NPPs.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2022

Neuromorphic Information Processing by Optical Media

Classification of features in a scene typically requires conversion of the incoming photonic field int the electronic domain. Recently, an alternative approach has emerged whereby passive structured materials can perform classification tasks by directly using free-space propagation and diffraction of light. In this manuscript, we present a theoretical and computational study of such systems and establish the basic features that govern their performance. We show that system architecture, material structure, and input light field are intertwined and need to be co-designed to maximize classification accuracy. Our simulations show that a single layer metasurface can achieve classification accuracy better than conventional linear classifiers, with an order of magnitude fewer diffractive features than previously reported. For a wavelength λ, single layer metasurfaces of size 100λ x 100λ with aperture density λ -2 achieve ~96% testing accuracy on the MNIST dataset, for an optimized distance ~100λ to the output plane. This is enabled by an intrinsic nonlinearity in photodetection, despite the use of linear optical metamaterials. Furthermore, we find that once the system is optimized, the number of diffractive features is the main determinant of classification performance. The slow asymptotic scaling with the number of apertures suggests a reason why such systems may benefit from multiple layer designs. Finally, we show a trade-off between the number of apertures and fabrication noise.

47 OTHER INSTRUMENTATION↗

DOE OSTI2022

High-order ( N = 4–6) multiphoton absorption and mid-infrared Kerr nonlinearity in GaP, ZnSe, GaSe, and ZGP crystals

We report a study of high-order multiphoton absorption, nonlinear refraction, and their anisotropy in four notable mid-infrared χ (2) crystals: GaP, ZnSe, GaSe, and ZGP using femtosecond pulses at 2.35 μm with peak intensity in excess of 200 GW/cm 2 . We found that the nonlinear absorption obeys a perturbation model with multiphoton absorption (MPA) orders from N = 4–6, in agreement with the bandgaps of the crystals. A study of the role of free carrier absorption, performed by changing the pulse duration from 30 to 70 fs while maintaining a constant peak intensity, showed that, at our intensity levels, free carriers generated during the MPA process absorb much more strongly than would be expected from their known linear absorption cross section. Possible mechanisms for this anomalous behavior are high-field effects, such as intravalley scattering in the conduction band and absorption to higher lying bands. Nonlinear refractive indices were measured using (i) closed aperture Z-scan and (ii) spectral broadening due to self-phase modulation, both methods agreeing with each other.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS2004

Electrical Transfer Function and Poling Mechanisms for Nonlinear Optical Polymer Modulators

Electro-Optic Polymers hold great promise in increased electro-optic coefficients as compared to their inorganic corollaries. Many researchers have focused on quantum chemistry to describe how the dipoles respond to temperature and electric fields. Much work has also been done for single layer films to confirm these results. For optical applications, waveguide structures are utilized to guide the optical waves in 3 layer stacks. Electrode poling is the only practical poling method for these structures. This research takes an electrical engineering approach to develop poling models and electrical and optical transfer functions of the waveguide structure. The key aspect of the poling model is the large boundary charge density deposited during the poling process. The boundary charge density also has a large effect on the electrical transfer function which is used to explain the transient response of the system. These models are experimentally verified. Exploratory experiment design is used to study poling parameters including time, temperature, and voltage. These studies verify the poling conditions for CLDX/APC and CLDZ/APEC guest host electro optic polymer films in waveguide stacks predicted by the theoretical developments.

Watson, Michael Dale↗

DOE OSTI2024

Non-resonant Bragg scattering four-wave mixing at near-visible wavelengths in low-confinement silicon nitride waveguides

Quantum state coherent frequency conversion processes—such as Bragg-scattering four-wave mixing (BSFWM)—hold promise as a flexible technique for networking heterogeneous and distant quantum systems. In this Letter, we demonstrate BSFWM within an extended (1.2-m) low-confinement silicon nitride waveguide and show that this system has the potential for near-unity frequency conversion in visible and near-visible wavelength ranges. Using sensitive classical heterodyne laser spectroscopy at low optical powers, we characterize the Kerr coefficient (∼1.55 W −1 m −1 ) and linear propagation loss (∼0.0175 dB/cm) of this non-resonant waveguide system, revealing a record-high nonlinear figure of merit (NFM = γ / α ≈ 3.85 W −1 ) for BSFWM of near-visible light in non-resonant silicon nitride waveguides. We predict how, at high yet achievable on-chip optical powers, this NFM would yield a comparatively large frequency conversion efficiency, opening the door to near-unity flexible frequency conversion without cavity enhancement and resulting bandwidth constraints.

