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The possibility of using axial spin color centers with $S=3/2$, oriented along the hexagonal $c$ axis in a silicon carbide (SiC) wafer, has been demonstrated for all-optical measurement of projection of the external magnetic field coinciding with the $c$ axis of the crystal, and the polar and azimuthal angles of the external measured magnetic field at room and significantly higher temperatures. A distinctive feature of spin centers in SiC, in which optically induced spin alignment is carried out, is the presence of a unique system of spin levels in a magnetic field, caused by fine structure interaction and hyperfine interaction with the $^{29}$Si nuclei and there is a wide range of level anticrossings (LACs), leading to an exceptionally strong change in photoluminescence in the region of LAC and the dependence of the LAC spectrum on the orientation of the external measured magnetic field, which made it possible to develop the all-optical vector magnetometry method. Such measurements do not require microwave radiation, it is possible to use single spin center for the all-optical vector magnetometry. The proposed magnetometer is based on an external magnetic field cancellation scheme, which leads to a LAC spectrum observed in a zero external magnetic field, called its reference spectrum, by maintaining a local region of zero magnetic field at the site of optical excitation of spin centers. 4H-SiC plate is placed on the scanning stage of a confocal microscope inside the Helmholtz coils. Sensitivity to a constant magnetic field for $z$ component of the magnetic field ${B}_{z}$ is better than $0.1\mu$T$/\sqrt{\text{Hz}}$ in a volume of $1\times10^{-8}$mm$^{3}$ at room temperature. The sensitivity of determining the angles polar and azimuthal is determined by the sensitivity to determining the perpendicular component of the magnetic field, which is better than $5~\mu$T$/\sqrt{\text{Hz}}$.

Periodic optical structures, such as diffraction grating and numerous photonic crystals, are one of the staples of modern nanophotonics for the manipulation of electromagnetic radiation. The array of subwavelength dielectric rods is one of the simplest platforms, which, despite its simplicity exhibits extraordinary wave phenomena, such as diffraction anomalies and narrow reflective resonances. Despite the well-documented properties of infinite periodic systems, the behavior of these diffractive effects in systems incorporating a finite number of elements is studied to a far lesser extent. Here we study theoretically and numerically the evolution of collective spectral features in finite arrays of dielectric rods. We develop an analytical model of light scattering by a finite array of circular rods based on the coupled dipoles approximation and analyze the spectral features of finite arrays within the developed model. Finally, we validate the results of the analytical model using full-wave numerical simulations.

Perfect light transmission into a dielectric at the Brewster angle is one of the simplest effects in macroscopic electromagnetism. The common wisdom states that absorption in the dielectric violates Brewster angle and leads to a non-vanishing reflection. Yet, incorporating anisotropy may recover perfect transmission of $p$-polarized light into the absorbing medium. Unlike the traditional "lossless" Brewster angle, perfect transmission in this case is accompanied by phase singularities of the reflection amplitude. In this paper, we examine theoretically phase singularities and the associated topological charges emerging in the wavelength-incidence angle space upon perfect transmission into absorbing uniaxial dielectrics. We derive the analytical criterion of perfect light transmission into an anisotropic medium, demonstrate phase singularities in these scenarios, and study their dynamics as a function of material parameters. Finally, by lowering the symmetry of the problem, we translate this phenomenon into a different parameter space of wave vector components, and illustrate the feasibility of this phenomenon with available optically anisotropic materials. Our results may could become valuable for the development of novel analog computing schemes and holography approaches.

Vacuum fluctuations are a fundamental and irremovable property of a quantized electromagnetic field. These fluctuations are the cause of the Casimir effect -- mutual attraction of two electrically neutral metallic plates in vacuum in the absence of any other interactions. For most geometries and materials, Casimir effect is strictly attractive, leading to the only stable equilibrium configuration with merged plates. Recent observation showed, however, that this unavoidable vacuum-induced attraction can be mitigated by the presence of electrostatic repulsion produced by the formation of double electric layers, and a stable equilibrium between two charged metallic plates in a solution of an organic salt can be reached. Here, we study theoretically in details equilibrium configurations and their dynamical behavior in the system of two parallel metallic films coupled by the Casimir and electrostatic interactions. We analyze the effect of various parameters of the system -- such as the salt concentartion and temperature -- on the equilibrium cavity thicknesses, inspect resonant properties of the resulting an-harmonic optomechanical system near equilibrium, and examine its stochastic dynamics under the influence of thermal fluctuations of the environment.

