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We present GERestaurant, a novel dataset consisting of 3,078 German language restaurant reviews manually annotated for Aspect-Based Sentiment Analysis (ABSA). All reviews were collected from Tripadvisor, covering a diverse selection of restaurants, including regional and international cuisine with various culinary styles. The annotations encompass both implicit and explicit aspects, including all aspect terms, their corresponding aspect categories, and the sentiments expressed towards them. Furthermore, we provide baseline scores for the four ABSA tasks Aspect Category Detection, Aspect Category Sentiment Analysis, End-to-End ABSA and Target Aspect Sentiment Detection as a reference point for future advances. The dataset fills a gap in German language resources and facilitates exploration of ABSA in the restaurant domain., Comment: Accepted in KONVENS 2024. Camera Ready submission

Cover songs are alternate versions of a song by a different artist. Long being a vital part of the music industry, cover songs significantly influence music culture and are commonly heard in public venues. The rise of online music platforms has further increased their prevalence, often as background music or video soundtracks. While current automatic identification methods serve adequately for original songs, they are less effective with cover songs, primarily because cover versions often significantly deviate from the original compositions. In this paper, we propose a novel method for cover song detection that utilizes the lyrics of a song. We introduce a new dataset for cover songs and their corresponding originals. The dataset contains 5078 cover songs and 2828 original songs. In contrast to other cover song datasets, it contains the annotated lyrics for the original song and the cover song. We evaluate our method on this dataset and compare it with multiple baseline approaches. Our results show that our method outperforms the baseline approaches., Comment: 6 pages, 3 figures

To optimize materials' stability, automated high-throughput workflows are of increasing interest. However, many of those workflows use processes not suitable for large-area depositions which limits the transferability of results. While combinatorial approaches based on vapour-based depositions are inherently scalable, their potential for controlled stability assessments has yet to be exploited. Based on MAPbI3 thin-films as a prototypical system, we demonstrate a combinatorial inert-gas workflow to study materials degradation based on intrinsic factors only, closely resembling conditions in encapsulated de-vices. Through a comprehensive set of automated X-Ray fluorescence (XRF), X-Ray diffraction (XRD) and UV-Vis characterizations, we aim to obtain a holistic understanding of thin-film properties of pristine and aged thin-films. From phase changes derived from XRD characterizations before and after aging, we observe simi-lar aging behaviours for MAPbI3 thin-films with varying PbI2 residuals. Using a custom-designed in-situ UV-Vis aging setup, the combinatorial libraries are exposed to relevant aging conditions, such as heat or light-bias exposure. Simultaneously, UV-Vis photospectroscopy is performed to gain kinetic insights into the aging process which can be linked to intrinsic degradation processes such as autocatalytic decomposition. Despite scattering effects, which complicate the conventional interpretation of in-situ UV-Vis results, we demonstrate how a machine learning model trained on the comprehensive characterization data before and after the aging process can link optical changes to phase changes during aging. Consequently, this approach does not only enable semi-quantitative comparisons of materials' stability but also provides detailed insights into the underlying degradation processes which are otherwise mostly reported for investigations on single samples.

We discuss the possibility of self-hybridisation in high-index dielectric nanoparticles, where Mie modes of electric or magnetic type can couple to the interband transitions of the material, leading to spectral anticrossings. Starting with an idealised system described by moderately high constant permittivity with a narrow Lorentzian, in which self-hybridisation is visible for both plane-wave and electron-beam excitation, we embark on a quest for realistic systems where this effect should be visible. We explore a variety of spherical particles made of traditional semiconductors such as Si, GaAs, and GaP. With the effect hardly discernible, we identify two major causes hindering observation of self-hybridisation: the very broad spectral fingerprints of interband transitions in most candidate materials, and the significant overlap between electric and magnetic Mie modes in nanospheres. We thus depart from the spherical shape, and show that interband--Mie hybridisation is indeed feasible in the example of GaAs cylinders, even with a simple plane-wave source. This so-far unreported kind of polariton has to be considered when interpreting experimental spectra of Mie-resonant nanoparticles and assigning modal characters to specific features. On the other hand, it has the potential to be useful for the characterisation of the optical properties of dielectric materials, through control of the hybridisation strength via nanoparticle size and shape.

