Optical Response Research Articles

Statistical and Correlative Characterization of Individual Nanoparticle in Gap Plasmon Resonator Sensors

AbstractPlasmonic nanocavities are receving increased attention from the nanophotonics, nanoelectronics, and quantum optics community due to their ability to confine light in extremely small volumes. Coupling colloidal plasmonic nanocrystals to metal films is an inexpensive approach to fabricate virtually unlimited individual resonators that can be tuned by adjusting nanoparticle size, gap thickness, and refractive index. The focus is on silver nanocubes separated from a gold mirror by thin amorphous dielectric layers (Al2O3, TiO2). The optical response is measured and correlative electron microscopy is performed on a large number (>800) of individual resonators to unveil the statistical distribution of gap plasmon modes and assess systematically their sensitivity. A sensitivity as large as 8 nm/nm to nanocube size variation, 50 nm/nm to Al2O3 thickness variation, and 130 nm/RIU for index change of the spacer layer is found. With the help of numerical simulations, this approach enables to infer a quantitative statistical distribution of molecular coatings present on the nanocubes surface, such as polyvinylpyrrolidone, which can affect the performance of nanoelectronic devices and assess the strategy to remove it. Finally, polarization‐resolved measurements enable to unveil a birefringent behavior when nanocubes are supported on annealed TiO2 layers (2–4 nm).

Yielding high photovoltaic conversion efficiency by Pd-decoration on Si-based interface: A density-functional theory study

There has been showing great interest in boosting the performance of III-V/Si multi-junction solar cell, which is low-cost and offering high photovoltaic conversion efficiency. Adding noble-metal nano-array at the interface between the Si and III-V materials is one of most effective ways. This theoretical work comprehensively studied the atomic structure, electronic properties, and optical response of Pd-decoration on the Si(111) surface by using density-functional theory calculations. The structural stability calculations showed that Pd atoms could exist on Si surface in many forms. The calculated differential charge density with Bader charge showed that the charge transfer between Pd and Si atoms would increase the generation of electron-hole pairs. At the same time, Pd-decoration could reduce the work function and improve the optical conductivity of Si surface. In addition, the modification of Pd atoms would create new energy levels near the Fermi level in the band gap of Si surface. These energy levels enable Si bottom cell to undergo electron inter-band transitions under weak light irradiation, improving the utilization of weak light. This work provided a micro physical explanation for the improvement of III-V/Si solar cell by using noble-metal nano-array.

Investigation of structural, morphological and optoelectronic properties of (Ni, Co)-doped and (Ni/Co) co-doped SnO2 (110) sprayed thin films

The manuscript details the application of spray pyrolysis for the deposition of an economically viable transparent conductive oxide film comprised of (Ni/Co) co-doped SnO2 on a glass substrate. The primary objective of this research was to systematically examine the impact of Ni/Co co-doping on diverse properties of the SnO2 thin film. These properties encompassed the film's structural composition, surface morphology, optical response, and electrical behaviors. A comparison was made with pure SnO2 film, as well as SnO2 films doped with 3 %Ni and 1 %Co. The results indicate that all the samples exhibited a tetragonal structureThe introduction of Co and Ni atoms had no impact on the favored alignment of the (110) plane or the crystal structure of the SnO2 film. The crystallite size of the pure SnO2 film, as well as the (Co, Ni)-doped and (Ni/Co) co-doped SnO2 films, varied within the range of 11 to 20 nm. Scanning electron microscopy (SEM) images were employed to assess how doping and co-doping influenced the surface characteristics of the films. The presence of pores and/or roughness on the surface resulted in a hydrophilic character and a decrease in the contact angle for the doped films (Ni, Co). However, the co-doped film exhibited a hydrophobic characteristic due to the surface enhancement provided by SnO2:3 %Ni:1 %Co. The research also focused on the optical characteristics of the films, showing a positive impact with the proper incorporation of Ni and Co atoms into the SnO2 lattice. It was notably observed that the addition of Ni and Co atoms improves the optical properties of the undoped transparent SnO2 film in the visible spectrum, with a high transmittance of 87 % achieved for the Ni-doped film. Furthermore, the hydrophobic nature achieved by adding a concentration of 3 %Ni to the SnO2:1 %Co film enhances its optical transmission in the range of 300 nm to 750 nm. The SnO2 film shows an improvement in the electrical resistivity upon doping and co-doping with low resistivity value of 2.22 × 10−2 Ω.cm for the film (3 %Ni/1 %Co)-SnO2. Drawing from these insightful results, the study proposes the potential utilization of (Ni/Co) co-doped SnO2 films as transparent electrodes in optoelectronic applications, especially in the manufacturing of thin film solar cells.