Chirality is probably the most mysterious among all symmetry transformations. Very readily broken in biological systems, it is practically absent in naturally occurring inorganic materials and is very challenging to create artificially. Chiral optical wavefronts are often used for the identification, control and discrimination of left- and right-handed biological and other molecules. Thus, it is crucially important to create materials capable of chiral interaction with light, which would allow one to assign arbitrary chiral properties to a light field. In this paper, we utilized van der Waals technology to assemble helical homostructures with chiral properties (e. g. circular dichroism). Because of the large range of van der Waals materials available such helical homostructures can be assigned with very flexible optical properties. We demonstrate our approach by creating helical homostructures based on multilayer As$_2$S$_3$, which offers the most pronounced chiral properties even in thin structures due to its strong biaxial optically anisotropy. Our work showcases that the chirality of an electromagnetic system may emerge at an intermediate level between the molecular and the mesoscopic one due to the tailored arrangement of non-chiral layers of van der Waals crystals and without additional patterning.

Variations of the weak magnetic fields of the photosphere with periods of the order of the solar magnetic cycle were investigated. Synoptic maps of the photospheric magnetic field produced by NSO Kitt Peak for the period from 1978 to 2016 were used as initial data. In order to study weak magnetic fields, the saturation threshold for synoptic maps was set at 5 G. On the base of transformed synoptic maps the time-latitude chart was built. 18 profiles of the magnetic field evenly distributed along the sine of latitude from the north to the south pole were selected in the diagram for the further analysis. Time dependencies were averaged by sliding smoothing over 21 Carrington rotations. The approximation of averaged time dependencies by the sinusoidal function made it possible to distinguish in weak magnetic fields a cyclic component with a period of about 22 years (the period of the Hale magnetic cycle). The dependence of 22-year variation on latitude was studied. In addition to the well-known 22-year change in the near-polar field, similar variations were found for the fields at all latitudes. The exception was latitudes $26^\circ$ and $33^\circ$ in the northern and $26^\circ$ in the southern hemisphere. These mid-latitude intervals were characterized by a predominance of short-period variations. The amplitude of the long-term variation decreased from the poles to the equator, with the period of variation remaining almost constant (T = 22.3 years)., Comment: 13 pages, 7 figures, 1 table; to appear in Geomagnetism and Aeronomy

Optical anapoles are intriguing charge-current distributions characterized by a strong suppression of electromagnetic radiation. They originate from the destructive interference of the radiation produced by electric and toroidal multipoles. Although anapoles in dielectric structures have been probed and mapped with a combination of near- and far-field optical techniques, their excitation using fast electron beams has not been explored so far. Here, we theoretically and experimentally analyze the excitation of optical anapoles in tungsten disulfide (WS$_2$) nanodisks using Electron Energy Loss Spectroscopy (EELS) in Scanning Transmission Electron Microscopy (STEM). We observe prominent dips in the electron energy loss spectra and associate them with the excitation of optical anapoles and anapole-exciton hybrids. We are able to map the anapoles excited in the WS$_2$ nanodisks with subnanometer resolution and find that their excitation can be controlled by placing the electron beam at different positions on the nanodisk. Considering current research on the anapole phenomenon, we envision EELS in STEM to become a useful tool for accessing optical anapoles appearing in a variety of dielectric nanoresonators., Comment: 4 figures

A global trend to miniaturization and multiwavelength performance of nanophotonic devices drives research on novel phenomena, such as bound states in the continuum and Mietronics, as well as the survey for high-refractive index and strongly anisotropic materials and metasurfaces. Hexagonal boron nitride (hBN) is one of promising materials for the future nanophotonics owing to its inherent anisotropy and prospects of high-quality monocrystals growth with atomically flat surface. Here, we present highly accurate optical constants of hBN in the broad wavelength range of 250-1700 nm combining the imaging ellipsometry measurements scanning near-field optical microscopy and first-principle quantum mechanical computations. hBN's high refractive index, up to 2.75 in ultraviolet (UV) and visible range, broadband birefringence of 0.7, and negligible optical losses make it an outstanding material for UV and visible range photonics. Based on our measurement results, we propose and design novel optical elements: handedness-preserving mirrors and subwavelength waveguides with dimensions of 40 nm operating in the visible and UV range, respectively. Remarkably, our results offer unique opportunity to bridge the size-gap between photonics and electronics., Comment: 12 pages, 4 figures

