Floating-gate memristor based on a MoS2/h-BN/AuNPs mixed-dimensional heterostructure.

Memristors have recently received substantial attention because of their promising and unique emerging applications in neuromorphic computing, which can achieve gains in computation speed by mimicking the topology of the brain in electronic circuits. Traditional memristors made of bulk MoO3and HfO2, for example, suffer from a low switching ratio and poor durability and stability. In this work, a floating-gate memristor is developed based on a mixed-dimensional heterostructure comprising two-dimensional (2D) molybdenum disulfide (MoS2) and zero-dimensional (0D) Au nanoparticles (AuNPs) separated by an insulating hexagonal boron nitride (h-BN) layer (MoS2/h-BN/AuNPs). We find that under the modulation of back-gate voltages, the MoS2/h-BN/AuNPs device operates reliably between a high-resistance state (HRS) and a low-resistance state (LRS) and shows multiple stable LRS states, demonstrating the excellent potential of our memristor in multibit storage applications. The modulation effect can be attributed to electron quantum tunneling between the AuNP charge-trapping layer and the MoS2channel. Our memristor exhibits excellent durability and stability: the HRS and LRS are retained for more than 104s without obvious degradation and the on/off ratio is >104after more than 3000 switching cycles. We also demonstrate frequency-dependent memory properties upon stimulation with electrical and optical pulses.

Microcavity-enhanced Kerr nonlinearity in a vertical-external-cavity surface-emitting laser: erratum.

We correct a mistake in [Opt. Express27, 11914 (2019)10.1364/OE.27.011914] when calculating the focal length of the Kerr lens with the measured values of the nonlinear refractive index n2 and parameters of a prototypical self-mode-locking VECSEL cavity. We therefore update Fig. 1 of the original publication. The new calculation yields a significantly larger value of the Kerr lens focal length leading to a smaller perturbation of the cavity beam profile.

Nonlinear refraction in CH3NH3PbBr3 single crystals.

We measure both nonlinear absorption and nonlinear refraction in a ${{\rm CH}_3}{{\rm NH}_3}{{\rm PbBr}_3}$CH3NH3PbBr3 single crystal using the Z-scan technique with femtosecond laser pulses. At 1000 nm, we obtain values of 5.2 cm/GW and ${+}{9.5} \cdot {{10}^{ - 14}}\;{{\rm cm}^2}/{\rm W}$+9.5⋅10-14cm2/W for nonlinear absorption and nonlinear refraction, respectively. The sign and magnitude of the observed refractive nonlinearity are reproduced well by the two-band model. Our results suggest that the large nonlinear refractive index measured in perovskite nanostructures cannot be explained by an intrinsically high bound-electronic nonlinear refractive index in this emerging material class but is possibly caused by free carriers or quantum confinement effects.

Lead-Free Antimony Halide Perovskite with Heterovalent Mn2+ Doping.

Lead toxicity is hindering the applications of conventional lead halide perovskites (PVKs), and antimony (Sb) is a promising nontoxic Pb alternative, showing huge potential in optoelectronic devices. Herein, pure and Mn-doped Cs3Sb2Cl9 crystals are synthesized in a facile route and studied both experimentally and theoretically. All the pure and Mn-doped Cs3Sb2Cl9 crystals show good crystallinity and similar crystal structures, exhibiting visible photoluminescence (PL) characteristics with emission peaks at 422 and 613 nm, respectively. Combined density functional theory (DFT) calculations and experimental analyses reveal that the structure of the host PVK compound Cs3Sb2Cl9 is not influenced by the formation of [MnCl6]4- octahedra and that Mn 3d orbitals generate impurity states in the forbidden energy gap of Cs3Sb2Cl9. Therefore, energy transfer from Cs3Sb2Cl9 to Mn 3d states is observed, resulting in the d-d transition and bright red luminescence. Mn-doped Sb-based PVK can be utilized as a new platform for optoelectronic applications.

Microcavity-enhanced Kerr nonlinearity in a vertical-external-cavity surface-emitting laser.

