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At least 289 records · Page 16
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

High‐Order Nonlinear Frequency Conversion in Transparent Conducting Oxide Thin Films

The study of conductive oxides has gained momentum within the photonics community due to their unique linear and nonlinear optical properties. Despite recent experiments reporting on high harmonic generation from thin films, the optical/electronic behavior of these compounds at the nanoscale is still not fully understood due to the lack of a suitable theoretical model. In the present work, aluminum zinc oxide is excited near its epsilon-near-zero crossing point using incident femtosecond pulses having peak power densities in the 1 TW cm −2 range. A relatively efficient frequency up-conversion including even and odd harmonics up to the seventh order is observed. A hydrodynamic-Maxwell theoretical approach is adopted, capable of simultaneously taking into account linear and nonlinear dispersions, nonlocal effects, surface, magnetic, and bulk nonlinearities in a spectral region that spans over two and a half octaves from the UV to the NIR region. The study enables a deeper understanding of the fundamental material parameters regulating optical nonlinearities, providing important insights to engineer this class of materials for applications in sensing, ultra-fast physics, and spectroscopy.

material modeling↗
DOE OSTI2022

Thin liquid film as an optical nonlinear-nonlocal medium and memory element in integrated optofluidic reservoir computer

Understanding light–matter interaction lies at the core of our ability to harness physical effects and to translate them into new capabilities realized in modern integrated photonics platforms. Here, we present the design and characterization of optofluidic components in an integrated photonics platform and computationally predict a series of physical effects that rely on thermocapillary-driven interaction between waveguide modes and topography changes of optically thin liquid dielectric film. Our results indicate that this coupling introduces substantial self-induced phase change and transmittance change in a single channel waveguide, transmittance through the Bragg grating waveguide, and nonlocal interaction between adjacent waveguides. We then employ the self-induced effects together with the inherent built-in finite relaxation time of the liquid film, to demonstrate that the light-driven deformation can serve as a reservoir computer capable of performing digital and analog tasks, where the gas–liquid interface operates both as a nonlinear actuator and as an optical memory element.

42 ENGINEERING↗
DOE OSTI2021

Wavelength conversion through plasmon-coupled surface states

Surface states generally degrade semiconductor device performance by raising the charge injection barrier height, introducing localized trap states, inducing surface leakage current, and altering the electric potential. We show that the giant built-in electric field created by the surface states can be harnessed to enable passive wavelength conversion without utilizing any nonlinear optical phenomena. Photo-excited surface plasmons are coupled to the surface states to generate an electron gas, which is routed to a nanoantenna array through the giant electric field created by the surface states. The induced current on the nanoantennas, which contains mixing product of different optical frequency components, generates radiation at the beat frequencies of the incident photons. We utilize the functionalities of plasmon-coupled surface states to demonstrate passive wavelength conversion of nanojoule optical pulses at a 1550 nm center wavelength to terahertz regime with efficiencies that exceed nonlinear optical methods by 4-orders of magnitude.

42 ENGINEERING↗
DOE OSTI2020

Nonlinear Spectroscopy of Collective Modes in an Excitonic Insulator

The nonlinear optical response of an excitonic insulator coupled to lattice degrees of freedom is shown to depend in strong and characteristic ways on whether the insulating behavior originates primarily from electron-electron or electron-lattice interactions. Linear response optical signatures of the massive phase mode and the amplitude (Higgs) mode are identified. Upon nonlinear excitation resonant to the phase mode, a new in-gap mode at twice the phase mode frequency is induced, leading to a huge second harmonic response. Excitation of in-gap phonon modes leads to different and much smaller effects. A Landau-Ginzburg theory analysis explains these different behaviors and reveals that a parametric resonance of the strongly excited phase mode is the origin of the photoinduced mode in the electron-dominant case. Here, the difference in the nonlinear optical response serves as a measure of the dominant mechanism of the ordered phase.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Nonlinear Dispersion Relation and Out‐of‐Plane Second Harmonic Generation in MoSSe and WSSe Janus Monolayers

