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Development of advanced optical data storage, information encryption, and security labeling technologies requires low-cost materials exhibiting local, pronounced, and diverse modification of their structure-dependent optical properties under external excitation. Herein, for these purposes, we propose and develop a novel platform relying on layered lead halide Ruddlesden-Popper (quasi-2D) phases that undergo a light-induced transition towards bulk (3D) halide perovskite and employ this phenomenon for the direct optical writing of various multicolor patterns. This transition causes the weakening of quantum confinement, and hence the bandgap reduction in these photoluminescent thin films. To significantly extend the color gamut of evolving photoluminescence, we make use of mixed-halide compositions exhibiting photoinduced halide segregation. As a result, the emission wavelength of the resulting films can be widely tuned across the entire 450-600 nm range depending on the illumination conditions. We show that pulsed near-infrared femtosecond laser irradiation provides high-resolution direct writing, whereas continuous-wave ultraviolet exposure is suitable for fast recording on larger scales. The luminescent micro- and macro-scale images created on such quasi-2D perovskite films can be erased during the visualization process, by which the persistence of these images to UV light exposure can be controlled and increased further with the increasing number of octahedral layers used in the perovskite stacks. This makes the proposed writing/erasing perovskite-based platform suitable for the manufacturing of both inexpensive optical data storage devices and light-erasable security labels.

Mixed halide perovskites undergo phase segregation, manifested as spectral red-shifting of photoluminescence spectra under illumination. In the iodine-bromide mixed perovskites, the origin of the low-energy luminescence is related to iodine-enriched domains formation. Such domains create favorable bands for the induced carrier funneling into them. Despite the phase segregation process is crucial for mixed halide perovskite-based optoelectronics, numerous gaps exist within the understanding of this phenomenon. One such gap pertains to the emergence of temporary and intermediate photoluminescence peaks during the initial stages of phase segregation. However, these peaks appear only within the first few seconds of illumination. Nevertheless, the decreasing temperature may prolong these initial stages. In this work, we carry out a detailed study of the temperature dependence of anion segregation in MAPbBr_2I and MAPbBr2.5I0.5 halide perovskites, to obtain a deeper comprehension of segregation processes, particularly during their initial stages. The temporal evolution of low-temperature photoluminescence reveals the undergoing of the intermediate stage during the segregation process and temperature-related phase transition from orthorhombic to tetragonal phase. To complement the phase segregation study, the temperature dependence of time-resolved photoluminescence spectroscopy is provided, allowing us to estimate the change in the photoluminescence lifetimes for the initial and segregated peaks with temperature., Comment: 28 pages, 7 figures

Halide perovskites belong to an important family of semiconducting materials with unique electronic properties that enable a myriad of applications, especially in photovoltaics and optoelectronics. Their optical properties, including photoluminescence quantum yield, are affected and notably enhanced at crystal imperfections where the symmetry is broken and the density of states increases. These lattice distortions can be introduced through structural phase transitions, allowing charge gradients to appear near the interfaces between phase structures. In this work, we demonstrate controlled multi-phase structuring in a single perovskite crystal. The concept uses cesium lead bromine (CsPbBr3) placed on a thermoplasmonic TiN/Si metasurface and enables single, double and triple phase structures to form on demand above the room temperature. This approach opens up application horizons of dynamically controlled heterostructures with distinctive electronic and enhanced optical properties.

Nanophotonics is an important branch of modern optics dealing with light-matter interaction at the nanoscale. Nanoparticles can exhibit enhanced light absorption under illumination by light, and they become nanoscale sources of heat that can be precisely controlled and manipulated. For metal nanoparticles, such effects have been studied in the framework of $\textit{thermoplasmonics}$ which, similar to plasmonics itself, has a number of limitations. Recently emerged $\textit{all-dielectric resonant nanophotonics}$ is associated with optically-induced electric and magnetic Mie resonances, and this field is developing very rapidly in the last decade. As a result, thermoplasmonics is being replaced by $\textit{all-dielectric thermonanophotonics}$ with many important applications such as photothermal cancer therapy, drug and gene delivery, nanochemistry, and photothermal imaging. This review paper aims to introduce this new field of non-plasmonic nanophotonics and discuss associated thermally-induced processes at the nanoscale.

The full control of the fundamental photophysics of nanosystems at frequencies as high as few THz is key for tunable and ultrafast nano-photonic devices and metamaterials. Here we combine geometrical and ultrafast control of the optical properties of halide perovskite nanoparticles, which constitute a prominent platform for nanophotonics. The pulsed photoinjection of free carriers across the semiconducting gap leads to a sub-picosecond modification of the far-field electromagnetic properties that is fully controlled by the geometry of the system. When the nanoparticle size is tuned so as to achieve the overlap between the narrowband excitons and the geometry-controlled Mie resonances, the ultrafast modulation of the transmittivity is completely reversed with respect to what is usually observed in nanoparticles with different sizes, in bulk systems and in thin films. The interplay between chemical, geometrical and ultrafast tuning offers an additional control parameter with impact on nano-antennas and ultrafast optical switches.

