Optical Response Research Articles

Enhanced Nonlinear Optical Responses in MoS2 via Femtosecond Laser‐Induced Defect‐Engineering

Abstract2D materials are a promising platform for applications in many fields as they possess a plethora of useful properties that can be further optimized by careful engineering, for example, by defect introduction. While reliable high‐yield defect engineering methods are in demand, most current technologies are expensive, harsh, or non‐deterministic. Optical modification methods offer a cost‐effective and fast mechanism to engineer the properties of 2D materials at any step of the device fabrication process. In this paper, the nonlinear optical responses of mono‐, bi‐, and trilayer molybdenum disulfide (MoS2) flakes are enhanced by deterministic defect‐engineering with a femtosecond laser. A 50‐fold enhancement in the third harmonic generation (THG) and a 3.3‐fold increase in the second harmonic generation (SHG) in the optically modified areas is observed. The enhancement is attributed to resonant SHG and THG processes arising from optically introduced mid‐band gap defect states. These results demonstrate a highly controllable, sub‐micrometer resolution tool for enhancing the nonlinear optical responses in 2D materials, paving the way for prospective future applications in optoelectronics, quantum technologies, and energy solutions.

Improved Charge Recombination Efficiency in Organic Light‐Emitting Transistors via Luminescent Radicals

AbstractLuminescent radicals are attracting attention as emitters in electroluminescent devices thanks to the exploitation of doublet excitons. Recent studies reveal that exciton formation in radical organic light‐emitting diodes (OLEDs) primarily occurs through a charge trapping mechanism. Although typically detrimental for OLEDs, this might be a key process to elucidate light emission in organic light‐emitting transistors (OLETs). Here, a unipolar n‐type architecture suitable for the implementation of radical emitters is introduced, designed based on computational calculations. The operation of the as‐realized devices incorporating the newly synthesized [2,6‐dichloro‐4‐(2,6‐dimethoxyphenyl)phenyl](3,5‐dichloro‐4‐pyridyl) (2,4,6‐trichlorophenyl)methyl radical is investigated via transient electroluminescence measurements to demonstrate the occurrence of long‐living emission ascribed to the charge trapping mechanisms. Moreover, a comprehensive understanding of the processes governing radical‐OLET is obtained by recording complete 2D maps of both optical and electrical response of the device as a function of applied voltages. Notably, the trapping of electrons by radical moieties is demonstrated to generate a negative charge density in the emissive layer that facilitates holes to be injected: increasing the balance of opposite charge carriers, a tenfold enhancement of the external quantum efficiency (EQE) at the proper source‐drain and source‐gate voltage conditions is reported to reach a maximum EQE value of 0.2%.

Electrostatic fence induced assembly of low-concentration colloidal nanospheres to form liquid photonic crystals

Liquid photonic crystals (LPCs) have great application potential in sensors, anti-counterfeiting materials and detection due to their sensitive dynamic responsiveness. Currently, the preparation of LPCs mainly relies on the supersaturation of colloidal nanospheres. However, the supersaturation method usually fails to obtain LPCs based on low-concentration colloidal nanospheres. In turn, the use of high-concentration colloidal nanospheres results in poor mobility of LPCs, which makes them inappropriate for subsequent utilization in responsive systems. In this study, self-assembly of LPCs with vibrant structural colors is achieved through the electrostatic fence effect by introducing an anionic carboxylate-containing polymer as an inducer into the system of low-concentration negatively charged colloidal nanospheres (≥1.25 wt%). It is shown that the anionic carboxylate groups on the inducer molecules and the appropriate molecular chain length are the decisive factors for the inducing effect. The obtained LPCs exhibit a typical non-close-packed structure with a face-centered cubic arrangement of nanospheres. The nearest inter-nanosphere surface distance is 12.10 nm, and the farthest one is as long as 40.30 nm. The LPCs possess good dynamic recovery performance and sensitive optical response characteristics, which are conducive to application in responsive optical sensors directly or after filling.