Jaber, Nicholas (ORCID:000900070106809X)↗

DOE OSTI2026

Efficiency-optimized relativistic plasma harmonics for extreme fields

Bright harmonic radiation from relativistically oscillating laser plasmas offers a direct route for generating extreme electromagnetic fields. Theory predicts that under optimized conditions, the plasma medium can support strong spatiotemporal compression of laser energy in a coherent harmonic focus (CHF), delivering intensity boosts many orders of magnitude greater than the incident driving laser pulse. Although diffraction-limited performance (spatial compression) and attosecond phase locking (temporal compression) have been demonstrated experimentally, efficient coupling of relativistically intense laser pulse energy into the emitted harmonic cone has not been realized so far. Here we demonstrate that this highly nonlinear interaction can be tailored to deliver the maximum conversion efficiencies predicted from simulations. By fine-tuning the temporal profile of the driving laser on sub-picosecond (<10 −12 s) timescales, energies >9 mJ between the 12th and 47th harmonics are observed. These results are in agreement with the theoretically expected efficiency dependence on harmonic order, verifying that optimal conditions have been achieved in the generation process. This is the important final element required to achieve the expected intensity boosts from a CHF in experiments. Although obtaining spatiotemporal compression and optimal efficiency simultaneously remains challenging, the path to realizing extreme optical field strengths approaching the critical field of quantum electrodynamics (the Schwinger limit at >10 16 V cm −1 or >10 29 W cm −2 ) is now open, permitting all-optical studies of the quantum vacuum and new frontiers for intense attosecond science.

High-harmonic generation↗

DOE OSTI2024

EXPLORING INTERFEROMETRY DIAGNOSTICS FOR OPTICAL STOCHASTIC COOLING AT FAST/IOTA

Optical Stochastic Cooling (OSC) is an advanced beam-cooling technique that will advance the traditional stochastic cooling. This method leverages optical radiation and high-precision feedback to cool the particles more efficiently than traditional stochastic methods by more than three orders of magnitude. As such, it is an enabler for the development of next generation discovery science machines at the frontiers of energy and intensity. This paper focuses on the development of the second phase of OSC and improving extreme beam cooling techniques in accelerators. The goal was to build and characterize a Mach-Zehnder Interferometer (MZI) in the FAST laser lab using known glass plates thickness which will allow future measurements of unknown phase change due to nonlinear amplification processes.

Teriba, Folashade↗

DOE OSTI2020

Broad Frequency Shift of Parametric Processes in Epsilon-Near-Zero Time-Varying Media

The ultrafast changes of material properties induced by short laser pulses can lead to a frequency shift of reflected and transmitted radiation. Recent reports highlight how such a frequency shift is enhanced in spectral regions where the material features a near-zero real part of the permittivity. Here, we investigate the frequency shift for fields generated by four-wave mixing. In our experiment, we observed a frequency shift of more than 60 nm (compared to the pulse width of ~40 nm) in the phase conjugated radiation generated by a 500 nm aluminium-doped zinc oxide (AZO) film pumped close to the epsilon-near-zero wavelength. Our results indicate applications of time-varying media for nonlinear optics and frequency conversion.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Impact of dynamic Jahn-Teller effect on magnetic excitations, lattice vibration, and thermal conductivity in U 𝑥 ⁢T⁢h 1−𝑥 ⁡O 2 system

