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DOE OSTI2024

A 2D chiral microcavity based on apparent circular dichroism

Abstract Engineering asymmetric transmission between left-handed and right-handed circularly polarized light in planar Fabry–Pérot (FP) microcavities would enable a variety of chiral light-matter phenomena, with applications in spintronics, polaritonics, and chiral lasing. Such symmetry breaking, however, generally requires Faraday rotators or nanofabricated polarization-preserving mirrors. We present a simple solution requiring no nanofabrication to induce asymmetric transmission in FP microcavities, preserving low mode volumes by embedding organic thin films exhibiting apparent circular dichroism (ACD); an optical phenomenon based on 2D chirality. Importantly, ACD interactions are opposite for counter-propagating light. Consequently, we demonstrated asymmetric transmission of cavity modes over an order of magnitude larger than that of the isolated thin film. Through circular dichroism spectroscopy, Mueller matrix ellipsometry, and simulation using theoretical scattering matrix methods, we characterize the spatial, spectral, and angular chiroptical responses of this 2D chiral microcavity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1980

Common time in a four-dimensional symmetry framework

Following the ideas of Poincare, Reichenbach, and Grunbaum concerning the convention of setting up clock systems, clock systems and light propagation are analyzed within the framework of four-dimensional symmetry. It is possible to construct a new four-dimensional symmetry framework incorporating common time: observers in different inertial frames of reference use one and the same clock system, which is located in any one of the frames. Consequently, simultaneity has a meaning independent of position and independent of frame of reference. A further consequence is that the two-way speeds of light alone are isotropic in any frame. By the choice of clock system there will be one frame in which the one-way speed of light is isotropic. This frame can be arbitrarily chosen. The difference between one-way speeds and two-way speeds of light signals is considered in detail.

Hsu, J. P.↗

NASA NTRS1999

Corrugated Quantum Well Infrared Photodetectors and Arrays

Quantum well infrared photodetectors (QWIPs) have many advantages in infrared detection, mainly due to the mature Ill-V material technology. The employment of the corrugation structure further advances the technology by providing a simple, yet efficient light-coupling scheme. A C-QWIP enjoys the same flexibility as a detector with intrinsic normal incident absorption. In this paper, we will discuss the utilities of C-QWIPs in different applications, including two-color detection and polarization-sensitive detection. Besides practical applications, C-QWIPs are also useful in detector characterization. They can be used for measuring the absorption coefficient of light propagating parallel to the layers under bias and providing information on the energy resolved photoconductive gain. These two quantities have never been measured before. Based on the corrugation design, we have made several modifications that further improve the detector sensitivity without increasing its complexity. Other than the C-QWIP structure, we also continue searching for other sensitive detector architectures. In a quantum grid infrared photodetector, 3-dimensional electron confinement can be achieved, with which the detector is able to absorb light in all directions. At the same time, the photoconductive gain can also be improved. We further improve the design using a blazed structure. All the experimental results are supported by a rigorous electromagnetic modal transmission-line theory developed especially for these types of structures. Preliminary thermal imaging using C-QWIP FPAs validates the advantages of the present approach.

Choi, K. K.↗

DOE OSTI2020

Measurement of the angular dependence of the spontaneous Raman scattering in anisotropic crystalline materials using spherical samples: Potassium dihydrogen phosphate as a case example

A specialized experimental configuration was created to allow for more-accurate characterization of the spontaneous Raman scattering properties in anisotropic materials. This need stems from the challenges, arising from the complexity of light propagation, in obtaining accurate measurements of the angular dependence of the Raman scattering cross section in birefringent materials. The nonlinear optical material KH 2 PO 4 (KDP) is used as a model medium. Our report is motivated by the need to improve our understanding and management of transverse stimulated Raman scattering in KDP crystals and its deuterated analog, DKDP, typically used for frequency conversion and polarization control in large-aperture laser systems. Key to this experimental platform is the use of high-quality spherical samples that enable one to measure the Raman scattering cross section in a wide range of geometries using only a single sample. The effect of polarization rotation of both the pump light and the collected Raman signal must be carefully considered in data analysis and can give rise to artifacts, which can, in part, be mitigated by reducing the input and collection cone angles.

