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At least 163 records · Page 9

Ultrafast thermal modification of strong coupling in an organic microcavity

There is growing interest in using strongly coupled organic microcavities to tune molecular dynamics, including the electronic and vibrational properties of molecules. However, very little attention has been paid to the utility of cavity polaritons as sensors for out-of-equilibrium phenomena, including thermal excitations. Here, we demonstrate that non-resonant infrared excitation of an organic microcavity system induces a transient response in the visible spectral range near the cavity polariton resonances. We show how these optical responses can be understood in terms of ultrafast heating of electrons in the metal cavity mirror, which modifies the effective refractive index and subsequently the strong coupling conditions. The temporal dynamics of the microcavity are strictly determined by carriers in the metal, including the cooling of electrons via electron–phonon coupling and excitation of propagating coherent acoustic modes in the lattice. We rule out multiphoton excitation processes and verify that no real polariton population exists despite their strong transient features. These results suggest the cavity polaritons to be promising as sensitive probes of non-equilibrium phenomena.

36 MATERIALS SCIENCE↗

Large-Area, Highly Crystalline DNA-Assembled Metasurfaces Exhibiting Widely Tunable Epsilon-Near-Zero Behavior

Metasurfaces prepared via bottom-up nanoparticle assembly enable the deliberate manipulation of light in the optical regime, resulting in media with unprecedented optical responses. Here, we report a scalable method to grow highly crystalline 2D metasurfaces comprised of colloidal gold nanocubes, over macroscopic areas, using DNA-mediated assembly under equilibrium conditions. Using an effective medium description, we predict that these plasmonic metasurfaces behave as dielectric media with high refractive indices that can be dynamically tuned by tuning DNA length. Furthermore, we predict that when coupled with an underlying thin gold film, the real permittivity of these metasurfaces exhibits a crossover region between positive and negative values, known as the epsilon-near-zero (ENZ) condition, which can be tuned between 1.5 - 2.6 μm by changing DNA length. Optical characterization performed on the DNA-assembled metasurfaces reveals that the predicted optical properties agree well with measured response. Overall, we propose an efficient method for realizing large-area plasmonic metasurfaces that enable dynamic control over unique optical characteristics. High-index and ENZ metasurfaces operating in the telecommunications regime could have significant implications in high-speed optical computing, optical communications, optical imaging, and other areas.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Nanoscale Imaging of Optical-Frequency Plasmonic Energy Transfer in Individual Nanoparticles and their Assemblies

The nonradiative transfer of energy from plasmonic metal nanostructures to their neighboring environments is a rapidly expanding research area because of its tremendous potential impact on photovoltaics and photocatalysis. Despite the significant progress achieved via optical spectroscopies, understanding the differing and competing energy transfer pathways available to these systems still presents a major challenge due to a lack of insight into their nanoscale optical responses. With the atom-scale spatial resolving power of the electron microscope and its ability to probe optical transitions, electron spectroscopies like EELS are uniquely suited for these challenges. Our proposal addressed STEM/EELS techniques (Camden) to directly measure and even control energy transfer pathways in hybrid plasmon-resonator systems and leveraged detailed theoretical models combined with simulation (Masiello) to understand the essential underlying physics. In particular, the outcome of our proposed studies deepened the fundamental understanding of how surface plasmons shed energy to their environment and the practical knowledge gained here will influence the design of future high-efficiency solar energy-harvesting devices and photocatalysts capable of operating throughout the visible and the infrared.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Coloration Determination of Spectral Darkening Occurring on a Broadband Earth Observing Radiometer: Application to Clouds and the Earth's Radiant Energy System (CERES)

