Multiresonant all-dielectric metasurfaces based on high-order multipole coupling in the visible.

In many cases, optical metasurfaces are studied in the single-resonant regime. However, a multiresonant behavior can enable multiband devices with reduced footprint, and is desired for applications such as display pixels, multispectral imaging and sensing. Multiresonances are typically achieved by engineering the array lattice (e.g., to obtain several surface lattice resonances), or by adopting a unit cell hosting one (or more than one) nanostructure with some optimized geometry to support multiple resonances. Here, we present a study on how to achieve multiresonant metasurfaces in the visible spectral range by exploiting high-order multipoles in dielectric (e.g., diamond or titanium dioxide) nanostructures. We show that in a simple metasurface (for a fixed particle and lattice geometry) one can achieve triple resonance occurring nearly at RGB (red, green, and blue) wavelengths. Based on analytical and numerical analysis, we demonstrate that the physical mechanism enabling the multiresonance behavior is the lattice induced coupling (energy exchange) between high-order Mie-type multipoles moments of the metasurface's particles. We discuss the influence on the resonances of the metasurface's finite size, surrounding material, polarization, and lattice shape, and suggest control strategies to enable the optical tunability of these resonances.

Low-frequency magnetic response of gold nanoparticles.

Gold nanoparticles (AuNPs) exposed to low frequency magnetic fields have shown promise in enhancing biological processes, such as cellular reprogramming. Despite the experimental evidence, a comprehensive understanding of the underlying physical principles and the corresponding theory remains elusive. The most common hypothesis is that functionalized nanoparticles transiently amplify magnetic fields, leading to improved cellular reprogramming efficiency. However, a detailed investigation on this topic is lacking. This paper bridges this knowledge gap by conducting a comprehensive investigation on the magnetic response of surface-modified AuNPs exposed to magnetic fields with frequencies up to hundreds of MHz. Starting with the inherent properties of bulk gold material, we explore a wide range of magnetic susceptibilities that might result from the redistribution of charge carriers due to bond molecules on the particle surfaces. Through analytical models and numerical electromagnetic simulations, we examine various geometric factors that can enhance the magnetic response, including the number of particles, spatial distribution, size, and shape. Our broad investigation provides researchers with analytical and numerical estimates of the magnetic response of nanoparticles, and the associated limits that can be expected. We found that a magnetic field enhancement comparable to the incident field requires very high magnetic susceptibilities, well beyond the values measured in functionalized gold nanoparticles thus far.

Lasing Effect in Symmetrical van der Waals Heterostructured Metasurfaces Due to Lattice-Induced Multipole Coupling.

New practical ways to reach the lasing effect in symmetrical metasurfaces have been developed and theoretically demonstrated. Our approach is based on excitation of the resonance of an octupole quasi-trapped mode (OQTM) in heterostructured symmetrical metasurfaces composed of monolithic disk-shaped van der Waals meta-atoms featured by thin photoluminescent layers and placed on a substrate. We revealed that the coincidence of the photoluminescence spectrum maximum of these layers with the wavelength of high-quality OQTM resonance leads to the lasing effect. Based on the solution of laser rate equations and direct full-wave simulation, it was shown that lasing is normally oriented to the metasurface plane and occurs from the entire area of metasurface consisting of MoS2/hBN/MoTe2 disks with line width of generated emission of only about 1.4 nm near the wavelength 1140 nm. This opens up new practical possibilities for creating surface emitting laser devices in subwavelength material systems.

Laser Synthesis of Cerium-Doped Garnet Nanoparticles.