Janus transition metal dichalcogenides are an emerging class of atomically thin materials with engineered broken mirror symmetry that gives rise to long‐lived dipolar excitons, Rashba splitting, and topologically protected solitons. They hold great promise as a versatile nonlinear optical platform due to their broadband harmonic generation tunability, ease of integration on photonic structures, and nonlinearities beyond the basal crystal plane. Here, second and third harmonic generation in MoSSe and WSSe Janus monolayers is studied. Polarization‐resolved spectroscopy is used to map the full second‐order susceptibility tensor of MoSSe, including its out‐of‐plane components. In addition, the effective third‐order susceptibility and the second‐order nonlinear dispersion close to exciton resonances for both MoSSe and WSSe are measured at room and cryogenic temperatures. This work sets a bedrock for understanding the nonlinear optical properties of Janus transition metal dichalcogenides and probing their use in the next‐generation on‐chip multifaceted photonic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Magnon-mediated exciton–exciton interaction in a van der Waals antiferromagnet

Excitons are fundamental excitations that govern the optical properties of semiconductors. Interactions between excitons can lead to various emergent phases of matter and large nonlinear optical responses. In most semiconductors, excitons interact via exchange interactions or phase-space filling. Correlated materials that host excitons coupled to other degrees of freedom could offer pathways for controlling these interactions. Here, in this study, we demonstrate magnon-mediated interactions between excitons in CrSBr, an antiferromagnetic semiconductor. These interactions manifest as the dependence of the exciton energy on the exciton density via a magnonic adjustment of the spin canting angle. Our study demonstrates the emergence of quasiparticle-mediated interactions in correlated quantum materials, leading to large nonlinear optical responses and potential device concepts such as magnon-mediated quantum transducers.

36 MATERIALS SCIENCE↗
NASA NTRS1989

Novel photovoltaic delta-doped GaAs superlattice structure

An asymmetric delta-doped GaAs structure is described which exhibits novel photovoltaic effects and low-intensity nonlinear optics. Of particular interest in this kind of structure is the ability to design the electrooptical and nonlinear optical properties and the material response time over a wide range by appropriate design of the doping profile.

Glass, A. M.↗
DOE OSTI2024

Nonlinear effects in manybody van der Waals interactions

Van der Waals interactions are ubiquitous and they play an important role for the stability of materials. Current understanding of this type of coupling is based on linear response theory, while optical nonlinearities are rarely considered in this context. Many materials, however, exhibit strong optical nonlinear response, which prompts further evaluation of dispersive forces beyond linear response. Here we present a approach that takes into account linear and nonlinear properties of all dipolar nanoparticles in a given system. This method is based on a Hamiltonian for nonlinear dipoles, which we apply in different systems uncovering a complex interplay of distance, anisotropy, polarizabilities, and hyperpolarizabilities in the vdW energy. This investigation broadens our basic understanding of dispersive interactions, especially in the context of nonlinear materials. Published by the American Physical Society 2024

Le, Dai-Nam (ORCID:0000000307568742)↗
DOE OSTI2020

Strong Coupling in All-Dielectric Intersubband Polaritonic Metasurfaces

Mie-resonant dielectric metasurfaces are excellent candidates for both fundamental studies related to light–matter interactions and for numerous applications ranging from holography to sensing to nonlinear optics. To date, however, most applications using Mie metasurfaces utilize only weak light-matter interaction. Furthermore, we go beyond the weak coupling regime and demonstrate for the first time strong polaritonic coupling between Mie photonic modes and intersubband (ISB) transitions in semiconductor heterostructures. Furthermore, along with demonstrating ISB polaritons with Rabi splitting as large as 10%, we also demonstrate the ability to tailor the strength of strong coupling by engineering either the semiconductor heterostructure or the photonic mode of the resonators. Unlike previous plasmonic-based works, our new all-dielectric metasurface approach to generate ISB polaritons is free from ohmic losses and has high optical damage thresholds, thereby making it ideal for creating novel and compact mid-infrared light sources based on nonlinear optics.