Self-mode-locking has become an emerging path to the generation of ultrashort pulses with vertical-external-cavity surface-emitting lasers. In our work, a strong Kerr nonlinearity that is so far assumed to give rise to mode-locked operation is evidenced and a strong nonlinearity enhancement by the microcavity is revealed. We present wavelength-dependent measurements of the nonlinear absorption and nonlinear refractive index change in a gain chip using the Z-scan technique. We report negative nonlinear refraction up to 5x10-12 cm2/W in magnitude in the (InGa)As/Ga(AsP) material system close to the laser design wavelength, which can lead to Kerr lensing. We show that by changing the angle of incidence of the probe beam with respect to the gain chip, the Kerr nonlinearity can be wavelength-tuned, shifting with the microcavity resonance. Such findings may ultimately lead to novel concepts with regard to tailored self-mode-locking behavior achievable by peculiar Kerr-lens chip designs for cost-effective, robust and compact fs-pulsed semiconductor lasers.

Shedding light on exciton's nature in monolayer quantum material by optical dispersion measurements.

Strong light-matter interactions based on two-dimensional excitons formed in quantum materials such as monolayer transition-metal dichalcogenides have become a major subject of research in recent years. Particularly attractive is the extraordinarily large oscillator strength as well as binding energy of the excitonic quasiparticles in these atomically-thin crystal lattices. Numerous theoretical studies and experiments have been devoted to the exploration of the excitonic systems that could be exploited in future nano-scaled optoelectronic devices. To obtain unique insight into the exciton's characteristics in an archetype monolayer quantum material, we directly measure the quasiparticle energy-momentum dispersion for the first time optically. Our results for h-BN encapsulated single-layer WSe2 clearly indicate an emission regime with a dispersion in the meV range in within the light cone at cryogenic temperatures. The amount of dispersion agrees well with calculations for an exciton-polariton based on the material's monolayer exciton, or energetic modifications caused by exciton exchange interactions predicted for this material family. The measurable dispersion slightly weakens for elevated excitation densities, whereas at elevated temperatures, it even becomes immeasurable. The obtained reduction in dispersion is attributed to an enhanced role of uncorrelated charge carriers as well as the formation of phonon sidebands above 100 K.

Two-chip power-scalable THz-generating semiconductor disk laser.

We demonstrate a compact two-chip terahertz-emitting vertical-external-cavity surface-emitting laser source, which provides 1 THz output based on intracavity frequency conversion of dual-wavelength emission in a periodically poled lithium niobate crystal. The type-I frequency conversion scheme at room temperature highly benefits from the power-scaling possibilities in a multi-chip cavity with intracavity powers in excess of 500 W.

An electrically pumped polariton laser.

Conventional semiconductor laser emission relies on stimulated emission of photons, which sets stringent requirements on the minimum amount of energy necessary for its operation. In comparison, exciton-polaritons in strongly coupled quantum well microcavities can undergo stimulated scattering that promises more energy-efficient generation of coherent light by 'polariton lasers'. Polariton laser operation has been demonstrated in optically pumped semiconductor microcavities at temperatures up to room temperature, and such lasers can outperform their weak-coupling counterparts in that they have a lower threshold density. Even though polariton diodes have been realized, electrically pumped polariton laser operation, which is essential for practical applications, has not been achieved until now. Here we present an electrically pumped polariton laser based on a microcavity containing multiple quantum wells. To prove polariton laser emission unambiguously, we apply a magnetic field and probe the hybrid light-matter nature of the polaritons. Our results represent an important step towards the practical implementation of polaritonic light sources and electrically injected condensates, and can be extended to room-temperature operation using wide-bandgap materials.

Characterization of an abnormal photoluminescence behavior upon crystal-phase transition of perovskite CH3NH3PbI3.

