2D-Material-Assisted GaN Growth on GaN Template by MOCVD and Its Exfoliation Strategy.

The production of freestanding membranes using two-dimensional (2D) materials often involves techniques such as van der Waals (vdW) epitaxy, quasi-vdW epitaxy, and remote epitaxy. However, a challenge arises when attempting to manufacture freestanding GaN by using these 2D-material-assisted growth techniques. The issue lies in securing stability, as high-temperature growth conditions under metal-organic chemical vapor deposition (MOCVD) can cause damage to the 2D materials due to GaN decomposition of the substrate. Even when GaN is successfully grown using this method, damage to the 2D material leads to direct bonding with the substrate, making the exfoliation of the grown GaN nearly impossible. This study introduces an approach for GaN growth and exfoliation on 2D material/GaN templates. First, graphene and hexagonal boron nitride (h-BN) were transferred onto the GaN template, creating stable conditions under high temperatures and various gases in MOCVD. GaN was grown in a two-step process at 750 and 900 °C, ensuring exfoliation in cases where the 2D materials remained intact. Essentially, while it is challenging to grow GaN on 2D material/GaN using only MOCVD, this study demonstrates that with effective protection of the 2D material, the grown GaN can endure high temperatures and still be exfoliated. Furthermore, these results support that vdW epitaxy and remote epitaxy principle are not only possible with specific equipment but also applicable generally.

Stability of Graphene and Influence of AlN Surface Pits on GaN Remote Heteroepitaxy for Exfoliation.

Remote epitaxy is a promising technology that has recently attracted considerable attention, which enables the growth of thin films that copy the crystallographic characteristics of the substrate through two-dimensional material interlayers. The grown films can be exfoliated to form freestanding membranes, although it is often challenging to apply this technique if the substrate materials are prone to damage under harsh epitaxy conditions. For example, remote epitaxy of GaN thin films on graphene/GaN templates has not been achieved by a standard metal-organic chemical vapor deposition (MOCVD) method due to such damages. Here, we report GaN remote heteroepitaxy on graphene/AlN templates by MOCVD and investigate the influence of surface pits in AlN on the growth and exfoliation of GaN thin films. We first show the thermal stability of graphene before GaN growth, based on which two-step growth of GaN on graphene/AlN is developed. The GaN samples are successfully exfoliated after the first step of the growth at 750 °C, whereas the exfoliation failed after the second step at 1050 °C. In-depth analysis confirms that the pits in AlN templates lead to the degradation of graphene near the area and thus the alteration of growth modes and the failure of exfoliation. These results exemplify the importance of chemical and topographic properties of growth templates for successful remote epitaxy. It is one of the key factors for III-nitride-based remote epitaxy, and these results are expected to be of great help in realizing complete remote epitaxy using only MOCVD.

Understanding the 2D-material and substrate interaction during epitaxial growth towards successful remote epitaxy: a review.

Remote epitaxy, which was discovered and reported in 2017, has seen a surge of interest in recent years. Although the technology seemed to be difficult to reproduce by other labs at first, remote epitaxy has come a long way and many groups are able to consistently reproduce the results with a wide range of material systems including III-V, III-N, wide band-gap semiconductors, complex-oxides, and even elementary semiconductors such as Ge. As with any nascent technology, there are critical parameters which must be carefully studied and understood to allow wide-spread adoption of the new technology. For remote epitaxy, the critical parameters are the (1) quality of two-dimensional (2D) materials, (2) transfer or growth of 2D materials on the substrate, (3) epitaxial growth method and condition. In this review, we will give an in-depth overview of the different types of 2D materials used for remote epitaxy reported thus far, and the importance of the growth and transfer method used for the 2D materials. Then, we will introduce the various growth methods for remote epitaxy and highlight the important points in growth condition for each growth method that enables successful epitaxial growth on 2D-coated single-crystalline substrates. We hope this review will give a focused overview of the 2D-material and substrate interaction at the sample preparation stage for remote epitaxy and during growth, which have not been covered in any other review to date.

Improving Ultraviolet Responses in Cu2ZnSn(S,Se)4 Thin-Film Solar Cells Using Quantum Dot-Based Luminescent Down-Shifting Layer.

Quantum dot (QD)-based luminescent down-shifting (LDS) layers were deposited on Cu2ZnSn(S,Se)4 (CZTSSe) solar cells via the drop-casting method. The LDS layers can easily widen the narrow absorption wavelength regions of single-junction solar cells and enable improvement of the short-circuit current. The optical properties of LDS layers deposited on glass and containing different QD contents were analyzed based on their transmittance, reflectance, and absorbance. The absorber films to be used in the CZTSSe solar cells were determined by X-ray diffraction measurements and Raman spectroscopy to determine their crystal structures and secondary phases, respectively. The completed CZTSSe solar cells with LDS layers showed increased ultraviolet responses of up to 25% because of wavelength conversion by the QDs. In addition, the impact of the capping layer, which was formed to protect the QDs from oxygen and moisture, on the solar cell performance was analyzed. Thus, a maximal conversion efficiency of 7.3% was achieved with the 1.0 mL QD condition; furthermore, to the best of our knowledge, this is the first time that LDS layers have been experimentally demonstrated for CZTSSe solar cells.

High-performance metal mesh/graphene hybrid films using prime-location and metal-doped graphene.

We introduce high-performance metal mesh/graphene hybrid transparent conductive layers (TCLs) using prime-location and metal-doped graphene in near-ultraviolet light-emitting diodes (NUV LEDs). Despite the transparency and sheet resistance values being similar for hybrid TCLs, there were huge differences in the NUV LEDs' electrical and optical properties depending on the location of the graphene layer. We achieved better physical stability and current spreading when the graphene layer was located beneath the metal mesh, in direct contact with the p-GaN layer. We further improved the contact properties by adding a very thin Au mesh between the thick Ag mesh and the graphene layer to produce a dual-layered metal mesh. The Au mesh effectively doped the graphene layer to create a p-type electrode. Using Raman spectra, work function variations, and the transfer length method (TLM), we verified the effect of doping the graphene layer after depositing a very thin metal layer on the graphene layers. From our results, we suggest that the nature of the contact is an important criterion for improving the electrical and optical performance of hybrid TCLs, and the method of doping graphene layers provides new opportunities for solving contact issues in other semiconductor devices.

Very thin ITO/metal mesh hybrid films for a high-performance transparent conductive layer in GaN-based light-emitting diodes.

In this paper, we introduce very thin Indium tin oxide (ITO) layers (5, 10, and 15 nm) hybridized with a metal mesh to produce high-performance transparent conductive layers (TCLs) in near-ultraviolet light-emitting diodes (NUV LEDs). Using UV-vis-IR spectrometry, Hall measurement, and atomic force microscopy, we found that 10 nm was the optimal thickness for the very thin ITO layers in terms of outstanding transmittance and sheet resistance values as well as stable contact properties when hybridized with the metal mesh. The proposed layers showed a value of 4.56 Ω/□ for sheet resistance and a value of 89.1% for transmittance. Moreover, the NUV LEDs fabricated with the hybrid TCLs achieved ∼140% enhanced light output power compared to that of 150 nm thick ITO layers. Finally, to verify the practical usage of the TCLs for industrial applications, we packaged the NUV LED chips and obtained improved turn-on voltage (3.48 V) and light output power (∼116%) performance.