42 ENGINEERING↗
DOE OSTI2023

Light-induced shift current vortex crystals in moiré heterobilayers

Transition metal dichalcogenide (TMD) moiré superlattices provide an emerging platform to explore various light-induced phenomena. Recently, the discoveries of novel moiré excitons have attracted great interest. The nonlinear optical responses of these systems are however still underexplored. Here, we report investigation of light-induced shift currents (a second-order response generating DC current from optical illumination) in the WSe 2 /WS 2 moiré superlattice. We identify a striking phenomenon of the formation of shift current vortex crystals—i.e., two-dimensional periodic arrays of moiré-scale current vortices and associated magnetic fields with remarkable intensity under laboratory laser setup. Furthermore, we demonstrate high optical tunability of these current vortices—their location, shape, chirality, and magnitude can be tuned by the frequency, polarization, and intensity of the incident light. Electron-hole interactions (excitonic effects) are found to play a crucial role in the generation and nature of the shift current intensity and distribution. Our findings provide a promising all-optical control route to manipulate nanoscale shift current density distributions and magnetic field patterns, as well as shed light on nonlinear optical responses in moiré quantum matter and their possible applications.

36 MATERIALS SCIENCE↗
NASA NTRS1995

Photodeposition of amorphous polydiacetylene films from monomer solutions onto transparent substrates

Polydiacetylenes are a very promising class of polymers for both photonic and electronic applications because of their highly conjugated structures. For these applications, high-quality thin polydiacetylene films are required. We have discovered a novel technique for obtaining such films of a polydiacetylene derivative of 2-methyl-4-nitroaniline using photodeposition from monomer solutions onto UV transparent substrates. This heretofore unreported process yields amorphous polydiacetylene films with thicknesses on the order of I micron that have optical quality superior to that of films grown by standard crystal growth techniques. Furthermore, these films exhibit good third-order nonlinear optical susceptibilities; degenerate four-wave mixing experiments give x(3) values on the order of 10(exp -8) - 10(exp -7) esu. We have conducted masking experiments which demonstrate that photodeposition occurs only where the substrate is directly irradiated, clearly indicating that the reaction occurs at the surface. Additionally, we have also been able to carry out photodeposition using lasers to form thin polymer circuits. In this work, we discuss the photodeposition of polydiacetylene thin films from solution, perform chemical characterization of these films, investigate the role of the substrate, speculate on the mechanism of the reaction, and make a preliminary determination of the third-order optical nonlinearity of the films. This simple, straightforward technique may ultimately make feasible the production of polydiacetylene thin films for technological applications.

Paley, M. S.↗
DOE OSTI2022

Broadband‐Tunable Third‐Harmonic Generation Using Phase‐Change Chalcogenides

Despite remarkable progress in passive nonlinear nanophotonics, dynamically controlled ultracompact nonlinear optical sources with high efficiency remain elusive. Nonvolatility, large refractive index contrast between amorphous and crystalline phases, low thermal threshold for crystallization, and particularly high‐third‐order nonlinear optical susceptibility of phase‐change alloy Ge 2 Sb 2 Te 5 (GST) make it a promising candidate for active subwavelength metaphotonic structures for realization of third‐harmonic generation (THG) devices. Herein, a GST‐based asymmetric Fabry–Perot cavity is numerically designed and experimentally demonstrated to show a dynamically reconfigurable structure with a large shift of the THG resonant band. In addition, continuous resonant spectral shifting bridged by a precisely controlled semicrystalline phase of GST is realized. Tunable THG with the fundamental wavelength ranging from 1150 to 1400 nm is presented, which corresponds to a broadband THG source in the violet‐blue visible wavelength range. Herein, the potential of GST subwavelength structures as a reliable platform for realization of the broadband‐tunable frequency‐conversion sources for applications such as THG microscopy and optical communication is indicated.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2025

