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Rare earth dopants are one of the most extensively studied optical emission centers for a broad range of applications such as laser optoelectronics, sensing, lighting, and quantum information technologies due to their narrow optical linewidth and exceptional coherence properties. Epitaxial doped oxide thin films can serve as a promising and controlled host to investigate rare-earth dopants suitable for scalable quantum memories, on-chip lasers and amplifiers. Here, we report high-quality epitaxial thin films of Tm-doped CaZrO$_3$ grown by pulsed laser deposition for infrared optoelectronic and quantum memory applications. We perform extensive structural and chemical characterization to probe the crystallinity of the films and the doping behavior. Low temperature photoluminescence measurements show sharp radiative transitions in the short-wave infrared range of 1.75 - 2 \mu m., Comment: 17 pages, 4 figures

The fascinating realm of strain engineering and wetting transitions in two-dimensional (2D) materials takes place when placed on a two-dimensional array of nanopillars or one-dimensional rectangular grated substrates. Our investigation encompasses a diverse set of atomically thin 2D materials, including transition metal dichalcogenides, hexagonal boron nitride, and graphene, with a keen focus on the impact of van der Waals adhesion energies to the substrate on the wetting/dewetting behavior on nanopatterned substrates. We find a critical aspect ratio of the nanopillar or grating heights to the period of the pattern when the wetting/dewetting transition occurs. Furthermore, energy hysteresis analysis reveals dynamic detachment and re-engagement events during height adjustments, shedding light on energy barriers of 2D monolayer transferred on patterned substrates. Our findings offer avenues for strain engineering in 2D materials, leading to promising prospects for future technological applications.

Subwavelength diffractive optics known as meta-optics have demonstrated the potential to significantly miniaturize imaging systems. However, despite impressive demonstrations, most meta-optical imaging systems suffer from strong chromatic aberrations, limiting their utilities. Here, we employ inverse-design to create broadband meta-optics operating in the long-wave infrared (LWIR) regime (8 - 12 $\mu$m). Via a deep-learning assisted multi-scale differentiable framework that links meta-atoms to the phase, we maximize the wavelength-averaged volume under the modulation transfer function (MTF) of the meta-optics. Our design framework merges local phase-engineering via meta-atoms and global engineering of the scatterer within a single pipeline. We corroborate our design by fabricating and experimentally characterizing all-silicon LWIR meta-optics. Our engineered meta-optic is complemented by a simple computational backend that dramatically improves the quality of the captured image. We experimentally demonstrate a six-fold improvement of the wavelength-averaged Strehl ratio over the traditional hyperboloid metalens for broadband imaging., Comment: 28 pages, 12 figures

Telecommunications and polarimetry both require the active control of the polarization of light, Currently, this is done by combining intrinsically anisotropic materials with tunable isotropic materials into heterostructures using complicated fabrication techniques due to the lack of scalable materials that possess both properties. Tunable birefringent and dichromic materials are scarce and rarely available in high-quality thin films over wafer scales. In this paper, we report semiconducting, highly aligned, single-walled carbon nanotubes (SWCNTs) over 4" wafers with normalized birefringence and dichroism values 0.09 and 0.58, respectively. The real and imaginary parts of the refractive index of the SWCNT films are tuned by up to 5.9% and 14.3% in the infrared at 2200 nm and 1660 nm, respectively, using electrostatic doping. Our results suggest that aligned SWCNTs are among the most anisotropic and tunable optical materials known and opens new avenues for their application in integrated photonics and telecommunications.

Excitons, bound electron-hole pairs, in Two-Dimensional Hybrid Organic Inorganic Perovskites (2D HOIPs) are capable of forming hybrid light-matter states known as exciton-polaritons (E-Ps) when the excitonic medium is confined in an optical cavity. In the case of 2D HOIPs, they can self-hybridize into E-Ps at specific thicknesses of the HOIP crystals that form a resonant optical cavity with the excitons. However, the fundamental properties of these self-hybridized E-Ps in 2D HOIPs, including their role in ultrafast energy and/or charge transfer at interfaces, remain unclear. Here, we demonstrate that > 0.5 um thick 2D HOIP crystals on Au substrates are capable of supporting multiple-orders of self-hybridized E-P modes. These E-Ps have high Q factors (> 100) and modulate the optical dispersion for the crystal to enhance sub-gap absorption and emission. Through varying excitation energy and ultrafast measurements, we also confirm energy transfer from higher energy upper E-Ps to lower energy, lower E-Ps. Finally, we also demonstrate that E-Ps are capable of charge transport and transfer at interfaces. Our findings provide new insights into charge and energy transfer in E-Ps opening new opportunities towards their manipulation for polaritonic devices., Comment: 5 figures plus supporting information