Meta-optics based on optically resonant all-dielectric structures is a rapidly developing research area driven by its potential applications for low-loss efficient metadevices. Active, light-emitting subwavelengh nanostructures and metasurfaces are of a particular interest for meta-optics, as they offer unique opportunities for novel types of compact light sources and nanolasers. Recently, the study of halide perovskites has attracted an enormous attention due to their exceptional optical and electrical properties. As a result, this family of materials can provide a prospective platform for modern nanophotonics and meta-optics, allowing to overcome many obstacles associated with the use of conventional semiconductor materials. Here we review the recent progress in the field of halide-perovskite meta-optics with the central focus on light-emitting nanoantennas and metasurfaces for the emerging field of active metadevices.

All-dielectric nanophotonics becomes a versatile tool for various optical applications, including nanothermometry and optical heating. Its general concept includes excitation of Mie resonances in nonplasmonic nanoparticles. However, the potential of resonant dielectric nanoparticles in drug delivery applications still have not been fully realized. Here, optically resonant dielectric iron oxide nanoparticles ($\alpha$-Fe$_2$O$_3$ NPs) are employed for remote rupture of microcontainers used as drug delivery platform. It is theoretically and experimentally demonstrated, that $\alpha$-Fe$_2$O$_3$ NPs has several advantages in light-to-heat energy conversion comparing to previously used materials, such as noble metals and silicon, due to the broader spectral range of efficient optical heating, and in enhancement of thermally sensitive Raman signal. The $\alpha$-Fe$_2$O$_3$ NPs embedded into the wall of universal drug carriers, polymer capsules, are used to experimentally determine the local temperature of the capsule rupture upon laser irradiation (170$^o$C). As a proof of principle, we successfully show the delivery and remote release of anticancer drug vincristine upon lowered laser irradiation (4.0$\times$10$^4$~W/cm$^2$) using polymer capsules modified with the $\alpha$-Fe$_2$O$_3$ NPs. The biological tests were performed on two primary cell types: (i) carcinoma cells, as an example of malignant tumor, and (ii) human stem cells, as a model of healthy cells. The developed delivery system consisting of polymer capsules modified with the dielectric nanoparticles provides multifunctional platform for remote drug release and temperature detection.

All-dielectric subwavelength structures utilizing Mie resonances provide a novel paradigm in nanophotonics for controlling and manipulating light. So far, only spontaneous emission enhancement was demonstrated with single dielectric nanoantennas, whereas stimulated emission was achieved only in large lattices supporting collective modes. Here, we demonstrate the first single-particle all-dielectric monolithic nanolaser driven by Mie resonances in visible and near-IR frequency range. We employ halide perovskite CsPbBr$_3$ as both gain and resonator material that provides high optical gain (up to $\sim 10^4$ cm$^{-1}$) and allows simple chemical synthesis of nanocubes with nearly epitaxial quality. Our smallest non-plasmonic Mie-resonant single-mode nanolaser with the size of 420 nm operates at room temperatures and wavelength 535 nm with linewidth $\sim 3.5$ meV. These novel lasing nanoantennas can pave the way to multifunctional photonic designs for active control of light at the nanoscale.

Nanoantennas for highly efficient excitation and manipulation of surface waves at nanoscale are key elements of compact photonic circuits. However, previously implemented designs employ plasmonic nanoantennas with high Ohmic losses, relatively low spectral resolution, and complicated lithographically made architectures. Here we propose an ultracompact and simple dielectric nanoantenna (silicon nanosphere) allowing for both directional launching of surface plasmon polaritons on a thin gold film and their demultiplexing with a high spectral resolution. We show experimentally that mutual interference of magnetic and electric dipole moments supported by the dielectric nanoantenna results in opposite propagation of the excited surface waves whose wavelengths differ by less than 50 nm in the optical range. Broadband reconfigurability of the nanoantennas operational range is achieved simply by varying the diameter of the silicon sphere. Moreover, despite subwavelength size ($<\lambda/3$) of the proposed nanoantennas, they demonstrate highly efficient and directional launching of surface waves both in the forward and backward directions with the measured front-to-back ratio having a contrast of almost two orders of magnitude within a 50 nm spectral band. Our lithography-free design has great potential as highly efficient, low-cost, and ultracompact demultiplexer for advanced photonic circuits., Comment: added relevant references; fixed typos in Supplementary eq. 8,9,11

Achievement of all-optical ultrafast signal modulation and routing by a low-loss nanodevice is a crucial step towards an ultracompact optical chip with high performance. Here, we propose a specifically designed silicon dimer nanoantenna, which is tunable via photoexcitation of dense electron-hole plasma with ultrafast relaxation rate. Basing on this concept, we demonstrate the effect of beam steering up to 20 degrees via simple variation of incident intensity, being suitable for ultrafast light routing in an optical chip. The effect is demonstrated both in the visible and near-IR spectral regions for silicon and germanium based nanoantennas. We also reveal the effect of electron-hole plasma photoexcitation on local density of states (LDOS) in the dimer gap and find that the orientation averaged LDOS can be altered by 50\%, whereas modification of the projected LDOS can be even more dramatic: almost 500\% for transverse dipole orientation. Moreover, our analytical model sheds light on transient dynamics of the studied nonlinear nanoantennas, yielding all temporal characteristics of the proposed ultrafast nanodevice. The proposed concept paves the ways to creation of low-loss, ultrafast, and compact devices for optical signal modulation and routing.