47 OTHER INSTRUMENTATION↗

DOE OSTI2022

Simulating the filamentation of smoothed laser beams with three-dimensional nonlinear dynamics

In a plasma, the ponderomotive force of an inhomogeneous electromagnetic field expels plasma from regions of high intensity. When a laser propagates through a plasma, this force creates density wells that subsequently modify the index of refraction. The beam refracts and focuses into these wells and may filament. In extreme cases, the laser beam will spray due to increasing angular divergence of the beam. The threshold for ponderomotive self-focusing is well established for isolated laser hotspots or speckles. Here, we define a practical threshold for characterizing the filamentation of thousands of speckles that are found in the focal plane of high-power laser beams spatially smoothed with random phase plates as used at high energy and power laser facilities studying inertial confinement fusion. This threshold is tested against three-dimensional simulations of speckled laser light propagating through plasma. Four metrics are applied to assess filamentation: the fraction of power above five times the average intensity, an effective f-number, the mean-squared perpendicular wavenumber, and the fraction of rarefied density with deviation from the initial density exceeding | δn/ n| = 0.1. The speckled beams studied are generated by random phase plates, both with and without additional polarization smoothing, in a parameter regime of relevance to indirect drive experiments. While filamentation has been discussed extensively in the literature, we believe this to be the first published simulation study with three-dimensional nonlinear hydrodynamics that addresses the onset threshold of ponderomotive filamentation and establishes the lengths and time scales necessary to reach a statistical steady state.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

NASA NTRS2009

Method for Measuring the Volume-Scattering Function of Water

The volume scattering function (VSF) of seawater affects visibility, remote sensing properties, in-water light propagation, lidar performance, and the like. Currently, it s possible to measure only small forward angles of VSF, or to use cumbersome, large, and non-autonomous systems. This innovation is a method of measuring the full range of VSF using a portable instrument. A single rapid-sensing photosensor is used to scan a green laser beam, which delivers the desired measurement. By using a single sensor, inter-calibration is avoided. A compact design is achieved by using drift-free detector electronics, fiber optics, and a new type of photomultiplier. This provides a high angular resolution of 1 or better, as well as the ability to focus in on a VSF region of particular interest. Currently, the total scattering of light is measured as a difference from the other two parts of the light budget equation. This innovation will allow the direct calculation of the total scattering of light by taking an integral of the VSF over all angles. This directly provides one of the three components of the light budget equation, allowing greater versatility in its calculation.

Agrawal, Yogesh C.↗

NASA NTRS2014

A Synthesis of Light Absorption Properties of the Arctic Ocean: Application to Semi-analytical Estimates of Dissolved Organic Carbon Concentrations from Space

The light absorption coefficients of particulate and dissolved materials are the main factors determining the light propagation of the visible part of the spectrum and are, thus, important for developing ocean color algorithms. While these absorption properties have recently been documented by a few studies for the Arctic Ocean [e.g., Matsuoka et al., 2007, 2011; Ben Mustapha et al., 2012], the datasets used in the literature were sparse and individually insufficient to draw a general view of the basin-wide spatial and temporal variations in absorption. To achieve such a task, we built a large absorption database at the pan-Arctic scale by pooling the majority of published datasets and merging new datasets. Our results showed that the total non-water absorption coefficients measured in the Eastern Arctic Ocean (EAO; Siberian side) are significantly higher 74 than in the Western Arctic Ocean (WAO; North American side). This higher absorption is explained 75 by higher concentration of colored dissolved organic matter (CDOM) in watersheds on the Siberian 76 side, which contains a large amount of dissolved organic carbon (DOC) compared to waters off 77 North America. In contrast, the relationship between the phytoplankton absorption (a()) and chlorophyll a (chl a) concentration in the EAO was not significantly different from that in the WAO. Because our semi-analytical CDOM absorption algorithm is based on chl a-specific a() values [Matsuoka et al., 2013], this result indirectly suggests that CDOM absorption can be appropriately erived not only for the WAO but also for the EAO using ocean color data. Derived CDOM absorption values were reasonable compared to in situ measurements. By combining this algorithm with empirical DOC versus CDOM relationships, a semi-analytical algorithm for estimating DOC concentrations for coastal waters at the Pan-Arctic scale is presented and applied to satellite ocean color data.

Pan-Arctic↗

NASA NTRS2005

Coherence Effects in Ring Laser Gyros

We predict the propagation of slow and fast light in two co-resonant coupled optical resonators. In coupled resonators, slow light can propagate without attenuation by a cancellation of absorption as a result of mode splitting and destructive interference, whereas transparent fast light propagation can be achieved by the assistance of gain and splitting of the intracavity resonances, which consequently change the dispersion from normal to anomalous. The effective steady-state response of coupled- resonators is derived using the temporal coupled-mode formalism, and the absorptive and dispersive responses are described. Specifically, the occurrence of slow light via coupled-resonator-induced transparency and gain-assisted fast light are discussed. Keywords: whispering gallery modes, optical resonators, slow light, fast light, superluminal pulse propagation, coupled optical resonators.

