Qiuyu Shang

Surface Plasmon Enhanced Strong Exciton–Photon Coupling in Hybrid Inorganic–Organic Perovskite Nanowires

Manipulating strong light-matter interaction in semiconductor microcavities is crucial for developing high-performance exciton polariton devices with great potential in next-generation all-solid state quantum technologies. In this work, we report surface plasmon enhanced strong exciton-photon interaction in CH3NH3PbBr3 perovskite nanowires. Characteristic anticrossing behaviors, indicating a Rabi splitting energy up to ∼564 meV, are observed near exciton resonance in hybrid perovskite nanowire/SiO2/Ag cavity at room temperature. The exciton-photon coupling strength is enhanced by ∼35% on average, which is mainly attributed to surface plasmon induced localized excitation field redistribution. Further, systematic studies on SiO2 thickness and nanowire dimension dependence of exciton-photon interaction are presented. These results provide new avenues to achieve extremely high coupling strengths and push forward the development of electrically pumped and ultralow threshold small lasers.

Fabry-Pérot Oscillation and Room Temperature Lasing in Perovskite Cube-Corner Pyramid Cavities

Recently, organometal halide perovskite-based optoelectronics, particularly lasers, have attracted intensive attentions because of its outstanding spectral coherence, low threshold, and wideband tunability. In this work, high-quality CH3 NH3 PbBr3 single crystals with a unique shape of cube-corner pyramids are synthesized on mica substrates using chemical vapor deposition method. These micropyramids naturally form cube-corner cavities, which are eminent candidates for small-sized resonators and retroreflectors. The as-grown perovskites show strong emission ≈530 nm in the vertical direction at room temperature. A special Fabry-Pérot (F-P) mode is employed to interpret the light confinement in the cavity. Lasing from the perovskite pyramids is observed from 80 to 200 K, with threshold ranging from ≈92 µJ cm-2 to 2.2 mJ cm-2 , yielding a characteristic temperature of T0 = 35 K. By coating a thin layer of Ag film, the threshold is reduced from ≈92 to 26 µJ cm-2 , which is accompanied by room temperature lasing with a threshold of ≈75 µJ cm-2 . This work advocates the prospect of shape-engineered perovskite crystals toward developing micro-sized optoelectronic devices and potentially investigating light-matter coupling in quantum optics.

Controlled Gas Molecules Doping of Monolayer MoS2 via Atomic-Layer-Deposited Al2O3 Films

MoS2 as atomically thin semiconductor is highly sensitive to ambient atmosphere (e.g., oxygen, moisture, etc.) in optical and electrical properties. Here we report a controlled gas molecules doping of monolayer MoS2 via atomic-layer-deposited Al2O3 films. The deposited Al2O3 films, in the shape of nanospheres, can effectively control the contact areas between ambient atmosphere and MoS2 that allows precise modulation of gas molecules doping. By analyzing photoluminescence (PL) emission spectra of MoS2 with different thickness of Al2O3, the doped carrier concentration is estimated at ∼2.7 × 1013 cm-2 based on the mass action model. Moreover, time-dependent PL measurements indicate an incremental stability of single layer MoS2 as the thicknesses of Al2O3 capping layer increase. Effective control of gas molecules doping in monolayer MoS2 provides us a valuable insight into the applications of MoS2 based optical and electrical devices.

