Jia Shi

3R MoS2 with Broken Inversion Symmetry: A Promising Ultrathin Nonlinear Optical Device

Nonlinear 2D layered crystals provide ideal platforms for applications and fundamental studies in ultrathin nonlinear optical (NLO) devices. However, the NLO frequency conversion efficiency constrained by lattice symmetry is still limited by layer numbers of 2D crystals. In this work, 3R MoS2 with broken inversion symmetry structure are grown and proved to be excellent NLO 2D crystals from monolayer (0.65 nm) toward bulk-like (300 nm) dimension. Thickness and wavelength-dependent second harmonic generation spectra offer the selection rules of appropriate working conditions. A model comprising of bulk nonlinear contribution and interface interaction is proposed to interpret the observed nonlinear behavior. Polarization enhancement with two petals along staggered stacking direction appears in 3R MoS2 is first observed and the robust polarization of 3R MoS2 crystal is caused by the retained broken inversion symmetry. The results provide a new arena for realizing ultrathin NLO devices for 2D layered materials.

Electrically Configurable Graphene Field-Effect Transistors with a Graded-Potential Gate

A device architecture for electrically configurable graphene field-effect transistor (GFET) using a graded-potential gate is present. The gating scheme enables a linearly varying electric field that modulates the electronic structure of graphene and causes a continuous shift of the Dirac points along the channel of GFET. This spatially varying electrostatic modulation produces a pseudobandgap observed as a suppressed conductance of graphene within a controllable energy range. By tuning the electrical gradient of the gate, a GFET device is reversibly transformed between ambipolar and n- and p-type unipolar characteristics. We further demonstrate an electrically programmable complementary inverter, showing the extensibility of the proposed architecture in constructing logic devices based on graphene and other Dirac materials. The electrical configurable GFET might be explored for novel functionalities in smart electronics.

Strong Exciton–Photon Coupling and Lasing Behavior in All-Inorganic CsPbBr3 Micro/Nanowire Fabry-Pérot Cavity

Macroscopic spontaneous coherence of exciton-polariton in semiconductor cavity is one important research field in condensed matter physics. All-inorganic micro/nanowire Fabry-Perot cavity with excellent optical performance makes it possible to realize strong coupling and lasing of exciton-photon at room temperature. In this work, we demonstrated strong coupling of exciton-photon and polariton lasing in CsPbBr3 micro/nanowires synthesized by CVD method. By exploring spatial resolved PL spectra of CsPbBr3 cavity, we observed mode volume dependent coupling strength , as well as significant increase in group index. Moreover, low threshold polariton lasing was achieved at room temperature within strong coupling regime; the polariton characteristic is confirmed by comparing lasing spectra with waveguided output spectra and the dramatically reduced lasing threshold. Our present results provide new avenues to achieve high coupling strengths potentially enabling application of exciting phenomena such as Bose-Einstein condensation of polaritons, efficient light-emitting diodes and lasers.

Tuning Excitonic Properties of Monolayer MoS2 with Microsphere Cavity by High-Throughput Chemical Vapor Deposition Method

Tuning the optical properties of 2D direct bandgap semiconductors is crucial for applications in photonic light source, optical communication, and sensing. In this work, the excitonic properties of molybdenum disulphide (MoS2 ) are successfully tuned by directly depositing it onto silica microsphere resonators using chemical vapor deposition method. Multiple whispering gallery mode (WGM) peaks in the emission wavelength range of ≈650-750 nm are observed under continuous wave excitation at room temperature. Time-resolved photoluminescence (TRPL) and femtosecond transient absorption (TA) spectroscopy are conducted to study light-matter interaction dynamics of the MoS2 microcavities. TRPL study suggests radiative recombination rate of carrier-phonon scattering and interband transition processes in MoS2 is enhanced by a factor of ≈1.65 due to Purcell effect in microcavities. TA spectroscopy study shows modulation of the interband transition process mainly occurs at PB-A band with an estimated F ≈ 1.60. Furthermore, refractive index sensing utilizing WGM peaks of MoS2 is established with sensitivity up to ≈150 nm per refractive index unit. The present work provides a large-scale and straightforward method for coupling atomically thin 2D gain media with cavities for high-performance optoelectronic devices and sensors.

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.

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.

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.