Ultrastrong coupling between optical and material excitations is a distinct regime of electromagnetic interaction that enables a variety of intriguing physical phenomena. Traditional ways to ultrastrong light-matter coupling involve the use of some sorts of quantum emitters, such as organic dyes, quantum wells, superconducting artificial atoms, or transitions of two-dimensional electron gases. Often, reaching the ultrastrong coupling domain requires special conditions, including high vacuum, strong magnetic fields, and extremely low temperatures. Recent report indicate that a high degree of light-matter coupling can be attained at ambient conditions with plasmonic meta-atoms -- artificial metallic nanostructures that replace quantum emitters. Yet, the fundamental limits on the coupling strength imposed on such systems have not been identified. Here, using a Hamiltonian approach we theoretically analyze the formation of polaritonic states and examine the upper limits of the collective plasmon-photon coupling strength in a number of dense assemblies of plasmonic meta-atoms. Starting off with spheres, we identify the universal upper bounds on the normalized collective coupling strength $g/\omega_0$ between ensembles of plasmonic meta-atoms and free-space photons. Next, we examine spheroidal metallic meta-atoms and show that a strongly elongated meta-atom is the optimal geometry for attaining the highest value of the collective coupling strength in the array of meta-atoms. The results could be valuable for the field of polaritonics studies, quantum technology, and modifying material properties.

Coupling between light and material excitations underlies a wide range of optical phenomena. Polaritons are eigenstates of a coupled system with hybridized wave function. Owing to their hybrid composition, polaritons exhibit at the same time properties typical for photonic and electronic excitations, thus offering new ways for controlling electronic transport and even chemical kinetics. While most theoretical and experimental efforts have been focused on polaritons with electric-dipole coupling between light and matter, in chiral quantum emitters, electronic transitions are characterized by simultaneously nonzero electric and magnetic dipole moments. Geometrical chirality affects the optical properties of materials in a profound way and enables phenomena that underlie our ability to discriminate enantiomers of chiral molecules. Thus, it is natural to wonder what kinds of novel effects chirality may enable in the realm of strong light-matter coupling. Right now, this field located at the intersection of nanophotonics, quantum optics, and chemistry is in its infancy. In this Perspective, we offer our view towards chiral polaritons. We review basic physical concepts underlying chirality of matter and electromagnetic field, discuss the main theoretical and experimental challenges that need to be solved, and consider novel effects that could be enabled by strong coupling between chiral light and matter.

Silicon vacancies in silicon carbide (SiC) have been proposed as interesting candidates for quantum technology applications such as quantum sensing and quantum repeaters. SiC exists in many polytypes with different plane stacking sequences, and in each polytype, the vacancies can occupy a variety of different lattice sites. In this work, we characterize and identify the three most important charged silicon vacancies in the 6H-SiC polytype. We record the photoluminescence and continuous-wave optically detected magnetic resonance spectra at different radio-frequency power levels and different temperatures. We individually select the zero-phonon lines of the different silicon vacancies at low temperatures and record the corresponding optically detected magnetic resonance (ODMR) spectra. ODMR allows us to correlate optical and magnetic resonance spectra and thereby resolve a controversy from earlier work.

The distribution of magnetic fields of positive and negative polarities over the surface of the Sun was studied on the basis of synoptic maps presented by the NSO/Kitt Peak (1978-2016). To emphasize the contribution of weak fields the following transformation of synoptic maps was made: for each synoptic map only magnetic fields with modulus less than 5G ($|B|\leq 5$G) were left unchanged while larger or smaller fields were replaced by the corresponding threshold values +5G or $-5$G. Cyclic variations of the magnetic field polarity have been observed associated with two types of magnetic field flows in the photosphere. Rush-to-the-Poles (RTTP) appear near the maximum of solar activity and have the same sign as the following sunspots. The lifetime of RTTP is $\sim 3$ yrs, during which time they drift from latitudes $30^\circ$-$40^\circ$ to the pole, causing the polarity change of the Sun's polar field. Our aim is the study of another type of variations which has the form of series of flows with individual flows of 0.5-1 yr with alternating polarity. These flows called ripples are located in time between two RTTP and drift from the equator to the latitudes of $~50^\circ$. The period of variation of ripples was shown to be 1.1 yr for the northern hemisphere and 1.3 yr for the southern hemisphere. It was found that the amplitude of variation was higher for the time intervals where the polar field had a positive sign. Within the same flow, fields of positive and negative signs developed in anti-phase. Two types of flows - RTTP and ripples - together formed a unique structure which had close connection to the magnetic solar cycle., Comment: 17 pages, 12 figures

