物理所高鸿钧、杜世萱AM: 石墨烯/硅烯范德华异质结构中的稳定硅烯
2018-10-12 15:17:09   来源:材料牛   评论:0 点击:

【引言】

作为石墨烯的二维类似物,硅烯最近成为科研人员广泛研究的材料。理论上预测的硅烯和基于硅烯的范德瓦尔斯异质结虽然具有令人感兴趣的物理性质,但是由于硅烯在空气中易于氧化,目前来说,在实验上制备此类器件仍然具有很大的挑战性。

【成果简介】

近日,中国科学院物理研究所高鸿钧、杜世萱(共同通讯)等研究人员通过硅插层方法成功制备了石墨烯/硅烯范德瓦尔斯异质结构。密度泛函理论计算显示石墨烯和硅烯层之间的相互作用较弱,证实了范德华异质结构的形成。他们首先在Ru(0001)衬底上生长石墨烯层,并在其下插入硅原子以构筑硅烯。同时,他们通过控制硅的量,在石墨烯下制备不同类型的硅烯纳米结构并通过扫描隧道显微镜(STM)成像分析。在低剂量下,在石墨烯摩尔图案的顶部(atop)区域下周期性排列的硅烯纳米片段阵列是一种新型的本征图案化的二维材料;而在较高剂量下,插入的Si形成硅烯单层。在更高的Si剂量下,在石墨烯和基底之间则形成多层硅烯。将所制备的石墨烯/硅烯异质结构在环境条件下暴露两周,没有显示出可观察到的损坏,表明了其良好的空气稳定性。该研究发表于Advanced Materials,题为“Stable Silicene in Graphene/Silicene Van der Waals Heterostructures”。文章第一作者为物理所李更。

【图文导读】

图1. 在石墨烯/Ru(0001)界面处的硅烯结构形成示意图

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在退火过程中,沉积的Si原子插入到石墨烯和Ru基底之间。Si含量较小时,Si原子在顶部区域下方形成蜂窝状硅烯纳米薄片。随着Si嵌入的增加,形成硅烯单层和多层。

图2. 硅烯纳米薄片的形成

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(a)STM形貌显示Si插层后的石墨烯/Ru(0001)结构。插图为(a)的放大图像。(b,c)分别为在-0.5V和-0.1V的不同偏压下在相同区域得到的原子级分辨率图像。(d)在atop位下方插层26个Si原子的原子结构模型。(e,f)分别为(d)中的模型在-0.5V和-0.1V的样品偏压下通过第一性原理计算模拟的STM图像。

图3. 单层硅烯的形成

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(a)封装在石墨烯和Ru(0001)之间的单层硅烯的STM图像。(b)为完整碳原子晶格的原子分辨率图像。(c)(7×7)Ru(0001)/(√21×√21)硅烯/(8×8)石墨烯构型的弛豫原子模型的顶视图和侧视图(超晶格元胞由红色菱形标记)。(d)(c)中构型的第一性原理模拟STM图像。

图4. 石墨烯/硅烯异质结构的电子局域函数(ELF)计算和输运特性

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(a,b)硅原子平面上的硅烯纳米片和单层的ELF图。c)在105 K下测量的石墨烯/硅烯/钌垂直异质结构的电流-电压曲线,显示典型的肖特基样整流行为。插图是样品结构和测量的示意图。d)伏安曲线的对数图。通过将其与Schockley模型拟合,可以得到 ~1.5的理想因子。

【小结】

本项研究表明,通过精确控制Si和石墨烯之间的插层过程,可以实现不同类型的石墨烯/硅烯异质结构:硅烯纳米片阵列和硅烯单层和多层。STM表征和DFT模拟都明确地支持观察到的结构。石墨烯和硅烯之间的相互作用属于范德瓦尔斯型,如ELF计算所证明。所展示的这些结构的空气稳定性在将来的硅烯器件制造中将是有用的。对垂直异质结构的测量确实显示出明确定义的肖特基整流行为,表明生长的石墨烯/硅烯异质结构代表了一类新兴的稳定和功能性二维异质结构。研究人员也注意到制备的异质结构仍然与金属钌衬底键合,这限制了其实际应用,而在未来,进一步将异质结构转移到绝缘基板上的研究则是很有必要的。

文献链接:Stable Silicene in Graphene/Silicene Van der Waals Heterostructures (Advanced Materials 2018, DOI: 10.1002/adma.201804650)

