Engineering the Impact of Phonon Dephasing on the Coherence of a WSe_{2} Single-Photon Source via Cavity Quantum Electrodynamics.

Emitter dephasing is one of the key issues in the performance of solid-state single-photon sources. Among the various sources of dephasing, acoustic phonons play a central role in adding decoherence to the single-photon emission. Here, we demonstrate that it is possible to tune and engineer the coherence of photons emitted from a single WSe_{2} monolayer quantum dot via selectively coupling it to a spectral cavity resonance. We utilize an open cavity to demonstrate spectral enhancement, leveling, and suppression of the highly asymmetric phonon sideband, finding excellent agreement with a microscopic description of the exciton-phonon dephasing in a truly two-dimensional system. Moreover, the impact of cavity tuning on the dephasing is directly assessed via optical interferometry, which points out the capability to utilize light-matter coupling to steer and design dephasing and coherence of quantum emitters in atomically thin crystals.

Photoluminescence Enhancement of Monolayer WS2 by n-Doping with an Optically Excited Gold Disk.

In nanophotonics and quantum optics, we aim to control and manipulate light with tailored nanoscale structures. Hybrid systems of nanostructures and atomically thin materials are of interest here, as they offer rich physics and versatility due to the interaction between photons, plasmons, phonons, and excitons. In this study, we explore the optical and electronic properties of a hybrid system, a naturally n-doped monolayer WS2 covering a gold disk. We demonstrate that the nonresonant excitation of the gold disk in the high absorption regime efficiently generates hot carriers via localized surface plasmon excitation, which n-dope the monolayer WS2 and enhance the photoluminescence emission by regulating the multiexciton population and stabilizing the neutral exciton emission. The results are relevant to the further development of nanotransistors in photonic circuits and optoelectronic applications.

Monolayer-Based Single-Photon Source in a Liquid-Helium-Free Open Cavity Featuring 65% Brightness and Quantum Coherence.

Solid-state single-photon sources are central building blocks in quantum information processing. Atomically thin crystals have emerged as sources of nonclassical light; however, they perform below the state-of-the-art devices based on volume crystals. Here, we implement a bright single-photon source based on an atomically thin sheet of WSe2 coupled to a tunable optical cavity in a liquid-helium-free cryostat without the further need for active stabilization. Its performance is characterized by high single-photon purity (g(2)(0) = 4.7 ± 0.7%) and record-high, first-lens brightness of linearly polarized photons of 65 ± 4%, representing a decisive step toward real-world quantum applications. The high performance of our devices allows us to observe two-photon interference in a Hong-Ou-Mandel experiment with 2% visibility limited by the emitter coherence time and setup resolution. Our results thus demonstrate that the combination of the unique properties of two-dimensional materials and versatile open cavities emerges as an inspiring avenue for novel quantum optoelectronic devices.

Enhanced surface second harmonic generation in nanolaminates.

Second-harmonic generation (SHG) is a second-order nonlinear optical process that is not allowed in media with inversion symmetry. However, due to the broken symmetry at the surface, surface SHG still occurs, but is generally weak. We experimentally investigate the surface SHG in periodic stacks of alternating, subwavelength dielectric layers, which have a large number of surfaces, thus enhancing surface SHG considerably. To this end, multilayer stacks of SiO2/TiO2 were grown by Plasma Enhanced Atomic Layer Deposition (PEALD) on fused silica substrates. With this technique, individual layers of a thickness of less than 2 nm can be fabricated. We experimentally show that under large angles of incidence (> 20 degrees) there is substantial SHG, well beyond the level, which can be observed from simple interfaces. We perform this experiment for samples with different periods and thicknesses of SiO2/TiO2 and our results are in agreement with theoretical calculations.

Hybridized Exciton-Photon-Phonon States in a Transition Metal Dichalcogenide van der Waals Heterostructure Microcavity.