Preferential selection of a given enantiomer over its chiral counterpart becomes increasingly relevant in the advent of the next era of medical drug design. In parallel, cavity quantum electrodynamics has grown into a solid framework to control energy transfer and chemical reactivity. In this work, we derive an analytical solution to a system of many chiral emitters interacting with a chiral cavity -- in analogy to the widely used Tavis-Cummings and Hopfield models of quantum optics. We are able to estimate the discriminating strength of chiral polaritonics, discuss possible future development directions, exciting applications such as elucidating homochirality, and deliver much needed intuition to foster the freshly flourishing field of chiral polaritonics., Comment: Small additions and clarifications

The distribution of magnetic fields of positive and negative polarities over the surface of the Sun was studied. Synoptic maps of the photospheric magnetic field (NSO Kitt Peak, 1978--2016) were used for the analysis. In the time-latitude diagram for weak magnetic fields ($B \leq 5 G$), inclined bands are clearly visible, indicating the alternating dominance of magnetic fields with positive or negative polarity drifting towards the poles of the Sun. Analysis of the time-latitude diagram using the method of empirical orthogonal functions (EOF) made it possible to establish a cyclic change in the polarity of magnetic field flows with a period of 1-3 years, which indicates a possible connection with quasi biennial variation. Similar period values are obtained by averaging over the latitude of the time-latitude diagram, Comment: 10 pages, 7 figures; accepted for publication in Geomagnetism and Aeronomy

Transition metal dichalcogenides (TMDCs), belonging to the class of van der Waals materials, are promising materials for optoelectronics and photonics. In particular, their giant optical anisotropy may enable important optical effects when employed in nanostructures with finite thickness. In this paper, we theoretically and numerically study light scattering behavior from anisotropic MoS2 nanocylinders, and highlight its distinct features advantageous over the response of conventional silicon particles of the same shape. We establish two remarkable phenomena, appearing in the same MoS2 particle with optimized geometry. The first one is a pure magnetic dipole scattering associated with the excitation of the electric-dipole anapole states. Previously reported in core-shell hybrid (metal/dielectric) systems only, it is now demonstrated in an all-dielectric particle. The second phenomenon is the super-deflection in the far field: the maximum scattering may occur over a wide range of directions, including forward-, backward- and side-scattering depending on the mutual orientation of the MoS2 nanocylinder and the incident wave. In contrast to the well-known Kerker and anti-Kerker effects, which appear in nanoparticles at different frequencies, the super-deflection can be achieved by rotating the particle at a constant frequency of incident light. Our results facilitate the development of functional optical devices incorporating nanostructured anisotropic TMDCs and may encourage further research in meta-optics based on highly anisotropic materials.

Transition metal dichalcogenides (TMDs) attract significant attention due to their exceptional optical, excitonic, mechanical, and electronic properties. Nanostructured multilayer TMDs were recently shown to be highly promising for nanophotonic applications, as motivated by their exceptionally high refractive indexes and optical anisotropy. Here, we extend this vision to more sophisticated structures, such as periodic arrays of nanodisks and nanoholes, as well as proof-of-concept waveguides and resonators. We specifically focus on various advanced nanofabrication strategies, including careful selection of resists for electron beam lithography and etching methods. The specific materials studied here include semiconducting WS$_2$, in-plane anisotropic ReS$_2$, and metallic TaSe$_2$, TaS$_2$ and NbSe$_2$. The resulting nanostructures can potentially impact several nanophotonic and optoelectronic areas, including high-index nanophotonics, plasmonics and on-chip optical circuits. The knowledge of TMD material-dependent nanofabrication parameters developed here will help broaden the scope of future applications of these materials in all-TMD nanophotonics.