We present an analytic, Mie theory-based solution for the energy-loss and the photon-emission probabilities in the interaction of spherical nanoparticles with electrons passing nearby and through them, in both cathodoluminescence and electron energy-loss spectroscopies. In particular, we focus on the case of penetrating electron trajectories, for which the complete fully electrodynamic and relativistic formalism has not been reported as yet. We exhibit the efficiency of this method in describing collective excitations in matter through calculations for a dispersive and lossy system, namely a sphere described by a Drude permittivity. Subsequently, we use the analytic solution to corroborate the implementation of electron-beam sources in a state-of-the-art numerical method for problems in electrodynamics, the discontinuous Galerkin time-domain (DGTD) method. We show that the two approaches produce spectra in good mutual agreement, and demonstrate the versatility of DGTD via simulations of spherical nanoparticles characterized by surface roughness. The possibility of simultaneously employing both kinds of calculations (analytic and numerical) facilitates a better understanding of the rich optical response of nanophotonic architectures excited by fast electron beams., Comment: 16 pages, 8 figures

The lowest energy states in transition metal dichalcogenide (TMD) monolayers follow valley selection rules, which have attracted vast interest due to the possibility of encoding and processing of quantum information. However, these quantum states are strongly affected by the temperature-dependent intervalley scattering causing complete valley depolarization, which is hampering any practical applications of TMD monolayers at room temperature. Therefore, for achieving clear and robust valley polarization in TMD monolayers one needs to suppress parasitic depolarization processes, which is the central challenge in the growing field of valleytronics. Here, in electron-doping experiments on TMD monolayers, we demonstrate that strong doping levels beyond $10^{13}$~cm$^{-2}$ can induce 61\% and 37\% valley contrast at room temperature in tungsten diselenide and molybdenum diselenide monolayers, respectively. Our results indicate that charged excitons in TMD monolayers can be utilized as quantum units in designing of practical valleytronic devices operating at 300 K.

Classical electrodynamics describes the optical response of systems using bulk electronic properties and infinitesimally thin boundaries. However, due to the quantum nature of electrons, interfaces have a finite thickness. Non-classical surface effects become increasingly important as ever smaller nanoscale systems are realized and eventually dominate over volume-related phenomena. Investigating the response of surface electrons in such systems, therefore, becomes imperative. One way to gain control over non-classical interface effects and study them is through electrical gating, as the static screening charges reside exclusively at the surface. Here, we investigate the modulation of the surface response upon direct electric charging of a single plasmonic nanoresonator by measuring the resulting changes in resonance. We analyze the observed effects within the general framework of surface-response functions and provide a basic model derived from electron spill-out within the local-response approximation (LRA). Our observed change in resonance frequency is well accounted for by assuming a modulation of the in-plane surface current. Surprisingly, we also measure a change in the resonance width, where adding electrons to the surface leads to a narrowing of the plasmonic resonance, i.e., reduced losses. The description of such effects requires considering nonlocal effects and the inclusion of a possible anisotropy of the perturbed surface permittivity. Our experiment, therefore, opens a vast field of investigations on how to gain control over the surface response in plasmonic resonators and to develop ultrafast and extremely small electrically driven plasmonic modulators and metasurfaces by leveraging electrical control over non-classical surface effects., Comment: 10 pages, 4 figures, 15 pages Supplementary

Impurity-vacancy centers in diamond offer a new class of robust photon sources with versatile quantum properties. While individual color centers commonly act as single-photon sources, their ensembles have been theoretically predicted to have tunable photon-emission statistics. Importantly, the particular type of excitation affects the emission properties of a color center ensemble within a diamond crystal. While optical excitation favors non-synchronized excitation of color centers within an ensemble, electron-beam excitation can synchronize the emitters and thereby provides a control of the second-order correlation function $g_2(0)$. In this letter, we demonstrate experimentally that the photon stream from an ensemble of color centers can exhibit $g_2(0)$ both above and below unity. Such a photon source based on an ensemble of few color centers in a diamond crystal provides a highly tunable platform for informational technologies operating at room temperature.