It is estimated that in order to best detect real changes in the Earth s climate system, space based instrumentation measuring the Earth Radiation Budget (ERB) must remain calibrated with a stability of 0.3% per decade. Such stability is beyond the specified accuracy of existing ERB programs such as the Clouds and the Earth s Radiant Energy System (CERES, using three broadband radiometric scanning channels: the shortwave 0.3 - 5microns, total 0.3. > 100microns, and window 8 - 12microns). It has been shown that when in low earth orbit, optical response to blue/UV radiance can be reduced significantly due to UV hardened contaminants deposited on the surface of the optics. Since typical onboard calibration lamps do not emit sufficient energy in the blue/UV region, this darkening is not directly measurable using standard internal calibration techniques. This paper describes a study using a model of contaminant deposition and darkening, in conjunction with in-flight vicarious calibration techniques, to derive the spectral shape of darkening to which a broadband instrument is subjected. Ultimately the model uses the reflectivity of Deep Convective Clouds as a stability metric. The results of the model when applied to the CERES instruments on board the EOS Terra satellite are shown. Given comprehensive validation of the model, these results will allow the CERES spectral responses to be updated accordingly prior to any forthcoming data release in an attempt to reach the optimum stability target that the climate community requires.

Matthews, Grant↗

Plasmonic Nonlinear Energy Transfer Enhanced Second Harmonic Generation Nanoscopy

Nonlinear optical response is a fingerprint of various physicochemical properties of materials related to symmetry, including crystallography, interfacial configuration, and carrier dynamics. However, the intrinsically weak nonlinear optical susceptibility and the diffraction limit of far-field optics restrict probing deep-subwavelength-scale nonlinear optics with measurable signal-to-noise ratio. Here, we propose an alternative approach toward efficient second harmonic generation (SHG) nanoscopy for SHG-active sample (zinc oxide nanowire; ZnO NW) using an SHG-active plasmonic nanotip. Our full-wave simulation suggests that the experimentally observed high near-field SHG contrast is possible when the nonlinear response of ZnO NW is enhanced and/or that of the tip is suppressed. Here, this result suggests possible evidence of quantum mechanical nonlinear energy transfer between the tip and the sample, modifying the nonlinear optical susceptibility. Further, this process probes the nanoscale corrosion of ZnO NW, demonstrating potential use in studying various physicochemical phenomena in nanoscale resolution.

36 MATERIALS SCIENCE↗

Time-varying gradient metasurface with applications in all-optical beam steering

Integrating the large, subpicosecond nonlinear optical response of epsilon-near-zero (ENZ) materials with the broad design freedoms of plasmonic metasurfaces shows potential for creating rapidly modulated optical devices with possible applications in telecommunications, sensing, and reactive beam steering. In this work, we experimentally investigate a metasurface consisting of a plasmonic gradient array on a thin layer of indium tin oxide (ITO), characterize how incident probe pulses diffract from a system as it is being dynamically modulated by a pump pulse at wavelengths near the ENZ region. Angular shifts in the diffraction orders are observed and can be principally attributed to the adiabatic wavelength conversion of the probe as it witnesses the temporal change of index induced by the pump. Of note, the asymmetric gradient metasurface, considered to be a blazed diffraction grating, shows significantly different dynamic responses for different diffraction orders. The free-space wavelength shift to +1 and -1 diffraction orders is 6 and 12 nm, resulting in steering angle changes of 0.65 and 1.5°, respectively.

42 ENGINEERING↗

Molecularly Imprinted Polymer Sensor Empowered by Bound States in the Continuum for Selective Trace-Detection of TGF-beta

The integration of advanced materials and photonic nanostructures can lead to enhanced biodetection capabilities, crucial in clinical scenarios and point-of-care diagnostics, where simplified strategies are essential. Herein, a molecularly imprinted polymer (MIP) photonic nanostructure is demonstrated, which selectively binding to transforming growth factor-beta (TGF-β), in which the sensing transduction is enhanced by bound states in the continuum (BICs). The MIP operating as a synthetic antibody matrix and coupled with BIC resonance, enhances the optical response to TGF-β at imprinted sites, leading to an augmented detection capability, thoroughly evaluated through spectral shift and optical lever analogue readout. The validation underscores the MIP-BIC sensor capability to detect TGF-β in spiked saliva, achieving a limit of detection of 10 fM and a resolution of 0.5 pM at physiological concentrations, with a precision of two orders of magnitude above discrimination threshold in patients. The MIP tailored selectivity is highlighted by an imprinting factor of 52, showcasing the sensor resistance to interference from other analytes. The MIP-BIC sensor architecture streamlines the detection process eliminating the need for complex sandwich immunoassays and demonstrates the potential for high-precision quantification. This positions the system as a robust tool for biomarker detection, especially in real-world diagnostic scenarios.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Single Crystal Optical Fiber and Perovskite Oxide Sensing Materials for Gas Monitoring above 500 °C