Non-local optical response of a multi-phased quantum material

Non-local optical response of a multi-phased quantum material

Theoretical calculations of nonlinear optical responses for interpreting nonconjugated molecular systems to affect non-optimal properties

Understanding the intricacies of polymorphic origins in nonconjugated crystal systems is crucial for optimizing their properties. This study focuses on the crystal growth, characterization, and nonlinear optical (NLO) responses of a system analyzed using single crystal X-ray analysis, revealing a monoclinic geometry. Hirschfeld surface analysis emphasized the significance of intermolecular interactions in driving polymorph development, shedding light on the structural nuances influencing the material’s properties. Through the evaluation of density functional theory parameters, the research found that the NLO responses of the system were as efficient as those of widely recognized materials like urea and KDP. Moreover, the stability of the system was confirmed through (NBO) analysis, showcasing its potential for practical applications. By manipulating the polymorphic crystal forms, researchers can potentially unveil new crystalline materials with tailored properties suitable for applications in optical and optoelectronic devices. This work underscores the importance of exploring novel crystal engineering strategies to harness the full potential of materials in the realm of advanced technologies.

A comprehensive study on optical properties of La2O3 and HfO2 for radiative cooling via multiscale simulations

Abstract Radiative cooling materials have gained prominence as a zero-energy solution to mitigate global warming. However, a comprehensive understanding of atomic-scale optical properties and macroscopic optical performance of radiative cooling materials remains elusive, limiting insights into the underlying physics of their optical response and cooling efficacy. La2O3 and HfO2, representing rare earth and third/fourth subgroup inorganic oxides respectively, which show promise for radiative cooling applications. In this work, we employed multiscale simulations to investigate the optical properties of La2O3 and HfO2 across a broad spectrum. First-principles calculations revealed their dielectric functions and intrinsic refractive indices and the results indicated that the slightly smaller bandgap of La2O3 compared to HfO2 induces a higher refractive index in the solar band. Additionally, three-phonon scattering was found to provide more accurate infrared optical properties than two-phonon scattering, which enhances the emissivity in the sky window. Monte Carlo simulations were also used to determine the macroscopic optical properties of La2O3 and HfO2 coatings. Based on simulated results, we identified that particle size and particle volume fraction play the dominant role in optical properties. Our findings underscore the potential of La2O3 and HfO2 nanocomposites for environmentally friendly cooling and offer a new approach for high-throughput screening of optical materials through multiscale simulations.

Plasmonic Coupling for High‐Sensitivity Detection of Low Molecular Weight Molecules

This article presents a novel plasmonic sensing platform designed for the detection of low molecular weight molecules, offering significant advancements in diagnostic applications. The platform features a periodic array of gold nanodisks on a 20 nm thin silica layer, supported by a 100 nm thick gold substrate. By leveraging the coupling between localized and propagating surface plasmon resonances, this design significantly enhances the sensitivity and specificity of molecular detection. Finite element method simulations are conducted to characterize the optical properties and reflectance response of the nanodisks array in the visible to near‐infrared range. Ellipsometric analysis is performed to measure the reflectance of the sample at various angles. Additionally, scanning near‐field optical microscopy in reflectance mode validates the design by revealing well‐defined plasmonic hot spots and interference patterns consistent with the simulated results. The findings demonstrate the platform's effectiveness in amplifying optical signals, achieving a limit of detection of 50 μM for molecules with a molecular weight of less than 1 KDa. This high sensitivity and specificity highlight the potential of the proposed plasmonic platform to advance the development of highly sensitive sensors for low molecular weight molecules, making it a valuable tool for diagnostics and precise molecular detection.