Numerical investigation of high-order harmonic generation by gold nanorod arrays in hybrid nanostructures: effect of number of gold nanorod

Hybrid metal-dielectric nanostructures are highly effective and helpful in generating and enhancing linear and nonlinear optical phenomena due to their unique optical properties. In this study, the linear optical responses and second- and third-order harmonics have been calculated numerically for this structure. Nonlinear optical response efficiency has been studied at the resonance wavelengths of the nanostructure by varying its parameters (radius and length). The desired efficiency can be achieved by adjusting the radius and length of the nanorods and matching the resonance wavelengths with the fundamental and generation frequencies of nonlinear optical phenomena in specific applications. Moreover, the effect of the number of gold nanorods on harmonic generation has been investigated. By increasing the number of nanorods in pairs, it is possible to generate high-order harmonics. The acquired results can be used to improve optical devices such as biomedical equipment, optical integrated circuits, and sensors.

Thermal radiation forces on planar structures with asymmetric optical response

Abstract Light carries momentum and, upon interaction with material structures, can exert forces on them. Here, we show that a planar structure with asymmetric optical response is spontaneously accelerated when placed in an environment at a different temperature. This phenomenon originates from the imbalance in the exchange rates of photons between both sides of the structure and the environment. Using a simple theoretical model, we calculate the force acting on the planar structure and its terminal velocity in vacuum, and analyze their dependence on the initial temperature and the geometrical properties of the system for different realistic materials. Our results unravel an alternative approach to manipulating objects in the nano and microscale that does not require an external source of radiation.

Effects of germanium content on the optical properties of GeO2-based organic-inorganic composite films doped with azobenzene

Organic-inorganic composite materials have great applications in integrated optics due to their good optical performance. In this study, GeO2-based organic-inorganic composite films doped with azobenzene were prepared by combining the solgel technique and the spin-coating method. The optical waveguide properties including the refractive index and film thickness and the optical response properties of the composite films with different germanium contents have been investigated. The results indicate that the refractive index of the film increases, but the film thickness decreases as the germanium content increases. The composite film with 0.2 mol of germanium exhibits the best optical response properties. Further, the optical switching characteristics of the optimal composite film shows good stability and reversibility. The photochemical and structural properties of the film were also investigated by using Fourier transform infrared spectroscopy and thermo-gravimetric analysis. Finally, hexagonal microlens arrays were built in the film by using the UV nanoimprint technique, resulting in neatly arranged structures with good optical imaging performance.

Linear and nonlinear optics in composite systems: From diagrammatic modeling to applications.

A bipartite system is defined as two microscopic entities being able to exchange energy. When excited by light, the complete optical response functions at first (polarizabilities) and second orders (first hyperpolarizabilities) of such a system are determined using the diagrammatic theory of optics. The generality of the method is ensured by the free choice of light-matter and matter-matter interaction Hamiltonians and by the arbitrary number of quanta involved in the energy exchange. In the dipolar approximation, the optical response functions of the system (i.e., of the interacting entities) are linked to the responses of the interaction-free entities by transfer matrices. These universal matrices identically modify the optical response functions at all orders in the electromagnetic field, allowing the implementation of matter-matter interactions in higher-order processes, such as stimulated or spontaneous Raman scattering and four-wave mixing. This formalism is then applied to various composite systems: dimers, multimers and lattices of nanoparticles and molecules, dense molecular layers, and substrate-induced image dipoles.