The application of a pulsed laser ablation technique for the generation of cerium-doped garnet nanoparticles in liquids is investigated. The morphological and optical properties of the obtained nanoparticles are demonstrated. Features introduced by the single crystals of Gd3Al2.4Ga2.6O12:Ce3+, Lu3Al5O12:Ce3+, and Y3Al1.25Ga3.75O12:Ce3+ from which the nanoparticles are generated, as well as the parameters of a liquid media on the garnet nanoparticle generation are experimentally studied using TEM and UV-Vis spectroscopy methods. It is shown how the size, shape, and internal structure of the nanoparticles are related to the external laser ablation conditions, as well as to the laser melting processes of NPs in the colloidal solutions. This work provides important information about the generated nanoparticles, which can be used as building blocks for specially designed structures with predetermined optical properties.

Trapped mode control in metasurfaces composed of particles with the form birefringence property.

Progress in developing advanced photonic devices relies on introducing new materials, discovered physical principles, and optimal designs when constructing their components. Optical systems operating on the principles of excitation of extremely high-quality factor trapped modes (also known as the bound states in the continuum, BICs) are of great interest since they allow the implementation of laser and sensor devices with outstanding characteristics. In this paper, we discuss how one can utilize the anisotropic properties of novel materials (transition metal dichalcogenides, TMDs), particularly, the bulk molybdenum disulfide (MoS2), to realize the excitation of trapped modes in dielectric metasurfaces. The bulk MoS2 is a thin-film structure in which the light wave behaves the same way as that in the uniaxial anisotropic material with the form birefringence property. Our metasurface is composed of an array of disk-shaped nanoparticles (resonators) made of the MoS2 material under the assumption that the anisotropy axis of MoS2 can be tilted to the rotation axis of the disks. We perform a detailed analysis of eigenwaves and scattering properties of such anisotropic resonators as well as the spectral features of the metasurface revealing dependence of the excitation conditions of the trapped mode on the anisotropy axis orientation of the MoS2 material used.

SERS uncovers the link between conformation of cytochrome c heme and mitochondrial membrane potential.

The balance between the mitochondrial respiratory chain activity and the cell's needs in ATP ensures optimal cellular function. Cytochrome c is an essential component of the electron transport chain (ETC), which regulates ETC activity, oxygen consumption, ATP synthesis and can initiate apoptosis. The impact of conformational changes in cytochrome c on its function is not understood for the lack of access to these changes in intact mitochondria. We have developed a novel sensor that uses unique properties of label-free surface-enhanced Raman spectroscopy (SERS) to identify conformational changes in heme of cytochrome c and to elucidate their role in functioning mitochondria. We have verified that molecule bond vibrations assessed by SERS are a reliable indicator of the heme conformation during changes in the inner mitochondrial membrane potential and ETC activity. We have demonstrated that cytochrome c heme reversibly switches between planar and ruffled conformations in response to the inner mitochondrial membrane potential (ΔΨ) and H+ concentration in the intermembrane space. This regulates the efficiency of the mitochondrial respiratory chain, thus, adjusting the mitochondrial respiration to the cell's consumption of ATP and the overall activity. We have found that under hypertensive conditions cytochrome c heme loses its sensitivity to ΔΨ that can affect the regulation of ETC activity. The ability of the proposed SERS-based sensor to track mitochondrial function opens broad perspectives in cell bioenergetics.

Transition metal dichalcogenide nanospheres for high-refractive-index nanophotonics and biomedical theranostics.

Recent developments in the area of resonant dielectric nanostructures have created attractive opportunities for concentrating and manipulating light at the nanoscale and the establishment of the new exciting field of all-dielectric nanophotonics. Transition metal dichalcogenides (TMDCs) with nanopatterned surfaces are especially promising for these tasks. Still, the fabrication of these structures requires sophisticated lithographic processes, drastically complicating application prospects. To bridge this gap and broaden the application scope of TMDC nanomaterials, we report here femtosecond laser-ablative fabrication of water-dispersed spherical TMDC (MoS2 and WS2) nanoparticles (NPs) of variable size (5 to 250 nm). Such NPs demonstrate exciting optical and electronic properties inherited from TMDC crystals, due to preserved crystalline structure, which offers a unique combination of pronounced excitonic response and high refractive index value, making possible a strong concentration of electromagnetic field in the NPs. Furthermore, such NPs offer additional tunability due to hybridization between the Mie and excitonic resonances. Such properties bring to life a number of nontrivial effects, including enhanced photoabsorption and photothermal conversion. As an illustration, we demonstrate that the NPs exhibit a very strong photothermal response, much exceeding that of conventional dielectric nanoresonators based on Si. Being in a mobile colloidal state and exhibiting superior optical properties compared to other dielectric resonant structures, the synthesized TMDC NPs offer opportunities for the development of next-generation nanophotonic and nanotheranostic platforms, including photothermal therapy and multimodal bioimaging.

