Discrete Dipole Approximation Research Articles

Plasmonic couplings in Ag-Au heterodimers.

The plasmonic coupling between silver (Ag) and gold (Au) nanoparticles (NPs) under four polarization modes was examined: a longitudinal mode (L-mode), where the electric field of a linearly polarized incident light parallels the dimer axis, and three transverse modes (T-modes), where the electric field of the light is perpendicular to the dimer axis. The coupling was studied using the discrete dipole approximation followed by an in-house postprocessing code that determines the extinction (Qext), absorption (Qabs), and near-field (Qnf) spectra from the individual NPs as well as the whole system. In agreement with the literature results, the extinction/absorption spectra of the whole dimer have two peaks, one near the Ag localized surface plasmon resonance (LSPR) region and the other at the Au LSPR region, with the peak at Ag LSPR being reduced in all modes and the peak at Au LSPR being red-shifted and increased in the L-mode but not in the T-modes. It is further shown that the scattering at the Ag LSPR region is reduced and becomes less than the isolated Ag NPs, but the absorption at the Ag LSPR is increased and becomes greater than the isolated Ag NPs for the 50nm Ag-Au heterodimer. This suggests that the scattering from Ag NPs is being reabsorbed by the neighboring Au NPs due to the interband electronic transition in Au at that wavelength range. The Qext from the individual NP in the heterodimer shows the presence of the Fano profile on the Au NP but not on the Ag NP. This phenomenon was further investigated by using a dielectric particle (DP) placed near the Ag or Au NPs. The Fano profile appears in the absorbing DP spectra placed near either Ag or Au NPs. However, the Fano profile is masked upon further increases in the refractive index value of the DP particle. This explains the absence of a Fano profile on the Ag NPs in the Ag-Au heterodimer. The large near-field enhancement on both Ag and Au NPs at the Au plasmonic wavelength in the L-mode for large NPs was investigated through a DP-Au system. The large enhancement was shown to arise from a large imaginary component of the DP refractive index and a small real component. Through examination of both the near- and far-field properties of the individual NPs as well as the whole system and examinations of DP-Ag and DP-Au systems, our study provides a new understanding of the couplings between Ag and Au NPs.

THEMIS 2.0: A self-consistent model for dust extinction, emission, and polarisation

Context. Recent observational constraints in emission, extinction, and polarisation have at least partially invalidated most of the astronomical standard grain models for the diffuse interstellar medium. Moreover, laboratory measurements on interstellar silicate analogues have shown quite significant differences with the optical properties used in these standard models. Aims. To address these issues, our objective is twofold: (i) to update the optical properties of silicates and (ii) to develop The Heterogeneous dust Evolution Model for Interstellar Solids (THEMIS) to allow the calculation of polarised extinction and emission. Methods. Based on optical constants measured in the laboratory from 5 µm to 1 mm for amorphous silicates and on observational constraints in mid-IR extinction and X-ray scattering, we defined new optical constants for the THEMIS silicates. Absorption and scattering efficiencies for spheroidal grains using these properties were subsequently derived with the discrete dipole approximation. Results. These new optical properties make it possible to explain the dust emission and extinction, both total and polarised. It is noteworthy that the model is not yet pushed to its limits since it does not require the perfect alignment of all grains to explain the observations and it therefore has the potential to accommodate the highest polarisation levels inferred from extinction measurements. Moreover, the dispersion of the optical properties of the different silicates measured in the laboratory naturally explain the variations in both the total and polarised emission and extinction observed in the diffuse interstellar medium. Conclusions. A single, invariant model calibrated on one single set of observations is obsolete for explaining contemporary observations. We are proposing a completely flexible dust model based entirely on laboratory measurements that has the potential to make major advances in understanding the exact nature of interstellar grains and how they evolve as a function of their radiative and dynamic environment. Even if challenging, this is also relevant for future cosmic microwave background (CMB) missions that will aim to perform precise measurements of the CMB spectral distortions and polarisation.

