Recent Advances on Pulsed Laser Deposition of Large-Scale Thin Films.

2D thin films, possessing atomically thin thickness, are emerging as promising candidates for next-generation electronic devices, due to their novel properties and high performance. In the early years, a wide variety of 2D materials are prepared using several methods (mechanical/liquid exfoliation, chemical vapor deposition, etc.). However, the limited size of 2D flakes hinders their fundamental research and device applications, and hence the effective large-scale preparation of 2D films is still challenging. Recently, pulsed laser deposition (PLD) has appeared to be an impactful method for wafer-scale growth of 2D films, owing to target-maintained stoichiometry, high growth rate, and efficiency. In this review, the recent advances on the PLD preparation of 2D films are summarized, including the growth mechanisms, strategies, and materials classification. First, efficacious strategies of PLD growth are highlighted. Then, the growth, characterization, and device applications of various 2D films are presented, such as graphene, h-BN, MoS2 , BP, oxide, perovskite, semi-metal, etc. Finally, the potential challenges and further research directions of PLD technique is envisioned.

Non-volatile optoelectronic memory based on a photosensitive dielectric.

Recently, the optoelectronic memory is capturing growing attention due to its integrated function of sense and memory as well as multilevel storage ability. Although tens of states have been reported in literature, there are still three obvious deficiencies in most of the optoelectronic memories: large programming voltage (>20 V), high optical power density (>1 mW cm-2), and poor compatibility originating from the over-reliance on channel materials. Here, we firstly propose an optoelectronic memory based on a new photosensitive dielectric (PSD) architecture. Data writing and erasing are realized by using an optical pulse to switch on the PSD. The unique design enables the memory to work with a programming voltage and optical power density as low as 4 V and 160 µW cm-2, respectively. Meanwhile, this device may be extended to different kinds of transistors for specific applications. Our discovery offers a brand-new direction for non-volatile optoelectronic memories with low energy consumption.

High Dielectric Transparent Film Tailored by Acceptor and Donor Codoping.

High dielectric constant materials are of particular current interests as indispensable components in transistors, capacitors, etc. In this context, there are emerging trends to exploit defect engineering in dielectric ceramics for enhancing the performance. However, demonstrations of similar high dielectric performance in integration-compatible crystalline films are rare. Herein, such a breakthrough via the functionalization of donor-acceptor dipoles by compositional tuning in GaCu codoped ZnO films is reported. The dielectric constant reaches ~200 at 1 kHz and the optical transmittance in visible light reaches ~80%. Importantly, by analyzing the impedance spectroscopy data, prominent relaxation mechanisms in correlation with the dipole properties, enabling consistent explanations of the dielectric constant as a function of frequency are discriminated. The atomistic nature of the dipoles is revealed by the systematic X-ray spectroscopy analysis. Spectacularly, similar trends for the dielectric properties are observed, while synthesizing samples by pulsed laser deposition and ion implantation, indicating the general character of the phenomena.

Higher-Order Multiphoton Absorption Upconversion Lasing Based on ZnO/ZnMgO Multiple Quantum Wells.

In the progress of nonlinear optics, multiphoton absorption (MPA) upconversion lasing enables many vital applications in bioimaging, three-dimensional optical data storage, and photodynamic therapy. Here, efficient four-photon absorption upconversion lasing from the ZnO/ZnMgO multiple quantum wells (MQWs) at room temperature is realized. Moreover, the MPA upconversion lasing and third-harmonic generation peak generated in the MQWs under the excitation of a femtosecond (fs) laser pulse were observed concurrently, and the essential differences between each other were studied comprehensively. Compared with the ZnO film, the upconversion lasing peak of the ZnO/ZnMgO MQWs exhibits a clear blue shift. In addition, the four-photon absorption upconversion photoluminescence (PL) intensity was enhanced in the MQWs/Au nanoparticles (NPs) by the metal-localized surface plasmons (LSPs). The work paves the way for short-wavelength lasers by taking advantage of the high stability and large exciton binding energy of the MQWs' structures.

Shape-control growth of 2D-In2Se3 with out-of-plane ferroelectricity by chemical vapor deposition.

For potential applications in ferroelectric switching and piezoelectric nano-generator devices, the promising ferroelectric properties of two dimensional (2D) layered In2Se3 attracted much attention. In the present study, 2D In2Se3 flakes down to monolayers are grown by the chemical vapor deposition (CVD) technique on a mica substrate with their structural, optical and ferroelectric properties being studied. The effect of growth parameters (time of growth and Ar flow rate) on the shape and size of the deposited flakes was studied. The optical microscopy study revealed that the flake changed from a circular shape to a sharp face triangle as the Ar flow rate and growth time increased. Raman spectroscopy and high-resolution scanning transmission electron microscopy (HR-STEM) studies revealed that the flakes were of α and ß phases, each of which has a hexagonal crystal structure. Strong second harmonic generation (SHG) was observed from α-In2Se3, demonstrating its non-centrosymmetric structure. The piezo-force microscopic (PFM) study showed the presence of out of plane (OOP) ferroelectricity with no in plane (IP) ferroelectricity in CVD grown α-In2Se3 indicating its vertically confined piezoresponse, which was tuned by the applied electric bias and the flake thickness. The present result of shape-controlled growth of In2Se3 with OOP ferroelectricity would open new pathways in the field of 2D ferroelectric switching devices.

Vacancy cluster in ZnO films grown by pulsed laser deposition.

Undoped and Ga-doped ZnO films were grown on c-sapphire using pulsed laser deposition (PLD) at the substrate temperature of 600 °C. Positron annihilation spectroscopy study (PAS) shows that the dominant VZn-related defect in the as-grown undoped ZnO grown with relative low oxygen pressure P(O2) is a vacancy cluster (most likely a VZn-nVO complex with n = 2, 3) rather than the isolated VZn which has a lower formation energy. Annealing these samples at 900 °C induces out-diffusion of Zn from the ZnO film into the sapphire creating the VZn at the film/sapphire interface, which favors the formation of vacancy cluster containing relatively more VZn. Increasing the P(O2) during growth also lead to the formation of the vacancy cluster with relatively more VZn. For Ga-doped ZnO films, the oxygen pressure during growth has significant influence on the electron concentration and the microstructure of the VZn-related defect. Green luminescence (GL) and yellow luminescence (YL) were identified in the cathodoluminescence study (CL) study, and both emission bands were quenched after hydrogen plasma treatment. The origin of the GL is discussed.