Solution-processed hybrid perovskite of CH3NH3PbI3 (MAPbI3) exhibits an abnormal luminescence behavior at around the tetragonal-orthorhombic phase transition temperature. The combination of time resolved photoluminescence (PL), variable excitation power PL, and variable-temperature X-ray diffraction (XRD) allows us to clearly interpret the abnormal luminescence features in the phase transition region of MAPbI3. Both PL and XRD results unambiguously prove the coexistence of the tetragonal and orthorhombic phases of MAPbI3 in the temperature range of 150 to 130 K. The two luminescence features observed in the orthorhombic phase at T < 130 K originate from free excitons and donor-acceptor-pair (DAP) transitions, respectively. The comprehensive understanding of optical properties upon phase transition in MAPbI3 will benefit the development of new optoelectronic devices.

Self-mode-locking semiconductor disk laser.

The development of mode-locked semiconductor disk lasers received striking attention in the last 14 years and there is still a vast potential of such pulsed lasers to be explored and exploited. While for more than one decade pulsed operation was strongly linked to the employment of a saturable absorber, self-mode-locking emerged recently as an effective and novel technique in this field - giving prospect to a reduced complexity and improved cost-efficiency of such lasers. In this work, we highlight recent achievements regarding self-mode-locked semiconductor devices. It is worth to note, that although nonlinear effects in the active medium are expected to give rise to self-mode-locking, this has to be investigated with care in future experiments. However, there is a controversy whether results presented with respect to self-mode-locking truly show mode-locking. Such concerns are addressed in this work and we provide a clear evidence of mode-locking in a saturable-absorber-free device. By using a BBO crystal outside the cavity, green light originating from second-harmonic generation using the out-coupled laser beam is demonstrated. In addition, long-time-span pulse trains as well as radiofrequency-spectra measurements are presented for our sub-ps pulses at 500 MHz repetition rate which indicate the stable pulse operation of our device. Furthermore, a long-time-span autocorrelation trace is introduced which clearly shows absence of a pedestal or double pulses. Eventually, a beam-profile measurement reveals the excellent beam quality of our device with an M-square factor of less than 1.1 for both axes, showing that self-mode-locking can be achieved for the fundamental transverse mode.

A 23-watt single-frequency vertical-external-cavity surface-emitting laser.

We report on a single-frequency semiconductor disk laser which generates 23.6 W output power in continuous wave operation, at a wavelength of 1013 nm. The high output power is a result of optimizing the chip design, thermal management and the cavity configuration. By applying passive stabilization techniques, the free-running linewidth is measured to be 407 kHz for a sampling time of 1 ms, while undercutting 100 kHz in the microsecond domain.

Self-mode-locked quantum-dot vertical-external-cavity surface-emitting laser.

We present the first self-mode-locked optically pumped quantum-dot semiconductor disk laser. Our mode-locked device emits sub-picosecond pulses at a wavelength of 1040 nm and features a record peak power of 460 W at a repetition rate of 1.5 GHz. In this work, we also investigate the temperature dependence of the pulse duration as well as the time-bandwidth product for stable mode locking.

From polariton condensates to highly photonic quantum degenerate states of bosonic matter.

Bose-Einstein condensation (BEC) is a thermodynamic phase transition of an interacting Bose gas. Its key signatures are remarkable quantum effects like superfluidity and a phonon-like Bogoliubov excitation spectrum, which have been verified for atomic BECs. In the solid state, BEC of exciton-polaritons has been reported. Polaritons are strongly coupled light-matter quasiparticles in semiconductor microcavities and composite bosons. However, they are subject to dephasing and decay and need external pumping to reach a steady state. Accordingly the polariton BEC is a nonequilibrium process of a degenerate polariton gas in self-equilibrium, but out of equilibrium with the baths it is coupled to and therefore deviates from the thermodynamic phase transition seen in atomic BECs. Here we show that key signatures of BEC can even be observed without fulfilling the self-equilibrium condition in a highly photonic quantum degenerate nonequilibrium system.

Enhancement of Interlayer Exciton Emission in a TMDC Heterostructure via a Multi-Resonant Chirped Microresonator Upto Room Temperature.