Anapole Meta-Atoms: Nonradiating Electric and Magnetic Sources.

The existence of classical nonradiating electromagnetic sources is one of the puzzling questions to date. Here, we investigate radiation properties of physical systems composed of a single ultrahigh permittivity dielectric hollow disk excited by electric or magnetic pointlike dipole antennas, placed inside the inner bore. Using analytical and numerical methods, we demonstrate that such systems can support anapole states with total suppression of far-field radiation and thereby exhibit the properties of electric or magnetic nonradiating sources. It is shown that the suppression of the far-field radiated power is a result of the destructive interference between radiative contributions of the pointlike dipole antennas and the corresponding induced dipole moments of the hollow disk. The experimental investigation of the nonradiating electric source has been performed to confirm our theoretical predictions. Our results pave the way to create and realize compact nonradiative sources for applications in modern wireless power transfer systems, sensors, RFID tags, and medical technologies.

Experimental Demonstration of Surface Plasmon Polaritons Reflection and Transmission Effects.

Special integrated photonic surface structures composed of a dielectric semicircle ridge and a dielectric block placed on a metal substrate are proposed for the investigation of surface plasmon polariton (SPP) reflection and transmission effects. A fabrication method called microscope projection photolithography was employed for the preparation of the structures. Leakage radiation microscopy was applied for the excitation and observation of surface plasmon polaritons (SPPs). It was observed that SPPs exhibit a remarkable decrease in intensity when impinging onto the rectangular dielectric block. Nevertheless, the transmitted wave out of the dielectric block was always observable. The propagation behavior of both the reflected waves at two boundaries (air/dielectric and dielectric/air) and the transmitted wave inside the dielectric block were demonstrated for different SPP incident conditions. The variation of the angles of reflection and transmission with respect to the incident angle was analytically and experimentally investigated. An agreement between the calculated results and the experimental results was obtained. Our findings might allow for novel applications in sensing and analytics once the structures will be functionalized.

Core-shell particles as efficient broadband absorbers in infrared optical range.

We demonstrate that efficient broadband absorption of infrared radiation can be obtained with deeply subwavelength spherical dielectric particles covered by a thin metal layer. Considerations based on Mie theory and the quasi-static approximation reveala wide range of configuration parameters, within which the absorption cross section reaches the geometrical one and exceeds more than by order of magnitude the scattering cross section in the infrared spectrum. We show that the absorption is not only efficient but also broadband with the spectral width being close to the resonant wavelength corresponding to the maximum of the absorption cross section. We obtain a simple analytical expression for the absorption resonance that allows one to quickly identify the configuration parameters ensuring strong infrared absorption in a given spectral range. Relation between the absorption resonance and excitation of the short-range surface palsmon modes in the metal shell of particles is demonstrated and discussed. Our results can be used as practical guidelines for realization of efficient broadband infrared absorbers of subwavelength sizes desirable in diverse applications.

Transverse Scattering and Generalized Kerker Effects in All-Dielectric Mie-Resonant Metaoptics.

