Guang-Xin Ni

Face-to-face transfer of wafer-scale graphene films

Graphene has attracted worldwide interest since its experimental discovery, but the preparation of large-area, continuous graphene film on SiO2/Si wafers, free from growth-related morphological defects or transfer-induced cracks and folds, remains a formidable challenge. Growth of graphene by chemical vapour deposition on Cu foils has emerged as a powerful technique owing to its compatibility with industrial-scale roll-to-roll technology. However, the polycrystalline nature and microscopic roughness of Cu foils means that such roll-to-roll transferred films are not devoid of cracks and folds. High-fidelity transfer or direct growth of high-quality graphene films on arbitrary substrates is needed to enable wide-ranging applications in photonics or electronics, which include devices such as optoelectronic modulators, transistors, on-chip biosensors and tunnelling barriers. The direct growth of graphene film on an insulating substrate, such as a SiO2/Si wafer, would be useful for this purpose, but current research efforts remain grounded at the proof-of-concept stage, where only discontinuous, nanometre-sized islands can be obtained. Here we develop a face-to-face transfer method for wafer-scale graphene films that is so far the only known way to accomplish both the growth and transfer steps on one wafer. This spontaneous transfer method relies on nascent gas bubbles and capillary bridges between the graphene film and the underlying substrate during etching of the metal catalyst, which is analogous to the method used by tree frogs to remain attached to submerged leaves. In contrast to the previous wet or dry transfer results, the face-to-face transfer does not have to be done by hand and is compatible with any size and shape of substrate; this approach also enjoys the benefit of a much reduced density of transfer defects compared with the conventional transfer method. Most importantly, the direct growth and spontaneous attachment of graphene on the underlying substrate is amenable to batch processing in a semiconductor production line, and thus will speed up the technological application of graphene.

Gate-controlled nonvolatile graphene-ferroelectric memory

In this letter, we demonstrate a nonvolatile memory device in a graphene field-effect-transistor structure using ferroelectric gating. The binary information, i.e., “1” and “0”, is represented by the high and low resistance states of the graphene working channels and is switched by controlling the polarization of the ferroelectric thin film using gate voltage sweep. A nonvolatile resistance change exceeding 200% is achieved in our graphene-ferroelectric hybrid devices. The experimental observations are explained by the electrostatic doping of graphene by electric dipoles at the ferroelectric/graphene interface.

Graphene field-effect transistors with ferroelectric gating.

Recent experiments on ferroelectric gating have introduced a novel functionality, i.e., nonvolatility, in graphene field-effect transistors. A comprehensive understanding in the nonlinear, hysteretic ferroelectric gating and an effective way to control it are still absent. In this Letter, we quantitatively characterize the hysteretic ferroelectric gating using the reference of an independent background doping (n(BG)) provided by normal dielectric gating. More importantly, we prove that n(BG) can be used to control the ferroelectric gating by unidirectionally shifting the hysteretic ferroelectric doping in graphene. Utilizing this electrostatic effect, we demonstrate symmetrical bit writing in graphene-ferroelectric field-effect transistors with resistance change over 500% and reproducible no-volatile switching over 10⁵ cycles.

Graphene-ferroelectric hybrid structure for flexible transparent electrodes.

Graphene has exceptional optical, mechanical, and electrical properties, making it an emerging material for novel optoelectronics, photonics, and flexible transparent electrode applications. However, the relatively high sheet resistance of graphene is a major constraint for many of these applications. Here we propose a new approach to achieve low sheet resistance in large-scale CVD monolayer graphene using nonvolatile ferroelectric polymer gating. In this hybrid structure, large-scale graphene is heavily doped up to 3 × 10(13) cm(-2) by nonvolatile ferroelectric dipoles, yielding a low sheet resistance of 120 Ω/□ at ambient conditions. The graphene-ferroelectric transparent conductors (GFeTCs) exhibit more than 95% transmittance from the visible to the near-infrared range owing to the highly transparent nature of the ferroelectric polymer. Together with its excellent mechanical flexibility, chemical inertness, and the simple fabrication process of ferroelectric polymers, the proposed GFeTCs represent a new route toward large-scale graphene-based transparent electrodes and optoelectronics.