Hyperbolic response and low-frequency ultra-flat plasmons in inhomogeneous charge-distributed transition-metal monohalides

Plasmon, the collective oscillations of free electron gas in materials, determines the long-wavelength excitation spectrum and optical response, are pivotal in the realm of nanophotonics and optoelectronics. In this study, using the first-principles calculations, we systematically investigated the dielectric response and plasmon properties of bulk transition-metal monohalides MXs (M = Zr, Mo; X = Cl, F). Due to the strong electronic anisotropy, MXs exhibit a broadband type-II hyperbolic response and direction-dependent plasmon modes. Particularly, local field effect (LFE) driven by the charge distribution inhomogeneity, significantly modifies the optical response and excitation spectra in MX along the out-of-plane direction. Taking into account LFE, the energy dissipation along the out-of-plane direction is almost completely suppressed, and an ultra-flat and long-lived plasmon mode with a slow group velocity is introduced. This finding reveals the role of charge density in modifying the optical response and excitation behavior, shedding light on potential applications in plasmonics.

Neural network driven sensitivity analysis of diffraction-based overlay metrology performance to target defect features

Overlay (OVL) is one significant performance indicator for the lithography process control in semiconductor manufacturing. The accuracy of the OVL metrology is extremely critical for guarantee the lithography quality. Currently, diffraction-based overlay (DBO) is one of the mainstream OVL metrology techniques. Unfortunately, the accuracy of the DBO metrology is largely affected by the defect features of the OVL target. Therefore, there is a strong need to investigate the impacts of these target defects on the DBO metrology performance. However, efficiently investigating the statistical and interactive impacts of various DBO target defects remains challenging. This study aims to address this issue through proposing an intelligent sensitivity analysis approach. A cumulative distribution based global sensitivity analysis (GSA) method is utilized to assess the nonlinear influences of multiple defects in the OVL target on the DBO inaccuracy. The scenarios with both known and unknown distributions of the OVL target defects are considered. For the former, a neural network driven forward model is constructed for fast calculating the optical diffraction responses to accelerate the GSA process. For the latter, another neural network based inverse model are built for efficiently estimating the distribution of the target defects. Finally, a series of simulation experiments are conduct for typical DBO targets with multiple common defect features. The results demonstrate the effectiveness and robustness of the proposed approach as well as give valuable insights into the DBO defect analysis. Our study provides a strong tool to assist the practitioners in achieving intelligent and efficient DBO analysis and thus in enhancing OVL metrology performance.

Evidence of multifunctional properties of ferromanganite La0.5Ca0.5Mn0.5Fe0.5O3

Synthesis and characterization of the magnetic and electrical properties of the perovskite-type ferro-magnetite La0.5Ca0.5Mn0.5Fe0.5O3 are reported. Structural analysis reveals crystallization of the material in an orthorhombic structure, space group Pbnm (#62). The optical response suggests semiconductor-type behavior with bandgap Eg=2.3 eV. Susceptibility curves as a function of temperature and magnetization as a function of applied field suggest a soft ferromagnetic type response below room temperature, with evidence of disorder characterized by magnetic irreversibility at low temperatures and low applied fields. Resistivity measurements as a function of temperature and corroborate the semiconductor nature of the material and hysteretic I-V curves enhance its applicability in programmable logic memory devices. Band structure calculations around the Fermi level result in two different band gap values for the two spin up and spin down polarizations, as expected in ferromagnetic semiconductor materials. The hybridizations observed in the density of states curves as a function of energy suggest that the ferromagnetic character is due to double exchange mechanisms, coexisting with antiferromagnetic super-exchange, which is essentially due to the disorder of Fe3+ and Mn4+ cations in the octahedra along the three crystallographic axes.

Electrical manipulation of telecom color centers in silicon

Silicon color centers have recently emerged as promising candidates for commercial quantum technology, yet their interaction with electric fields has yet to be investigated. In this paper, we demonstrate electrical manipulation of telecom silicon color centers by implementing novel lateral electrical diodes with an integrated G center ensemble in a commercial silicon on insulator wafer. The ensemble optical response is characterized under application of a reverse-biased DC electric field, observing both 100% modulation of fluorescence signal, and wavelength redshift of approximately 1.24 ± 0.08 GHz/V above a threshold voltage. Finally, we use G center fluorescence to directly image the electric field distribution within the devices, obtaining insight into the spatial and voltage-dependent variation of the junction depletion region and the associated mediating effects on the ensemble. Strong correlation between emitter-field coupling and generated photocurrent is observed. Our demonstration enables electrical control and stabilization of semiconductor quantum emitters.