Metamaterials and metasurfaces operating in the visible and near-infrared (NIR) offer a promising route towards next-generation photodetectors and devices for solar energy harvesting. While numerous metamaterials and metasurfaces using metals and semiconductors have been demonstrated, semimetals-based metasurfaces in the vis-NIR range are notably missing. Here, we experimentally demonstrate a broadband metasurface superabsorber based on large area, semimetallic, van der Waals PtSe2 thin films in agreement with electromagnetic simulations. Our results show that PtSe2 is an ultrathin and scalable semimetal that concurrently possesses high index and high extinction across the vis-NIR range. Consequently, the thin-film PtSe2 on a reflector separated by a dielectric spacer can absorb > 85 % for the unpatterned case and ~97 % for the optimized 2D metasurface in the 400-900 nm range making it one of the strongest and thinnest broadband perfect absorbers to date. Our results present a scalable approach to photodetection and solar energy harvesting, demonstrating the practical utility of high index, high extinction semimetals for nanoscale optics.

Two-dimensional chalcogenide semiconductors have recently emerged as a host material for quantum emitters of single photons. While several reports on defect and strain-induced single photon emission from 2D chalcogenides exist, a bottom-up, lithography-free approach to producing a high density of emitters remains elusive. Further, the physical properties of quantum emission in the case of strained 2D semiconductors are far from being understood. Here, we demonstrate a bottom-up, scalable, and lithography-free approach to creating large areas of localized emitters with high density (~150 emitters/um2) in a WSe2 monolayer. We induce strain inside the WSe2 monolayer with high spatial density by conformally placing the WSe2 monolayer over a uniform array of Pt nanoparticles with a size of 10 nm. Cryogenic, time-resolved, and gate-tunable luminescence measurements combined with near-field luminescence spectroscopy suggest the formation of localized states in strained regions that emit single photons with a high spatial density. Our approach of using a metal nanoparticle array to generate a high density of strained quantum emitters opens a new path towards scalable, tunable, and versatile quantum light sources., Comment: 45 pages, 20 figures (5 main figures, 15 supporting figures)

The generation of rapidly tunable Optical Vortex (OV) beams is one of the most demanding research areas of the present era as they possess Orbital Angular Momentum (OAM) with additional degrees of freedom that can be exploited to enhance signal-carrying capacity by using mode division multiplexing and information encoding in optical communication. Particularly, rapidly tunable OAM devices at a fixed wavelength in the telecom band stir extensive interest among researchers for both classical and quantum applications. This article demonstrates the realistic design of a Si-integrated photonic device for rapidly tunable OAM wave generation at a 1550-nm wavelength by using an ultra-low-loss Phase Change Material (PCM) embedded with a Si-ring resonator with angular gratings. Different OAM modes are achieved by tuning the effective refractive index using rapid electrical switching of Sb2Se3 film from amorphous to crystalline states and vice versa. The generation of OAM waves relies on a traveling wave modulation of the refractive index of the micro-ring, which breaks the degeneracy of oppositely oriented whispering gallery modes. The proposed device is capable of producing rapidly tunable OV beams, carrying different OAM modes by using electrically controllable switching of ultra-low-loss PCM Sb2Se3., Comment: 13 Pages and 8 Figures

Chiral nanostructures offer the ability to respond to the vector nature of a light beam at the nanoscale. While naturally chiral materials offer a path towards scalability, engineered structures offer a path to wavelength tunability through geometric manipulation. Neither approach, however, allows for temporal control of chirality. Therefore, in the best of all worlds, it is crucial to realize chiral materials that possess the quality of scalability, tailored wavelength response, and dynamic control at high speeds. Here, a new class of intrinsically chiral phase change nanomaterials (PCNMs) is proposed and explored, based on a scalable bottom-up fabrication technique with a high degree of control in three dimensions. Angular resolved Mueller Matrix and spectroscopic ellipsometry are performed to characterize the optical birefringence and dichroism, and a numerical model is provided to explain the origin of optical activity. This work achieves the critical goal of demonstrating high-speed dynamic switching of chirality over 50,000 cycles via the underlying PCNM., Comment: 21 pages, 10 page supplement, 16 figures

