Ultrastrong magnon-magnon coupling and chiral spin-texture control in a dipolar 3D multilayered artificial spin-vortex ice.

Strongly-interacting nanomagnetic arrays are ideal systems for exploring reconfigurable magnonics. They provide huge microstate spaces and integrated solutions for storage and neuromorphic computing alongside GHz functionality. These systems may be broadly assessed by their range of reliably accessible states and the strength of magnon coupling phenomena and nonlinearities. Increasingly, nanomagnetic systems are expanding into three-dimensional architectures. This has enhanced the range of available magnetic microstates and functional behaviours, but engineering control over 3D states and dynamics remains challenging. Here, we introduce a 3D magnonic metamaterial composed from multilayered artificial spin ice nanoarrays. Comprising two magnetic layers separated by a non-magnetic spacer, each nanoisland may assume four macrospin or vortex states per magnetic layer. This creates a system with a rich 16N microstate space and intense static and dynamic dipolar magnetic coupling. The system exhibits a broad range of emergent phenomena driven by the strong inter-layer dipolar interaction, including ultrastrong magnon-magnon coupling with normalised coupling rates of Δ f ν = 0.57 , GHz mode shifts in zero applied field and chirality-control of magnetic vortex microstates with corresponding magnonic spectra.

Breakdown of Temporal Coherence in Photon Condensates.

The temporal coherence of an ideal Bose gas increases as the system approaches the Bose-Einstein condensation threshold from below, with coherence time diverging at the critical point. However, counterexamples have been observed for condensates of photons formed in an externally pumped, dye-filled microcavity, wherein the coherence time decreases rapidly for increasing particle number above threshold. This Letter establishes intermode correlations as the central explanation for the experimentally observed dramatic decrease in the coherence time beyond critical pump power.

Optical Gain Spectrum and Confinement Factor of a Monolayer Semiconductor in an Ultrahigh-Quality Cavity.

Two-dimensional (2D) semiconductors have attracted great attention as a novel class of gain materials for low-threshold, on-chip coherent light sources. Despite several experimental reports on lasing, the underlying gain mechanism of 2D materials remains elusive due to a lack of key information, including modal gain and the confinement factor. Here, we demonstrate a novel approach to directly determine the absorption coefficient of monolayer WS2 by characterizing the whispering gallery modes in a van der Waals microdisk cavity. By exploiting the cavity's high intrinsic quality factor of 2.5 × 104, the absorption coefficient spectrum and confinement factor are experimentally resolved with unprecedented accuracy. The excitonic gain reduces the WS2 absorption coefficient by 2 × 104 cm-1 at room temperature, and the experimental confinement factor is found to agree with the theoretical prediction. These results are essential for unveiling the gain mechanism in emergent, low-threshold 2D-semiconductor-based laser devices.

Crystalline AuNP-Decorated Strontium Niobate Thin Films: Strain-Controlled AuNP Morphologies and Optical Properties for Plasmonic Applications.

Gold nanoparticle (AuNP) decoration is a commonly used method to enhance the optical responses in many applications such as photocatalysis, biosensing, solar cells, etc. The morphology and structure of AuNPs are essential factors determining the functionality of the sample. However, tailoring the growth mechanism of AuNPs on an identical surface is not straightforward. In this study, AuNPs were deposited on the surface of a perovskite thin film, strontium niobate (SNO), using pulsed laser deposition (PLD). AuNPs exhibited a dramatic variation in their growth mechanisms, depending on whether they were deposited on SNO thin films grown on magnesium oxide (SNO/MgO) or strontium titanate (SNO/STO) substrates. On SNO/MgO, the Au aggregates form large NPs with an average size of up to 3500 nm2. These AuNPs are triangular with sharp edges and corners. The out-of-plane direction of growth is favored, and the surface coverage ratio by AuNPs is low. When deposited on SNO/STO, the average size of AuNPs is much smaller, i.e., ∼250 nm2. This reduction in the average size is accompanied by an increase in the number density of NPs. AuNPs on SNO/STO have a round shape and high coverage ratio. Such an impact from the substrate selection on the AuNP structure is significant when the sandwiched SNO film is below 80 nm thickness and is weakened for 200 nm of SNO films. X-ray diffraction (XRD) and scanning electron microscopy (SEM) were used to characterize all samples. Strain analysis was used to explain the growth mechanism of AuNPs. The average height of AuNPs was measured by using atomic force microscopy (AFM). Ellipsometry in the visible-near-infrared (vis-NIR) region was used to characterize the optical response of all samples. AuNP-decorated SNO/MgO and SNO/STO thin films exhibit different optical properties, with only gold-decorated SNO/MgO samples showing a size-dependent epsilon-near-zero behavior of nanoparticles. These results provide an additional route to control the structure of AuNPs. They can be used for various plasmonic applications like the design and development of strain-engineered gold-nanoparticle-decorated devices for surface-enhanced Raman spectroscopy (SERS) and photocatalysis.