All-dielectric resonant nanophotonics lies at the heart of modern optics and nanotechnology due to the unique possibilities to control scattering of light from high-index dielectric nanoparticles and metasurfaces. One of the important concepts of dielectric Mie-resonant nanophotonics is associated with the Kerker effect that drives the unidirectional scattering of light from nanoantennas and Huygens metasurfaces. Here we suggest and demonstrate experimentally a novel effect manifested in the nearly complete simultaneous suppression of both forward and backward scattered fields. This effect is governed by the Fano resonance of an electric dipole and off-resonant quadrupoles, providing necessary phases and amplitudes of the scattered fields to achieve the transverse scattering. We extend this concept to dielectric metasurfaces that demonstrate zero reflection with transverse scattering and strong field enhancement for resonant light filtering, nonlinear effects, and sensing.

Enhanced absorption in all-dielectric metasurfaces due to magnetic dipole excitation.

All-dielectric nanophotonics lies at a forefront of nanoscience and technology as it allows to control light at the nanoscale using its electric and magnetic components. Bulk silicon does not experience any magnetic response, nevertheless, we demonstrate that the metasurface made of silicon parallelepipeds allows to excite the magnetic dipole moment leading to the broadening and enhancement of the absorption. Our investigations are underpinned by the numerical predictions and the experimental verifications. Also surprisingly we found that the resonant electric quadrupole moment leads to the enhancement of reflection. Our results can be applied for a development of absorption based devices from miniature dielectric absorbers, filters to solar cells and energy harvesting devices.

Resonant suppression of light transmission in high-refractive-index nanoparticle metasurfaces.

High-refractive-index nanoparticle two-dimensional arrays have attracted a lot of interest recently, as they support both electric and magnetic resonances and can be implemented as functional metasurfaces. Here we show that under particular conditions, the all-dielectric nanoparticle metasurfaces can resonantly suppress transmission. As an important example, resonant electric and magnetic dipole (MD) responses of silicon nanoparticle arrays are considered in the air, as well as in the dielectric matrix in visible and infrared spectral ranges. We show that the wave resonantly scattered forward by one or both electric and MD moments of nanoparticles can destructively interfere with the incident wave, providing significant suppression of the transmission through the array. The reported effect can find important applications in different fields related to optics and photonics such as the development of filters, sensors, and solar cells.

Direct Amplitude-Phase Near-Field Observation of Higher-Order Anapole States.

Anapole states associated with the resonant suppression of electric-dipole scattering exhibit minimized extinction and maximized storage of electromagnetic energy inside a particle. Using numerical simulations, optical extinction spectroscopy, and amplitude-phase near-field mapping of silicon dielectric disks, we demonstrate high-order anapole states in the near-infrared wavelength range (900-1700 nm). We develop the procedure for unambiguously identifying anapole states by monitoring the normal component of the electric near-field and experimentally detect the first two anapole states as verified by far-field extinction spectroscopy and confirmed with the numerical simulations. We demonstrate that higher-order anapole states possess stronger energy concentration and narrower resonances, a remarkable feature that is advantageous for their applications in metasurfaces and nanophotonics components, such as nonlinear higher-harmonic generators and nanoscale lasers.

Highly Stable Monocrystalline Silver Clusters for Plasmonic Applications.

Plasmonic sensor configurations utilizing localized plasmon resonances in silver nanostructures typically suffer from the rapid degradation of silver under ambient atmospheric conditions. In this work, we report on the fabrication and detailed characterization of ensembles of monocrystalline silver nanoparticles (NPs), which exhibit a long-term stability of optical properties under ambient conditions without any protective treatments. Ensembles with different densities (surface coverages) of size-selected NPs (mean diameters of 12.5 and 24 nm) on quartz substrates are fabricated using the cluster-beam technique and characterized by linear spectroscopy, two-photon-excited photoluminescence, surface-enhanced Raman scattering microscopy, and transmission electron, helium ion, and atomic force microscopies. It is found that the fabricated ensembles of monocrystalline silver NPs preserve their plasmonic properties (monitored with optical spectroscopy) and strong field enhancements (revealed by surface-enhanced Raman spectroscopy) at least 5 times longer as compared to chemically synthesized silver NPs with similar sizes. The obtained results are of high practical relevance for the further development of sensors, resonators, and metamaterials utilizing the plasmonic properties of silver NPs.