Angular momentum is an important physical property that plays a key role in light-matter interactions such as spin-orbit interaction. Here, we investigate theoretically and experimentally the spin-orbit interaction between a circularly polarized optical (spin) and a transverse vortex acoustic wave (orbital) using Brillouin backscattering in a silica optical nanofiber. We specifically explore the state of polarization of Brillouin backscattering induced by the TR21 torso-radial vortex acoustic mode that carries an orbital angular momentum. Using a full-vectorial theoretical model, we predict and observe two operating regimes for which the backscattered Brillouin signal is either depolarized or circularly polarized depending on the input pump polarization. We demonstrate that when the pump is circularly polarized and thus carries a spin angular momentum, the backscattered signal undergoes a handedness reversal of circular polarization due to optoacoustic spin-orbit interaction and the conservation of overall angular momentum.

Tin fluoride (SnF2) is an indispensable additive for high-efficiency Pb-Sn perovskite solar cells (PSCs). However, the spatial distribution of SnF2 in the perovskite absorber is seldom investigated while essential for a comprehensive understanding of the exact role of the SnF2 additive. Herein, we revealed the spatial distribution of SnF2 additive and made structure-optoelectronic properties-flexible photovoltaic performance correlation. We observed the chemical transformation of SnF2 to a fluorinated oxy-phase on the Pb-Sn perovskite film surface, due to its rapid oxidation. In addition, at the buried perovskite interface, we detected and visualized the accumulation of F- ions. We found that the photoluminescence quantum yield of Pb-Sn perovskite reached the highest value with 10 mol% SnF2 in the precursor solution. When integrating the optimized absorber in flexible devices, we obtained the flexible Pb-Sn perovskite narrow bandgap (1.24 eV) solar cells with an efficiency of 18.5% and demonstrated 23.1%-efficient flexible 4-terminal all-perovskite tandem cells.

We propose an efficient approach for actively controlling the Rabi oscillations in emitter-cavity hybrids based on the presence of an element with optical gain. Inspired by recent developments in parity-time ($\mathcal{PT}$)-symmetry photonics, we show that nano- or micro-cavities where intrinsic losses are partially or fully compensated by an externally controllable amount of gain offer unique capabilities for manipulating the dynamics of emitters. In particular, one can drastically modify the dynamics of the system, increase the overall occupation numbers, enhance the longevity of the Rabi oscillations, and even decelerate them to the point where their experimental observation becomes less challenging. Furthermore, we show that there is a specific gain value that leads to an exceptional point, where both emitter and cavity occupation oscillate practically in phase, with occupation numbers that can significantly exceed unity. By revisiting a recently-introduced Rabi-visibility measure, we provide robust guidelines for quantifying the coupling strength and achieving strong-coupling with adaptable Rabi frequency via loss compensation.

We explore the emergence and active control of optical bistability in a two-level atom near a graphene sheet. Our theory incorporates self-interaction of the optically-driven atom and its coupling to electromagnetic vacuum modes, both of which are sensitive to the electrically-tunable interband transition threshold in graphene. We show that electro-optical bistability and hysteresis can manifest in the intensity, spectrum, and quantum statistics of the light emitted by the atom, which undergoes critical slow-down to steady-state. The optically-driven atom-graphene interaction constitutes a platform for active control of driven atomic systems in quantum coherent control and atomic physics., Comment: 16 pages, 7 figures

Coherent control of traveling acoustic excitations in a waveguide system is an interesting way to manipulate and transduce classical and quantum information. So far, these interactions, often based on optomechanical resonators or Brillouin scattering, have been studied in the steady-state regime using continuous waves. However, waveguide experiments are often based on optical pump pulses which require treatment in a dynamic framework. In this paper, we present an effective Hamiltonian formalism in the dynamic regime using optical pulses that links waveguide optomechanics and cavity optomechanics, which can be used in the classical and quantum regime including quantum noise. Based on our formalism, a closed solution for coupled-mode equation under the undepleted assumption is provided and we found that the strong coupling regime is already accessible in current Brillouin waveguides by using pulses. We further investigate several possible experiments within waveguide optomechanics, including Brillouin-based coherent transfer, Brillouin cooling, and optoacoustic entanglement.