Numerical simulations of the optical properties of SiO2@Au core–shell nanoparticles: The effect of geometrical parameters on the tunability and sensitivity of their plasmon response

Based on systematic numerical simulations, the effect of geometrical parameters of SiO2@Au core-shells (nanoshells) on the tunability and sensitivity of their optical response was elucidated. The surface plasmon resonance (SPR) of nanoshells experiences a blueshift-redshift crossover with the increase in shell thickness, and this phenomenon is ascribed to the competition between the two effects, that is, the hybridization effect dominated in the thin shells and the retardation effect dominated in the thick shells. The relative strength of absorption/scattering in the extinction spectra and the relative strength of dipolar/multipolar modes can be selectively tuned by controlling the total volume of nanoshells. The sensitivity of the SPR peak wavelength to the shell thickness is primarily dependent on the core-to-shell ratio; the higher this ratio is, the larger the sensitivity. The tailorable properties of nanoshells make them promising and well-suited platforms in various applications.

Flexible epitaxial LiNbO3 thin film with ferroelectricity and nonlinear optical response

Flexible or wearable devices are of great interests in the modern technologies, and oxide thin films are critical components for such applications. In this work, epitaxial LiNbO3 (LNO) thin film integrated on flexible mica substrate has been achieved. Al-doped ZnO (AZO) layer has been first deposited as buffer layer to obtain the epitaxial LNO film, furthermore AZO serves as bottom electrode for electrical measurement. The as-deposited LNO film exhibits high epitaxial quality with c-direction growth. The transmittance measurement indicates the high transparency of the film, ～85 % in visible range and ～90 % in near infrared region up to 1500 nm. The second harmonic generation (SHG) measurement confirms the nonlinearity of the flexible LNO film. The LNO/AZO/mica film also presents apparent ferroelectric response. Overall, the high-quality LNO integrated on flexible mica could be potentially applied in wearable optical and electrical devices.

Effect of the Contribution of the Local and Nonlocal Optical Response of an Isotropic Gyrotropic Medium on the Components of the Minkowski Energy–Momentum Tensor of the Electromagnetic Field of the Self-Focusing Beam

Effect of the Contribution of the Local and Nonlocal Optical Response of an Isotropic Gyrotropic Medium on the Components of the Minkowski Energy–Momentum Tensor of the Electromagnetic Field of the Self-Focusing Beam

Integration of conventional surface science techniques with surface-sensitive azimuthal and polarization dependent femtosecond-resolved sum frequency generation spectroscopy.

Experimental insight into the elementary processes underlying charge transfer across interfaces has blossomed with the wide-spread availability of ultra-high vacuum (UHV) setups that allow the preparation and characterization of solid surfaces with well-defined molecular adsorbates over a wide range of temperatures. Within the last 15 years, such insights have extended to charge transfer heterostructures containing solids overlain by one or more atomically thin two dimensional materials. Such systems are of wide potential interest both because they appear to offer a path to separate surface reactivity from bulk chemical properties and because some offer completely novel physics, unrealizable in bulk three dimensional solids. Thick layers of molecular adsorbates or heterostructures of 2D materials generally preclude the use of electrons or atoms as probes. However, with linear photon-in/photon-out techniques, it is often challenging to assign the observed optical response to a particular portion of the interface. We and prior workers have demonstrated that by full characterization of the symmetry of the second order nonlinear optical susceptibility, i.e., the χ(2), in sum frequency generation (SFG) spectroscopy, this problem can be overcome. Here, we describe an UHV system built to allow conventional UHV sample preparation and characterization, femtosecond and polarization resolved SFG spectroscopy, the azimuthal sample rotation necessary to fully describe χ(2) symmetry, and sufficient stability to allow scanning SFG microscopy. We demonstrate these capabilities in proof-of-principle measurements on CO adsorbed on Pt(111) and on the clean Ag(111) surface. Because this setup allows both full characterization of the nonlinear susceptibility and the temperature control and sample preparation/characterization of conventional UHV setups, we expect it to be of great utility in the investigation of both the basic physics and applications of solid, 2D material heterostructures.

