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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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89 records · Page 5

Understanding and Controlling the Formation of Nonradiative Defects in Blue Organic Triplet Emitters

Phosphorescent organic light-emitting devices (PHOLEDs) suffer from destructive molecular processes due to triplet-polaron and triplet-triplet annihilation. These processes are energetically driven and hence are particularly active in decreasing the lifetime of blue PHOLEDs. It has recently been shown that increasing triplet radiative rates via the Purcell effect effectively extends the device operational lifetime by reducing the triplet radiative lifetime, thus decreasing their density and the probability of triplet-annihilation reactions. We provide an analytical framework using Marcus theory to explain the observed, approximately exponential relationship between exciton energy and device lifetime. From transient drift-diffusion dynamics, we show that the Purcell effect reduces the exciton density in the steady state and increases the photoluminescent yield, thereby reducing defect generation rates and extending the device lifetime. We control the radiative rate of excitons in microcavities, thereby connecting the exciton energy and decay rates with the observed device lifetime. The device lifetime is shown to follow a power-law dependence on the Purcell factor ( PF m ) with m = 1.5 to 2.5, dependent on the TTA-to-TPA ratio and photoluminescence quantum yield. From our analysis, a fivefold increase in PF has the potential to extend the blue PHOLED lifetime by up to 2 orders of magnitude, making the blue PHOLED lifetime comparable to that of state-of-the-art green PHOLEDs. Published by the American Physical Society 2024

Zhao, Haonan (ORCID:0000000190584422)↗

Spin-orbit–coupled exciton-polariton condensates in lead halide perovskites

Spin-orbit coupling (SOC) is responsible for a range of spintronic and topological processes in condensed matter. Here, we show photonic analogs of SOCs in exciton-polaritons and their condensates in microcavities composed of birefringent lead halide perovskite single crystals. The presence of crystalline anisotropy coupled with splitting in the optical cavity of the transverse electric and transverse magnetic modes gives rise to a non-Abelian gauge field, which can be described by the Rashba-Dresselhaus Hamiltonian near the degenerate points of the two polarization modes. With increasing density, the exciton-polaritons with pseudospin textures undergo phase transitions to competing condensates with orthogonal polarizations. Unlike their pure photonic counterparts, these exciton-polaritons and condensates inherit nonlinearity from their excitonic components and may serve as quantum simulators of many-body SOC processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Chiral flat-band optical cavity with atomically thin mirrors

A fundamental requirement for photonic technologies is the ability to control the confinement and propagation of light. Widely used platforms include two-dimensional (2D) optical microcavities in which electromagnetic waves are confined in either metallic or distributed Bragg reflectors. Recently, transition metal dichalcogenides hosting tightly bound excitons with high optical quality have emerged as promising atomically thin mirrors. In this work, we propose and experimentally demonstrate a subwavelength 2D nanocavity using two atomically thin mirrors with degenerate resonances. Angle-resolved measurements show a flat band, which sets this system apart from conventional photonic cavities. We demonstrate how the excitonic nature of the mirrors enables the formation of chiral and tunable optical modes upon the application of an external magnetic field. Moreover, we show the electrical tunability of the confined mode. Our work demonstrates a mechanism for confining light with high-quality excitonic materials, opening perspectives for spin-photon interfaces, and chiral cavity electrodynamics.

36 MATERIALS SCIENCE↗

Cavity-enabled enhancement of ultrafast intramolecular vibrational redistribution over pseudorotation

Vibrational strong coupling (VSC) between molecular vibrations and microcavity photons yields a few polaritons (light-matter modes) and many dark modes (with negligible photonic character). Although VSC is reported to alter thermally activated chemical reactions, its mechanisms remain opaque. To elucidate this problem, we followed ultrafast dynamics of a simple unimolecular vibrational energy exchange in iron pentacarbonyl [Fe(CO) 5 ] under VSC, which showed two competing channels: pseudorotation and intramolecular vibrational-energy redistribution (IVR). We found that under polariton excitation, energy exchange was overall accelerated, with IVR becoming faster and pseudorotation being slowed down. However, dark-mode excitation revealed unchanged dynamics compared with those outside of the cavity, with pseudorotation dominating. Thus, despite controversies around thermally activated VSC modified chemistry, our work shows that VSC can indeed alter chemistry through a nonequilibrium preparation of polaritons.

Science & Technology - Other Topics↗

Radiative pumping of exciton-polaritons in 2D hybrid perovskites

In addition to their attractive technological applications in photovoltaics and light emitters, the perovskite family of semiconductors has recently emerged as an excellent excitonic material for fundamental studies. Specifically, the 2D hybrid organic-inorganic perovskite (HOIP) offers the added advantage of room temperature investigations owing to their large exciton binding energy. In this work, we strongly couple excitons in 2D HOIP crystals to planar microcavity photons sustaining exciton-polaritons under ambient conditions resulting in a Rabi splitting of 290 meV. Dark excitons directly pump the polariton branch along its dispersion in resonance with the Stokes shifted emission state (radiative pumping), creating a high density of polaritons at higher in-plane momentum ( k || ). We further probe the nonlinear polariton dispersion dynamics at varying input laser fluence, which indicates efficient polariton-polariton scattering and decay to k || = 0 from higher k || . The observation of Stokes shift-assisted energy exchange of dark states with lower polaritons coupled with evidence of efficient polariton-polariton scattering makes 2D HOIPs an attractive platform to study exciton-polariton many-body physics and Bose-Einstein like condensation (BEC) at room temperature.