Vibrational and magnetic properties of single-crystal uranium-thorium dioxide (U 𝑥 ⁢T⁢h 1−𝑥⁡ O 2 ) with a full range of 0 < 𝑥 < 1 are investigated. Thorium dioxide is a diamagnet whose thermal properties are governed by lattice vibration. The addition of paramagnetic uranium ions leads to the emergence of magnetic effects that alter the thermophysical properties noticeably even at room temperature. The interaction of phonons with magnetic moments of uranium 5⁢𝑓 electrons mediated by magnetoelastic coupling results in an anomalous low-temperature thermal conductivity profile. Analysis of the magnetic susceptibility measurements indicates a departure from the Curie-Weiss relationship characteristic of noninteracting paramagnetic ions, previously associated with the dynamic Jahn-Teller (DJT) effect characterized by coupling between spin and the oxygen sublattice. The T 2⁢g Raman peak position follows a nonlinear trend as a function of uranium concentration and hints that these Raman active optical modes play a role in either DJT or in mediating quadrupole-quadrupole interactions. A first-principle-based thermal transport model is implemented to explain the low-temperature transport measurements, where the anomalous reduction is attributed to phonon-spin resonant scattering. The interplay between spins and phonons is also captured using high-resolution inelastic x-ray scattering (IXS) measurements of phonon linewidths. Our results provide insights into the phonon interactions with the magnetic excitations governing DJT effect and impacting the low-temperature thermal transport processes in this material system. Furthermore, these findings have implications for understanding low-temperature thermal transport and magnetic properties in advanced materials for information processing and energy applications.

36 - MATERIALS SCIENCE↗

NASA NTRS2019

First Steps in the Creation of a Joint MISR/MODIS Ocean Color Atmospheric Correction Algorithm

We are creating a new algorithm that combines observations from MISR and MODIS (both on the NASA Terra spacecraft) to improve atmospheric correction and coverage for ocean color data products. The algorithm utilizes information rich, multi-angle MISR observations for atmospheric correction, applied to MODIS. Our goal is to produce atmospherically corrected Remote Sensing Reflectance from MODIS with enhanced coverage and accuracy, for input to downstream bio-optical ocean parameter retrieval algorithms.An important aspect of this work is the utilization of multi-angle views of the reflected ocean surface sun glint. Usually, such observations are avoided, since the intensity of the glint overwhelms any contribution from the ocean body. However, MISR's multi-angle observations see varying degrees of glint, which means they can be used to better determine aerosol optical properties (Kaufman et al., 2002, Ottaviani et al., 2013), and to identify surface wind speeds that govern the glint pattern. The latter could be utilized to replace the wind speeds taken from ancillary sources that are currently used to conservatively mask potential glint contamination in MODIS observations.To assess this capability, and to identify the appropriate parameterization, we present an analysis using the Generalized Nonlinear Retrieval Analysis (GENRA, Vukicevic et al., 2009) information content assessment. This technique is also easily modified to act as a Bayesian retrieval algorithm, for which initial results are discussed. Finally, we describe the status of integrating MISR data into the processing capabilities of the Ocean Biology Processing Group (OBPG) at NASA, and show the first ocean color vicarious calibration (Franz et al., 2007) of the MISR instrument.

Knobelspiesse, Kirk↗

DOE OSTI2024

Silicon-On-Silicon Carbide Platform for Integrated Photonics

Silicon carbide (SiC)'s nonlinear optical properties and applications to quantum information have recently brought attention to its potential as an integrated photonics platform. However, despite its many excellent material properties, such as large thermal conductivity, wide transparency window, and strong optical nonlinearities, it is generally a difficult material for microfabrication. Here, it is shown that directly bonded silicon-on-silicon carbide can be a high-performing hybrid photonics platform that does not require the need to form SiC membranes or directly pattern in SiC. The optimized bonding method yields defect-free, uniform films with minimal oxide at the silicon–silicon–carbide interface. Ring resonators are patterned into the silicon layer with standard, complimentary metal–oxide–semiconductor (CMOS) compatible (Si) fabrication and measure room-temperature, near-infrared quality factors exceeding 10 5 . The corresponding propagation loss is 5.7 dB cm -1 . The process offers a wafer-scalable pathway to the integration of SiC photonics into CMOS devices.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Ultrafast nano-imaging and nano-spectroscopy