Resonant forward scattering of light by high-refractive-index dielectric nanoparticles with toroidal dipole contribution.

In this Letter, we demonstrate and investigate the Kerker-type effect in high-index dielectric nanoparticles for which the third-order multipoles give a considerable contribution to the light scattering process. It is shown that the Kerker-type effect (strong suppression of the backward light scattering and, simultaneously, resonant forward light scattering) can be associated with the resonant excitation of a toroidal dipole moment in the system. This effect is realized due to the interference of the scattered waves generated by electric, magnetic, and toroidal dipole moments of high-index nanoparticles.

Probing cytochrome c in living mitochondria with surface-enhanced Raman spectroscopy.

Selective study of the electron transport chain components in living mitochondria is essential for fundamental biophysical research and for the development of new medical diagnostic methods. However, many important details of inter- and intramembrane mitochondrial processes have remained in shadow due to the lack of non-invasive techniques. Here we suggest a novel label-free approach based on the surface-enhanced Raman spectroscopy (SERS) to monitor the redox state and conformation of cytochrome c in the electron transport chain in living mitochondria. We demonstrate that SERS spectra of living mitochondria placed on hierarchically structured silver-ring substrates provide exclusive information about cytochrome c behavior under modulation of inner mitochondrial membrane potential, proton gradient and the activity of ATP-synthetase. Mathematical simulation explains the observed enhancement of Raman scattering due to high concentration of electric near-field and large contact area between mitochondria and nanostructured surfaces.

Nonradiating anapole modes in dielectric nanoparticles.

Nonradiating current configurations attract attention of physicists for many years as possible models of stable atoms. One intriguing example of such a nonradiating source is known as 'anapole'. An anapole mode can be viewed as a composition of electric and toroidal dipole moments, resulting in destructive interference of the radiation fields due to similarity of their far-field scattering patterns. Here we demonstrate experimentally that dielectric nanoparticles can exhibit a radiationless anapole mode in visible. We achieve the spectral overlap of the toroidal and electric dipole modes through a geometry tuning, and observe a highly pronounced dip in the far-field scattering accompanied by the specific near-field distribution associated with the anapole mode. The anapole physics provides a unique playground for the study of electromagnetic properties of nontrivial excitations of complex fields, reciprocity violation and Aharonov-Bohm like phenomena at optical frequencies.

The interplay between localized and propagating plasmonic excitations tracked in space and time.

In this work, the mutual coupling and coherent interaction of propagating and localized surface plasmons within a model-type plasmonic assembly is experimentally demonstrated, imaged, and analyzed. Using interferometric time-resolved photoemission electron microscopy the interplay between ultrashort surface plasmon polariton wave packets and plasmonic nanoantennas is monitored on subfemtosecond time scales. The data reveal real-time insights into dispersion and localization of electromagnetic fields as governed by the elementary modes determining the functionality of plasmonic operation units.

Laser printing of silicon nanoparticles with resonant optical electric and magnetic responses.

Silicon nanoparticles with sizes of a few hundred nanometres exhibit unique optical properties due to their strong electric and magnetic dipole responses in the visible range. Here we demonstrate a novel laser printing technique for the controlled fabrication and precise deposition of silicon nanoparticles. Using femtosecond laser pulses it is possible to vary the size of Si nanoparticles and their crystallographic phase. Si nanoparticles produced by femtosecond laser printing are initially in an amorphous phase (a-Si). They can be converted into the crystalline phase (c-Si) by irradiating them with a second femtosecond laser pulse. The resonance-scattering spectrum of c-Si nanoparticles, compared with that of a-Si nanoparticles, is blue shifted and its peak intensity is about three times higher. Resonant optical responses of dielectric nanoparticles are characterized by accumulation of electromagnetic energy in the excited modes, which can be used for the realization of nanoantennas, nanolasers and metamaterials.