Optical non-reciprocity, which breaks the symmetry between forward and backward propagating optical waves, has become vital in photonic systems and enables many key devices, such as optical isolators, circulators and optical routers. Most conventional optical isolators involve magneto-optic materials, but devices based on optical nonlinearities, optomechanically induced transparency and stimulated Brillouin scattering (SBS) have also been demonstrated. So far, however, they have only been implemented for linearly or randomly polarized LP01-like fundamental modes. Here we report a light-driven nonreciprocal isolator for optical vortex modes, based on topology-selective SBS in chiral photonic crystal fibre. The device can be reconfigured as an amplifier or an isolator by adjusting the frequency of the control signal. The experimental results show vortex isolation of 22 dB, which is at the state-of-the-art in fundamental mode isolators using SBS. This unique device may find applications in optical communications, fibre lasers, quantum information processing and optical tweezers.

We analyse the emergence of unphysical superluminal group velocities in Su--Schrieffer--Heeger (SSH) parity-time ($\mathcal{PT}$) symmetric chains, and explore the origins of such a behaviour. By comparing the band structure of an infinite loss-gain SSH chain with that of a one-dimensional Bragg stack, we first exclude insufficient coupling consideration in the tight-binding description as the cause of group-velocity divergence. We then focus on material dispersion, and show that indeed, restoring causality in the description of both the lossy and the gain components resolves the problem and recovers finite group velocities, whose real part can only exceed the speed of light in vacuum when accompanied by a significant imaginary part. Our analysis introduces thus the required practical limits in the performance of common $\mathcal{PT}$-symmetric systems., Comment: 9 pages, 3 figures

Cathodoluminescence spectroscopy performed in an electron microscope has proven a versatile tool for analysing the near- and far-field optical response of plasmonic and dielectric nanostructures. Nevertheless, the transition radiation produced by electron impact is often disregarded in the interpretation of the spectra recorded from resonant nanoparticles. Here we show, experimentally and theoretically, that transition radiation can by itself generate distinct resonances which, depending on the time of flight of the electron beam inside the particle, can result from constructive or destructive interference in time. Superimposed on the eigenmodes of the investigated structures, these resonances can distort the recorded spectrum and lead to potentially erroneous assignment of modal characters to the spectral features. We develop an intuitive analogy that helps distinguish between the two contributions. As an example, we focus on the case of silicon nanospheres, and show that our analysis facilitates the unambiguous interpretation of experimental measurements on Mie-resonant nanoparticles.

Cathodoluminescence spectroscopy in conjunction with second-order auto-correlation measurements of $g_2(\tau)$ allows to extensively study the synchronization of quantum light sources in low-dimensional structures. Co-existing excitons in two-dimensional transition metal dichalcogenide monolayers provide a great source of identical quantum emitters which can be simultaneously excited by an electron. In this article, we demonstrate large photon bunching with $g_2(0)$ up to $156\pm16$ of a tungsten disulfide monolayer, exhibiting a strong dependence on the electron-beam current density. To further improve the excitation synchronization and the electron-emitter interaction, we show exemplary that the careful selection of a simple and compact geometry -- a thin, monocrystalline gold nanodisk -- can be used to realize a record-high bunching $g_2(0)$ of up to $2152\pm236$. This approach to control the electron excitation of excitons in a \ce{WS2} monolayer allows for the synchronization of quantum emitters in an ensemble, which is important to further advance quantum information processing and computing technologies., Comment: Supporting information is available upon request to authors

Historically, the field of plasmonics has been relying on the framework of classical electrodynamics, with the local-response approximation of material response being applied even when dealing with nanoscale metallic structures. However, when approaching the atomic-scale confinement of the electromagnetic radiation, mesoscopic effects are anticipated to become observable, e.g., those associated with the nonlocal electrodynamic surface response of the electron gas. We investigate nonlocal effects in propagating gap surface plasmon modes in ultrathin metal--dielectric--metal planar waveguides, exploiting monocrystalline gold flakes separated by atomic-layer-deposited aluminum oxide. We use scanning near-field optical microscopy to directly access the near-field of such confined gap plasmon modes and measure their dispersion relation (via their complex-valued propagation constants). We compare our experimental findings with the predictions of the generalized nonlocal optical response theory to unveil signatures of nonlocal damping, which becomes appreciable for smaller dielectric gaps., Comment: Supporting information is available upon request to authors