【团队介绍】

中国科学院物理研究所高鸿钧课题组长期从事低维信息材料、低维有机功能材料以及以石墨烯为代表的新型二维材料的构筑和探索其物理性质方面的工作。课题组长高鸿钧是国际知名的凝聚态物理学家、中国科学院院士、第三世界科学院院士,是我国低维信息材料和低维物理研究领域的领军人物之一。他的相关研究成果两次入选“中国十大科技进展/新闻”,发表SCI论文350余篇,总引用18000余次,在国际/国内重要会议上作大会报告和邀请报告100余次。他获得了德国“洪堡研究奖”、第三世界科学院“物理奖”、全球华人物理学会“亚洲成就奖”、“中国科学院杰出科技成就奖”、“何梁何利科学与技术进步奖”、国家自然科学二等奖、第七届中国青年科技奖、陈嘉庚科学奖等。近年来他带领团队成功制备了以硅烯、锗烯、铪烯、锑烯等多种超越石墨烯的新型二维原子晶体材料,其中锗烯、铪烯等材料均是在国际上首次制备合成;利用分子束外延的方法制备了包括PtSe2, CuSe等在内的多种二维双元原子晶体材料;利用插层技术首次构筑了石墨烯/硅烯范德华异质结构。

【团队在该领域代表性工作】

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Y. Pan, H.G. Zhang, D.X. Shi, J.T. Sun, S.X. Du, F. Liu, H. -J. Gao, "Highly Ordered, Millimeter-Scale, Continuous, Single-Crystalline Graphene Monolayer Formed on Ru (0001) ", Adv. Mater. 21, 2777-2780 (2009)

Y. Pan, M. Gao, L. Huang, F. Liu, H. -J. Gao, "Directed self-assembly of monodispersed platinum nanoclusters on graphene Moiré template", Appl. Phys. Lett. 95, 093106(2009)

H. T. Zhou, J. H. Mao, G. Li, Y. L. Wang, X. L. Feng, S. X. Du, K. Mu llen, and H.-J. Gao, “Direct Imaging of Intrinsic Molecular Orbitals Using Two-dimensional, Epitaxially-grown, Nanostructured Graphene for Study of Single Molecule and Interactions", Appl. Phys. Lett. 99, 153101 (2011)

Li Huang, Yi Pan, Lida Pan, Min Gao, Wenyan Xu, Yande Que, Haitao Zhou, Yeliang Wang, Shixuan Du, and H.-J. Gao, “Intercalation of Metal Islands and Films at the Interface of Epitaxially Grown Graphene and Ru(0001) Surfaces", Appl. Phys. Lett. 99, 163107 (2011)

Jinhai Mao, Li Huang, Yi Pan, Min Gao, Junfeng He, Haitao Zhou, Haiming Guo,Yuan Tian, Qiang Zou, Lizhi Zhang, Haigang Zhang, Yeliang Wang, Shixuan Du, Xingjiang Zhou, A. H. Castro Neto, and Hong-Jun Gao, "Silicon layer intercalation of centimeter-scale, epitaxially grown monolayer graphene on Ru(0001)", Appl. Phys. Lett. 100, 093101 (2012)

Lei Meng, Yeliang Wang, Lizhi Zhang, Shixuan Du, Rongting Wu, Linfei Li, Yi Zhang, Geng Li, Haitao Zhou, Werner A. Hofer,and Hong-Jun Gao, "Buckled Silicene Formation on Ir(111)", Nano Lett. 13, 685 (2013)

Linfei Li, Yeliang Wang, Shengyi Xie, Xian-Bin Li, Yu-Qi Wang, Rongting Wu, Hongbo Sun, Shengbai Zhang, and Hong-Jun Gao, "Two-Dimensional Transition Metal Honeycomb Realized: Hf on Ir(111)", Nano Lett. 13, 4671 (2013)

Linfei Li , Shuang-zan Lu , Jinbo Pan , Zhihui Qin , Yu-qi Wang , Yeliang Wang , Geng-yu Cao , Shixuan Du , and Hong-Jun Gao, "Buckled Germanene Formation on Pt(111)", Adv. Mater. 2014, 26, 4820–4824

Yeliang Wang, Linfei Li, Wei Yao, Shiru Song, J. T. Sun, Jinbo Pan, Xiao Ren, Chen Li, Eiji Okunishi, Yu-Qi Wang, Eryin Wang, Yan Shao, Y. Y. Zhang, Hai-tao Yang,Eike F. Schwier, Hideaki Iwasawa, Kenya Shimada, Masaki Taniguchi, Zhaohua Cheng, Shuyun Zhou, Shixuan Du, Stephen J. Pennycook, Sokrates T. Pantelides, and Hong-Jun Gao, "Monolayer PtSe2, a New Semiconducting Transition-Metal- Dichalcogenide, Epitaxially Grown by Direct Selenization of Pt", Nano Lett. 15(6),4013 (2015)

Geng Li, Haitao Zhou, Lida Pan, Yi Zhang, Li Huang, Wenyan Xu, Shixuan Du, Min Ouyang, Andrea C. Ferrari, and Hong-Jun Gao, "Role of Cooperative Interactions in the Intercalation of Heteroatoms between Graphene and a Metal Substrate", J. Am. Chem. Soc. 137(22),7099 (2015)

Lili Jiang, Zhiwen Shi, Bo Zeng, Sheng Wang, Ji-Hun Kang, Trinity Joshi, Chenhao Jin, Long Ju, Jonghwan Kim, Tairu Lyu, Yuen-Ron Shen, Michael Crommie, Hong-Jun Gao, and Feng Wang, "Soliton-dependent plasmon reflection at bilayer graphene domain walls", Nat. Mater. 15, 840, (2016)