Optimizing Hot Electron Harvesting at Planar Metal-Semiconductor Interfaces with Titanium Oxynitride Thin Films.

Understanding metal-semiconductor interfaces is critical to the advancement of photocatalysis and sub-bandgap solar energy harvesting where electrons in the metal can be excited by sub-bandgap photons and extracted into the semiconductor. In this work, we compare the electron extraction efficiency across Au/TiO2 and titanium oxynitride (TiON)/TiO2-x interfaces, where in the latter case the spontaneously forming oxide layer (TiO2-x) creates a metal-semiconductor contact. Time-resolved pump-probe spectroscopy is used to study the electron recombination rates in both cases. Unlike the nanosecond recombination lifetimes in Au/TiO2, we find a bottleneck in the electron relaxation in the TiON system, which we explain using a trap-mediated recombination model. Using this model, we investigate the tunability of the relaxation dynamics with oxygen content in the parent film. The optimized film (TiO0.5N0.5) exhibits the highest carrier extraction efficiency (NFC ≈ 2.8 × 1019 m-3), slowest trapping, and an appreciable hot electron population reaching the surface oxide (NHE ≈ 1.6 × 1018 m-3). Our results demonstrate the productive role oxygen can play in enhancing electron harvesting and prolonging electron lifetimes, providing an optimized metal-semiconductor interface using only the native oxide of titanium oxynitride.

Emission enhancement of erbium in a reverse nanofocusing waveguide.

Since Purcell's seminal report 75 years ago, electromagnetic resonators have been used to control light-matter interactions to make brighter radiation sources and unleash unprecedented control over quantum states of light and matter. Indeed, optical resonators such as microcavities and plasmonic antennas offer excellent control but only over a limited spectral range. Strategies to mutually tune and match emission and resonator frequency are often required, which is intricate and precludes the possibility of enhancing multiple transitions simultaneously. In this letter, we report a strong radiative emission rate enhancement of Er3+-ions across the telecommunications C-band in a single plasmonic waveguide based on the Purcell effect. Our gap waveguide uses a reverse nanofocusing approach to efficiently enhance, extract and guide emission from the nanoscale to a photonic waveguide while keeping plasmonic losses at a minimum. Remarkably, the large and broadband Purcell enhancement allows us to resolve Stark-split electric dipole transitions, which are typically only observed under cryogenic conditions. Simultaneous radiative emission enhancement of multiple quantum states is of great interest for photonic quantum networks and on-chip data communications.

Near-unity Raman ß-factor of surface-enhanced Raman scattering in a waveguide.