Surface-response functions are one of the most promising routes for bridging the gap between fully quantum-mechanical calculations and phenomenological models in quantum nanoplasmonics. Within all the currently available recipes for obtaining such response functions, \emph{ab initio} calculations remain one of the most predominant, wherein the surface-response function are retrieved via the metal's non-equilibrium response to an external perturbation. Here, we present a complementary approach where one of the most appealing surface-response functions, namely the Feibelman $d$-parameters, yield a finite contribution even in the case where they are calculated directly from the equilibrium properties described under the local-response approximation (LRA), but with a spatially varying equilibrium electron density. Using model calculations that mimic both spill-in and spill-out of the equilibrium electron density, we show that the obtained $d$-parameters are in qualitative agreement with more elaborate, but also more computationally demanding, \emph{ab initio} methods. The analytical work presented here illustrates how microscopic surface-response functions can emerge out of entirely local electrodynamic considerations., Comment: Supplementary material is available upon request to authors

Highly integrated active nanophotonics addressing both device footprint and operation speed demands is a key enabling technology for the next generation optical networks. Plasmonic systems have proven to be a serious contender to alleviate current performance limitations in electro-optic devices. Here, we demonstrate a plasmonic optical phased array (OPA) consisting of two 10-$\mu$m-long plasmonic phase shifters, utilized to control the far-field radiation pattern of two subwavelength-separated emitters for aliasing-free beam steering with an angular range of $\pm5^\circ$ and flat frequency response up to 18 GHz (with the potential bandwidth of 1.2 THz). Extreme optical and electrostatic field confinement with great spatial overlap results in high phase modulation efficiency ($V_{\pi}L=0.24\: \text{Vcm}$). The demonstrated approach of using plasmonic lithium niobate technology for optical beam manipulation offers inertia-free, robust, ultra-compact and high-speed beam steering., Comment: 8 pages, 3 figures

Noble metals with well-defined crystallographic orientation constitute an appealing class of materials for controlling light-matter interactions on the nanoscale. Nonlinear optical processes, being particularly sensitive to anisotropy, are a natural and versatile probe of crystallinity in nano-optical devices. Here we study the nonlinear optical response of monocrystalline gold flakes, revealing a polarization dependence in second-harmonic generation from the {111} surface that is markedly absent in polycrystalline films. Apart from suggesting an approach for directional enhancement of nonlinear response in plasmonic systems, we anticipate that our findings can be used as a rapid and non-destructive method for characterization of crystal quality and orientation that may be of significant importance in future applications., Comment: 5 pages, 4 figures, color

The recent generalised nonlocal optical response (GNOR) theory for plasmonics is analysed, and its main input parameter, namely the complex hydrodynamic convection-diffusion constant, is quantified in terms of enhanced Landau damping due to diffusive surface scattering of electrons at the surface of the metal. GNOR has been successful in describing plasmon damping effects, in addition to the frequency shifts originating from induced-charge screening, through a phenomenological electron diffusion term implemented into the traditional hydrodynamic Drude model of nonlocal plasmonics. Nevertheless, its microscopic derivation and justification is still missing. Here we discuss how the inclusion of a diffusion-like term in standard hydrodynamics can serve as an efficient vehicle to describe Landau damping without resorting to computationally demanding quantum-mechanical calculations, and establish a direct link between this term and the Feibelman $d$ parameter for the centroid of charge. Our approach provides a recipe to connect the phenomenological fundamental GNOR parameter to a frequency-dependent microscopic surface-response function. We therefore tackle one of the principal limitations of the model, and further elucidate its range of validity and limitations, thus facilitating its proper application in the framework of nonclassical plasmonics.