Excitons in atomically thin transition-metal dichalcogenides (TMDs) have been established as an attractive platform to explore polaritonic physics, owing to their enormous binding energies and giant oscillator strength. Basic spectral features of exciton polaritons in TMD microcavities, thus far, were conventionally explained via two-coupled-oscillator models. This ignores, however, the impact of phonons on the polariton energy structure. Here we establish and quantify the threefold coupling between excitons, cavity photons, and phonons. For this purpose, we employ energy-momentum-resolved photoluminescence and spatially resolved coherent two-dimensional spectroscopy to investigate the spectral properties of a high-quality-factor microcavity with an embedded WSe_{2} van der Waals heterostructure at room temperature. Our approach reveals a rich multibranch structure which thus far has not been captured in previous experiments. Simulation of the data reveals hybridized exciton-photon-phonon states, providing new physical insight into the exciton polariton system based on layered TMDs.

Nanostructure-modulated planar high spectral resolution spectro-polarimeter.

We present a planar spectro-polarimeter based on Fabry-Pérot cavities with embedded polarization-sensitive high-index nanostructures. A 7 µm-thick spectro-polarimetric system for 3 spectral bands and 2 linear polarization states is experimentally demonstrated. Furthermore, an optimal design is theoretically proposed, estimating that a system with a bandwidth of 127 nm and a spectral resolution of 1 nm is able to reconstruct the first three Stokes parameters with a signal-to-noise ratio of -13.14 dB with respect to the the shot noise limited SNR. The pixelated spectro-polarimetric system can be directly integrated on a sensor, thus enabling applicability in a variety of miniaturized optical devices, including but not limited to satellites for Earth observation.

Discrete dispersion scan setup for measuring few-cycle laser pulses in the mid-infrared.

In this work, we demonstrate a discrete dispersion scan scheme using a low number of flat windows to vary the dispersion of laser pulses in discrete steps. Monte Carlo simulations indicate that the pulse duration can be retrieved accurately with less than 10 dispersion steps, which we verify experimentally by measuring few-cycle pulses and material dispersion curves at 3 and 10 µm wavelength. This minimal measuring scheme using only five optical components without the need for linear positioners and interferometric alignment can be readily implemented in many wavelength ranges and situations.

Adaptive pre-amplification pulse shaping in a high-power, coherently combined fiber laser system.

We report on the successful implementation of an adaptive pre-amplification pulse shaping technique in a high-power, coherently combined fiber laser system to achieve sub-300-fs pulse durations at 320 W average power and 3.2 mJ pulse energy. The pulse shaper is utilized to impose a gain flattening mask to increase the spectral width of the amplified pulse by 60%. Simultaneously, it pre-compensates the spectral phase acquired in the multi-stage amplification and subsequent compression including the eight-channel, coherently combined main amplification stage. This result does significantly enhance the performance of the fiber laser system and the subsequent nonlinear compression stages.

Quantitative Investigation of Quantum Emitter Yield in Drop-Casted Hexagonal Boron Nitride Nanoflakes.

Single photon emitters (SPEs) are a key component for their use as pure photon source in quantum technologies. In this study, we investigate the generation of SPEs from drop-casted hexagonal boron nitride (hBN) nanoflakes, examining the influence of the immersion solution and the source of hBN. We show that, depending on the utilized supplier and solution, the number and quality of the emitters change. We perform a comprehensive optical characterization of the deposited nanoflakes to assess the quality of the generated SPEs. Importantly, we provide quantitative data on SPE yields, highlighting significant variations among solvents and different sources of hBN. We find that hBN from Merck drop-casted in acetone provided the best quality emitters with a g (2) < 0.1 and photoluminescence intensities above 300 kCounts/s. Their number of SPEs among all photon emitters was also the highest, with about 14%, rendering a total yield of about 1.25% of all drop-casted flakes. These numbers hold particular significance when evaluating drop-casting as a practical method for the generation of SPEs and their deposition and incorporation within existing nanophotonic systems. By choosing appropriate solvents and source materials' quality and yield of SPEs can be significantly increased, showcasing further optimization potential for the development of future quantum applications.