The Raman scattering of light by molecular vibrations is a powerful technique to fingerprint molecules through their internal bonds and symmetries. Since Raman scattering is weak1, methods to enhance, direct and harness it are highly desirable, and this has been achieved using optical cavities2, waveguides3-6 and surface-enhanced Raman scattering (SERS)7-9. Although SERS offers dramatic enhancements2,6,10,11 by localizing light within vanishingly small hot-spots in metallic nanostructures, these tiny interaction volumes are only sensitive to a few molecules, yielding weak signals12. Here we show that SERS from 4-aminothiophenol molecules bonded to a plasmonic gap waveguide is directed into a single mode with >99% efficiency. Although sacrificing a confinement dimension, we find a SERS enhancement of ~103 times across a broad spectral range enabled by the waveguide's larger sensing volume and non-resonant waveguide mode. Remarkably, this waveguide SERS is bright enough to image Raman transport across the waveguides, highlighting the role of nanofocusing13-15 and the Purcell effect16. By analogy to the ß-factor from laser physics10,17-20, the near-unity Raman ß-factor we observe exposes the SERS technique to alternative routes for controlling Raman scattering. The ability of waveguide SERS to direct Raman scattering is relevant to Raman sensors based on integrated photonics7-9 with applications in gas sensing and biosensing.

Learning the Fuzzy Phases of Small Photonic Condensates.

Phase transitions, being the ultimate manifestation of collective behavior, are typically features of many-particle systems only. Here, we describe the experimental observation of collective behavior in small photonic condensates made up of only a few photons. Moreover, a wide range of both equilibrium and nonequilibrium regimes, including Bose-Einstein condensation or laserlike emission are identified. However, the small photon number and the presence of large relative fluctuations places major difficulties in identifying different phases and phase transitions. We overcome this limitation by employing unsupervised learning and fuzzy clustering algorithms to systematically construct the fuzzy phase diagram of our small photonic condensate. Our results thus demonstrate the rich and complex phase structure of even small collections of photons, making them an ideal platform to investigate equilibrium and nonequilibrium physics at the few particle level.

Efficient ultrafast all-optical modulation in a nonlinear crystalline gallium phosphide nanodisk at the anapole excitation.

High-refractive index nanostructured dielectrics have the ability to locally enhance electromagnetic fields with low losses while presenting high third-order nonlinearities. In this work, we exploit these characteristics to achieve efficient ultrafast all-optical modulation in a crystalline gallium phosphide (GaP) nanoantenna through the optical Kerr effect (OKE) and two-photon absorption (TPA) in the visible/near-infrared range. We show that an individual GaP nanodisk can yield differential reflectivity modulations of up to ~40%, with characteristic modulation times between 14 and 66 fs, when probed at the anapole excitation (AE). Numerical simulations reveal that the AE represents a unique condition where both the OKE and TPA contribute with the same modulation sign, maximizing the response. These findings highly outperform previous reports on sub-100-fs all-optical switching from resonant nanoscale dielectrics, which have demonstrated modulation depths no larger than 0.5%, placing GaP nanoantennas as a promising choice for ultrafast all-optical modulation at the nanometer scale.

Plasmon-Driven Hot Electron Transfer at Atomically Sharp Metal-Semiconductor Nanojunctions.

Recent advances in guiding and localizing light at the nanoscale exposed the enormous potential of ultrascaled plasmonic devices. In this context, the decay of surface plasmons to hot carriers triggers a variety of applications in boosting the efficiency of energy-harvesting, photocatalysis, and photodetection. However, a detailed understanding of plasmonic hot carrier generation and, particularly, the transfer at metal-semiconductor interfaces is still elusive. In this paper, we introduce a monolithic metal-semiconductor (Al-Ge) heterostructure device, providing a platform to examine surface plasmon decay and hot electron transfer at an atomically sharp Schottky nanojunction. The gated metal-semiconductor heterojunction device features electrostatic control of the Schottky barrier height at the Al-Ge interface, enabling hot electron filtering. The ability of momentum matching and to control the energy distribution of plasmon-driven hot electron injection is demonstrated by controlling the interband electron transfer in Ge, leading to negative differential resistance.

Stimulated Raman Scattering in Ge Nanowires.

