Beijing National Laboratory for Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, People's Republic of China.
Acc Chem Res. 2013 Jan 15;46(1):106-15. doi: 10.1021/ar300103f. Epub 2012 Jul 19.
Because of its atomic thickness, excellent properties, and widespread applications, graphene is regarded as one of the most promising candidate materials for nanoelectronics. The wider use of graphene will require processes that produce this material in a controllable manner. In this Account, we focus on our recent studies of the controllable chemical vapor deposition (CVD) growth of graphene, especially few-layer graphene (FLG), and the applications of this material in electronic devices. CVD provides various means of control over the morphologies of the produced graph ene. We studied several variables that can affect the CVD growth of graphene, including the catalyst, gas flow rate, growth time, and growth temperature and successfully achieved the controlled growth of hexagonal graphene crystals. Moreover, we developed several modified CVD methods for the controlled growth of FLGs. Patterned CVD produced FLGs with desired shapes in required areas. By introducing dopant precursor in the CVD process, we produced substitutionally doped FLGs, avoiding the typically complicated post-treatment processes for graphene doping. We developed a template CVD method to produce FLG ribbons with controllable morphologies on a large scale. An oxidation-activated surface facilitated the CVD growth of polycrystalline graphene without the use of a metal catalyst or a complicated postgrowth transfer process. In devices, CVD offers a controllable means to modulate the electronic properties of the graphene samples and to improve device performance. Using CVD-grown hexagonal graphene crystals as the channel materials in field-effect transistors (FETs), we improved carrier mobility. Substitutional doping of graphene in CVD opened a band gap for efficient FET operation and modulated the Fermi energy level for n-type or p-type features. The similarity between the chemical structure of graphene and organic semiconductors suggests potential applications of graphene in organic devices. We used patterned CVD FLGs as the bottom electrodes in pentacene FETs. The strong π-π interactions between graphene and pentacene produced an excellent interface with low contact resistance and a reduced injection barrier, which dramatically enhances the device performance. We also fabricated reversible nanoelectromechanical (NEM) switches and a logic gate using the FLG ribbons produced using our template CVD method. In summary, CVD provides a controllable means to produce graphene samples with both large area and high quality. We developed several modified CVD methods to produce FLG samples with controlled shape, location, edge, layer, dopant, and growth substrate. As a result, we can modulate the properties of FLGs, which provides materials that could be used in FETs, OFETs, and NEM devices. Despite remarkable advances in this field, further exploration is required to produce consistent, homogeneous graphene samples with single layer, single crystal, and large area for graphene-based electronics.
由于其原子级厚度、优异的性能和广泛的应用,石墨烯被认为是最有前途的纳米电子候选材料之一。为了更广泛地使用石墨烯,需要开发能够以可控方式生产这种材料的工艺。在本专题介绍中,我们重点介绍了我们最近在可控化学气相沉积(CVD)生长石墨烯,特别是少层石墨烯(FLG)方面的研究,以及该材料在电子器件中的应用。CVD 为所生产石墨烯的形貌提供了多种控制手段。我们研究了几种可能影响石墨烯 CVD 生长的变量,包括催化剂、气流速率、生长时间和生长温度,并成功实现了六方石墨烯晶体的可控生长。此外,我们还开发了几种用于 FLG 可控生长的改良 CVD 方法。图案化 CVD 可在所需区域内生产出具有所需形状的 FLG。通过在 CVD 过程中引入掺杂剂前体,我们生产出了取代掺杂的 FLG,避免了通常对石墨烯掺杂所需要的复杂后处理过程。我们开发了一种模板 CVD 方法,可以大规模生产具有可控形貌的 FLG 带状物。氧化激活表面促进了多晶石墨烯的 CVD 生长,而无需使用金属催化剂或复杂的后生长转移工艺。在器件中,CVD 提供了一种可控的手段来调节石墨烯样品的电子性质并提高器件性能。我们使用 CVD 生长的六方石墨烯晶体作为场效应晶体管(FET)的沟道材料,提高了载流子迁移率。CVD 中的石墨烯替代掺杂为高效 FET 操作打开了带隙,并调节了费米能级以实现 n 型或 p 型特征。石墨烯与有机半导体在化学结构上的相似性表明了其在有机器件中的潜在应用。我们使用图案化 CVD FLG 作为并五苯 FET 的底电极。石墨烯与并五苯之间的强π-π相互作用产生了具有低接触电阻和减小的注入势垒的优异界面,从而极大地增强了器件性能。我们还使用我们的模板 CVD 方法制造的 FLG 带状物制造了可逆的纳米机电(NEM)开关和逻辑门。总之,CVD 提供了一种可控的手段,可以生产出具有大面积和高质量的石墨烯样品。我们开发了几种改良的 CVD 方法来生产具有可控形状、位置、边缘、层、掺杂剂和生长衬底的 FLG 样品。因此,我们可以调节 FLG 的性质,从而提供可用于 FET、OFET 和 NEM 器件的材料。尽管在这一领域取得了显著进展,但仍需要进一步探索以生产具有一致性、均匀性、单层、单晶和大面积的石墨烯样品,以用于基于石墨烯的电子学。