Synthesis, photophysical properties, and in-silico nonlinear optics of 3-hydroxy-N-phenyl-2-naphthamide and its acetate, acrylate, and benzoate derivative

In this study, we report the successful growth of single crystals of 3-hydroxynaphthalene-2-carboxanilides (NAS) with a monoclinic structure in the P21/c space group and space group number of 14 for the first time. We have developed a yield and time-effective modified synthetic procedure using a synthetic reactor by replacing the traditional microwave method. Additionally, acylated derivatives of NAS, including novel acryloyl derivative (NAS AC), are synthesized with a modified procedure, replacing pyridine with triethylamine.We investigate the structural, photophysical, and quantum chemical properties of N-(4-acetylphenyl)-2-oxo-2H-chromene-3-carboxamide (NAS) and its acylated derivatives (NAS AC, NAS ACT, NAS BZ). Photophysical studies reveal significant Stokes shifts observed in different solvents, including time-enhanced fluorescence in DMSO, attributed to solvent relaxation processes. Natural bond orbital (NBO) analysis, molecular electrostatic potential (MEP) maps, and frontier molecular orbital (FMO) provide insights into electronic interactions and asymmetric charge distribution. Low-lying LUMO values of these compounds (-2.31 eV to -1.95 eV) support candidature for the electron acceptor applications. Nonlinear optical properties were thoroughly investigated, with NAS displaying the highest static first-order hyperpolarizability (17.89 × 10−30 esu) and NAS BZ exhibiting the highest second-order hyperpolarizability (113.09 × 10−36 esu), indicating significant nonlinear optical responses. Thermal stability (TGA and DTA) highlights the significant range of temperatures for the NLO applications.

Enhanced high-harmonic generation in a polarization-insensitive all-dielectric metasurface exploiting dual-Fano resonance

Nonlinear optics demands efficacious techniques for nonlinear properties engineering. Metasurfaces, as a flat technology with easy fabrication in various arrangements and without the need for phase-matching conditions, are suitable platforms for nonlinear optics. This study proposes a silicon metasurface with special geometry that provides high conversion efficiency by exploiting Fano resonances and the excitation of magnetic and toroidal dipoles. The results indicate the high efficiencies of third harmonic generation of 5.17×10−3 W−2 and fifth harmonic generation of 7.92×10−9 W−4 under 1 GW/cm2 pump intensity in the near-infrared regime. More specifically, linear and nonlinear optical responses of the structure are completely polarization-independent.

Numerical modeling of SNSPD absorption utilizing optical conductivity with quantum corrections

Superconducting nanowire single-photon detectors are widely used in various fields of physics and technology, due to their high efficiency and timing precision. Although, in principle, their detection mechanism offers broadband operation, their wavelength range has to be optimized by the optical cavity parameters for a specific task. We present a study of the optical absorption of a superconducting nanowire single photon detector with an optical cavity. The optical properties of the niobium nitride films, measured by spectroscopic ellipsometry, were modeled using the Drude–Lorentz model with quantum corrections. The numerical simulations of the optical response of the detectors show that the wavelength range of the detector is not solely determined by its geometry, but the optical conductivity of the disordered thin metallic films contributes considerably. This contribution can be conveniently expressed by the ratio of imaginary and real parts of the optical conductivity. This knowledge can be utilized in detector design.

Broadband self-powered MoS2/PdSe2/WSe2 PSN heterojunction photodetector for high-performance optical imaging and communication

Two-dimensional (2D) semi-metal transition metal dichalcogenides (TMDs) have drawn significant attention for their distinctive physical properties. However, the inherent high dark current of these materials and the single structure of detectors hinder the further development of photodetectors with high performance. Here, we construct a PSN (p-type semiconductor/semi-metal/n-type semiconductor) architecture by sandwiching 2D semi-metal between two semiconductor layers. In this architecture, the top and bottom layers generate an internal built-in electric field, while the middle layer serves as an absorption layer for low-energy photons and facilitates the dissociation of photo-generated carriers. As a result, the heterojunction device demonstrates a wide spectrum optical response from visible to infrared light (405 nm to 1550 nm) without requiring an external voltage. Working in self-powered mode at room temperature, the device achieves a responsivity of 0.56 A/W, a detectivity of 5.63 × 1011 Jones, and a rapid response speed of 190/74 µs. Additionally, the device shows potential for applications in fast optical communication and multi-wavelength optical imaging. This work presents a novel approach for developing a new type of broadband, self-powered, high-performance miniaturized semi-metal-based photodetector.