Smith, David D.↗

DOE OSTI2022

Broadband Asymmetric Transmission of Linearly Polarized Mid‐Infrared Light Based on Quasi‐3D Metamaterials

Abstract Metamaterials consisting of subwavelength resonators offer an exciting opportunity for realizing asymmetric transmission (AT) of linearly polarized light. However, to date, only moderate/narrow‐band AT responses have been obtained in metadevices based on stacked planar nanostructures. Here, leveraging a combination of a genetic algorithm (GA) based optimization method and a membrane projection lithography (MPL) fabrication approach, a quasi‐3D metamaterial for broadband AT of linearly polarized mid‐infrared light is demonstrated. Facilitated by the customized GA, an efficient exploration of 3D plasmonic meta‐atoms with broken mirror symmetry in the light propagation direction allows the satisfaction of the rigorous conditions for AT of linearly polarized waves over a broad wavelength range. Confirmed by surface current analysis, the observed AT behavior is attributed to the resonant coupling between the plasmonic nanostructures located on the two orthogonal walls of the MPL cavities. Incorporating an advanced inverse‐design method and a state‐of‐art fabrication technique, the methodology used in the present study provides a promising route for exploiting 3D metamaterials with sophisticated functionalities via effectively exploring the high‐dimensional parametric space offered by true 3D meta‐atoms.

Whiting, Eric B.↗

DOE OSTI2022

Tunable, Homoepitaxial Hyperbolic Metamaterials Enabled by High Mobility CdO

We report propagating light exhibits hyperbolicity in strongly anisotropic materials where the principal components of the dielectric tensor are opposite in sign. While hyperbolicity occurs naturally in anisotropic polar dielectrics, wherein optical phonons along orthogonal crystal axes are nondegenerate, such optical anisotropy can also be engineered in hyperbolic metamaterials (HMMs): thin film superlattices of alternating dielectric and metallic layers. Contrasted with the severely limited tunability of natural hyperbolic materials, the hyperbolic behavior of HMMs can be tailored significantly both through superlattice design and material selection. However, so far HMMs have suffered from high optical losses, hindering their performance. In this report, broadly tunable (λ = 2–5 µm) Type I and II hyperbolic modes with low losses (quality (Q)-factors up to 19.7) are observed through attenuated total reflectance measurements of monolithic, homoepitaxial superlattices of high- and low-doped cadmium oxide (CdO). Further, the low losses offered by CdO enable the first demonstration of real-space imaging of hyperbolic plasmon polaritons in nanoresonators by scattering-type scanning near-field optical microscopy—previously only possible for hyperbolic phonon polariton materials. Tunable, low-loss CdO HMMs promise designability for applications such as on-chip photonics, super-resolution imaging (hyperlensing), enhanced emission, novel emitter designs, and possibly quantum nanophotonic and time variant metasurfaces.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Time‐Lapse Image Classification Using a Diffractive Neural Network

Diffractive deep neural networks (D 2 NNs), comprised of spatially engineered passive surfaces, collectively process optical input information at the speed of light propagation through a thin diffractive volume, without any external computing power. Diffractive networks were demonstrated to achieve all‐optical object classification and perform universal linear transformations. Herein, a “time‐lapse” image classification scheme using a diffractive network is demonstrated for the first time, significantly advancing its classification accuracy and generalization performance on complex input objects by using the lateral movements of the input objects and/or the diffractive network, relative to each other. In a different context, such relative movements of the objects and/or the camera are routinely being used for image super‐resolution applications; inspired by their success, a time‐lapse diffractive network is designed to benefit from the complementary information content created by controlled or random lateral shifts. The design space and performance limits of time‐lapse diffractive networks are numerically explored, revealing a blind testing accuracy of 62.03% on the optical classification of objects from the CIFAR‐10 dataset. This constitutes the highest inference accuracy achieved so far using a single diffractive network on the CIFAR‐10 dataset. Time‐lapse diffractive networks will be broadly useful for the spatiotemporal analysis of input signals using all‐optical processors.