Silicon vacancy centers in silicon carbide are promising candidates for storing and manipulating quantum information. Implementation of fast quantum gates is an essential requirement for quantum information processing. In a low magnetic field, the resonance frequencies of silicon vacancy spins are in the range of a few MHz, the same order of magnitude as the Rabi frequencies of typical control fields. As a consequence, the rotating wave approximation becomes invalid and nonlinear processes like the absorption and emission of multiple photons become relevant. This work focuses on multi-photon transitions of negatively charged silicon vacancies driven by a strong RF field. We present continuous-wave optically detected magnetic resonance (ODMR) spectra measured at different RF powers to identify the 1-, 2-, and 3-RF photon transitions of different types of the silicon vacancy in the 6$H$-SIC polytype. Time-resolved experiments of Rabi oscillations and free induction decays of these multiple RF photon transitions were observed for the first time. Apart from zero-field data, we also present spectra in magnetic fields with different strength and orientation with respect to the system's symmetry axis.

Optically controllable solid-state spin qubits are one of the basic building blocks for applied quantum technology. Efficient extraction of emitted photons and a robust spin-photon interface are crucial for the realization of quantum sensing protocols and essential for the implementation of quantum repeaters. Though silicon carbide (SiC) is a very promising material platform hosting highly-coherent silicon vacancy spin qubits, a drawback for their practical application is the unfavorable ordering of the electronic levels in the optically excited state. Here, we demonstrate that due to polytypism of SiC, a particular type of silicon vacancy qubits in 6H-SiC possesses an unusual inverted fine structure. This results in the directional emission of light along the hexagonal crystallographic axis, making photon extraction more efficient and integration into photonic structures technologically straightforward. From the angular polarization dependencies of the emission, we reconstruct the spatial symmetry and determine the optical selection rules depending on the local deformation and spin-orbit interaction, enabling direct implementation of robust spin-photon entanglement schemes. Furthermore, the inverted fine structure leads to unexpected behavior of the spin readout contrast. It vanishes and recovers with lattice cooling due to two competing optical spin pumping mechanisms. Our experimental and theoretical approaches provide a deep insight into the optical and spin properties of atomic-scale qubits in SiC required for quantum communication and distributed quantum information processing., Comment: 11 pages, 7 figures

Atomically thin transition metal dichalcogenides (TMDCs) present a promising platform for numerous photonic applications due to excitonic spectral features, possibility to tune their constants by external gating, doping, or light, and mechanical stability. Utilization of such materials for sensing or optical modulation purposes would require a clever optical design, as by itself the 2D materials can offer only a small optical phase delay - consequence of the atomic thickness. To address this issue, we combine films of 2D semiconductors which exhibit excitonic lines with the Fabry-Perot resonators of the standard commercial SiO$_2$/Si substrate, in order to realize topological phase singularities in reflection. Around these singularities, reflection spectra demonstrate rapid phase changes while the structure behaves as a perfect absorber. Furthermore, we demonstrate that such topological phase singularities are ubiquitous for the entire class of atomically thin TMDCs and other high-refractive-index materials, making it a powerful tool for phase engineering in flat optics. As a practical demonstration, we employ PdSe$_2$ topological phase singularities for a refractive index sensor and demonstrate its superior phase sensitivity compared to typical surface plasmon resonance sensors.

Thermal emission is a universal phenomenon of stochastic electromagnetic emission from an object composed of arbitrary materials at elevated temperatures. A defining feature of this emission is the monotonic and rapid growth of its intensity with the object's temperature for most known materials. This growth originates from the Bose-Einstein statistics of the thermal photonic field. The fact that the material's ability to absorb and emit light may change with temperature, however, is often ignored. Here, we carry out a theoretical study of thermal emission from structures incorporating ensembles of two-level media. We investigate this effect in a range of geometries including thin films and compact nanoparticles, and establish the general dependencies in the evolution of thermal emission from systems including two-level media. Thermal emission from such structures is essentially Non-Planckian and exhibits a universal asymptotic behavior in the limit of high temperatures. These results might have important implications for the design of thermal energy harvesting and thermal vision systems.