A wide range of high-value applications, including power generation and chemical manufacturing, involve harsh chemical conditions and extreme temperatures. In this work, we discuss the pairing of single crystal optical fiber with optically responsive, high-temperature stable perovskite oxide materials for monitoring of oxidizing and reduction gas streams up to 1000 °C. Optical sensing will be presented for hydrogen and oxygen monitoring in this temperature regime. Strategies will be discussed for improving stability and eliminating drift via multi-wavelength detection. The application of spatially resolved interrogation techniques, such as optical time domain reflectometry (OTDR) will be addressed for these sensors.

Wuenschell, Jeffrey↗

NASA's LCOT (Low-Cost Optical Terminal) FSOS (Free-Space Optical Subsystem): Concept, Design, Build, & Test

We present the status of ongoing work at NASA’s Goddard Space Flight Center (GSFC) to build a prototype, low-cost-of-production, flexibly-configured ground terminal for space optical communication. For laser telecommunication to be cost effective for future missions, a wide-spread global network of operationally responsive optical terminals should be established. There has been a decades-old need for a single modular open systems approach (MOSA) ground terminal architecture capable of supporting multiple space missions ranging from LEO to Lunar distances with 2-way laser communications. At the heart of LCOT’s design concept is the Free-Space Optical Subsytem (FSOS). The major subassemblies of LCOT/FSOS that address most optical comms configurations are : (1) Single 700mm F/12 Nasmyth folded Rx R-C Telescope, (2) Four independent 150mm diameter high-power all-reflective Tx beam directors (XOA), (3) Non-coherent direct detection Rx bench on starboard side of telescope (SOB), and (4) Coherent (possibly Quantum) optical communications bench on port side (POB). The Low-Cost Optical Terminal (LCOT) research and development (R&D) prototype is designed to be a generalized system that can be quickly field-reconfigured to support a wide variety of laser communications missions past, present, & future.

COTS↗

NASA's Low-Cost Optical Terminal (LCOT) Free-Space Optical Subsystem (FSOS): Concept, Design, Build, & Test

We present the status of ongoing work at NASA’s Goddard Space Flight Center (GSFC) to build a prototype, low-cost-of-production, flexibly-configured ground terminal for space optical communication. For laser telecommunication to be cost effective for future missions, a wide-spread global network of operationally responsive optical terminals should be established. There has been a decades-old need for a single modular open systems approach (MOSA) ground terminal architecture capable of supporting multiple space missions ranging from LEO to Lunar distances with 2-way laser communications. At the heart of LCOT’s design concept is the Free-Space Optical Subsystem (FSOS). The major subassemblies of LCOT/FSOS that address most optical common configurations are : (1) Single 700mm F/12 Nasmyth folded Rx R-C Telescope, (2) Four independent 150mm diameter high-power all-reflective Tx beam directors (XOA), (3) Non-coherent direct detection Rx bench on starboard side of telescope (SOB), and (4) Coherent (possibly Quantum) optical communications bench on port side (POB). The Low-Cost Optical Terminal (LCOT) research and development (R&D) prototype is designed to be a generalized system that can be quickly field-reconfigured to support a wide variety of laser communications missions past, present, & future.

COTS↗

Low-energy interband transition in the infrared response of the correlated metal SrVO 3 in the ultraclean limit

We studied the low-energy electronic response of the prototypical correlated metal SrVO 3 in the ultraclean and disordered limit using infrared spectroscopy and density functional theory plus dynamical mean field theory calculations (DFT+DMFT). A strong optical excitation at 70 meV is observed in the optical response of the ultraclean samples but is hidden by the low-energy Drude-like response from intraband excitations in the more disordered samples. DFT+DMFT calculations reveal that this optical excitation originates from interband transitions between the bands split by orbital off-diagonal hopping, which has often been ignored in cubic systems, such as SrVO 3 . A memory function analysis of the optical data shows that this interband transition can lead to deviations of optical self-energy from the expected Fermi-liquid behavior. Our findings demonstrate that analysis schemes employed to extract many-body effects from optical spectra may be oversimplified to study the true electronic ground state and that improvements in material quality can guide efforts to refine theoretical approaches.