Optically generated electron-hole plasma in high-index dielectric nanostructures was demonstrated as a means of tuning of their optical properties. However, until now an ultrafast operation regime of such plasma driven nanostructures has not been attained. Here, we perform pump-probe experiments with resonant silicon nanoparticles and report on dense optical plasma generation near the magnetic dipole resonance with ultrafast (about 2.5 ps) relaxation rate. Basing on experimental results, we develop an analytical model describing transient response of a nanocrystalline silicon nanoparticle to an intense laser pulse and show theoretically that plasma induced optical nonlinearity leads to ultrafast reconfiguration of the scattering power pattern. We demonstrate 100 fs switching to unidirectional scattering regime upon irradiation of the nanoparticle by an intense femtosecond pulse. Our work lays the foundation for developing ultracompact and ultrafast all-optical signal processing devices.

Enhancement of optical response with high-index dielectric nanoparticles is attributed to the excitation of their Mie-type magnetic and electric resonances. Here we study Raman scattering from crystalline silicon nanoparticles and reveal that magnetic dipole modes have much stronger effect on the scattering than electric modes of the same order. We demonstrate experimentally a 140-fold enhancement of Raman signal from individual silicon spherical nanoparticles at the magnetic dipole resonance. Our results confirm the importance of the optically-induced magnetic response of subwavelength dielectric nanoparticles for enhancing light-matter interactions.

Hybrid nanophotonics based on metal-dielectric nanostructures unifies the advantages of plasmonics and all-dielectric nanophotonics providing strong localization of light, magnetic optical response and specifically designed scattering properties. Here we demonstrate a novel approach for fabrication of ordered hybrid nanostructures via femtosecond laser melting of asymmetrical metal-dielectric (Au-Si) nanoparticles created by lithographical methods. The approach allows selective reshaping of the metal components of the hybrid nanoparticles without affecting dielectric ones. We apply the developed approach for tuning of the hybrid nanostructures scattering properties in the visible range. The experimental results are supported by molecular dynamics simulation and numerical solving of Maxwell equations., Comment: Published in Advanced Materials

Dewetting of thin metal films is one of the most widespread method for functional plasmonic nanostructures fabrication. However, simple thermal-induced dewetting does not allow to control degree of nanostructures order without additional lithographic process steps. Here we propose a novel method for lithography-free and large-scale fabrication of plasmonic nanostructures via controllable femtosecond laser-induced dewetting. The method is based on femtosecond laser surface pattering of a thin film followed by a nanoscale hydrodynamical instability, which is found to be very controllable under specific irradiation conditions. We achieve control over degree of nanostructures order by changing laser irradiation parametrs and film thickness. This allowed us to exploit the method for the broad range of applications: resonant light absorbtion and scattering, sensing, and potential improving of thin-film solar cells., Comment: to be published in Laser and Photonics Reviews. arXiv admin note: substantial text overlap with arXiv:1505.03041

We propose a novel concept for efficient dynamic tuning of optical properties of a high refractive index subwavelength nanoparticle with a magnetic Mie-type resonance by means of femtosecond laser radiation. This concept is based on ultrafast generation of electron-hole plasma within such nanoparticle, drastically changing its transient dielectric permittivity. This allows to manipulate by both electric and magnetic nanoparticle responses, resulting in dramatic changes of its extinction cross section and scattering diagram. Specifically, we demonstrate the effect of ultrafast switching-on a Huygens source in the vicinity of the magnetic dipole resonance. This approach enables to design ultrafast and compact optical switchers and modulators based on the "ultrafast magnetic light" concept., Comment: Silicon nanoparticles, femtosecond laser pulses, magnetic light

A novel method for single-step, lithography-free, and large-scale laser writing of nanoparticle-based plasmonic structures has been developed. Changing energy of femtosecond laser pulses and thickness of irradiated gold film it is possible to vary diameter of the gold nanoparticles, while the distance between them can be varied by laser scanning parameters. This method has an advantage over the most previously demonstrated methods in its simplicity and versatility, while the quality of the structures is good enough for many applications. In particular, resonant light absorbtion/scattering and surface-enhanced Raman scattering have been demonstrated on the fabricated nanostructures.