36 MATERIALS SCIENCE↗

DOE OSTI2025

RSPECT: A PROSPECT-based model incorporating the real structure of rice leaves

Radiative transfer models (RTMs) describe how light is absorbed, scattered, and transmitted within leaves by simulating mechanistic light propagation processes. The PROSPECT model is based on measurable parameters (the leaf biochemical content) and a non-measurable parameter (the leaf anatomical structure represented by the leaf structure parameter (N)). The effect of N on the optical properties of leaves has been investigated through a number of local and global sensitivity analyses. Other studies have directly evaluated the effect of the leaf anatomical structure on spectral reflectance, particularly in the near infrared region. However, the relationship between N and the anatomical structure is unclear. Here, in this study, we leveraged eLeaf, a ray tracing-based 3D rice leaf simulator, to establish relationships between leaf anatomical features and spectral properties, enabling us to replace N in the PROSPECT-4 model with measurable leaf anatomical parameters and develop the RSPECT model. The leaf thickness at minor vein, leaf thickness at bulliform cells, mesophyll thickness at minor vein, and distance between two minor veins could be used to predict N effectively. The RSPECT model achieved spectral simulation accuracy comparable to PROSPECT-4 and was more suitable for parameter inversion of the physical and chemical properties of rice leaves, with relative root mean square errors of 7.4% for chlorophyll content, 5.6% for equivalent water thickness, and 7.5% for dry matter content. In conclusion, RSPECT improves radiative transfer modeling by integrating measurable anatomical features and provides a framework for extending this approach to other vegetation types.

hyperspectral↗

DOE OSTI2025

Nonlinear Topological Photonics: Capturing Nonlinear Dynamics and Optical Thermodynamics

Combining multiple optical resonators or engineering dispersion of complex media has provided an effective method for demonstrating topological physics controlling photons in unprecedented ways such as unidirectional light propagation and spatially localized modes between an interface or on a corner. Further, adding nonlinear responses to those topological photonic systems has enabled achieving diverse phases of photons in both space and time, allowing for more functionalities in photonic devices that provide a new playground for studying dynamic features of nonlinear topological systems. However, most methods for describing nonlinear topological photonic systems rely on linear topological theories, making it challenging to accurately characterize the topology of nonlinear systems. Thus, substantial efforts have focused on rigorously describing nonlinear topological phases and developing effective tools to analyze nonlinear topological effects. Meanwhile, coupled multimode optical waveguides with nonlinear dynamic responses provide an excellent platform for the statistical description of photons, opening a new paradigm called “optical thermodynamics”. This review will introduce the basic concepts of nonlinear topological photonics and the recent development of theoretical approaches focusing on data-driven approaches for creating phase diagrams as well as the spectral localizer framework and the pseudospectrum method for understanding optical nonlinearities in topological systems. In addition, the new concept of optical thermodynamics will be introduced with some recent theoretical works.

Topological photonics↗

DOE OSTI2020

Nonreciprocal directional dichroism of a chiral magnet in the visible range

Nonreciprocal directional dichroism is an unusual light–matter interaction that gives rise to diode-like behavior in low-symmetry materials. The chiral varieties are particularly scarce due to the requirements for strong spin–orbit coupling, broken time-reversal symmetry, and a chiral axis. Here we bring together magneto-optical spectroscopy and first-principles calculations to reveal high-energy, broadband nonreciprocal directional dichroism in Ni 3 TeO 6 with special focus on behavior in the metamagnetic phase above 52 T. In addition to demonstrating this effect in the magnetochiral configuration, we explore the transverse magnetochiral orientation in which applied field and light propagation are orthogonal to the chiral axis and, by so doing, uncover an additional configuration with a unique nonreciprocal response in the visible part of the spectrum. In a significant conceptual advance, we use first-principles methods to analyze how the Ni 2+ d-to-d on-site excitations develop magneto-electric character and present a microscopic model that unlocks the door to theory-driven discovery of chiral magnets with nonreciprocal properties.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2025