Geometrical chirality is a universal property encountered on very different length scales ranging from geometrical shapes of living organisms to protein and DNA molecules. Interaction of chiral matter with chiral light - that is, electromagnetic field possessing a certain handedness - underlies our ability to discriminate enantiomers of chiral molecules. In this context, it is often desired to have an optical cavity that efficiently couples to only a specific (right or left) molecular enantiomer, and does not couple to the opposite one. Here, we demonstrate a single-handedness chiral optical cavity supporting only an eigenmode of a given handedness and lacking modes having the opposite one. Resonant excitation of the cavity with light of appropriate handedness enables formation of a helical standing wave with a uniform chirality density, while the light of opposite handedness does not cause any resonant effects. Furthermore, only chiral emitters of the matching handedness efficiently interact with such a chiral eigenmode, enabling the handedness-selective strength of light-matter coupling. The proposed system expands the set of tools available for investigations of chiral matter and opens the door to studies of chiral electromagnetic vacuum.

Nanostructured dielectric metasurfaces offer unprecedented opportunities to manipulate light by imprinting an arbitrary phase-gradient on an impinging wavefront. This has resulted in the realization of a range of flat analogs to classical optical components like lenses, waveplates and axicons. However, the change in linear and angular optical momentum associated with phase manipulation also results in previously unexploited forces acting on the metasurface itself. Here, we show that these optomechanical effects can be utilized to construct optical metavehicles - microscopic particles that can travel long distances under low-power plane-wave illumination while being steered through the polarization of the incident light. We demonstrate movement in complex patterns, self-correcting motion, and an application as transport vehicles for microscopic cargo, including unicellular organisms. The abundance of possible optical metasurfaces attests to the prospect of developing a wide variety of metavehicles with specialized functional behavior., Comment: Main Text: 16 pages, 4 figures. Supporting Information: 6 pages, 9 figures

We report the influence of static mechanical deformation on the zero-field splitting of silicon vacancies in silicon carbide at room temperature. We use AlN/6H-SiC heterostructures deformed by growth conditions and monitor the stress distribution as a function of distance from the heterointerface with spatially-resolved confocal Raman spectroscopy. The zero-field splitting of the V1/V3 and V2 centers in 6H-SiC, measured by optically-detected magnetic resonance, reveal significant changes at the heterointerface compared to the bulk value. This approach allows unambiguous determination of the spin-deformation interaction constant, which turns out to be $0.75 \, \mathrm{GHz}$ for the V1/V3 centers and $0.5 \, \mathrm{GHz}$ for the V2 centers. Provided piezoelectricity of AlN, our results offer a strategy to realize the on-demand fine tuning of spin transition energies in SiC by deformation., Comment: 13 pages, 3 figures

We grow AlN/4H-SiC and AlN/6H-SiC heterostructures by physical vapor deposition and characterize the heterointerface with nanoscale resolution. Furthermore, we investigate the spatial stress and strain distribution in these heterostructures using confocal Raman spectroscopy. We measure the spectral shifts of various vibrational Raman modes across the heterointerface and along the entire depth of the 4H- and 6H-SiC layers. Using the earlier experimental prediction for the phonon-deformation potential constants, we determine the stress tensor components in SiC as a function of the distance from the AlN/SiC heterointerface. In spite that the lattice parameter of SiC is smaller than that of AlN, the SiC layers are compressively strained at the heterointerface. This counterintuitive behavior is explained by different coefficients of thermal expansion of SiC and AlN when the heterostructures are cooled from growth to room temperature. The compressive stress values are maximum at the heterointerface, approaching one GPa, and relaxes to the equilibrium value on the scale of several tens of microns from the heterointerface., Comment: 19 pages, 6 figures, 3 table

Hybrid light-matter states, polaritons, are one of the central concepts in modern quantum optics and condensed matter physics. Polaritons emerge as a result of strong interaction between an optical mode and a material resonance, which is frequently realized in molecular, van der Waals, or solid-state platforms (1-7). However, this route requires accurate (nano)fabrication and often lacks simple means for tunability, which could be disadvantageous in some applications. Here, we use a different approach to realize polaritonic states by employing a stable equilibrium between two parallel gold nanoflakes in an aqueous solution (8). Such plates form a self-assembled Fabry-Perot microcavity with the fundamental optical mode in the visible spectral range. The equilibrium distance between the plates is determined by a balance between attractive Casimir and repulsive electrostatic forces (9-11) and can be controlled by concentration of ligand molecules in the solution, temperature, and light pressure, which allows active and facile tuning of the cavity resonance by external stimuli. Using this Casimir approach, we demonstrate self-assembled polaritons by placing an excitonic medium in the microcavity region, as well as observe their laser-induced modulations in and out of the strong coupling regime. These Casimir microcavities can be used as sensitive and tunable polaritonic platforms for a variety of applications, including opto-mechanics (12), nanomachinery (13), and cavity-induced effects, like polaritonic chemistry (14).