Ultrafast Charge Transfer in Perovskite Nanowire/2D Transition Metal Dichalcogenide Heterostructures

Mixed-dimensional van der Waals (vdW) heterostructures between one-dimensional (1D) perovskite nanowires and two-dimensional (2D) transition metal dichalcogenides (TMDCs) hold great potential for novel optoelectronics and light-harvesting applications. However, the ultrafast carrier dynamics between the 1D perovskite nanowires and 2D TMDCs are currently not well understood, which is critical for related optoelectronic applications. Here we demonstrate vdW heterostructures of CsPbBr3 nanowire/monolayer MoS2 and CsPbBr3 nanowire/monolayer WSe2 and further present systematic investigations on their charge transfer dynamics. We show that CsPbBr3/MoS2 and CsPbBr3/WSe2 are type-I and type-II heterostructures, respectively. Both electrons and holes transfer from CsPbBr3 to MoS2 with an efficiency of 71%. As a contrast, holes transfer from CsPbBr3 to WSe2 with a carrier transfer efficiency of 70% and electrons transfer inversely within 7 ps. The ultrafast and efficient charge transfer in the 1D/2D perovskite-TMDC heterostructures suggest great promise in light emission, photodetector, and photovoltaic devices.

Ultrathin CsPbX3 Nanowire Arrays with Strong Emission Anisotropy

1D nanowires of all-inorganic lead halide perovskites represent a good architecture for the development of polarization-sensitive optoelectronic devices due to their high absorption efficient, emission yield, and dielectric constants. However, among as-fabricated perovskite nanowires with the lateral dimensions of hundreds nanometers so far, the optical anisotropy is hindered and rarely explored owing to the invalidating of electrostatic dielectric mismatch in the physical dimensions. Here, well-aligned CsPbBr3 and CsPbCl3 nanowires with thickness T down to 15 and 7 nm, respectively, are synthesized using a vapor phase van der Waals epitaxial method. Strong emission anisotropy with polarization ratio up to ≈0.78 is demonstrated in the nanowires with T < 40 nm due to the electrostatic dielectric confinement. With the increasing of thickness, the polarization ratio remarkably reduces monotonously to ≈0.17 until T ≈140 nm; and further oscillates in a small amplitude owing to the wave characteristic of light. These findings not only represent a demonstration of perovskite-based polarization-sensitive light sources, but also advance fundamental understanding of their polarization properties of perovskite nanowires.

Low Threshold Fabry-Pérot Mode Lasing from Lead Iodide Trapezoidal Nanoplatelets

Lead Iodide (PbI2 ) is a layered semiconductor with direct band gap holding great promises in green light emission and detection devices. Recently, PbI2 planar lasers are demonstrated using hexagonal whispering-gallery-mode microcavities, but the lasing threshold is quite high. In this work, lasing from vapor phase deposition derived PbI2 trapezoidal nanoplatelets (NPs) with threshold that is at least an order of magnitude lower than the previous value is reported. The growth mechanism of the trapezoidal NPs is explored and attributed to the synergistic effects of van der Waals interactions and lattice mismatching. The lasing is enabled by the population inversion of n = 1 excitons and the optical feedback is provided by the Fabry-Pérot oscillation between the side facets of trapezoidal NPs. The findings not only advance the understanding of growth and photophysics mechanism of PbI2 nanostructures but also provide ideas to develop low threshold ultrathin lasers.

High-Temperature Continuous-Wave Pumped Lasing from Large-Area Monolayer Semiconductors Grown by Chemical Vapor Deposition

The realization of low-energy-consumption lasers based on atomically thin two-dimensional (2D) transition metal dichalcogenides (TMDCs) is crucial for the development of optical communications, flexible displays, and lasers on the chip level. However, among the as-demonstrated TMDC-based lasers so far, the gain materials are mainly achieved by a mechanical exfoliation approach accompanied by poor reproducibility and controllability. In this work, we report a controllable design for generating large-scale lasing from chemical vapor deposition (CVD)-derived high-quality monolayer MoS2 film. Strong continuous-wave optically driven whispering-gallery-mode lasing is achieved in a wide temperature range from 77 to 400 K. The eminent lasing performances result from the strong spatial confinement of carriers and the enhanced efficiency of spontaneous emission owing to the lensing and screening effects of silica microsphere cavities. These findings not only advance the fundamental understanding of 2D lasing effects but also provide solutions to fabricate low-cost, scalable, and integratable TMDC-based lasers.