Transfer learning for metamaterial design and simulation

Abstract We demonstrate transfer learning as a tool to improve the efficacy of training deep learning models based on residual neural networks (ResNets). Specifically, we examine its use for study of multi-scale electrically large metasurface arrays under open boundary conditions in electromagnetic metamaterials. Our aim is to assess the efficiency of transfer learning across a range of problem domains that vary in their resemblance to the original base problem for which the ResNet model was initially trained. We use a quasi-analytical discrete dipole approximation (DDA) method to simulate electrically large metasurface arrays to obtain ground truth data for training and testing of our deep neural network. Our approach can save significant time for examining novel metasurface designs by harnessing the power of transfer learning, as it effectively mitigates the pervasive data bottleneck issue commonly encountered in deep learning. We demonstrate that for the best case when the transfer task is sufficiently similar to the target task, a new task can be effectively trained using only a few data points yet still achieve a test mean absolute relative error of 3 % with a pre-trained neural network, realizing data reduction by a factor of 1000.

RDDA method for characterization of photonic nanojets.

This paper presents a reduced discrete dipole approximation (RDDA) method as a flexible and powerful tool for computing the field distribution of photonic nanojets (PNJs) based on superposition of the induced dipole radiation fields with a low number of lattice points at the surface of microparticles. Microparticles with spherical and ellipsoidal shapes have been studied using the RDDA method to produce PNJs. The incident beam polarization and filling factor effects in the PNJs' shape and confinement strength have been characterized by quality factor Q. The best confined PNJs have been found in microellipsoids with a specific range of the shape parameter and filling factor values.

Numerical study of near-field radiative heat transfer between bio-inspired spiny particles

The spine-like structure appears on some smooth organisms and has a high light absorption cross-section. Inspired by the spiny structure in the nature, this study establishes models of solid and hollow spiny particles. The effects of spine cross-section size, uniform and nonuniform spine distribution, hollow size, gap, and spine dislocation on near-field radiative heat transfer of spiny particles are investigated based on the thermal discrete dipole approximations method. The spectral radiative conductance and volumetric net power distribution are obtained. The results indicate that the coupling of localized surface phonons between two particles is affected by spine cross-section size and spine distribution. Near-field radiative heat transfer of spiny particles is enhanced maximumly when the frequencies are slightly lower than the resonance frequency of smooth particles. The peak of the spectral conductance is red-shifted and decreases with the increase of hollow size. The uniformity of volumetric power absorbed distribution increases and the variation of the relative spectral conductance decreases with increasing gap. The influence of two particles’ spine dislocation on near-field radiative heat transfer and volumetric power absorbed distribution is not obvious.

Computational modeling of Chlamydomonas reinhardtii cellular radiation properties with synergistic consideration of complex structures and compositions.

The radiation characteristics of microalgae are of great significance for the design of photobioreactors and ocean optical remote sensing. Yet the complex structure of microalgae makes it difficult to theoretically predict its radiation characteristics based on traditional Mie theory. In this work, taking Chlamydomonas reinhardtii as an example, a multi-component cell model with a complex structure is proposed, which considers the organelles and shape of microalgae, and the volume change during the production of Chlamydomonas reinhardtii lipids. The theoretical calculation is carried out using the discrete dipole approximation method, and an improved transmission method is used for experimental measurement. The experimental data are compared and analyzed with the multi-component complex structure model, the homogeneous sphere model and the coated sphere model. The results show that the calculation accuracy of the multi-component complex structure model is higher, the error of the scattering cross-section is reduced by more than 8.6% compared with the homogeneous sphere model and coated sphere model, and the absorption cross-section and the scattering phase function are in good agreement with the experimental results. With the increase of lipids, the absorption cross-section and the scattering phase function vary slightly. However, the scattering cross-section has an observed change with increasing wavelength. In addition, the theoretical calculation error can be reduced when the influence of the culture medium is taken into account.