Multistate Geometry of Shift Current and Polarization

The quantum metric and Berry curvature capture essential properties of nontrivial Bloch states and underpin many fascinating phenomena. However, it becomes increasingly evident that a more comprehensive understanding of quantum state geometry is necessary to explain properties involving Bloch states of multiple bands, such as optical transitions. To this end, we employ quantum state projectors to develop an explicitly gauge-invariant formalism and demonstrate its power with applications to nonlinear optics and the theory of electronic polarization. We provide a simple expression for the shift current that resolves its precise relation to the moments of electronic polarization, clarifies the treatment of band degeneracies, and reveals its decomposition into the sum of the skewness of the occupied states and intrinsically multistate geometry. The projector approach is applied to calculate nonlinear optical properties of transition metal dichalcogenides (TMDs) layers, using previously calculated minimal tight-binding models, and demonstrated analytically on a three-band generalization of the Rice-Mele chain to elucidate the different contributions. We close with comments on further applications of the projector operator approach to multistate geometry.

electric polarization↗
DOE OSTI2024

InAs Terahertz Metalens Emitter for Focused Terahertz Beam Generation

Metasurfaces have opened doors to combining multiple photonic functionalities in a single compact device. In particular, the ability to generate short terahertz (THz) pulses with precise wavefront engineering in a single THz metasurface redefined the role metasurfaces can play in THz systems. Here, an InAs metalens emitter which generates and focuses a THz pulse beam is demonstrated using a 130 nm thick InAs metasurface designed as a binary‐phase Fresnel zone plate. The THz beam is focused to a spot of ≈430 μm at 1 THz with a short focal length of 5 mm and large numerical aperture of 0.5. Nanoscale InAs Mie resonators comprising the metasurface enable THz generation with an amplitude as high as 20 times compared to plasmonic THz emitters and several times compared to a 1 mm thick ZnTe crystal. This InAs metasurface emitter provides a new paradigm for designing THz imaging, spectroscopy, and communication systems, where THz beam generation and shaping are performed with a single device without compromising the generation efficiency, while eliminating losses and avoiding limitations of phase matching of conventional nonlinear optics approaches.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Large Enhancements in Optical and Piezoelectric Properties in Ferroelectric Zn 1- x Mg x O Thin Films through Engineering Electronic and Ionic Anharmonicities

Multifunctionality as a paradigm requires materials exhibiting multiple superior properties. Integrating second-order optical nonlinearity and large bandgap with piezoelectricity can, for example, enable broadband, strain-tunable photonics. Though very different phenomena at distinct frequencies, both second-order optical nonlinearity and piezoelectricity are third-rank polar tensors present only in acentric crystal structures. However, simultaneously enhancing both phenomena is highly challenging since it involves competing effects with tradeoffs. Recently, a large switchable ferroelectric polarization of ≈80 μC cm –2 was reported in Zn 1-x Mg x O films. Here, ferroelectric Zn 1-x Mg x O is demonstrated to be a platform that hosts simultaneously a 30% increase in the electronic bandgap, a 50% enhancement in the second harmonic generation (SHG) coefficients, and a near 200% improvement in the piezoelectric coefficients over pure ZnO. These enhancements are shown to be due to a 400% increase in the electronic anharmonicity and a ≈200% decrease in the ionic anharmonicity with Mg substitution. Precisely controllable periodic ferroelectric domain gratings are demonstrated down to 800 nm domain width, enabling ultraviolet quasi-phase-matched optical harmonic generation as well as domain-engineered piezoelectric devices.