36 MATERIALS SCIENCE↗

Optical Forces on an Oscillating Dipole Near VO2 Phase Transition

We investigate optical forces on oscillating dipoles close to a phase change vanadium dioxide (VO2) film, which exhibits a metal-insulator transition around 340 K and low thermal hysteresis. This configuration emulates the interaction between an illuminated nanosphere and an interface and we employ a classical description to capture its important aspects. We consider both electric and magnetic dipoles for two different configurations, namely with the dipole moments parallel and perpendicular to the VO2 film. By using Bruggeman theory to describe the effective optical response of the material, we show that the thermal hysteresis present in the VO2 transition clearly shows up in the behavior of optical forces. In the near-field regime, the force on both dipoles can change from attractive to repulsive just by heating (or cooling) the film for a selected frequency range. We also verified that the optical forces are comparable to the Casimir-Polder force in a similar system, revealing the possibility of modulating or even changing the sign of the resultant force on an illuminated nano-object due to the presence of a thermochromic material. We hope that this work contributes to set the grounds for alternative approaches to control light-matter interactions using phase-change materials.

36 MATERIALS SCIENCE↗

Effects of RAM Exposure on a Low Earth Orbit BroadBand Radiometer (BBR): CERES Experience and Implications for EarthCARE

In order to best detect real changes in the Earth's climate system it is estimated that space based instrumentation measuring the global Earth Radiation Budget (ERB) must remain calibrated with a stability of 0.3% per decade. This level of stability is beyond the specified accuracy of existing ERB programs such as the Clouds and the Earth's Radiant Energy System (CERES, using three broadband radiometric scanning channels: the shortwave (SW 0.3 - 5?m), total (0.3 - >100 micron), and window (8 - 12 micron)). When in low earth orbit, it has been shown that optical response to blue-UV radiance can be reduced significantly (> 3%) due to UV hardened contaminants deposited on the surface of the optics. Evidence suggests that exposure of telescope optics to the forward looking ram direction is the primary cause of this contamination build up. With typical onboard calibration lamps emitting very low energy in the blue-UV region, this darkening is not directly measurable using standard internal calibration techniques. This paper describes a study using a model of ram exposure induced contaminant deposition and darkening, in conjunction standard established in-flight vicarious and internal calibration techniques to derive the spectral shape of the darkening to which a broadband instrument is subjected. The results of the model when applied to the CERES instruments are shown. These findings are of great importance to the EarthCARE project, whose BBR uses one broadband telescope permanently looking forward at 45 degrees, with continual exposure to the ram direction. Specific attention may therefore be needed in the design of BBR optics and on-board calibration in order to prevent or compensate for the spectral darkening seen in the CERES project.

Matthews, Grant↗

Measuring an ultrashort, ultraviolet pulse in a slowly responding, absorbing medium

Frequency-resolved optical gating (FROG) is a common technique for measuring ultrashort laser pulses using an instantaneous, nonlinear-optical interaction as a fast time-gate to measure the pulse intensity and phase. But at high frequencies, materials are often absorbing and it is not always possible to find a medium with a fast nonlinear-optical response. Here we show that an ultrashort, ultraviolet (UV) pulse can be measured in a strongly absorbing medium, using the absorption as the nonlinear-optical time-gate. To do this, we build on our recent implementation of FROG, known as induced-grating cross-correlation FROG (IG XFROG), where an unknown, higher-frequency pulse creates a transient grating that is probed with a lower-frequency, more easily detectable reference pulse. We demonstrate this with an 800 nm reference pulse to characterize 400 nm or 267 nm pulses using ZnS as the nonlinear-optical medium, which is absorptive at and below 400 nm. By scanning the delay between the two UV pulses which create the transient grating, we show that the phase-sensitive instantaneous four-wave-mixing contribution to the nonlinear signal field can be detected and separated from the slower, incoherent part of the response. Measuring a spectrally-resolved cross-correlation in this way and then applying a simple model for the response of the medium, we show that a modified generalized projections (GP) phase-retrieval algorithm can be used to extract the pulse amplitude and phase. We test this approach by measuring chirped UV pulses centered at 400 nm and 267 nm. Since interband absorption (or even photoionization) is not strongly wavelength-dependent, we expect IG XFROG to be applicable deeper into the UV.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Polarization Control via Artificial Optical Nonlinearity in Dielectric Metasurfaces