Experimental and Theoretical Studies on Ag Nanoparticles with Enhanced Plasmonic Response, Formed Within Al2O3 Thin Films Deposited by Magnetron Sputtering

AbstractReactive magnetron sputtering was employed to prepare nanocomposite thin films of Ag/Al2O3, on a glass substrate. The films are characterized by the formation of Ag nanoparticles embedded in the Al2O3 matrix, after thermal treatment at 600 °C, which are responsible for the appearance of an outstanding pronounced and narrow localized surface plasmon resonance (LSPR) band. Electron microscopy analysis also revealed the presence of larger Ag fractal aggregates at the film’s surface, responsible for a broad band absorption. Noteworthily, the LSPR band maximum remains at the same position (about 412 nm) for Ag concentrations ranging from 23 to 34 at.%, despite some discernible alterations in both LSPR band intensity and width. An optimized thin film is characterized by full transparency in non-resonant wavelengths due to suppression of Ag aggregates at the film’s surface, while maintaining the LSPR behavior. To better explain the plasmonic behavior of the Ag/Al2O3 films, discrete dipole approximation was used to determine the extinction, scattering, and absorption efficiencies of Ag spheres surrounded by an Al2O3 cap layer. This allowed to ascertain some nanostructural features of the films, pointing to the formation of Ag nanoparticles with average sizes in the order of 40 nm.

Surface enhanced infrared absorption mechanism and modification of the plasmonic response

Surface enhanced infrared absorption (SEIRA) is an experimental method where trace amount of a compound can be detected with high sensibility. This high detection sensibility is the result of the interaction of the molecules with a localized plasmon, usually from a metallic nanoparticle. In this study we numerically investigate by discrete dipole approximation the origin of the Fano-like response of the system, including the induced transparency when the plasmon resonance and the molecular vibrational mode coincide. The detailed analysis of the localization of the absorption shows that the modification of the absorption cross-section when the molecule is present comes from a change of the plasmonic resonance, not from the direct molecular response which is negligible. This sheds a new light on the SEIRA mechanism. In particular, it demonstrates that the sensibility is associated with the influence of the molecule on the plasmon resonance rather than with the local field enhancement itself.

Asymmetric imaging through engineered Janus particle obscurants using a Monte Carlo approach for highly asymmetric scattering media

The advancement of imaging systems has significantly ameliorated various technologies, including Intelligence Surveillance Reconnaissance Systems and Guidance Systems, by enhancing target detection, recognition, identification, positioning, and tracking capabilities. These systems can be countered by deploying obscurants like smoke, dust, or fog to hinder visibility and communication. However, these counter-systems affect the visibility of both sides of the cloud. In this sense, this manuscript introduces a new concept of a smoke cloud composed of engineered Janus particles to conceal the target image on one side while providing clear vision from the other. The proposed method exploits the unique scattering properties of Janus particles, which selectively interact with photons from different directions to open up the possibility of asymmetric imaging. This approach employs a model that combines a genetic algorithm with Discrete Dipole Approximation to optimize the Janus particles' geometrical parameters for the desired scattering properties. Moreover, we propose a Monte Carlo-based approach to calculate the image formed as photons pass through the cloud, considering highly asymmetric particles, such as Janus particles. The effectiveness of the cloud in disguising a target is evaluated by calculating the Probability of Detection (PD) and the Probability of Identification (PID) based on the constructed image. The optimized Janus particles can produce a cloud where it is possible to identify a target more than 50% of the time from one side (PID > 50%) while the target is not detected more than 50% of the time from the other side (PD < 50%). The results demonstrate that the Janus particle-engineered smoke enables asymmetric imaging with simultaneous concealment from one side and clear visualization from the other. This research opens intriguing possibilities for modern obscurant design and imaging systems through highly asymmetric and inhomogeneous particles besides target detection and identification capabilities in challenging environments.