Organic Room-Temperature Polariton Condensate in a Higher-Order Topological Lattice.

Organic molecule exciton-polaritons in photonic lattices are a versatile platform to emulate unconventional phases of matter at ambient temperatures, including protected interface modes in topological insulators. Here, we investigate bosonic condensation in the most prototypical higher-order topological lattice: a 2D-version of the Su-Schrieffer-Heeger model. Under strong optical pumping, we observe bosonic condensation into both 0D and 1D topologically protected modes. The resulting 1D macroscopic quantum state reaches a coherent spatial extent of 10 µm, as evidenced by interferometric measurements of first order coherence. We account for the spatial mode patterns resulting from fluorescent protein-filled, structured microcavities by tight-binding calculations and theoretically characterize the topological invariants of the lattice. Our findings pave the way toward organic on-chip polaritonics using higher-order topology as a tool for the generation of robustly confined polaritonic lasing states.

A tunable transition metal dichalcogenide entangled photon-pair source.

Entangled photon-pair sources are at the core of quantum applications like quantum key distribution, sensing, and imaging. Operation in space-limited and adverse environments such as in satellite-based and mobile communication requires robust entanglement sources with minimal size and weight requirements. Here, we meet this challenge by realizing a cubic micrometer scale entangled photon-pair source in a 3R-stacked transition metal dichalcogenide crystal. Its crystal symmetry enables the generation of polarization-entangled Bell states without additional components and provides tunability by simple control of the pump polarization. Remarkably, generation rate and state tuning are decoupled, leading to equal generation efficiency and no loss of entanglement. Combining transition metal dichalcogenides with monolithic cavities and integrated photonic circuitry or using quasi-phasematching opens the gate towards ultrasmall and scalable quantum devices.

Imaging cross-correlation FROG: measuring ultrashort, complex, spatiotemporal fields.

We present imaging cross-correlation frequency-resolved optical gating (ImXFROG), a new method for the spatiotemporal phase retrieval of ultrashort pulses. It is demonstrated that ImXFROG can measure phase and intensity of arbitrary, spatiotemporally distorted pulses with femtosecond resolution and up to 10(7) independent variables. ImXFROG is implemented as a plug-in upgrade to an existing correlator and used to demonstrate the reconstruction of highly complex, optical pulses with femtosecond features and massive spatiotemporal distortion.

Precision Tailoring Quasi-BIC Resonance of a-Si:H Metasurfaces.

The capability of tailoring the resonance wavelength of metasurfaces is important as it can alleviate the manufacturing precision required to produce the exact structure according to the design of the nanoresonators. Tuning of Fano resonances by applying heat has been theoretically predicted in the case of silicon metasurfaces. Here, we experimentally demonstrate the permanent tailoring of quasi-bound states in the continuum (quasi-BIC) resonance wavelength in an a-Si:H metasurface and quantitatively analyze the modification in the Q-factor with gradual heating. A gradual increment in temperature leads to a spectral shift in the resonance wavelength. With the support of ellipsometry measurements, the spectral shift resulting from the short-duration (ten minutes) heating is identified to be due to refractive index variations in the material rather than a geometric effect or amorphous/polycrystalline phase transition. In the case of quasi-BIC modes in the near-infrared, resonance wavelength could be adjusted from T = 350 °C to T = 550 °C without affecting the Q-factor considerably. Apart from the temperature-induced resonance trimming, large Q-factors can be attained at the highest analyzed temperature (T = 700 °C) in the near-infrared quasi-BIC modes. Resonance tailoring is just one of the possible applications of our results. We expect that our study is also insightful in the design of a-Si:H metasurfaces where large Q-factors are required at high temperatures.

Approaching optimal entangling collective measurements on quantum computing platforms.