We report on multi-resonance chirped distributed Bragg reflector (DBR) microcavities. These systems are employed to investigate the light-mater interaction with both intra- and inter-layer excitons of transition metal dichalcogenide (TMDC) bilayer heterostructures. The chirped DBRs consisting of SiO2 and Si3N4 layers of gradually varying thickness exhibit a broad stopband with a width exceeding 600 nm. Importantly, the structures provide multiple resonances across a broad spectral range, which can be matched to resonances of the embedded TMDC heterostructures. Studying cavity-coupled emission of both intra- and inter-layer excitons from an integrated WSe2/MoSe2 heterostructure in a chirped microcavity system, an enhanced interlayer exciton emission with a Purcell factor of 6.67 ± 1.02 at 4 K is observed. The cavity-enhanced emission of the interlayer exciton is used to investigate its temperature-dependent luminescence lifetime of 60 ps at room temperature. The cavity system modestly suppresses intralayer exciton emission by intentional detuning, thereby promoting a higher IX population and enhancing cavity-coupled interlayer exciton emission. This approach provides an intriguing platform for future studies of energetically distant and confined excitons in different semiconducting materials, which paves the way for various applications such as microlasers and single-photon sources by enabling precise emission control and utilizing multimode resonance light-matter interaction.

Evolution of multi-mode operation in vertical-external-cavity surface-emitting lasers.

The longitudinal multi-mode emission in a vertical-external-cavity surface-emitting laser is investigated using both single shot streak camera measurements and interferometric measurement techniques. For this, the laser is operated in the single- and two-color emission regime using both an etalon and a free-running configuration without etalon, respectively. The laser emission is analyzed with respect to pump power and output coupling losses for a long and for a short resonator. We observe a steep increase of emission bandwidth close to the laser threshold and monitor the transition between longitudinal single- and multi-mode operation. Additionally, the results indicate that a stable two-color operation is related to a sufficiently high number of oscillating longitudinal modes within each color.

Near-IR Light-Tunable Omnidirectional Broadband Terahertz Wave Antireflection Based on a PEDOT:PSS/Graphene Hybrid Coating.

Omnidirectional broadband terahertz (THz) antireflection (AR) with an actively configurable coating promises the achievement of next-generation efficient and versatile THz components with high performance. We demonstrate a near-infrared (NIR) light-tunable and omnidirectional broadband THz AR coating based on an impedance matching method and composed of a poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS)/graphene composite film. The omnidirectional broadband properties of the active AR coating can be efficiently achieved by tunable NIR optical excitation of less than 0.27 W·cm-2, which exhibits omnidirectional suppression of THz-wave reflection for incidence angles from 0 to 70°, concerning the broadband frequency range of 0.1-3.0 THz, with an ultrafast response time of ∼5 ps. Furthermore, we demonstrate that the active AR coating can improve the performance of a reflectance-tunable THz-wave polarization reflector by the elimination of Fabry-Pérot interference. The NIR irradiance-dependent active AR mechanism of the hybrid system is investigated, which demonstrates the essential role of the PEDOT:PSS/graphene layers in promoting the charge separation at the interface and therefore changing the photoconductivity of the composite film to achieve impedance matching under optical excitation. Several crucial advantages of the proposed and proven concept, including the wide-angle range, broad spectral range, flexible tunability, and easier fabrication, may revolutionize the AR strategy at THz frequencies for a wide range of THz applications.

Radiative pattern of intralayer and interlayer excitons in two-dimensional WS2/WSe2 heterostructure.

