Large Single‐Crystal Cu Foils with High‐Index Facets by Strain‐Engineered Anomalous Grain Growth

Li, Yanglizhi; Sun, Luzhao; Chang, Zhenghua; Liu, Haiyang; Wang, Yuechen; Liang, Yu; Chen, Buhang; Ding, Qingjie; Zhao, Zhenyong; Wang, Ruoyu; Wei, Yujie; Peng, Hailin; Lin, Li; Liu, Zhongfan

doi:10.1002/adma.202002034

Cited by 55 publications

(58 citation statements)

References 29 publications

(33 reference statements)

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“…The high quality of the as-grown tBLG was corroborated by clear Moiré patterns in the HR-TEM and carrier mobility exceeding 68,000 cm 2 V −1 s −1 at room temperature. Our work brings inspiration for controlled growth of graphene and other 2D materials with interlayer twist, and future works still need to be done to grow tBLGs with certain twist angles, possibly by controlling the nucleation density, designing the growth substrate 48 , utilizing the axial screw dislocation 49 , 50 , or introducing intermediate layers 11 , 12 . Meanwhile, the torque toward smaller twist angles, which increases rapidly near the zero-angle, should be overcome to improve the portion of very small twist angle (near magic angle).…”

Section: Discussionmentioning

confidence: 99%

Hetero-site nucleation for growing twisted bilayer graphene with a wide range of twist angles

et al. 2021

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Twisted bilayer graphene (tBLG) has recently attracted growing interest due to its unique twist-angle-dependent electronic properties. The preparation of high-quality large-area bilayer graphene with rich rotation angles would be important for the investigation of angle-dependent physics and applications, which, however, is still challenging. Here, we demonstrate a chemical vapor deposition (CVD) approach for growing high-quality tBLG using a hetero-site nucleation strategy, which enables the nucleation of the second layer at a different site from that of the first layer. The fraction of tBLGs in bilayer graphene domains with twist angles ranging from 0° to 30° was found to be improved to 88%, which is significantly higher than those reported previously. The hetero-site nucleation behavior was carefully investigated using an isotope-labeling technique. Furthermore, the clear Moiré patterns and ultrahigh room-temperature carrier mobility of 68,000 cm2 V−1 s−1 confirmed the high crystalline quality of our tBLG. Our study opens an avenue for the controllable growth of tBLGs for both fundamental research and practical applications.

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Section: Discussionmentioning

confidence: 99%

Hetero-site nucleation for growing twisted bilayer graphene with a wide range of twist angles

et al. 2021

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“…Such a graphene film, without any GBs and adlayers, is essential for constructing 'stacked graphene single crystals' with controlled rotation angles and number of layers by a layer-by-layer assembly method, which we will discuss later. Very recently, Wu and Li independently reported the preparation of large-area single-crystal highindex Cu surfaces [77,78]. Epitaxial growth of graphene has been reported on various indices, such as 112, 311, and 436 [77][78][79].…”

Section: Single-crystal Slg Grown From Multiple Nucleimentioning

confidence: 99%

“…Very recently, Wu and Li independently reported the preparation of large-area single-crystal highindex Cu surfaces [77,78]. Epitaxial growth of graphene has been reported on various indices, such as 112, 311, and 436 [77][78][79]. Density function theory calculations indicated that this is due to the single lowest energy state of graphene nucleation on high-index Cu surface [79].…”