Optimizing Color Saturation in Colloidal Photonic Crystals by Control of Absorber Amount and Distribution

AbstractNanostructured materials that mimic structural coloration in nature can be synthetically created by colloidal self‐assembly. To maximize optical effects, the natural world integrates melanin as a broadband absorber to remove incoherently scattered light. Polydopamine (PDA) is used as a synthetic analog of natural melanin to systematically investigate the influence of absorber quantity and distribution on color saturation in colloidal photonic crystals. The absorbing PDA is integrated into two distinct ways: homogenous colloidal crystals are produced from core–shell particles with incrementally increasing polydopamine shells, and heterogeneous colloidal crystals are formed by co‐assembly of varying ratios of polystyrene (PS) and absorbing PS@PDA particles. The chromaticity is quantified by converting the measured spectra to reconstructed colors in the L*a*b* color sphere to identify structures with optimal color saturation. Simulations based on the discrete dipole approximation (DDA) indicate that a homogeneous absorber distribution is most efficient in creating saturated structural coloration. Experiments, however, demonstrate that the heterogeneous absorber incorporation outperforms the homogeneous strategies, as it allows for a more precise adjustment of the absorber content in the required concentration range. These results underline the importance of incorporating absorbers and indicate efficient ways in which colloidal photonic crystals with saturated structural colors can be prepared.

Theoretical and experimental study on the radiative properties of Parachlorella kessleri: considering the effect of internal microstructure.

A microalgal cell model with multiple organelles considering both the irregular overall shape and internal microstructure was proposed. The radiative properties of Parachlorella kessleri during the normal phase, starch-rich phase, and lipid-rich phase were calculated by the discrete dipole approximation method in the visible wavelengths. The accuracy of the model is verified with experimental measurements. The results showed that the theoretical calculation of the established microalgal cell model is more accurate than those of the equal volume spheres, such as the homogeneous sphere and the coated sphere, with the errors of the scattering cross-section reduced by more than 10.7%. The calculated scattering phase function of the multi-component model is basically in good agreement with the experimental results. Compared to the normal growth phase, the lipid enrichment during the lipid-rich phase leads to a sharp increase in the scattering cross-section by three to four times, while the absorption cross-section remains stable. Remarkably, in the starch-rich phase, the abundant production of starch results in a reduction of two to three times in the absorption cross-section compared to the normal growth phase, while the scattering cross-section varies little. The results can provide basic data and theoretical support for the design and optimization of photobioreactors.

Determining intrinsic potentials and validating optical binding forces between colloidal particles using optical tweezers

Understanding the interactions between small, submicrometer-sized colloidal particles is crucial for numerous scientific disciplines and technological applications. In this study, we employ optical tweezers as a powerful tool to investigate these interactions. We utilize a full image reconstruction technique to achieve high precision in characterizing particle pairs that enable nanometer-scale measurement of their positions. This approach captures intricate details and provides a comprehensive understanding of the spatial arrangement between particles, overcoming previous limitations in resolution. Moreover, our research demonstrates that properly accounting for optical binding forces to determine the intrinsic interaction potential is vital. We employ a discrete dipole approximation approach to calculate optical binding potentials and achieve a good agreement between the calculated and observed binding forces. We incorporate the findings from these simulations into the assessment of the intrinsic interaction potentials and validate our methodology by using short-range depletion attraction induced by micelles as an example.

Multiplexed Surface Protein Detection and Cancer Classification Using Gap-Enhanced Magnetic-Plasmonic Core-Shell Raman Nanotags and Machine Learning Algorithm.