Magnetic field-engineered optical nonlinearity in germanene nanotubes

Abstract The linear and nonlinear optical properties of germanene nanotubes (GeNTs) under the influence of magnetic fields are investigated through theoretical analysis. By employing a tight-binding model beyond the Dirac cone approximation, the electronic band structure, density of states, dipole matrix elements, and third-order nonlinear optical susceptibilities are calculated. The application of a magnetic field induces a Zeeman splitting of the energy levels, breaking the band degeneracy. Consequently, the dipole matrix elements exhibit a magnetic field dependence, altering the intensity and number of allowed transitions. In the infrared and ultraviolet energy regions, the linear optical absorption spectrum displays the splitting of peaks into dual neighboring peaks, with the splitting distance linearly dependent on the magnetic field strength. The third-order nonlinear optical susceptibilities, χTHG(3)3ω and χIDIR(3)ω, reveal the emergence of multiple resonance peaks in different energy regions due to two-photon and three-photon absorption processes. The magnetic field significantly influences the number, position, and height of these optical peaks, enabling effective control over the nonlinear optical response. By investigating the scaled energy (E/E_g) dependence, a universal behavior is observed for the three- and two photon resonance peaks, where their positions remain constant, but their peak intensities are significantly enhanced under the influence of the magnetic field. These findings demonstrate the potential of GeNTs as tunable nonlinear optical materials, with the magnetic field serving as an effective parameter for engineering their optical properties for various applications in optoelectronics, photonics, and related fields.

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.

Pulse length effects in the nonresonant long-wave infrared nonlinear optical response of n-Ge, GaAs, and ZnSe

Nonlinear optical refraction and nonlinear absorption are characterized in important long-wave infrared optical materials with picosecond and femtosecond laser pulses. The effective nonlinear refractive indices are found to be constant across a range of pulse parameters. Nonlinear absorption far from resonance is observed at relatively low (∼1GW/cm2) intensities in these materials, and the onset intensity and fluence scale strongly with pulse length. A free carrier dominated nonlinear absorption mechanism is identified for picosecond pulses, whereas nonperturbative photoionization causes femtosecond absorption.

Error rates of optically pre-amplified PPM wireless systems with coding and arbitrary optical filter response

We present novel results for the uncoded and coded bit-error probability (BEP) of optically pre-amplified pulse-position modulation (PPM) wireless systems. For uncoded systems, a novel analytic method for the evaluation of the BEP is derived. The method takes into account the non-ideal optical filter response and utilizes a finite Karhunen–Loève series expansion to calculate the BEP. Using the proposed approach, it is possible to accurately evaluate the PPM BEP for arbitrarily shaped filters where the well-established χ2 method only provides approximate results. Considering a Lorentzian filter response, the discrepancy between the two methods amounts to 0.5 dB in a variety of filter bandwidths and PPM modulation orders. The Lorentzian filter response was chosen as an illustrative practical example whose series can be calculated analytically. The proposed method is also valid for any type of optical filter for which the Karhunen–Loève series expansion can be calculated analytically or numerically. Due to the finite number of terms that are required irrespective of the signal energy level, the proposed method can also be applied without loss of accuracy to assess the system performance under the effects of turbulence and adverse weather conditions. For coded systems with Lorentzian filters, Monte-Carlo simulations are utilized to evaluate the BEP performance of the 5G LDPC codes, and it is demonstrated that they impart an energy gain up to 3.3 dB for 4–PPM and 2.3 dB for 16–PPM at a target BEP of 10−5. The optimal code rates are also discussed for several combinations of the optical filter bandwidth and PPM modulation order and it is shown that in almost all of the cases the optimal code rate is 11/13. Moreover, the sum-product and min-sum decoders perform within 0.1 dB from each other for the best code rates, which points towards the utilization of the min-sum decoder in all settings, since its operation does not require knowledge of the filter parameters. Finally, the comparison between the coded systems with Lorentzian and ideal passband filters exhibits the same 0.5 dB discrepancy that was observed for uncoded systems.