Section: Single-crystal Slg Grown From Multiple Nucleimentioning

confidence: 99%

Synthesis of Large-Area Single-Crystal Graphene

Wang

Luo

Wang

et al. 2021

Trends in Chemistry

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There have been breakthroughs in the mass production of graphene by chemical vapor deposition (CVD) and its practical applications have also been identified. Grain boundaries are typically present in 'CVD graphene' and adversely impact its properties. We summarize recent progress in growing large-area singlecrystal graphene. Centimeter-scale single-crystal, truly single-layer graphene (SLG) films have been reportedly achieved on single-crystal Cu(111) foils by CVD growth, while meter-scale single-crystal SLG films have been reportedly produced with assistance of a roll-to-roll technique. The growth of uniform single crystals of bilayer or multilayer graphene over a large area remains an exciting challenge. Layer-by-layer transfer and the stacking of single-crystal SLG is considered a promising route to making new types of 'single' crystals or quasicrystals with specific numbers of layers and different stacking angles. Structure and Properties of Single-Crystal GrapheneGraphene, a single layer of carbon atoms arranged in a honeycomb lattice (Figure 1A), has attracted worldwide attention due to its unique 2D structure and excellent physical properties [1][2][3][4][5]. When two graphene layers are stacked on top of each other, the properties of the bilayer material [6] depend on the stacking angle (Figure 1B,C) [7,8]. AB-stacked bilayer graphene (BLG) (see Glossary) reportedly has a continuously tunable bandgap of up to 250 meV when a vertical electrical field is applied, which enables the fabrication of semiconductor devices [9][10][11]. An AB-stacked BLG film was reportedly converted to an ultra-thin 'diamond' film (F-diamane) by fluorine chemisorption [12]. In addition, twisted bilayer graphene (tBLG) reportedly presents θ-dependent interfacial conductivity [13], van Hove singularities [14], and particular electronic structures [15] that are reported to have potential for use in ultra-sensitive sensors and ultra-thin capacitors. A Mott insulator and unconventional superconductivity with a critical temperature up to 1.7 K was reported for a twist angle of 1.1 o in BLG [10,11]. Compared with AB-stacked BLG, tBLG reportedly has a higher chemical reactivity, which was said to be due to distinct variations in the density-of-states distribution in the gap region [16]. Among various synthesis methods, chemical vapor deposition (CVD) has shown to be the most promising for the scalable production of large-area high-quality graphene films [17]. Ruoff and colleagues first reported the preparation of a centimeter-scale single-layer graphene (SLG) film on a commercial Cu foil by CVD in 2009 [18]. Unlike Ni with high carbon solubility (~0.9 at.% at 900°C [19]), Cu has a much lower carbon solubility, even up to 1000°C (7.4 at. ppm at 1020°C [20]), which is believed to predominantly contribute to the surface-mediated mechanism of graphene growth and good uniformity of the number of layers of the as-grown graphene [21]. As a result, Cu-based foils or films are the most common substrates for studying the behavior of graphene growt...

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“…Recently, a technology has been developed to prepare large-area single-crystal copper foil by abnormal grain growth during the annealing of polycrystalline copper foil [14][15][16]. The abnormal grain growth is affected by multiple factors, such as driving force [17] and temperature [18][19][20]. The tension can activate the grain boundary energy of Cu foil and promote its abnormal grain growth to single crystals [17].…”

Section: Introductionmentioning

confidence: 99%

“…For example, when the surface energy as the main diving force, the abnormal grain growth trends to formation of Cu (111) with minimum surface energy [21]. When the thermal stress that arises as a result of interfacial contact as the major driving force for grain growth, abnormal grown grain with a high-index facet can be obtained [19]. High temperature (close to the metals' melting temperatures) can accelerate the abnormal grain growth [21].…”

Section: Introductionmentioning

confidence: 99%

The Effect of Ethanol on Abnormal Grain Growth in Copper Foils

Zhang

Duan

et al. 2021

Nanomaterials

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Single-crystal Cu not only has high electrical and thermal conductivity, but can also be used as a promising platform for the epitaxial growth of two-dimensional materials. Preparing large-area single-crystal Cu foils from polycrystalline foils has emerged as the most promising technique in terms of its simplicity and effectiveness. However, the studies on transforming polycrystalline foil into large-area single-crystal foil mainly focus on the influence of annealing temperature and strain energy on the recrystallization process of copper foil, while studies on the effect of annealing atmosphere on abnormal grain growth behavior are relatively rare. It is necessary to carry out more studies on the effect of annealing atmosphere on grain growth behavior to understand the recrystallization mechanism of metal. Here, we found that introduction of ethanol in pure argon annealing atmosphere will cause the abnormal grain growth of copper foil. Moreover, the number of abnormally grown grains can be controlled by the concentration of ethanol in the annealing atmosphere. Using this technology, the number of abnormally grown grains on the copper foil can be controlled to single one. This abnormally grown grain will grow rapidly to decimeter-size by consuming the surrounding small grains. This work provides a new perspective for the understanding of the recrystallization of metals, and a new method for the preparation of large-area single-crystal copper foils.

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Large Single‐Crystal Cu Foils with High‐Index Facets by Strain‐Engineered Anomalous Grain Growth

Cited by 55 publications

References 29 publications

Hetero-site nucleation for growing twisted bilayer graphene with a wide range of twist angles

Hetero-site nucleation for growing twisted bilayer graphene with a wide range of twist angles

Synthesis of Large-Area Single-Crystal Graphene

The Effect of Ethanol on Abnormal Grain Growth in Copper Foils

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