Entanglement is a fundamental feature of quantum mechanics and holds great promise for enhancing metrology and communications. Much of the focus of quantum metrology so far has been on generating highly entangled quantum states that offer better sensitivity, per resource, than what can be achieved classically. However, to reach the ultimate limits in multi-parameter quantum metrology and quantum information processing tasks, collective measurements, which generate entanglement between multiple copies of the quantum state, are necessary. Here, we experimentally demonstrate theoretically optimal single- and two-copy collective measurements for simultaneously estimating two non-commuting qubit rotations. This allows us to implement quantum-enhanced sensing, for which the metrological gain persists for high levels of decoherence, and to draw fundamental insights about the interpretation of the uncertainty principle. We implement our optimal measurements on superconducting, trapped-ion and photonic systems, providing an indication of how future quantum-enhanced sensing networks may look.

Bistability suppression and low threshold switching using frozen light at a degenerate band edge waveguide.

We predict that nonlinear waveguides which support frozen light associated with a degenerate photonic band edge, where the dispersion relation is locally quartic, exhibit a tunable, all-optical switching response. The thresholds for switching are orders-of-magnitude lower than at regular band edges. By adjusting the input condition, bistability can be eliminated, preventing switching hysteresis.

Optical limiting and spectral stabilization in segmented photonic lattices.

We propose photonic lattices with segmentation-based linear self imaging as integrated optical limiters. Starting from unity transmission in the linear regime, nonlinear delocalization leads to a continuous decrease of the overall transmission for increasing input powers. The diffractive propagation between input and output port offers the additional benefit of substantially decreased nonlinear spectral distortions. The functionality is demonstrated experimentally in a waveguide lattice realized in bulk fused silica with the femtosecond laser writing technique.

Digital holography from shadowgraphic phase estimates.

We show experimentally that the recently proposed iterative shadowgraphic method can be applied to in-line digital holography, provided a suitable regularization step is introduced. We show that the method correctly solves the "twin-image" problem using just two samples of the intensity field scattered by a phase object. Field retrieval accuracy is significantly improved when compared to a reconstruction obtained with the defocusing variation algorithms.

Temporal switching induced by cascaded third order nonlinearity.

We investigate the impact of cascaded third harmonic generation and the intrinsic n4 material nonlinearity on the propagation of ultrashort pulses in noble-gas filled Kagome fibers. We show that the pressure tunability of the cascade allows for the implementation of temporal switching. We also investigate the relative strengths of both effects and show their ratio to be pressure tunable.

Higher-order Kerr effect and harmonic cascading in gases.

The higher-order Kerr effect (HOKE) has recently been advocated to explain measurements of the saturation of the nonlinear refractive index in gases. Here we show that cascaded third-harmonic generation results in an effective fifth-order nonlinearity that is negative and significant. Higher-order harmonic cascading will also occur from the HOKE, and the cascading contributions may significantly modify the observed nonlinear index change. At lower wavelengths, cascading increases the HOKE saturation intensity, while for longer wavelengths cascading will decrease the HOKE saturation intensity.

Patterned Growth of Transition Metal Dichalcogenide Monolayers and Multilayers for Electronic and Optoelectronic Device Applications.

A simple, large area, and cost-effective soft lithographic method is presented for the patterned growth of high-quality 2D transition metal dichalcogenides (TMDs). Initially, a liquid precursor (Na2 MoO4 in an aqueous solution) is patterned on the growth substrate using the micromolding in capillaries technique. Subsequently, a chemical vapor deposition step is employed to convert the precursor patterns to monolayer, few layers, or bulk TMDs, depending on the precursor concentration. The grown patterns are characterized using optical microscopy, atomic force microscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy, and photoluminescence spectroscopy to reveal their morphological, chemical, and optical characteristics. Additionally, electronic and optoelectronic devices are realized using the patterned TMDs and tested for their applicability in field effect transistors and photodetectors. The photodetectors made of MoS2 line patterns show a very high responsivity of 7674 A W-1 and external quantum efficiency of 1.49 × 106 %. Furthermore, the multiple grain boundaries present in patterned TMDs enable the fabrication of memtransistor devices. The patterning technique presented here may be applied to many other TMDs and related heterostructures, potentially advancing the fabrication of TMDs-based device arrays.