Investigating group-IV-based photonic components is a very active area of research with extensive interest in developing complementary metal-oxide-semiconductor (CMOS) compatible light sources. However, due to the indirect band gap of these materials, effective light-emitting diodes and lasers based on pure Ge or Si cannot be realized. In this context, there is considerable interest in developing group-IV based Raman lasers. Nevertheless, the low quantum yield of stimulated Raman scattering in Si and Ge requires large device footprints and high lasing thresholds. Consequently, the fabrication of integrated, energy-efficient Raman lasers is challenging. Here, we report the systematic investigation of stimulated Raman scattering (SRS) in Ge nanowires (NWs) and axial Al-Ge-Al NW heterostructures with Ge segments that come into contact with self-aligned Al leads with abrupt metal-semiconductor interfaces. Depending on their geometry, these quasi-one-dimensional (1D) heterostructures can reassemble into Ge nanowires, Ge nanodots, or Ge nanodiscs, which are monolithically integrated within monocrystalline Al (c-Al) mirrors that promote both optical confinement and effective heat dissipation. Optical mode resonances in these nanocavities support in SRS thresholds as low as 60 kW/cm2. Most notably, our findings provide a platform for elucidating the high potential of future monolithically integrated, nanoscale low-power group-IV-based Raman lasers.

Ten years of spasers and plasmonic nanolasers.

Ten years ago, three teams experimentally demonstrated the first spasers, or plasmonic nanolasers, after the spaser concept was first proposed theoretically in 2003. An overview of the significant progress achieved over the last 10 years is presented here, together with the original context of and motivations for this research. After a general introduction, we first summarize the fundamental properties of spasers and discuss the major motivations that led to the first demonstrations of spasers and nanolasers. This is followed by an overview of crucial technological progress, including lasing threshold reduction, dynamic modulation, room-temperature operation, electrical injection, the control and improvement of spasers, the array operation of spasers, and selected applications of single-particle spasers. Research prospects are presented in relation to several directions of development, including further miniaturization, the relationship with Bose-Einstein condensation, novel spaser-based interconnects, and other features of spasers and plasmonic lasers that have yet to be realized or challenges that are still to be overcome.

Non-stationary statistics and formation jitter in transient photon condensation.

While equilibrium phase transitions are easily described by order parameters and free-energy landscapes, for their non-stationary counterparts these quantities are usually ill-defined. Here, we probe transient non-equilibrium dynamics of an optically pumped, dye-filled microcavity. We quench the system to a far-from-equilibrium state and find delayed condensation close to a critical excitation energy, a transient equivalent of critical slowing down. Besides number fluctuations near the critical excitation energy, we show that transient phase transitions exhibit timing jitter in the condensate formation. This jitter is a manifestation of the randomness associated with spontaneous emission, showing that condensation is a stochastic, rather than deterministic process. Despite the non-equilibrium character of this phase transition, we construct an effective free-energy landscape that describes the formation jitter and allows, in principle, its generalization to a wider class of processes.

Ultrafast All-Optical Modulation in 2D Hybrid Perovskites.

Two-dimensional (2D) hybrid organic-inorganic Ruddlesden-Popper perovskites (RPPs) have been recently shown to exhibit large nonlinear optical properties due to the strong excitonic effects present in their multiple quantum wells. In this work, we use nondegenerate pump-probe spectroscopy in the 600-1000 nm wavelength range to study the influence of nonlinear effects on the ultrafast dynamics of 2D RPP thin flakes. We find that, under sub-bandgap excitation, ∼100 nm thick perovskite sheets allow up to ∼2% reflectivity modulation within a 20 fs period, due to the nonlinear optical Kerr effect and two-photon absorption, surpassing by a factor of ∼5 the reported nonlinear performance of photonic metasurfaces and single nanoantennas. When the excitation is resonant with the excitonic absorption, the ultrafast nature of the nonlinear response is lost due to the presence of linear absorption creating long-lived free carriers. Our results suggest that 2D RPPs are potential nanoscale all-optical modulators in the visible/near-infrared waveband for applications such as ultrafast information processing, optical data transmission, and high-performance computing.

Giant and Tunable Optical Nonlinearity in Single-Crystalline 2D Perovskites due to Excitonic and Plasma Effects.