36 MATERIALS SCIENCE↗

Contribution to the study of composite materials and their damage

Chapter 1 describes the homogenization techniques used for defining the overall behavior of composite materials for conventional cases of linear and perfectly glued elastic constituents. Chapters 2 and 3 focus on solving the problems inherent in two types of degenerated situations: elastic media with microcavities, and elastic media containing rigid inclusions. Through suitable definitions of deformation concepts and macroscopic stresses it is shown that conventional theory results apply naturally to these limits.

Lene, F.↗

Carbon Nanotube-Based Digital Vacuum Electronics and Miniature Instrumentation for Space Exploration

JPL has developed high performance cold cathodes using arrays of carbon nanotube bundles that produce > 15 A/sq cm at applied fields of 5 to 8 V/micron without any beam focusing. They have exhibited robust operation in poor vacuums of 10(exp -6) to 10(exp -4) Torr- a typically achievable range inside hermetically sealed microcavities. Using these CNT cathodes JPL has developed miniature X-ray tubes capable of delivering sufficient photon flux at acceleration voltages of <20kV to perform definitive mineralogy on planetary surfaces; mass ionizers that offer two orders of magnitude power savings, and S/N ratio better by a factor of five over conventional ionizers. JPL has also developed a new class of programmable logic gates using CNT vacuum electronics potentially for Venus in situ missions and defense applications. These digital vacuum electronic devices are inherently high-temperature tolerant and radiation insensitive. Device design, fabrication and DC switching operation at temperatures up to 700 C are presented in this paper.

Carbon Nanotube↗

On Perspectives of Generating Quasi-Fock State via Resonant Self-Phase-Modulation

Optical resonators with cubic nonlinearity were among the ?rst simplest physical systems proposed for generation of squeezed states of light as well as for veri?cation of quantum nondemolition measurement concept. These conventional squeezed states are characterized with Gaussian statistics and positive Wigner function and are frequently treated as semiclassical. In contrast, it is known that the quantum states resulting from the higher order self-phase modulation are characterized with negative Wigner function. Such states can be transformed to an imperfect Fock state via classical biasing. Using these known features, we have developed an experiment strategy for observation and characterization of the nonclassical state in a system based on a high-Q nonlinear optical microcavity. We discuss technical limitations for the state observation associated with the losses in the system and technical noise of the classical optical sources involved in the measurement.

Bilenko, I. A.↗

On Parametric Generation of Deep UV Light in Monolithic Cavities With Cubic Nonlinearity

Coherent ultra violet (UV) light has broad applications in optical atomic clocks and quantum computers. Since availability of semiconductor tunable monochromatic lasers is limited at short wavelengths, optical nonlinear processes are frequently used to produce the desirable radiation wavelength. Optical crystals with quadratic nonlinearity are promising for this purpose because of their transparency and high optical damage threshold. In this paper we discuss a possibility of generation of coherent deep UV light utilizing high quality factor (-Q) monolithic optical microcavities made of crystalline optical materials characterized with cubic nonlinearities. We show that the generation is feasible in spite of the relatively small cubic nonlinearities, due to the ultra-broad-band high optical transparency of the crystals and associated high-Q achievable in the cavities created out of the materials. We found that the birefringence as well as the tensor nature of the nonlinear susceptibility of the crystalline optical materials can simplify the phase matching of the nonlinear processes.

Matsko, A.B.↗

Bound States in the Continuum on a Silicon Chip with Dynamic Tuning

Expanding bound states in the continuum (BIC) beyond photonic crystal systems may enable broader applications benefiting from the unique properties of BIC states. We use photonic integrated circuit to realize a Fabry-Pérot BIC on a silicon chip. The devices consist of cascaded ring resonators with tunable resonance frequencies and phase delays. As a result, the BIC state is dynamically tuned with electrical I/O. We analyze the mechanism of the formation of BIC states in this waveguide system and point out the fundamental differences between the BIC states and electromagnetically induced transparency states in integrated photonics. The high transmission protected by the BIC state enables versatile optical filters, which are capable of independent control over switching, peak position, and quality factor. We also demonstrate the scalability of this platform. As a result, this integrated silicon photonic platform brings opportunities for practical BIC applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Room Temperature Lasing from Semiconducting Single-Walled Carbon Nanotubes

