Unraveling the Heterointegration of 3D Semiconductors on Graphene by Anchor Point Nucleation.

The heterointegration of graphene with semiconductor materials and the development of graphene-based hybrid functional devices are heavily bound to the control of surface energy. Although remote epitaxy offers one of the most appealing techniques for implementing 3D/2D heterostructures, it is only suitable for polar materials and is hugely dependent on the graphene interface quality. Here, the growth of defect-free single-crystalline germanium (Ge) layers on a graphene-coated Ge substrate is demonstrated by introducing a new approach named anchor point nucleation (APN). This powerful approach based on graphene surface engineering enables the growth of semiconductors on any type of substrate covered by graphene. Through plasma treatment, defects such as dangling bonds and nanoholes, which act as preferential nucleation sites, are introduced in the graphene layer. These experimental data unravel the nature of those defects, their role in nucleation, and the mechanisms governing this technique. Additionally, high-resolution transmission microscopy combined with geometrical phase analysis established that the as-grown layers are perfectly single-crystalline, stress-free, and oriented by the substrate underneath the engineered graphene layer. These findings provide new insights into graphene engineering by plasma and open up a universal pathway for the heterointegration of high-quality 3D semiconductors on graphene for disruptive hybrid devices.

Wafer-scale detachable monocrystalline germanium nanomembranes for the growth of III-V materials and substrate reuse.

Germanium (Ge) is increasingly used as a substrate for high-performance optoelectronics, photovoltaics, and electronic devices. These devices are usually grown on thick and rigid Ge substrates manufactured by classical wafering techniques. Nanomembranes (NMs) provide an alternative to this approach while offering wafer-scale lateral dimensions, weight reduction, waste limitation, and cost effectiveness. Herein, we introduce the Porous germanium Efficient Epitaxial LayEr Release (PEELER) process, which consists of the fabrication of wafer-scale detachable Ge NMs on porous Ge (PGe) and substrate reuse. We demonstrate the growth of Ge NMs with monocrystalline quality as revealed by high-resolution transmission electron microscopy (HRTEM) characterization. Together with the surface roughness below 1 nm, it makes the Ge NMs suitable for growth of III-V materials. Additionally, the embedded nanoengineered weak layer enables the detachment of the Ge NMs. Finally, we demonstrate the wet-etch-reconditioning process of the Ge substrate, allowing its reuse, to produce multiple free-standing NMs from a single parent wafer. The PEELER process significantly reduces the consumption of Ge in the fabrication process, paving the way for a new generation of low-cost flexible optoelectronic devices.

In-Situ Transmission Electron Microscopy Observation of Germanium Growth on Freestanding Graphene: Unfolding Mechanism of 3D Crystal Growth During Van der Waals Epitaxy.

Breakthroughs in cutting-edge research fields such as hetero-integration of materials and the development of quantum devices are heavily bound to the control of misfit strain during heteroepitaxy. While remote epitaxy offers one of the most intriguing avenues, demonstrations of functional hybrid heterostructures are hardly possible without a deep understanding of the nucleation and growth kinetics of 3D crystals on graphene and their mutual interactions. Here, the kinetics of such processes from real-time observations of germanium (Ge) growth on freestanding single layer graphene (SLG) using in-situ transmission electron microscopy are unraveled. This powerful technique provides a unique opportunity to observe new and yet unexplored phenomena, which are not accessible to the standard ex situ characterizations. Through direct observations, remote interactions are elucidated between Ge crystals through the graphene layer in double heterostructures of Ge/graphene/Ge. Notably, the data show real-time evidence of vertical Ge atoms diffusion through the graphene layer. This phenomenon is attributed to the remote interactions of Ge atoms through the graphene lattice, due to its interatomic interaction transparency. Additionally, key mechanisms governing nucleation and initial growth in graphene were systematically determined. These findings enlighten the growth mechanism of graphene and provide a new pathway for disruptive hybrid semiconductor-graphene devices.