Ultrafast pump–probe nano-imaging combines scanning probe-based optical near-field microscopy with ultrafast spectroscopy to enable imaging with deep sub-wavelength spatial resolution, femtosecond temporal resolution and simultaneous spectral resolution. Ultrafast nano-imaging has gained increased attention for its ability to provide far-from-equilibrium excitation and excited-state contrast. With coherent and nonlinear probing, coupled electron, spin and lattice dynamics on elementary timescale and length scale can be resolved. Through nano-movies, ultrafast nano-imaging visualizes correlated quantum dynamics underlying the properties of solid-state materials, semiconductors, molecular electronic, photonic, photovoltaic and other functional materials. With nanometre spatial resolution, this method probes elementary dynamic processes across multiple length scales that are otherwise obscured in conventional ultrafast spectroscopy in which heterogeneities are spatially averaged. Furthermore, this Primer describes the theoretical background and experimental implementation of ultrafast nano-imaging; signal interpretation and modelling; representative examples and a perspective for the future development of the field.

Microscopy↗

DOE OSTI2022

Polariton relaxation under vibrational strong coupling: Comparing cavity molecular dynamics simulations against Fermi’s golden rule rate

Under vibrational strong coupling (VSC), the formation of molecular polaritons may significantly modify the photo-induced or thermal properties of molecules. In an effort to understand these intriguing modifications, both experimental and theoretical studies have focused on the ultrafast dynamics of vibrational polaritons. Here, following our recent work [Li et al., J. Chem. Phys. 154, 094124 (2021)], we systematically study the mechanism of polariton relaxation for liquid CO 2 under a weak external pumping. Classical cavity molecular dynamics (CavMD) simulations confirm that polariton relaxation results from the combined effects of (i) cavity loss through the photonic component and (ii) dephasing of the bright-mode component to vibrational dark modes as mediated by intermolecular interactions. The latter polaritonic dephasing rate is proportional to the product of the weight of the bright mode in the polariton wave function and the spectral overlap between the polariton and dark modes. Both these factors are sensitive to parameters such as the Rabi splitting and cavity mode detuning. Compared to a Fermi’s golden rule calculation based on a tight-binding harmonic model, CavMD yields a similar parameter dependence for the upper polariton relaxation lifetime but sometimes a modest disagreement for the lower polariton. We suggest that this disagreement results from polariton-enhanced molecular nonlinear absorption due to molecular anharmonicity, which is not included in our analytical model. Finally, we also summarize recent progress on probing nonreactive VSC dynamics with CavMD.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1998

Predicting Ecologically Important Vegetation Variables from Remotely Sensed Optical/Radar Data Using Neural Networks

A number of satellite sensor systems will collect large data sets of the Earth's surface during NASA's Earth Observing System (EOS) era. Efforts are being made to develop efficient algorithms that can incorporate a wide variety of spectral data and ancillary data in order to extract vegetation variables required for global and regional studies of ecosystem processes, biosphere-atmosphere interactions, and carbon dynamics. These variables are, for the most part, continuous (e.g. biomass, leaf area index, fraction of vegetation cover, vegetation height, vegetation age, spectral albedo, absorbed photosynthetic active radiation, photosynthetic efficiency, etc.) and estimates may be made using remotely sensed data (e.g. nadir and directional optical wavelengths, multifrequency radar backscatter) and any other readily available ancillary data (e.g., topography, sun angle, ground data, etc.). Using these types of data, neural networks can: 1) provide accurate initial models for extracting vegetation variables when an adequate amount of data is available; 2) provide a performance standard for evaluating existing physically-based models; 3) invert multivariate, physically based models; 4) in a variable selection process, identify those independent variables which best infer the vegetation variable(s) of interest; and 5) incorporate new data sources that would be difficult or impossible to use with conventional techniques. In addition, neural networks employ a more powerful and adaptive nonlinear equation form as compared to traditional linear, index transformations, and simple nonlinear analyses. These neural networks attributes are discussed in the context of the authors' investigations of extracting vegetation variables of ecological interest.

Kimes, Daniel S.↗