Two-dimensional (2D) heterostructures (HS) formed by transition-metal dichalcogenide (TMDC) monolayers offer a unique platform for the study of intralayer and interlayer excitons as well as moiré-pattern-induced features. Particularly, the dipolar charge-transfer exciton comprising an electron and a hole, which are confined to separate layers of 2D semiconductors and Coulomb-bound across the heterojunction interface, has drawn considerable attention in the research community. On the one hand, it bears significance for optoelectronic devices, e.g. in terms of charge carrier extraction from photovoltaic devices. On the other hand, its spatially indirect nature and correspondingly high longevity among excitons as well as its out-of-plane dipole orientation render it attractive for excitonic Bose-Einstein condensation studies, which address collective coherence effects, and for photonic integration schemes with TMDCs. Here, we demonstrate the interlayer excitons' out-of-plane dipole orientation through angle-resolved spectroscopy of the HS photoluminescence at cryogenic temperatures, employing a tungsten-based TMDC HS. Within the measurable light cone, the directly-obtained radiation profile of this species clearly resembles that of an in-plane emitter which deviates from that of the intralayer bright excitons as well as the other excitonic HS features recently attributed to artificial superlattices formed by moiré patterns.

Continuously-tunable light-matter coupling in optical microcavities with 2D semiconductors.

A theoretical variation between the two distinct light-matter coupling regimes, namely weak and strong coupling, becomes uniquely feasible in open optical Fabry-Pérot microcavities with low mode volume, as discussed here. In combination with monolayers of transition-metal dichalcogenides (TMDCs) such as WS2, which exhibits a large exciton oscillator strength and binding energy, the room-temperature observation of hybrid bosonic quasiparticles, referred to as exciton-polaritons and characterized by a Rabi splitting, comes into reach. In this context, our simulations using the transfer-matrix method show how to tailor and alter the coupling strength actively by varying the relative field strength at the excitons' position - exploiting a tunable cavity length, a transparent PMMA spacer layer and angle-dependencies of optical resonances. Continuously tunable coupling for future experiments is hereby proposed, capable of real-time adjustable Rabi splitting as well as switching between the two coupling regimes. Being nearly independent of the chosen material, the suggested structure could also be used in the context of light-matter-coupling experiments with quantum dots, molecules or quantum wells. While the adjustable polariton energy levels could be utilized for polariton-chemistry or optical sensing, cavities that allow working at the exceptional point promise the exploration of topological properties of that point.

Direct Measurement of the Radiative Pattern of Bright and Dark Excitons and Exciton Complexes in Encapsulated Tungsten Diselenide.

The optical properties of particularly the tungsten-based transition-metal dichalcogenides are strongly influenced by the presence of dark excitons. Recently, theoretical predictions as well as indirect experimental insights have shown that two different dark excitons exist within the light cone. While one is completely dark, the other one is only dipole forbidden out-of-plane, hence referred to as grey exciton. Here, we present angle-resolved spectroscopic data of a high-quality hexagonal-BN-encapsulated WSe2 monolayer with which we directly obtain the radiation pattern of this grey exciton that deviates from that of the bright exciton and other exciton complexes obtained at cryogenic temperatures.

Enhancement of the Monolayer Tungsten Disulfide Exciton Photoluminescence with a Two-Dimensional Material/Air/Gallium Phosphide In-Plane Microcavity.

Light-matter interactions with two-dimensional materials gained significant attention in recent years, leading to the reporting of weak and strong coupling regimes and effective nanolaser operation with various structures. Particularly, future applications involving monolayer materials in waveguide-coupled on-chip-integrated circuitry and valleytronic nanophotonics require controlling, directing, and optimizing photoluminescence. In this context, photoluminescence enhancement from monolayer transition-metal dichalcogenides on patterned semiconducting substrates becomes attractive. It is demonstrated in our work using focused-ion-beam-etched GaP and monolayer WS2 suspended on hexagonal boron nitride buffer sheets. We present an optical microcavity approach capable of efficient in-plane and out-of-plane confinement of light, which results in a WS2 photoluminescence enhancement by a factor of 10 compared to that of the unstructured substrate at room temperature. The key concept is the combination of interference effects in both the horizontal direction using a bull's-eye-shaped circular Bragg grating and in the vertical direction by means of a multiple-reflection model with optimized etch depth of circular air-GaP structures for maximum constructive interference effects of the applied pump and expected emission light.