Cancer is the second leading cause of death attributed to disease worldwide. Current standard detection methods often rely on a single cancer marker, which can lead to inaccurate results, including false negatives, and an inability to detect multiple cancers simultaneously. Here, we developed a multiplex method that can effectively detect and classify surface proteins associated with three distinct types of breast cancer by utilizing gap-enhanced Raman scattering nanotags and machine learning algorithm. We synthesized anisotropic magnetic core-gold shell gap-enhanced Raman nanotags incorporating three different Raman reporters. These multicolor Raman nanotags were employed to distinguish specific surface protein markers in breast cancer cells. The acquired signals were deconvoluted and analyzed using classical least-squares regression to generate a surface protein profile and characterize the breast cancer cells. Furthermore, computational data obtained via finite-difference time-domain and discrete dipole approximation showed the amplification of the electric fields within the gap region due to plasmonic coupling between the two gold layers. Finally, a random forest classifier achieved an impressive classification and profiling accuracy of 93.9%, enabling effective distinguishing between the three different types of breast cancer cell lines in a mixed solution. With the combination of immunomagnetic multiplex target specificity and separation, gap-enhancement Raman nanotags, and machine learning, our method provides an accurate and integrated platform to profile and classify different cancer cells, giving implications for identification of the origin of circulating tumor cells in the blood system.

Simulation of Highly Sensitive Multi-Core-Satellite Plasmonic Structures for Detection of Gastric Cancer Agent MicroRNA-21 Using Modified Discrete Dipole Approximation

Simulation of Highly Sensitive Multi-Core-Satellite Plasmonic Structures for Detection of Gastric Cancer Agent MicroRNA-21 Using Modified Discrete Dipole Approximation

Sensitivity of Polarization to Grain Shape. I. Convex Shapes

Aligned interstellar grains produce polarized extinction (observed at wavelengths from the far-ultraviolet to the mid-infrared) and polarized thermal emission (observed at far-infrared and submm wavelengths). The grains must be quite nonspherical, but the actual shapes are unknown. The relative efficacy for aligned grains to produce polarization at optical versus infrared wavelengths depends on particle shape. The discrete dipole approximation is used to calculate polarization cross sections for 20 different convex shapes, for wavelengths from 0.1 to 100 μm, and grain sizes a eff from 0.05 to 0.3 μm. Spheroids, cylinders, square prisms, and triaxial ellipsoids are considered. Minimum aspect ratios required by the observed starlight polarization are determined. Some shapes can also be ruled out because they provide too little or too much polarization at far-infrared and submm wavelengths. The ratio of 10 μm polarization to integrated optical polarization is almost independent of grain shape, varying by only ±8% among the viable convex shapes; thus, at least for convex grains, uncertainties in grain shape cannot account for the discrepancy between predicted and observed 10 μm polarization toward Cyg OB2-12.

Multipole Excitation of Localized Plasmon Resonance in Asymmetrically Coated Core–Shell Nanoparticles Using Optical Vortices

AbstractPlasmonic interactions between an asymmetrically coated ore–shell (ACCS) nanoparticle and an optical vortex produce a novel engagement of the spin angular momentum (SAM) and the orbital angular momentum (OAM) of the input. Simulations based on a discrete dipole approximation (DDA) indicate that the SAM and the OAM of the incident beam determine the modal order of resonance, correctly identifying the peak wavelength, and both the direction and magnitude of optical torque exerted upon the excited, localized plasmon resonance in the ACCS particle. These simulations also indicate higher‐order resonances, including hexapole and octupole modes, and a zero‐order resonance (expressible as a monopole mode), can be excited by judicious selection of the SAM and OAM. A detailed symmetry analysis shows how the multipoles associated with eigenmode excitations connect to the radiation multipoles at the heart of the multipole expansion. It is also shown how additional, distorted resonance modes due to the asymmetricity of the structure are also exhibited. These specific plasmonic characteristics, which cannot be realized by plane wave excitation, become possible through the ACCS asymmetry engaging with the distinct optical vortex nature of the excitation.