Modeling the optical response of plasmonic nanoparticles

Modeling the optical response of plasmonic nanoparticles

Microwave Absorption Properties of Hexagonal Ba3(VO4)2 through Zn Doping: A Comprehensive Analysis of Ba3–xZnx(VO4)2

The current study explores the influence of Zinc (Zn) doping on the crystallography, optical behavior, dielectric properties, and microwave absorption characteristics of hexagonal Barium Vanadate (Ba3(VO4)2). Samples were systematically synthesized with Zn doping concentrations of x = 0, 0.05, 0.1, 0.15, and 0.2 mol%, resulting in Ba3–xZnx(VO4)2. Employing various characterization techniques, the alterations in structural, optical, and electrical responses due to incremental Zn incorporation are reported. The UV–VIS DRS absorption spectra reveal a decrease in energy bandgap with increasing concentration of Zn. The lowest optical energy band gap observed was 3.65 eV for x = 0.2 mol% Zn. Notably, at a thickness of 6.5 mm, the material achieved a high reflection loss of −82.37 dB at 12.47 GHz for x = 0.05 mol% of Zn. Similarly, the same material configuration exhibited a maximum effective absorption bandwidth (EAB) of 5.01 GHz, spanning a frequency range from 12.24 to 17.25 GHz when the thickness was set to 5.5 mm. Furthermore, as the Zn concentration increased from x = 0.05 to 0.2 mol%, a decreasing trend in reflection loss was observed, correlating well with the dielectric parameters of samples with different Zn concentrations. The work provides insightful correlations between Zn doping levels and the material’s performance in potential applications ranging from optoelectronics to electromagnetic wave absorption.

Linear and nonlinear optical response of Mie-resonant Si nanoparticles and its modification induced by femtosecond irradiation post-treatment

Silicon nanoparticles with Mie resonances are among the most prospective building blocks for state-of-the-art all-dielectric metasurfaces. Here we focus on linear and nonlinear optical responses of silicon nanoparticles printed by laser-induced transfer from silicon-on-insulator wafer. Second-harmonic generation and broadband multiphoton-absorption-induced luminescence are studied as a function of pump wavelength. The key role of magnetic quadrupole Mie resonances in the nonlinear optical response from silicon nanoparticles is revealed. We also show the influence of Si nanoparticle shape and structure modification, realized by additional femtosecond laser irradiation, on their linear and nonlinear optical properties.

Micrometric patterning of a borogermanate glass containing terbium by thermal poling to manage luminescence and second order optical properties

Borogermanate glasses containing terbium ions are interesting materials due to their luminescent and magnetic properties. Terbium can present two different oxidation states and the thermal poling technique can be a pertinent way to modulate spatially the oxidation state of these ions. In this work, we demonstrate using a thermo-electrical imprinting process the transfer of micro scaled motifs on the surface of a borogermanate glass containing Tb3+ resulting in a micrometric structuring of the oxidation state of Tb3+/Tb4+ ions. A large change in absorption and luminescence optical properties is observed, arising from the distinct properties of trivalent and tetravalent terbium ions. Correlative micro luminescence, Raman and second harmonic generation measurements were carried out on the patterned poled glass surface. This has demonstrated an accurate concomitant modification of the glass structure accompanying large luminescence changes and the appearance of a second order optical response which could be attributed to a localized space charge implantation. These original results demonstrate how a simple electrical process allows managing multi optical properties but also paves the way to induce static electrical functionalities in a magnetic optical glassy system.

A Stable Perovskite Sensitized Photonic Crystal P-N Junction with Enhanced Photoelectrochemical Hydrogen Production.

The slow photon effect in inverse opal photonic crystals represents a promising approach to manipulate the interactions between light and matter through the design of material structures. This study introduces a novel ordered inverse opal photonic crystal (IOPC) sensitized with perovskite quantum dots (PQDs), demonstrating its efficacy for efficient visible-light-driven H2 generation via water splitting. The rational structural design contributes to enhanced light harvesting. The sensitization of the IOPC with PQDs improves optical response performance and enhances photocatalytic H2 generation under visible light irradiation compared to the IOPC alone. The designed photoanode exhibits a photocurrent density of 3.42 mA cm-2 at 1.23 V vs RHE. This work advances the rational design of visible light-responsive photocatalytic heterostructure materials based on wide band gap metal oxides for photoelectrochemical applications.