An innovative way of etching MoS2: Characterization and mechanistic investigation

We report a systematic study of the etching of MoS2 crystals by using XeF2 as a gaseous reactant. By controlling the etching process, monolayer MoS2 with uniform morphology can be obtained. The Raman and photoluminescence spectra of the resulting material were similar to those of exfoliated MoS2. Utilizing this strategy, different patterns such as a Hall bar structure and a hexagonal array can be realized. Furthermore, the etching mechanism was studied by introducing graphene as an etching mask. We believe our technique opens an easy and controllable way of etching MoS2, which can be used to fabricate complex nanostructures, such as nanoribbons, quantum dots, and transistor structures. This etching process using XeF2 can also be extended to other interesting two-dimensional crystals.Graphical abstract

Quasi-Periodic Nanoripples in Graphene Grown by Chemical Vapor Deposition and Its Impact on Charge Transport

The technical breakthrough in synthesizing graphene by chemical vapor deposition methods (CVD) has opened up enormous opportunities for large-scale device applications. To improve the electrical properties of CVD graphene grown on copper (Cu-CVD graphene), recent efforts have focused on increasing the grain size of such polycrystalline graphene films to 100 μm and larger. While an increase in grain size and, hence, a decrease of grain boundary density is expected to greatly enhance the device performance, here we show that the charge mobility and sheet resistance of Cu-CVD graphene is already limited within a single grain. We find that the current high-temperature growth and wet transfer methods of CVD graphene result in quasi-periodic nanoripple arrays (NRAs). Electron-flexural phonon scattering in such partially suspended graphene devices introduces anisotropic charge transport and sets limits to both the highest possible charge mobility and lowest possible sheet resistance values. Our findings provide guidance for further improving the CVD graphene growth and transfer process.

Wafer-scale graphene/ferroelectric hybrid devices for low-voltage electronics

Preparing graphene and its derivatives on functional substrates may open enormous opportunities for exploring the intrinsic electronic properties and new functionalities of graphene. However, efforts in replacing SiO2 have been greatly hampered by a very low sample yield of the exfoliation and related transferring methods. Here, we report a new route in exploring new graphene physics and functionalities by transferring large-scale chemical-vapor deposition single-layer and bilayer graphene to functional substrates. Using ferroelectric Pb(Zr0.3Ti0.7)O3 (PZT), we demonstrate ultra-low-voltage operation of graphene field effect transistors within ±1 V with maximum doping exceeding 1013 cm− 2 and on-off ratios larger than 10 times. After polarizing PZT, switching of graphene field effect transistors are characterized by pronounced resistance hysteresis, suitable for ultra-fast non-volatile electronics.

Tuning Optical Conductivity of Large-Scale CVD Graphene by Strain Engineering

A controllable optical anisotropy in CVD graphene is shown. The transparency in the visible range of pre-strained CVD graphene exhibits a periodic modulation as a function of polarization direction. The strain sensitivity of the optical response of graphene demonstrated here can be effectively utilized towards novel ultra-thin optical devices and strain sensing applications.

Plasmons in graphene moire superlattices

Moiré patterns are periodic superlattice structures that appear when two crystals with a minor lattice mismatch are superimposed. A prominent recent example is that of monolayer graphene placed on a crystal of hexagonal boron nitride. As a result of the moiré pattern superlattice created by this stacking, the electronic band structure of graphene is radically altered, acquiring satellite sub-Dirac cones at the superlattice zone boundaries. To probe the dynamical response of the moiré graphene, we use infrared (IR) nano-imaging to explore propagation of surface plasmons, collective oscillations of electrons coupled to IR light. We show that interband transitions associated with the superlattice mini-bands in concert with free electrons in the Dirac bands produce two additive contributions to composite IR plasmons in graphene moiré superstructures. This novel form of collective modes is likely to be generic to other forms of moiré-forming superlattices, including van der Waals heterostructures.

A new route to graphene layers by selective laser ablation

Selectively creating regions of spatially varying thickness may enable the utilization of the electronic properties of N-layer (N=1 or more) graphene and other similar layered materials (e.g., topological insulators or layered superconductors) for novel devices and functionalities on a single chip. The ablation threshold energy density increases dramatically for decreasing layer numbers of graphene originating from the dimensional crossover of the specific heat. For the 2D regime of graphite (up to N≈7) the dominant flexural mode specific heat (due to its N-1 dependence) gives rise to a strong layer number-dependence on the pulsed laser ablation threshold energy density, while for 3D regime (N>>7) the ablation threshold saturates due to dominant acoustic mode specific heat. As a result, several energy density windows exist between the minimum energy densities that are required for ablating single, bi, or more layers of graphene, allowing layer number selectivity.