Monolayer transition metal dichalcogenide (TMD) semiconductors such as MoSe$_2$ host strongly bound excitons which are known to exhibit a strong resonant third-order nonlinear response. Although there have been numerous studies of the ultrafast nonlinear response of monolayer TMDs, a study of the steady-state nonlinear response is lacking. We report a comprehensive study of the steady-state two-color nonlinear response of excitons in hBN-encapsulated monolayer MoSe$_2$ at 7 K. We observe differential transmission (DT) signals associated with the neutral and charged exciton species, which is strongly dependent on the polarization of the pump and probe. Our results are compared to a theoretical model based on a T-matrix formulation for exciton-exciton, exciton-trion, and trion-trion correlations. The parameters are chosen such that the theory accurately reproduces the experimental DT spectrum, which is found to be dominated by two-exciton correlations without strong biexciton binding, exciton-trion attractive interactions, and strong spin mixing through incoherent relaxation.

Light-matter coupling in excitonic materials has been the subject of intense investigation due to emergence of new excitonic materials. Two-dimensional layered hybrid organic/inorganic perovskites (2D HOIPs) support strongly bound excitons at room-temperatures with some of the highest oscillator strengths and electric loss tangents among the known excitonic materials. Here, we report strong light-matter coupling in Ruddlesden-Popper phase 2D-HOIPs crystals without the necessity of an external cavity. We report concurrent occurrence of multiple-orders of hybrid light-matter states via both reflectance and luminescence spectroscopy in thick (> 100 nm) crystals and near-unity absorption in thin (< 20 nm) crystals. We observe resonances with quality factors > 250 in hybridized exciton-polaritons and identify a linear correlation between exciton-polariton mode splitting and extinction coefficient of the various 2D-HOIPs. Our work opens the door to studying polariton dynamics in self-hybridized and open cavity systems with broad applications in optoelectronics and photochemistry.

High-speed electrical switching of Ge2Sb2Te5 (GST) remains a challenging task due to the large impedance mismatch between the low-conductivity amorphous state and the high-conductivity crystalline state. In this letter, we demonstrate an effective doping scheme using nickel to reduce the resistivity contrast between the amorphous and crystalline states by nearly three orders of magnitude. Most importantly, our results show that doping produces the desired electrical performance without adversely affecting the film's optical properties. The nickel doping level is approximately 2% and the lattice structure remains nearly unchanged when compared with undoped-GST. The refractive indices at amorphous and crystalline states were obtained using ellipsometry which echoes the results from XRD. The material's thermal transport properties are measured using time-domain thermoreflectance (TDTR), showing no change upon doping. The advantages of this doping system will open up new opportunities for designing electrically reconfigurable high speed optical elements in the near-infrared spectrum., Comment: 5 pages, 5 figures, 1 table

We develop a quantum master equation (QME) approach to investigate the electroluminesence (EL) of molecules confined between metallic electrodes and coupled to quantum plasmonic modes. Within our general state-based framework, we describe electronic tunneling, vibrational damping, environmental dephasing, and the quantum coherent dynamics of coupled quantum electromagnetic field modes. As an example, we calculate the STM-induced spontaneous emission of a tetraphenylporphyrin (TPP) molecule coupled to a nanocavity plasmon. In the weak molecular exciton-plasmon coupling regime we find excellent agreement with experiments, including above-threshold hot luminescence, an effect not described by previous semiclassical calculations. In the strong coupling regime, we analyze the spectral features indicative of the formation of plexcitonic states., Comment: 10 pages, 4 figures

Strong coupling is a phenomenon which occurs when the interaction between two resonance systems is so strong that the oscillatory energy exchange between them exceeds all dissipative loss channels. Each resonance can then no longer be described individually but only as a part of the coupled, hybrid system. Here, we show that strong coupling can occur in a deep subwavelength nanofilm supporting an epsilon near zero mode which is integrated into a metal-insulator-metal gap plasmon structure. To generate an epsilon near zero mode resonance in the short-wave infrared region, an indium tin oxide nanofilm of ~lambda/100 thickness is used. A polariton splitting value of 27%, corresponding to a normalized coupling rate of 0.135, is experimentally demonstrated. Simulations indicate that much larger coupling rates, well within the ultra-strong regime where the energy exchange rate is comparable with the frequency of light, are possible.