36 MATERIALS SCIENCE↗
NASA NTRS2004

A Resonator for Low-Threshold Frequency Conversion

A proposed toroidal or disklike dielectric optical resonator (dielectric optical cavity) would be made of an optically nonlinear material and would be optimized for use in parametric frequency conversion by imposition of a spatially periodic permanent electric polarization. The poling (see figure) would suppress dispersions caused by both the material and the geometry of the optical cavity, thereby effecting quasi-matching of the phases of high-resonance-quality (high-Q) whispering-gallery electromagnetic modes. The quasi-phase-matching of the modes would serve to maximize the interactions among them. Such a resonator might be a prototype of a family of compact, efficient nonlinear devices for operation over a broad range of optical wavelengths. A little background information is prerequisite to a meaningful description of this proposal: (1) Described in several prior NASA Tech Briefs articles, the whispering-gallery modes in a component of spheroidal, disklike, or toroidal shape are waveguide modes that propagate circumferentially and are concentrated in a narrow toroidal region centered on the equatorial plane and located near the outermost edge. (2) For the sake of completeness, it must be stated that even though optical resonators of the type considered here are solid dielectric objects and light is confined within them by total internal reflection at dielectric interfaces without need for mirrors, such components are sometimes traditionally called cavities because their effects upon the light propagating within them are similar to those of true cavities bounded by mirrors. (3) For a given set of electromagnetic modes interacting with each other in an optically nonlinear material (e.g., modes associated with the frequencies involved in a frequency-conversion scheme), the threshold power for oscillation depends on the mode volumes and the mode-overlap integral. (4) Whispering-gallery modes are attractive in nonlinear optics because they maximize the effects of nonlinearities by occupying small volumes and affording high Q values

Iltchenko, Vladimir↗
DOE OSTI2026

Experimental Studies of Nonlinear Integrable Optics with Elliptic Potentials

The stable transport of charged particle beams is the core challenge in designing and operating accelerators. The current paradigm for transverse focusing is based on quadrupole and dipole elements, described as a linear integrable Hamiltonian by Courant and Snyder. The operational limits of high intensity accelerators are often determined by collective instabilities within the beam. Nonlinear elements may be added to suppress certain forms of these collective effects, but restrict the range of stable trajectories. These shortcomings motivate extending to a nonlinear integrable system which can offer the benefits of suppressing collective instabilities without limiting the stable trajectories. Danilov and Nagaitsev proposed a novel nonlinear integrable system with elliptical potentials, which could be implemented as magnetic elements in an accelerator. Such a system has been implemented for practical verification in the integrable optics test accelerator (IOTA), a small storage ring constructed for beam dynamics studies. Electron beam studies in IOTA treat the low-emittance beam as a macroparticle for detailed probing of the expected single particle dynamics. This dissertation details new measurements of the nonlinear integrable system relevant for practical implementation. Turn-by-turn measurements of the kicked beam responses are used for phase space reconstruction and analysis of the predicted nonlinear dynamics. The stability and aperture for various nonlinear configurations are measured with beam losses. Amplitude dependent detuning, a core figure of merit for suppressing instabilities, is measured and compared with high fidelity particle tracking simulations. The synchrotron radiation images of circulating beam allow direct measurements of the topology and lifetime in configurations where nonlinear focusing terms dominate.

Wieland, John [Michigan U.] (ORCID:000000028971852↗
DOE OSTI2020

Nonlinear spectroscopy in the condensed phase: The role of Duschinsky rotations and third order cumulant contributions

First-principles modeling of nonlinear optical spectra in the condensed phase is highly challenging because both environment and vibronic interactions can play a large role in determining spectral shapes and excited state dynamics. In this work, we compute two dimensional electronic spectroscopy (2DES) signals based on a cumulant expansion of the energy gap fluctuation operator, with specific focus on analyzing mode mixing effects introduced by the Duschinsky rotation and the role of the third order term in the cumulant expansion for both model and realistic condensed phase systems. We show that for a harmonic model system, the third order cumulant correction captures effects introduced by a mismatch in curvatures of ground and excited state potential energy surfaces, as well as effects of mode mixing. We also demonstrate that 2DES signals can be accurately reconstructed from purely classical correlation functions using quantum correction factors. We then compute nonlinear optical spectra for the Nile red and methylene blue chromophores in solution, assessing the third order cumulant contribution for realistic systems. We show that the third order cumulant correction is strongly dependent on the treatment of the solvent environment, revealing the interplay between environmental polarization and the electronic-vibrational coupling.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