YuQi Wang, Xu Wu, Yeliang Wang, Yan Shao, Tao Lei, Jia-Ou Wang, Shi-Yu Zhu, Hai-Ming Guo, Ling-Xiao Zhao, Gen-Fu Chen, Si-Min Nie, Hong-Ming Weng, Kurash Ibrahim, Xi Dai, Zhong Fang, Hong-Jun Gao, “Spontaneous Formation of a Superconductor–Topological Insulator–Normal Metal Layered Heterostructure”, Adv. Mater. 28, 5013, (2016)

X. Lin, J. C. Lu, Y. Shao, Y. Y. Zhang, X. Wu, J. B. Pan, L. Gao, S. Y. Zhu, K. Qian, Y. F. Zhang, D. L. Bao, L. F. Li, Y. Q. Wang, Z. L. Liu, J. T. Sun, T. Lei, C. Liu, J. O. Wang, K. Ibrahim, D. N. Leonard, W. Zhou, H. M. Guo, Y. L. Wang, S. X. Du, S. T. Pantelides and H.-J. Gao, "Intrinsically patterned two-dimensional materials for selective adsorption of molecules and nanoclusters", Nat. Mater., 16, 717 (2017)

W. Yao, E.Y. Wang, H.Q. Huang, K. Deng, M.Z. Yan, K.N. Zhang, K. Miyamoto, T. Okuda, L.F. Li, Y.L. Wang, H.J. Gao, C.X. Liu, W.H. Duan, S.Y. Zhou, “Direct observation of spin-layer locking by local Rashba effect in monolayer semiconducting PtSe2 film”, Nat. Commun, 8, 14216 (2017)

J.D. Ren, H.M. Guo, J.B. Pan, Y.F. Zhang, Y.F. Yang, X. Wu, S.X. Du, M. Ouyang, H.J. Gao, “Interatomic Spin Coupling in Manganese Clusters Registered on Graphene” , Phys. Rev. Lett., 119, 176806 (2017)

Z.H. Qin, J.B. Pan, S.Z. Lu, S. Yan, Y.L. Wang, S.X. Du, H.J. Gao, G.Y. Cao, "Direct Evidence of Dirac Signature in Bilayer Germanene Islands on Cu(111)", Adv. Mater. (Weinheim, Ger.), 29, 1606046 (2017)

X. Wu, Y. Shao, H. Liu, Z. Feng, Y.L. Wang, J.T. Sun, C. Liu, J.O. Wang, Z.L. Liu, S.Y. Zhu, Y.Q. Wang, S.X. Du, Y.G. Shi, K. Ibrahim, H.J. Gao,“Epitaxial Growth and Air-Stability of Monolayer Antimonene on PdTe2”, Adv. Mater. (Weinheim, Ger.), 29, 1605407 (2017)

L. Huang, Y.F. Zhang, Y.Y. Zhang, W.Y. Xu, Y.D. Que, E. Li, J.B. Pan, Y.L. Wang, Y.Q. Liu, S.X. Du, S.T. Pantelides, H.J. Gao, “Sequence of Silicon Monolayer Structures Grown on a Ru Surface: from a Herringbone Structure to Silicene”, Nano Lett., 17, 1161-1166 (2017)

Lili Jiang, Sheng Wang, Zhiwen Shi, Chenhao Jin, M. Iqbal Bakti Utama, Sihan Zhao, Yuen-Ron Shen, Hong-Jun Gao, Guangyu Zhang, and Feng Wang, "Manipulation of domain-wall solitons in bi- and trilayer graphene", Nature nanotechnology 13 (3), 204(2018)

Geng Li, Yu-Yang Zhang, Hui Guo, Li Huang, Hongliang Lu, Xiao Lin, Ye-Liang Wang, Shixuan Du, and Hong-Jun Gao, "Epitaxial growth and physical properties of 2D materials beyond graphene: from monatomic materials to binary compounds," Chem. Soc. Rev. 47 (16), 6073-6100 (2018)

Lei Gao, Jia-Tao Sun, Jian-Chen Lu, Hang Li, Kai Qian, Shuai Zhang, Yu-Yang Zhang, Tian Qian, Hong Ding, Xiao Lin, Shixuan Du, and Hong-Jun Gao, "Epitaxial Growth of Honeycomb Monolayer CuSe with Dirac Nodal Line Fermions," Advanced Materials 30 (16) (2018)

Yan Shao, Zhong-Liu Liu, Cai Cheng, Xu Wu, Hang Liu, Chen Liu, Jia-Ou Wang, Shi-Yu Zhu, Yu-Qi Wang, Dong-Xia Shi, Kurash Ibrahim, Jia-Tao Sun, Ye-Liang Wang, and Hong-Jun Gao, "Epitaxial Growth of Flat Antimonene Monolayer: A New Honeycomb Analogue of Graphene," Nano letters 18 (3), 2133-2139 (2018)


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