Strong coupling between various kinds of material excitations and optical modes has recently shown potential to modify chemical reaction rates in both excited and ground states. The ground-state modification in chemical reaction rates has usually been reported by coupling a vibrational mode of an organic molecule to the vacuum field of an external optical cavity, such as a planar Fabry-P\'erot microcavity made of two metallic mirrors. However, using an external cavity to form polaritonic states might: (i) limit the scope of possible applications of such systems, and (ii) be unnecessary. Here we highlight the possibility of using optical modes sustained by materials themselves to self-couple to their own electronic or vibrational resonances. By tracing the roots of the corresponding dispersion relations in the complex frequency plane, we show that electronic and vibrational polaritons are natural eigenstates of bulk and nanostructured resonant materials that require no external cavity. Several concrete examples, such as a slab of excitonic material and a spherical water droplet in vacuum are shown to reach the regime of such cavity-free self-strong coupling. The abundance of cavity-free polaritons in simple and natural structures questions their relevance and potential practical importance for the emerging field of polaritonic chemistry, exciton transport, and modified material properties., Comment: 14 pages, 6 figures

Vibrational strong coupling is emerging as a promising tool to modify molecular properties, by making use of hybrid light-matter states known as polaritons. Fabry-Perot cavities filled with organic molecules are typically used, and the molecular concentration limits the maximum reachable coupling strength. Developing methods to increase the coupling strength beyond the molecular concentration limit are highly desirable. In this letter, we investigate the effect of adding a gold nanorod array into a cavity containing pure organic molecules, using FT-IR microscopy and numerical modeling. Incorporation of the plasmonic nanorod array, that acts as artificial molecules, leads to an order of magnitude increase in the total coupling strength for the cavity filled with organic molecules. Additionally, we observe a significant narrowing of the plasmon linewidth inside the cavity. We anticipate that these results will be a step forward in exploring vibropolaritonic chemistry and may be used in plasmon based bio-sensors.

High-frequency pulse electron paramagnetic resonance (EPR) and electron nuclear double resonance (ENDOR) were used to clarify the electronic structure of the color centers with an optically induced high-temperature spin-3/2 alignment in hexagonal 4H-, 6H- and rhombic 15R- silicon carbide (SiC) polytypes. The identification is based on resolved ligand hyperfine interactions with carbon and silicon nearest, next nearest and the more distant neighbors and on the determination of the spin state. The ground state and the excited state were demonstrated to have spin S = 3/2. The microscopic model suggested from the EPR and ENDOR results is as follows: a paramagnetic negatively charged silicon vacancy that is noncovalently bonded to a non-paramagnetic neutral carbon vacancy, located on the adjacent site along the SiC symmetry c-axis., Comment: 50 pages, 14 figures, 2 tables

Silicon vacancies in silicon carbide have been proposed as an alternative to nitrogen vacancy centers in diamonds for spintronics and quantum technologies. An important precondition for these applications is the initialization of the qubits into a specific quantum state. In this work, we study the optical alignment of the spin 3/2 negatively charged silicon vacancy in 6H-SiC. Using a time-resolved optically detected magnetic resonance technique, we coherently control the silicon vacancy spin ensemble and measure Rabi frequencies and spin-lattice relaxation time of all three transitions. Then to study the optical initialization process of the silicon vacancy spin ensemble, the vacancy spin ensemble is prepared in different ground states and optically excited. We describe a simple rate equation model that can explain the observed behaviour and determine the relevant rate constants., Comment: 11 pages, 12 figures