Nonlinear optical phenomena are generally governed by geometry in matter systems, as they depend on the spatial arrangement of atoms within materials or molecules. Metasurfaces, through precisely designed geometries on a subwavelength scale, allow the optical response of a material to be tailored far beyond its natural properties. Therefore, metasurfaces are highly appealing for enabling the engineering of nonlinear optical interactions. Current studies of nonlinear metasurfaces predominantly focus on the phase control of the generated light. Nonetheless, investigating the tensorial nature of the nonlinearity of metasurfaces and its effect on the polarization of the generated light is critical to fully unlocking a range of applications, such as nonlinear vector beam generation and nonlinear polarization imaging. Here, we study the artificial optical nonlinearity of a dielectric metasurface originating from its meta-atom symmetry and describe the third-order nonlinear behavior by considering the polarization degree of freedom. We establish an effective nonlinear medium model that serves as a design toolbox for developing amorphous silicon-based geometric metasurfaces with customizable features for third-harmonic generation. We further extract quantitative values of the artificial nonlinear susceptibility tensor elements related to the investigated nonlinear process and geometry. The implemented functional devices demonstrate the versatility of dielectric metasurfaces in shaping the emitted light in terms of amplitude, phase, and polarization for the precise engineering of advanced nonlinear architectures targeting applications in nonlinear imaging and complex light generation.

Diffraction↗

Disentangling High Harmonic Generation from Surface and Bulk States of a Topological Insulator

The discovery of topological phases has introduced a new dimension to materials science. Three-dimensional (3D) topological insulators (TIs) are a remarkable class of matter that is insulating in the bulk while hosting conductive topological surface states (TSSs) with unique charge and spin properties. High-order harmonic generation (HHG) has emerged as a powerful tool to probe condensed matter systems by providing insights into their electronic structure and dynamic behavior. Here, we investigate HHG in the prototype 3D-TI Bi$_2$Se$_3$. We demonstrate that the contributions of bulk and surface states to the harmonic emission can be controlled by tuning the thickness of thin film samples. An ultrathin (6 nm) film substantially enhances HHG from the surface states, while the bulk states dominate HHG in a thicker (50 nm) film. By applying a quasi-static terahertz perturbing field, we disentangle the bulk and surface responses and reveal the significant impact of the surface states' shift vector and Berry curvature on HHG. Our study provides effective methods for isolating the optical responses of TSSs from those of the bulk, which opens the door to resolving an ongoing debate regarding whether it is possible to reliably extract topological signatures in HHG.

Atomic Physics (physics.atom-ph)↗

Thin-film light-intensity measurement strain-analysis technique.

The optical response to loading of a thin metallic film deposited on a low-modulus structural substrate is studied theoretically and experimentally. Two types of optical properties called total and central-image transmittance (or reflectance) are shown to be related to the mechanical state of the substrate. Empirical optical-mechanical relationships are proposed between these optical properties and the substrate strain field of a general plane-stress problem. A technique based on wrinkle and microfracture patterns is described for determining principal directions of strain. Experimental results for uniaxially loaded specimens show that it is possible to obtain a nearly linear relationship between transmittance and strain for certain materials combinations.

Williams, J. G.↗

Optically controlled microwave devices and circuits: Emerging applications in space communications systems

Optical control of microwave devices and circuits by an optical fiber has the potential to simplify signal distribution networks in high frequency communications systems. The optical response of two terminal and three terminal (GaAs MESFET, HEMT, PBT) microwave devices are compared and several schemes for controlling such devices by modulated optical signals examined. Monolithic integration of optical and microwave functions on a single semiconductor substrate is considered to provide low power, low loss, and reliable digital and analog optical links for signal distribution.

Bhasin, Kul B.↗