Optical interference effect in the hybrid quantum dots/two-dimensional materials: photoluminescence enhancement and modulation.

The optical interference effect originating from the multiple reflections between the two-dimensional (2D) materials and the substrates has been used to dramatically enhance their Raman signal. However, this effect in the hybrid structures of colloidal quantum dots (QD) coupled to 2D materials is always overlooked. Here we theoretically prove that the photoluminescence (PL) intensities of the QD films in the QD-2D hybrid structures can be strongly enhanced and modulated by the optical interference effect between QD and 2D interfaces, breaking the inherent standpoint that PL intensities of the QD films are always prominently quenched in these hybrid structures. The theoretical predictions have been well confirmed by experimental measurements of PL properties of CdSe/ZnS and CdSeTe/ZnS QD on different 2D materials (such as WSe2, MoS2, and h-BN). PL intensities of these QD films have been periodically modulated from almost disappearing to strong enhancement (with the enhancement of about 6 times). The optical interference effect uncovered in this work enables a powerful method to manipulate the PL property of the QD films in the different QD-2D hybrid structures. These results can boost the optical performance of the QD-based electronic and optoelectronic devices in the hybrid QD-2D structures.

Criteria for Assessing the Interlayer Coupling of van der Waals Heterostructures Using Ultrafast Pump-Probe Photoluminescence Spectroscopy.

van der Waals (vdW) heterostructures of transition metal dichalcogenides (TMDCs) provide an excellent paradigm for next-generation electronic and optoelectronic applications. However, the reproducible fabrications of vdW heterostructure devices and the boosting of practical applications are severely hindered by their unstable performance, due to the lack of criteria to assess the interlayer coupling in heterostructures. Here we propose a physical model involving ultrafast electron transfer in the heterostructures and provide two criteria, η (the ratio of the transferred electrons to the total excited electrons) and ζ (the relative photoluminescence variation), to evaluate the interlayer coupling by considering the electron transfer in TMDC heterostructures and numerically simulating the corresponding rate equations. We have proved the effectiveness and robustness of two criteria by measuring the pump-probe photoluminescence intensity of monolayer WS2 in the WS2/WSe2 heterostructures. During thermal annealing of WS2/WSe2, ζ varies from negative to positive values and η changes between 0 and 4.5 × 10-3 as the coupling strength enhanced; both of them can well characterize the tuning of interlayer coupling. We also design a scheme to image the interlayer coupling by performing PL imaging at two time delays. Our scheme offers powerful criteria to assess the interlayer coupling in TMDC heterostructures, offering opportunities for the implementation of vdW heterostructures for broadband and high-performance electronic and optoelectronic applications.

Exploration of exciton dynamics in GaTe nanoflakes via temperature- and power-dependent time-resolved photoluminescence spectra.

GaTe nanoflakes have been receiving much research attention recently due to their applications in optoelectronic devices, such as anisotropic non-volatile memory, solar cells, and high-sensitivity photodetectors from the ultraviolet to the visible region. Further applications, however, have been impeded due to the limited understanding of their exciton dynamics. In this work we perform temperature- and power-dependent time-resolved photoluminescence (PL) spectra to comprehensively investigate the exciton dynamics of GaTe nanoflakes. Temperature-dependent PL measurements manifest that spectral profiles of GaTe nanoflakes change dramatically from cryogenic to room temperature, where the bound exciton and donor-to-acceptor pair transition normally disappear above 100 K, while the charged exciton survives to room temperature. The lifetimes of these excitons and their evolution vs temperature have been uncovered by time-resolved PL spectra. Further measurements reveal the entirely different power-dependent exciton behaviors of GaTe nanoflakes between room and cryogenic temperatures. The underlying mechanisms have been proposed to explore the sophisticated exciton dynamics within GaTe nanoflakes. Our results offer a more thorough understanding of the exciton dynamics of GaTe nanoflakes, enabling further progress in engineering GaTe-based applications, such as photodetectors, light-emitting diodes, and nanoelectronics.

Photostable fluorescent molecules on layered hexagonal boron nitride: Ideal single-photon sources at room temperature.

Photoblinking and photobleaching are commonly encountered problems for single-photon sources. Numerous methods have been devised to suppress these two impediments; however, either the preparation procedures or the operating conditions are relatively harsh, making them difficult to apply to practical applications. Here, we reported giant suppression of both photoblinking and photobleaching of a single fluorescent molecule, terrylene, via the utilization of hexagonal boron nitride (h-BN) flakes as substrates. Experimentally, a much-prolonged survival time of terrylene has been determined, which can have a photostable emission over 2 h at room temperature under ambient atmospheres. Compared with single molecules on a SiO2/Si substrate or glass coverslip, a more than 100-fold increase in the total number of photons collected from each terrylene on h-BN flakes has been demonstrated. We also proved that the photostability of terrylene molecules can be well maintained for more than 6 months even under ambient conditions without any further protection. Our results demonstrate that the utilization of h-BN flakes to suppress photoblinking and photobleaching of fluorescent molecules has promising applications in the production of high-quality single-photon sources at room temperature.

Boost of single-photon emission by perfect coupling of InAs/GaAs quantum dot and micropillar cavity mode.

We proposed a precise calibration process of Al 0.9Ga0.1As/GaAs DBR micropillar cavity to match the single InAs/GaAs quantum dot (QD) exciton emission and achieve cavity mode resonance and a great enhancement of QD photoluminescence (PL) intensity. Light-matter interaction of single QD in DBR micropillar cavity (Q ∼ 3800) under weak coupling regime was investigated by temperature-tuned PL spectra; a pronounced enhancement (14.6-fold) of QD exciton emission was observed on resonance. The second-order autocorrelation measurement shows g(2)(0)=0.070, and the estimated net count rate before the first objective lens reaches 1.6×107 counts/s under continuous wave excitation, indicating highly pure single-photon emission at high count rates.