Large optical anisotropy observed in a broad spectral range is of paramount importance for efficient light manipulation in countless devices. Although a giant anisotropy was recently observed in the mid-infrared wavelength range, for visible and near-infrared spectral intervals, the problem remains acute with the highest reported birefringence values of 0.8 in BaTiS3 and h-BN crystals. This inspired an intensive search for giant optical anisotropy among natural and artificial materials. Here, we demonstrate that layered transition metal dichalcogenides (TMDCs) provide an answer to this quest owing to their fundamental differences between intralayer strong covalent bonding and weak interlayer van der Walls interaction. To do this, we carried out a correlative far- and near-field characterization validated by first-principle calculations that reveals an unprecedented birefringence of 1.5 in the infrared and 3 in the visible light for MoS2. Our findings demonstrate that this outstanding anisotropy allows for tackling the diffraction limit enabling an avenue for on-chip next-generation photonics., Comment: 20 pages, 5 figures

Absorption of electromagnetic energy by a dissipative material is one of the most fundamental electromagnetic processes that underlies a plethora of applied problems, including sensing and molecular detection, radar detection, wireless power transfer, and photovoltaics. Perfect absorption is a particular regime when all of the incoming electromagnetic energy is absorbed by the system without scattering. Commonly, the incident energy is delivered to the absorbing system by a plane wave, hence perfect absorption of this wave requires an infinitely extended planar structure. Here, we demonstrate theoretically that a confined incident beam carrying a finite amount of electromagnetic energy can be perfectly absorbed by a finite size deep subwavelength scatterer on a substrate. We analytically solve the self-consistent scattering problem in the dipole approximation and find a closed-form expression for the spatial spectrum of the incident field and the required complex polarizability of the particle. All analytical predictions are confirmed with full-wave simulations., Comment: 4 figures

Silicon carbide (SiC) hosts many interesting defects that can potentially serve as qubits for a range of advanced quantum technologies. Some of them have very interesting properties, making them potentially useful, e.g. as interfaces between stationary and flying qubits. Here we present a detailed overview of the relevant properties of the spins in silicon vacancies of the 6H-SiC polytype. This includes the temperature-dependent photoluminescence, optically detected magnetic resonance, and the relaxation times of the longitudinal and transverse components of the spins, during free precession as well as under the influence of different refocusing schemes., Comment: 9 pages, 13 figures

Ultrastrong coupling is a distinct regime of electromagnetic interaction that enables a rich variety of intriguing physical phenomena. Traditionally, this regime has been reached by coupling intersubband transitions of multiple quantum wells, superconducting artificial atoms, or two-dimensional electron gases to microcavity resonators. However, employing these platforms requires demanding experimental conditions such as cryogenic temperatures, strong magnetic fields, and high vacuum. Here, we use plasmonic nanorods array positioned at the antinode of the resonant optical Fabry-P\'erot microcavity to reach the ultrastrong coupling (USC) regime at ambient conditions and without the use of magnetic fields. From optical measurements we extract the value of the interaction strength over the transition energy as high as g/{\omega}~0.55, deep in the USC regime, while the nanorods array occupies only ~4% of the cavity volume. Moreover, by comparing the resonant energies of the coupled and uncoupled systems, we indirectly observe up to ~10% modification of the ground-state energy, which is a hallmark of USC. Our results suggest that plasmon-microcavity polaritons are a promising new platform for room-temperature USC realizations in the optical and infrared range., Comment: 4 figures

Strong coupling between a single quantum emitter and an electromagnetic mode is one of the key effects in quantum optics. In the cavity QED approach to plasmonics, strongly coupled systems are usually understood as single-transition emitters resonantly coupled to a single radiative plasmonic mode. However, plasmonic cavities also support non-radiative (or "dark") modes, which offer much higher coupling strengths. On the other hand, realistic quantum emitters often support multiple electronic transitions of various symmetry, which could overlap with higher order plasmonic transitions -- in the blue or ultraviolet part of the spectrum. Here, we show that vacuum Rabi splitting with a single emitter can be achieved by leveraging dark modes of a plasmonic nanocavity. Specifically, we show that a significantly detuned electronic transition can be hybridized with a dark plasmon pseudomode, resulting in the vacuum Rabi splitting of the bright dipolar plasmon mode. We develop a simple model illustrating the modification of the system response in the "dark" strong coupling regime and demonstrate single photon non-linearity. These results may find important implications in the emerging field of room temperature quantum plasmonics.