Biomass particle-radiation-interaction and the effect of shape and structure simplifications

Particle radiation significantly contributes to the overall heat transfer in pulverized solid fuel combustion. For a lower computational effort in numerical simulations, the particles are often assumed to be spherical without an internal structure. In particular, biomass particles deviate strongly from this shape assumption and consist of a structured porosity. To investigate the influence of these aspects, pulverized beech wood particles are modeled as realistic as possible, considering the asymmetric three-dimensional shape and tube-like pores. The numerically created particle is then used to calculate single-scattering properties (absorption-, scattering cross-section, and scattering phase function) by applying the discrete dipole approximation (DDA). Afterward, the shape and internal structure of the representative biomass particle are step-wise simplified, while comparing the impact on the radiation interaction with the detailed modeled particle.The calculations reveal that simplifications of the internal structure are acceptable as long as a similar shape is maintained. Here, an extruded ellipsis with no internal structure and an effective complex index of refraction indicates the best alternative and is recommended for future particle radiation simulations. While the deviations of the radiation cross-section between the extruded ellipsis and the realistic particle are below 10%, the deviations of the radiation cross-section between a sphere and the realistic particle are around 50%. The orientation averaged phase function of all particle models scatters more than 99.5% of the scattered radiation forward. Thus, a purely forward scattering model in combustion simulations is recommended.

The study of optical properties of single soot aggregate using three-dimension soft X-ray tomographic reconstruction

The linear depolarization ratio (LDR) is a key parameter used in remote sensing to distinguish particle types. The LDR of the soot fractal model is uneasy to match the measured values. In this paper we used three-dimensional (3D) synchrotron soft X-ray tomography (SXT) for the 3D reconstruction of the toluene-burning soot particles and used discrete dipole approximation to calculate optical properties. The obtained results showed the 3D reconstructed soot particles can efficiently reproduce the measured LDR. The results of this study will encourage us to develop a new morphology model, completely different from the traditional fractal model, for bare soot based on 3D reconstruction. This study is helpful for the understanding and explanation of LDR of bare soot particles.

A comprehensive study on the Rod-based plasmonic structures sensing using the modified discrete dipole approximation method

Using the previously introduced modified discrete dipole approximation (DDA) method by applying the full details of the nanoparticle and its surrounding environment, the detection sensitivity of molecules by plasmonic Rod-based nanosensors, including U-shaped and Rod-shaped structures, was investigated. In the calculations, the two factors of the magnitude of the wavelength shift and the ability to distinguish molecules with similar properties were of significant interest. The results indicated that the sensitivity of Rod-based nanostructures is significantly higher than that of spherical nanoparticles. Among the plasmonic Rod-based nanosensors, the silver U-shaped structure performs better than others. The wavelength shift of the absorption spectrum of different nanosensors for a given molecule was very different, making it possible to detect very similar molecules from each other by testing different sensors.

Reducing shape errors in the discrete dipole approximation using effective media.

The discrete dipole approximation (DDA) simulates optical properties of particles with any given shape based on the volume discretization. These calculations cost a large amount of time and memory to achieve high accuracy, especially for particles with large sizes and complex geometric structures, such as mixed black-carbon aerosol particles. We systematically study the smoothing of the DDA discretization using the effective medium approximation (EMA) for boundary dipoles. This approach is tested for optical simulations of spheres and coated black-carbon (BC) aggregates, using the Lorenz-Mie and multiple-sphere T-Matrix as references. For spheres, EMA significantly improves the DDA accuracy of integral scattering quantities (up to 60 times), when the dipole size is only several times smaller than the sphere diameter. In these cases, the application of the EMA is often comparable to halving the dipole size in the original DDA, thus reducing the simulation time by about an order of magnitude for the same accuracy. For a coated BC model based on transmission electron microscope observations, the EMA (specifically, the Maxwell Garnett variant) significantly improves the accuracy when the dipole size is larger than ¼ of the monomer diameter. For instance, the relative error of extinction efficiency is reduced from 4.7% to 0.3% when the dipole size equals that of the spherical monomer. Moreover, the EMA-DDA achieves the accuracy of 1% for extinction, absorption, and scattering efficiencies using three times larger dipoles than that with the original DDA, corresponding to about 30 times faster simulations.