Materials with large optical nonlinearity, especially in the visible spectral region, are in great demand for applications in all-optical information processing and quantum optics. 2D hybrid Ruddlesden-Popper-type halide perovskites (RPPs) with tunable ultraviolet-to-visible direct bandgaps exhibit large nonlinear optical responses due to the strong excitonic effects present in their multiple quantum wells. Using a microscopic Z-scan setup with femtosecond laser pulses tunable across the visible spectrum, it is demonstrated that single-crystalline lead halide RPP nanosheets possess unprecedentedly large nonlinear refraction and absorption coefficients near excitonic resonances. A room-temperature insulator (exciton)-metal (plasma) Mott transition is found to occur near the exciton resonance of the thinnest qunatum-well RPPs, boosting the nonlinear response. Owing to the rapidly changing refractive index near resonance, a single RPP crystal can exhibit different nonlinear functionalities across the excitation spectrum. The results suggest that RPPs are efficient nonlinear materials in the visible waveband, indicating their potential use in integrated nonlinear photonic applications such as optical modulation and switching.

Ultrafast sub-30-fs all-optical switching based on gallium phosphide.

Gallium phosphide (GaP) is one of the few available materials with strong optical nonlinearity and negligible losses in the visible (λ > 450 nm) and near-infrared regime. In this work, we demonstrate that a GaP film can generate sub-30-fs (full width at half maximum) transmission modulation of up to ~70% in the 600- to 1000-nm wavelength range. Nonlinear simulations using parameters measured by the Z-scan approach indicate that the transmission modulation arises from the optical Kerr effect and two-photon absorption. Because of the absence of linear absorption, no slower free-carrier contribution is detected. These findings place GaP as a promising ultrafast material for all-optical switching at modulation speeds of up to 20 THz.

Applications of nanolasers.

Nanolasers generate coherent light at the nanoscale. In the past decade, they have attracted intense interest, because they are more compact, faster and more power-efficient than conventional lasers. Thanks to these capabilities, nanolasers are now an emergent tool for a variety of practical applications. In this Review, we explain the intrinsic merits of nanolasers and assess recent progress on their applications, particularly for optical interconnects, near-field spectroscopy and sensing, optical probing for biological systems and far-field beam synthesis through near-field eigenmode engineering. We highlight the scientific and engineering challenges that remain for forging nanolasers into powerful tools for nanoscience and nanotechnology.

Plasmon induced thermoelectric effect in graphene.

Graphene has emerged as a promising material for optoelectronics due to its potential for ultrafast and broad-band photodetection. The photoresponse of graphene junctions is characterized by two competing photocurrent generation mechanisms: a conventional photovoltaic effect and a more dominant hot-carrier-assisted photothermoelectric (PTE) effect. The PTE effect is understood to rely on variations in the Seebeck coefficient through the graphene doping profile. A second PTE effect can occur across a homogeneous graphene channel in the presence of an electronic temperature gradient. Here, we study the latter effect facilitated by strongly localised plasmonic heating of graphene carriers in the presence of nanostructured electrical contacts resulting in electronic temperatures of the order of 2000 K. At certain conditions, the plasmon-induced PTE photocurrent contribution can be isolated. In this regime, the device effectively operates as a sensitive electronic thermometer and as such represents an enabling technology for development of hot carrier based plasmonic devices.

Sub-20 fs All-Optical Switching in a Single Au-Clad Si Nanodisk.

Dielectric nanoantennas have recently emerged as promising elements for nonlinear and ultrafast nanophotonics due to their ability to concentrate light on the nanometer scale with low losses, while exhibiting large nonlinear susceptibilities. In this work, we demonstrate that single Si nanodisks covered with a thin 30 nm thick layer of Au can generate positive and negative sub-20 fs reflectivity modulations of ∼0.3% in the vicinity of the first-order anapole mode, when excited around the second-order anapole mode. The experimental results, characterized in the visible to near-infrared spectral range, suggest that the nonlinear optical Kerr effect is the responsible mechanism for the observed all-optical switching phenomena. These findings represent an important step toward nanoscale ultrafast all-optical signal processing.