Miniaturized near-infrared semiconductor lasers that are able to generate coherent light with low energy consumption have widespread applications in fields such as optical interconnects, neuromorphic computing, and deep-tissue optogenetics. With optical transitions at near-infrared wavelengths, diameter-tunable electronic structures, and superlative optoelectronic properties, semiconducting single-walled carbon nanotubes (SWCNTs) are promising candidates for nanolaser applications. However, despite significant efforts in this direction and recent progress toward enhancing spontaneous emission from SWCNTs through Purcell effects, SWCNT-based excitonic lasers have not yet been demonstrated. Leveraging an optimized cavity-emitter integration scheme enabled by a self-assembly process, here we couple SWCNT emission to the whispering gallery modes supported by polymer microspheres, resulting in room temperature excitonic lasing with an average lasing threshold of 4.5 kW/cm 2 . The high photostability of SWCNTs allows stable lasing for prolonged duration with minimal degradation. Finally, this experimental realization of excitonic lasing from SWCNTs, combined with their versatile electronic and optical properties that can be further controlled by chemical modification, offers far-reaching opportunities for tunable near-infrared nanolasers that are applicable for optical signal processing, in vivo biosensing, and optoelectronic devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Optimal sensing on an asymmetric exceptional surface

We study the connection between exceptional points (EPs) and optimal parameter estimation, in a simple system consisting of two counterpropagating traveling wave modes in a microring resonator. The unknown parameter to be estimated is the strength of a perturbing cross-coupling between the two modes. Partially reflecting the output of one mode into the other creates a non-Hermitian Hamiltonian that exhibits a family of EPs, creating an exceptional surface (ES). We use a fully quantum treatment of field inputs and noise sources to obtain a quantitative bound on the estimation error by calculating the quantum Fisher information (QFI) in the output fields, whose inverse gives the Cramér-Rao lower bound on the mean-squared error of any unbiased estimator. We determine the bounds for two input states, namely, a semiclassical coherent state and a highly nonclassical NOON state. We find that the QFI is enhanced in the presence of an EP for both of these input states and that both states can saturate the Cramér-Rao bound. We then identify idealized yet experimentally feasible measurements that achieve the minimum bound for these two input states. We also investigate how the QFI changes for parameter values that do not lie on the ES, finding that these can have a larger QFI, suggesting alternative routes to optimize the parameter estimation for this problem.

Exceptional points↗

Er : Li Nb O 3 with High Optical Coherence Enabling Optical Thickness Control

Integrated photonics capable of incorporating rare-earth ions with high optical coherence is desirable for realizing efficient quantum transducers, compact quantum memories, and hybrid quantum systems. Here we describe a photonic platform based on the SmartCut erbium-doped lithium niobate thin film, and explore its stable optical transitions at telecom wavelength in a dilution refrigerator. Optical coherence time of up to 180μs, rivaling the value of bulk crystals, is achieved in optical ridge waveguides and ring resonators. With this integrated platform, we demonstrate tunable light-ion interaction and flexible control of optical thickness by exploiting long waveguides, whose lengths are in principle variable. This unique ability to obtain high optical density using low-concentration ions further leads to the observation of multiecho pulse trains in centimeter-long waveguides. Our results establish a promising photonic platform for quantum information processing with rare-earth ions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Light-Induced Dynamic Frequency Shifting of Microwave Photons in a Superconducting Electro-Optic Converter

Hybrid superconducting-photonic microresonators are a promising platform for realizing microwave-to-optical transduction. However, the absorption of scattered photons by the superconductors leads to unintended microwave resonance-frequency variation and line-width broadening. Here, we experimentally study the dynamics of this effect and its impact on microwave-to-optics conversion in an integrated lithium niobate–superconductor hybrid-resonator platform. Here, we unveil an adiabatic frequency shifting of the intracavity microwave photons induced by the fast photoresponses of the thin-film superconducting resonator. As a result, the temporal and spectral responses of electro-optics transduction are modified and well described by our theoretical model. This work provides insights into the light-induced conversion dynamics that must be considered in future designs of hybrid superconducting-photonic system.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach

We present a microscopic theory for nonlinear optical spectroscopy of N molecules in an optical cavity. Using the Heisenberg-Langevin equation, an analytical expression is derived for the time- and frequency-resolved signals accounting for arbitrary numbers of vibrational excitations. We identify clear signatures of the polariton-polaron interaction from multidimensional projections of the signal, e.g., pathways and timescales. Cooperative dynamics of cavity polaritons against intramolecular vibrations is revealed, along with a crosstalk between long-range coherence and vibronic coupling that may lead to localization effects. Our results further characterize the polaritonic coherence and the population transfer that is slower.

74 ATOMIC AND MOLECULAR PHYSICS↗

Microsphere Integration in Active and Passive Photonics Devices

An important step towards integration of microspheres in compact functional photonics devices, we demonstrate direct efficient coupling of light in and out of high-Q whispering-gallery (WG) modes in silica microspheres using angle-polished single mode fibers.

photonics↗