Dark plasmonic modes have interesting properties, such as a longer lifetime and a narrower linewidth than their radiative counterpart, as well as little to no radiative losses. However, they have not been extensively studied yet due to their optical inaccessibility. Using electron-energy loss (EEL) and cathodoluminescence (CL) spectroscopy, the dark radial breathing modes (RBMs) in thin, monochrystalline gold nanodisks are systematically investigated in this work. It is found that the RBMs can be detected in a CL set-up despite only collecting the far-field. Their visibility in CL is attributed to the breaking of the mirror symmetry by the high-index substrate, creating an effective dipole moment. The outcoupling into the far-field is demonstrated to be enhanced by a factor of 4 by increasing the thickness of the supporting SiN membrane from 5 to 50 nm due to the increased net electric dipole moment in the substrate. Furthermore, it is shown that the resonance energy of RBMs can be easily tuned by varying the diameter of the nanodisk, making them promising candidates for nanophotonic applications.

From the onset of high-speed optical communications, lithium niobite (LN) has been the material of choice for electro-optic modulators owing to its large electro-optic response, wide transparent window, excellent thermal stability and long-term material reliability. Conventional LN electro-optic modulators while continue to be the workhorse of the optoelectronic industry become progressively too bulky, expensive and power hungry to fully serve the needs of this industry rapidly progressing towards highly integrated, cost-effective and energy efficient components and circuits. Recently developed monolithic LN nanophotonic platform enables the realization of electro-optic modulators that are significantly improved in terms of compactness, bandwidth and energy efficiency, while still demanding relatively long, on the mm-scale, interaction lengths. Here we successfully deal with this challenge and demonstrate plasmonic electro-optic directional coupler switches consisting of two closely spaced nm-thin gold nanostripes monolithically fabricated on LN substrates that guide both coupled electromagnetic modes and electrical signals influencing their coupling and thereby enabling ultra-compact switching and modulatiofunctionalities. The extreme confinement of both slow-plasmon modes and electrostatic fields created by two nanostripes along with their nearly perfect spatial overlap allowed us to achieve a 90% modulation depth with 20-$\mu$m-long switches characterized by a electro-optic modulation efficiency of 0.3 Vcm. Our monolithic LN plasmonic platform enables ultra-dense integration of high-performance active photonic components, enabling a wide range of cost-effective optical communication applications demanding $\mu$m-scale footprints, ultrafast operation, robust design and high environmental stability., Comment: 19 pages, 4 figures

Light-matter interactions at the nanoscale constitute a fundamental ingredient for engineering applications in nanophotonics and quantum optics. To this regard electromagnetic Mie resonances excited in high-refractive index dielectric nanoparticles have recently attracted interest because of their lower losses and better control over the scattering patterns compared to their plasmonic metallic counterparts. The emergence of several resonances in those systems results in an overall high complexity, where the electric and magnetic dipoles have significant overlap in the case of spherical symmetry, thus concealing the contributions of each resonance separately. Here we show, experimentally and theoretically, the emergence of strong light-matter coupling between the magnetic and electric-dipole resonances of individual silicon nanodisks coupled to a J-aggregated organic semiconductor resonating at optical frequencies, evidencing how the different properties of the two resonances results in two different coupling strengths. The energy splittings observed are of the same order of magnitude as in similar plasmonic systems, thus confirming dielectric nanoparticles as promising alternatives for localized strong coupling studies. The coupling of both the electric and magnetic dipole resonances can offer interesting possibilities for the control of directional light scattering in the strong-coupling regime and the dynamic tuning of nanoscale light-matter coupled states by external fields.