Understanding the optoelectronic and vibrational properties of MB[formula omitted]O[formula omitted], using density functional theory, where M = Yb or Ce

This work aims to use density functional theory (DFT) and density functional perturbation theory (DFPT) to study the structure, optoelectronics, phonon dispersion and energetic stability of two new tetraborates, MB4O7, where M = Yb or Ce. The estimated values of the band gap energy (Eg) and power conversion efficiency (PCE) for the systems were calculated. The Shockley-Queisser was also taken into account to measure the maximum theoretical efficiency of a photovoltaic source cell based on a p-n union. The estimated average gap energy values for the YbB4O7 and CeB4O7 systems, calculated using the GGA-PBE, HSE06, and GGA+U functionals, were 3.64 eV and 0.97 eV, respectively. The average PCEs calculated for the YbB4O7 and CeB4O7 systems were 11.28% and 25.66%, respectively. The PCE and energy stability suggest that CeB4O7 may be a more viable candidate for a solar device than YbB4O7, at least in terms of these specific parameters. The results reported here, as well as those related to absorption calculations, showed that the structures have optical responses in the visible region, suggesting that both systems can be used as optoelectronic devices and in solar cell designs.

Efficiency-aware machine-learning driven design of solar harvester for renewable energy application

Although MIM structures have been studied for solar thermal applications for decades, the multilayer MI-MIM structure is the subject of this study's investigation for batter absorption. In order to identify an effective solar absorber, two configurations Gold-MgF2-Gold (GMGSA) and Gold-MgF2-Gold-MgF2-Gold (GMGMGSA) are examined in this work. By using machine learning approaches, this research was able to get an MSE of 2.8091 × 10−5 and an R2 value of 0.998836. The optical response and parameter optimization analysis have been examined in this work in the wavelength range of 0.4 μm–1.6 μm. When exposed to AM 1.5 spectrum radiation, the GMGMGSA absorbs 93.10 % of the radiation, compared to 88.30 % for the single-layer GMGSA. Furthermore, both structures show steady absorption that is independent of polarization up to a 70° incidence angle. The aforementioned discoveries render the structure a plausible contender for solar thermal uses, including battery-integrated photovoltaic (BIPV), commercial solar power (CSP), and solar water heating. This might lead to a future where energy is more sustainably produced.

Unveiling the Effect of Dilution on the Optical Response of Folic Acid Derived Carbon Dots: Role of Surface Interactions and Inner Filter Effect

Unveiling the Effect of Dilution on the Optical Response of Folic Acid Derived Carbon Dots: Role of Surface Interactions and Inner Filter Effect

Pioneering the future with silicon carbide integrated photonics

Silicon carbide (SiC) integrated photonics is advancing rapidly, promising to overcome the limitations of other integrated photonics platforms and enable new quantum devices. This progress is driven by SiC’s exceptional optical properties and significant advancements in epitaxial growth technologies, enabling wafer-scale production and manufacturability. The development of photonic components in SiC and SiC on Insulators at the wafer scale marks a paradigm shift in the role of SiC in photonics, a field dating back over 20 years. These advancements are seamlessly incorporating SiC into both integrated photonics and the emerging quantum photonics sector. SiC’s wide bandgap, high thermal conductivity, and robust nonlinear optical response make it ideal for a range of applications, from resilient photonic circuits in harsh environments to quantum devices that could revolutionize computing and communication. As research progresses, SiC-integrated photonics is poised to deliver cutting-edge, energy-efficient, and high-performance solutions that align with the goals of a sustainable and technologically advanced future.

Experimental magnetic-semiconductor features of the theoretically half-metallic perovskite CaLaTiFeO6

Abstract In this manuscript, the synthesis process of the CaLaTiFeO6 material is shown. The crystallographic structure analysis reveals its monoclinic perovskite type nature (space group P21/n, #14), its morphological strongly granular characteristics, its optical response yields its semiconducting character with a 0.61 eV bandgap and its ferromagnetic property at temperatures T>350 K are reported. Likewise, calculations and analysis of the electronic properties are performed through Density Functional Theory, which showed correlation with the experimental results. The results allow classifying the CaLaTiFeO6 material as a ferromagnetic semiconductor at room temperature, making it a good candidate for the design of spintronic devices.