Impurities produced during the synthesis process of a material pose detrimental impacts upon the intrinsic properties and device performances of the as-obtained product. This effect is especially pronounced in graphene, where surface contamination has long been a critical, unresolved issue, given graphene’s two-dimensionality. Here we report the origins of surface contamination of graphene, which is primarily rooted in chemical vapour deposition production at elevated temperatures, rather than during transfer and storage. In turn, we demonstrate a design of Cu substrate architecture towards the scalable production of super-clean graphene (>99% clean regions). The readily available, super-clean graphene sheets contribute to an enhancement in the optical transparency and thermal conductivity, an exceptionally lower-level of electrical contact resistance and intrinsically hydrophilic nature. This work not only opens up frontiers for graphene growth but also provides exciting opportunities for the utilization of as-obtained super-clean graphene films for advanced applications.

Directly incorporating heteroatoms into the hexagonal lattice of graphene during growth has been widely used to tune its electrical properties with superior doping stability, uniformity, and scalability. However the introduction of scattering centers limits this technique because of reduced carrier mobilities and conductivities of the resulting material. Here, we demonstrate a rapid growth of graphitic nitrogen cluster–doped monolayer graphene single crystals on Cu foil with remarkable carrier mobility of 13,000 cm2 V−1 s−1 and a greatly reduced sheet resistance of only 130 ohms square−1. The exceedingly large carrier mobility with high n-doping level was realized by (i) incorporation of nitrogen-terminated carbon clusters to suppress the carrier scattering and (ii) elimination of all defective pyridinic nitrogen centers by oxygen etching. Our study opens up an avenue for the growth of high-mobility/conductivity doped graphene with tunable work functions for scalable graphene-based electronic and device applications.

Contamination is a major concern in surface and interface technologies. Given that graphene is a 2D monolayer material with an extremely large surface area, surface contamination may seriously degrade its intrinsic properties and strongly hinder its applicability in surface and interfacial regions. However, large‐scale and facile treatment methods for producing clean graphene films that preserve its excellent properties have not yet been achieved. Herein, an efficient postgrowth treatment method for selectively removing surface contamination to achieve a large‐area superclean graphene surface is reported. The as‐obtained superclean graphene, with surface cleanness exceeding 99%, can be transferred to dielectric substrates with significantly reduced polymer residues, yielding ultrahigh carrier mobility of 500 000 cm2 V−1 s−1 and low contact resistance of 118 Ω µm. The successful removal of contamination is enabled by the strong adhesive force of the activated‐carbon‐based lint roller on graphene contaminants.

Future applications of graphene rely highly on the production of large-area high-quality graphene, especially large single-crystalline graphene, due to the reduction of defects caused by grain boundaries. However, current large single-crystalline graphene growing methodologies are suffering from low growth rate and as a result, industrial graphene production is always confronted by high energy consumption, which is primarily caused by high growth temperature and long growth time. Herein, a new growth condition achieved via ethane being the carbon feedstock to achieve low-temperature yet rapid growth of large single-crystalline graphene is reported. Ethane condition gives a growth rate about four times faster than methane, achieving about 420 µm min for the growth of sub-centimeter graphene single crystals at temperature about 1000 °C. In addition, the temperature threshold to obtain graphene using ethane can be reduced to 750 °C, lower than the general growth temperature threshold (about 1000 °C) with methane on copper foil. Meanwhile ethane always keeps higher graphene growth rate than methane under the same growth temperature. This study demonstrates that ethane is indeed a potential carbon source for efficient growth of large single-crystalline graphene, thus paves the way for graphene in high-end electronical and optoelectronical applications.

Graphitic nitrogen-doped graphene is an excellent platform to study scattering processes of massless Dirac fermions by charged impurities, in which high mobility can be preserved due to the absence of lattice defects through direct substitution of carbon atoms in the graphene lattice by nitrogen atoms. In this work, we report on 2 electrical and magnetotransport measurements of high-quality graphitic nitrogen-doped graphene. We show that the substitutional nitrogen dopants in graphene introduce atomically sharp scatters for electrons but long-range Coulomb scatters for holes and, thus, graphitic nitrogen-doped graphene exhibits clear electron-hole asymmetry in transport properties. Dominant scattering processes of charge carriers in graphitic nitrogen-doped graphene are analyzed. It is shown that the electron-hole asymmetry originates from a distinct difference in intervalley scattering of electrons and holes. We have also carried out the magnetotransport measurements of graphitic nitrogen-doped graphene at different temperatures and the temperature dependences of intervalley scattering, intravalley scattering and phase coherent scattering rates are extracted and discussed. Our results provide an evidence for the electron-hole asymmetry in the intervalley scattering induced by substitutional nitrogen dopants in graphene and shine a light on versatile and potential applications of graphitic nitrogen-doped graphene in electronic and valleytronic devices. KEYWORDS: graphene, charge transport, intervalley scattering, graphitic nitrogen doping, atomically sharp scattering center Graphene, a honeycomb lattice of single layer carbon atoms with a Dirac-like energy dispersion, has attracted extensive interests in recent years owing to its extraordinary charge transport properties and potential applications in electronic devices. [1][2][3][4][5] However, charge impurities universally exist in graphene and influence its electronic properties. [6][7][8][9][10] A particular case is when approaching the Dirac point at which, because of the vanishing density of states, the transport properties of graphene are expected to be highly sensitive to 3 scattering from charged impurities. [6][7][8][9][10] Previous studies of charge carrier scattering in graphene are mainly achieved with the scattering centers introduced by physical methods, such as ion irradiation, 7, 8 adsorption of adlayers, 9 low temperature deposition 10 and spin coating [11][12][13] of nanoparticles, and atomic hydrogen adsorption. 14 These methods could inevitably induce randomness and disorder in graphene and thereby largely degrade its transport properties. Compared with the physical methods, chemical doping has the advantage to achieve scattering centers in graphene with good replicability, lattice stability, and tunablity of doping concentration through the substitution of carbon atoms in the graphene lattice by dopant atoms. Among numerous dopants, nitrogen (N) atoms can be chemically incorporated into graphene forming covalent bonds with carbon (...