Acoustic waves can serve as memory for optical information, however, acoustic phonons in the GHz regime decay on the nanosecond timescale. Usually this is dominated by intrinsic acoustic loss due to inelastic scattering of the acoustic waves and thermal phonons. Here we show a way to counteract the intrinsic acoustic decay of the phonons in a waveguide by resonantly reinforcing the acoustic wave via synchronized optical pulses. This scheme overcomes the previous constraints of phonon-based optical signal processing for light storage and memory. We experimentally demonstrate on-chip storage up to 40 ns, four times the intrinsic acoustic lifetime in the waveguide. We confirm the coherence of the scheme by detecting the phase of the delayed optical signal after 40 ns using homodyne detection. Through theoretical considerations we anticipate that this concept allows for storage times up to microseconds within realistic experimental limitations while maintaining a GHz bandwidth of the optical signal. The refreshed phonon-based light storage removes the usual bandwidth-delay product limitations of e.g. slow-light schemes., Comment: 6 pages, 5 figures, BS and MM contributed equally

Non-Hermitian exceptional points (EPs) represent a special type of degeneracy where not only the eigenvalues coalesce, but also the eigenstates tend to collapse on each other. Recent studies have shown that in the presence of an EP, light-matter interactions are profoundly modified, leading to a host of novel optical phenomena ranging from enhanced sensitivity to chiral light transport. As of now, however, in order to stabilize a system at the vicinity of an exceptional point, its related parameters must be carefully tuned and/or continuously controlled. To overcome this limitation, here we introduce a new family of broadband exceptional points based on unidirectional coupling, implemented by incorporating an Sshaped waveguide in a microring cavity. In active settings, the resulting unidirectionality exhibits unprecedented resilience to perturbations, thus providing a robust and tunable approach for directly generating beams with distinct orbital angular momentum (OAM). This work could open up new possibilities for manipulating OAM degrees of freedom in applications pertaining to telecommunications and quantum computing, while at the same time may expand the notions of non-Hermiticity in the orbital angular momentum space.

We analyze intrinsic nonlinearities in two-dimensional polaritonic materials interacting with an optical wave. Focusing on the case of graphene, we show that the second-order nonlinear optical conductivity due to carrier density fluctuations associated with the excitation of a plasmon polariton is closely related to the ponderomotive force due to the oscillating optical field. This relation is first established through an elegant thermodynamic approach for a Drude-like plasma, in the frequency range where intraband scattering is the dominant contribution to conductivity. Subsequently, we extend our analysis to the interband regime, and show that for energies approximately half the Fermi energy, the intraband contribution to the ponderomotive force diverges. In practice, thermal broadening regularizes this divergence as one would expect, but even at room temperature typically leaves a strong ponderomotive enhancement. Finally, we study the impact of nonlocal corrections and find that nonlocality does not lead to further broadening (as one would expect in the case of Landau damping), but rather to a splitting of the ponderomotive interband resonance. Our analysis should prove useful to the open quest for exploiting nonlinearities in graphene and other two-dimensional polaritonic materials, through effects such as second harmonic generation and photon drag., Comment: 7 pages, 2 figures, 1 appendix

The plasmon and phonon polaritons of two-dimensional (2d) and van-der-Waals materials have recently gained substantial interest. Unfortunately, they are notoriously hard to observe in linear response because of their strong confinement, low frequency and longitudinal mode symmetry. Here, we propose a fundamentally new approach of harnessing nonlinear resonant scattering that we call stimulated plasmon polariton scattering (SPPS) in analogy to the opto-acoustic stimulated Brillouin scattering (SBS). We show that SPS allows to excite, amplify and detect 2d plasmon and phonon polaritons all across the THz-range while requiring only optical components in the near-IR or visible range. We present a coupled-mode theory framework for SPS and based on this find that SPS power gains exceed the very top gains observed in on-chip SBS by at least an order of magnitude. This opens exciting new possibilities to fundamental studies of 2d materials and will help closing the THz gap in spectrocopy and information technology., Comment: 7 pages, 3 figures