Attosecond control and measurement of chiral photoionization dynamics

Many chirality-sensitive light–matter interactions are governed by chiral electron dynamics. Therefore, the development of advanced technologies making use of chiral phenomena would critically benefit from measuring and controlling chiral electron dynamics on their natural attosecond timescales. Such endeavours have so far been hampered by the lack of characterized circularly polarized attosecond pulses, an obstacle that has recently been overcome. Here we introduce chiroptical spectroscopy with attosecond pulses and demonstrate attosecond coherent control over photoelectron circular dichroism (PECD), as well as the measurement of chiral asymmetries in the forward–backward and angle-resolved photoionization delays of chiral molecules. We show that co-rotating attosecond and near-infrared (IR) pulses can nearly double the PECD and even change its sign compared with single-photon ionization. We demonstrate that chiral photoionization delays depend on both polar and azimuthal angles of photoemission in the light-propagation frame, requiring 3D momentum resolution. We measure forward–backward chiral-sensitive delays of up to 60 as and polar-angle-resolved photoionization delays of up to 240 as, which include an asymmetry of about 60 as originating from chirality in the continuum–continuum transitions. Attosecond chiroptical spectroscopy opens the door to quantitatively understanding and controlling the dynamics of chiral molecules on the electronic timescale.

Atomic and molecular interactions with photons↗

DOE OSTI2020

Determination of the Raman polarizability tensor in the optically anisotropic crystal potassium dihydrogen phosphate and its deuterated analog

Abstract The Raman tensor of the dominant A 1 modes of the nonlinear optical crystalline material potassium dihydrogen phosphate and its 70% deuterated analog have been ascertained. Challenges in determining the A 1 mode tensor element values based on previous reports have been resolved using a specially designed experimental setup that makes use of spherical crystal samples. This novel experimental design enabled the determination of measurement artifacts, including polarization rotation of the pump and/or scattered light propagating through the sample and the contribution of additional overlapping phonon modes, which have hindered previous efforts. Results confirmed that the polarization tensor is diagonal, and matrix elements were determined with high accuracy.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Using the Gerchberg-Saxton algorithm to reconstruct nonmodulated pyramid wavefront sensor measurements

Adaptive optics (AO) is a technique to improve the resolution of ground-based telescopes by correcting, in real-time, optical aberrations due to atmospheric turbulence and the telescope itself. With the rise of Giant Segmented Mirror Telescopes (GSMT), AO is needed more than ever to reach the full potential of these future observatories. One of the main performance drivers of an AO system is the wavefront sensing operation, consisting of measuring the shape of the above mentioned optical aberrations. Aims. The non-modulated pyramid wavefront sensor (nPWFS) is a wavefront sensor with high sensitivity, allowing the limits of AO systems to be pushed. The high sensitivity comes at the expense of its dynamic range, which makes it a highly non-linear sensor. We propose here a novel way to invert nPWFS signals by using the principle of reciprocity of light propagation and the Gerchberg-Saxton (GS) algorithm. We test the performance of this reconstructor in two steps: the technique is first implemented in simulations, where some of its basic properties are studied. Then, the GS reconstructor is tested on the Santa Cruz Extreme Adaptive optics Laboratory (SEAL) testbed located at the University of California Santa Cruz. This new way to invert the nPWFS measurements allows us to drastically increase the dynamic range of the reconstruction for the nPWFS, pushing the dynamics close to a modulated PWFS. The reconstructor is an iterative algorithm requiring heavy computational burden, which could be an issue for real-time purposes in its current implementation. However, this new reconstructor could still be helpful in the case of many wavefront control operations. In conclusion, this reconstruction technique has also been successfully tested on the Santa Cruz Extreme AO Laboratory (SEAL) bench where it is now used as the standard way to invert nPWFS signal.

47 OTHER INSTRUMENTATION↗

DOE OSTI2021

Investigations of radiation damaged arranged scintillating particle composites

Composites consisting of periodically arranged scintillating particles within an acrylic (poly methyl methacrylate) matrix are excellent templates for the gamma-insensitive detection of fast neutrons. In order to study the impact of radiation damage on acrylic-based scintillating particle composites, we exposed acrylic samples to different doses of fast neutrons up to 119.7 kGy and investigated the change in optical characteristics using optical absorption spectroscopy in the 200–800 nm wavelength range. The experimental results are compared to coupled MCNP6 and optical ray-tracing (FRED) simulations, and qualitative agreement is found. Neutron-induced radiation damage in the acrylic matrix manifests as a red-shift in the ultra-violet absorption edge of the acrylic and a corresponding decrease in the light propagation efficiency, which leads to detector performance degradation. We show for the first time that the effects of radiation damage can be mitigated by the use of wavelength-shifting coatings. We predict that composites with wavelength-shifting coatings can enable neutron detectors with high tolerance against neutron-induced radiation damage, a property that is particularly desired for neutron detection in high radiation environments.

36 MATERIALS SCIENCE↗