The incorporation of even small amounts of strontium (Sr) into lead-based quadruple cation hybrid perovskite solar cells results in a systematic increase of the open circuit voltage (Voc) in pin-type perovskite solar cells. We demonstrate via transient and absolute photoluminescence (PL) experiments how the incorporation of Sr significantly reduces the non-radiative recombination losses in the neat perovskite layer and specifically at the perovskite/C60 interface. We show that Sr segregates at the perovskite surface, where it induces important changes of morphology and energetics. Notably, the Sr-enriched surface exhibits a wider band gap and a more n-type character, accompanied with significantly stronger surface band bending. As a result, we observe a significant increase of the quasi-Fermi level splitting in the neat perovskite by reduced surface recombination and more importantly, a strong reduction of losses attributed to non-radiative recombination at the interface to the C60 electron-transporting layer. The resulting solar cells exhibited a Voc of 1.18 V, which could be further improved to nearly 1.23 V through addition of a thin polymer interlayer, bringing the non-radiative voltage loss to only 110 meV. Our work shows that simply adding a small amount of Sr to the precursor solutions induces a beneficial surface modification in the perovskite, without requiring any post treatment, resulting in high efficiency solar cells with power conversion efficiency (PCE) up to 20.3%. Our results demonstrate very high Voc values and efficiencies in Sr-containing quadruple cation perovskite pin solar cells and highlight the imperative importance of addressing and minimizing the recombination losses at the interface between perovskite and charge transporting layer., Comment: Manuscript and supporting information merged together in one file

We theoretically evaluate the impact of drift-free noise on the dynamics of $\mathcal{PT}$-symmetric non-Hermitian systems with an exceptional point, which have recently been proposed for sensors. Such systems are currently considered as promising templates for sensing applications, because of their intrinsically extremely sensitive response to external perturbations. However, this applies equally to the impact of fabrication imperfections and fluctuations in the system parameters. Here we focus on the influence of such fluctuations caused by inevitable (thermal) noise and show that the exceptional-point eigenstate is not stable in its presence. To this end, we derive an effective differential equation for the mean time evolution operator averaged over all realizations of the noise field and via numerical analysis we find that the presence of noise leads to exponential divergence of any initial state after some characteristic period of time. We therefore show that it is rather demanding to design sensor systems based on continuous operation at an exceptional point., Comment: 7 pages, 2 figures

On-chip manipulating and controlling the temporal and spatial evolution of light is of crucial importance for information processing in future planar integrated nanophotonics. The spin and orbital angular momentum of light, which can be treated independently in classical macroscopic geometrical optics, appear to be coupled on subwavelength scales. We use spin-orbit interactions in a plasmonic achiral nano-coupler to unidirectionally excite surface plasmon polariton modes propagating in seamlessly integrated plasmonic slot waveguides. The spin-dependent flow of light in the proposed nanophotonic circuit allows on-chip electrical detection of the spin state of incident photons by integrating two germanium-based plasmonic-waveguide photodetectors. Consequently, our device serves as a compact ($\sim$ 6 $\times$ 18 $\mu$m$^2$) electrical sensor for photonic spin Hall dynamics. The demonstrated configuration opens new avenues for developing highly-integrated polarization-controlled optical devices that would exploit the spin-degree of freedom for manipulating and controlling subwavelength optical modes in nanophotonic systems., Comment: 15 pages, 4 figures

Charge transport layers (CTLs) are key components of diffusion controlled perovskite solar cells, however, they can induce additional non-radiative recombination pathways which limit the open circuit voltage (V_OC) of the cell. In order to realize the full thermodynamic potential of the perovskite absorber, both the electron and hole transport layer (ETL/HTL) need to be as selective as possible. By measuring the quasi-Fermi level splitting (QFLS) of perovskite/CTL heterojunctions, we quantify the non-radiative interfacial recombination current for a wide range of commonly used CTLs, including various hole-transporting polymers, spiro-OMeTAD, metal oxides and fullerenes. We find that all studied CTLs limit the V_OC by inducing an additional non-radiative recombination current that is significantly larger than the loss in the neat perovskite and that the least-selective interface sets the upper limit for the V_OC of the device. The results also show that the V_OC equals the internal QFLS in the absorber layer of (pin, nip) cells with selective CTLs and power conversion efficiencies of up to 21.4%. However, in case of less selective CTLs, the V_OC is substantially lower than the QFLS which indicates additional losses at the contacts and/or interfaces. The findings are corroborated by rigorous device simulations which outline several important considerations to maximize the V_OC. This work shows that the real challenge to supress non-radiative recombination losses in perovskite cells on their way to the radiative limit lies in the suppression of carrier recombination at the perovskite/CTL interfaces., Comment: Update of Figure 3 and Figure S9 and new Figure S10 added