二硫化钼的电子能带结构和低温输运实验进展

吴帆帆; 季怡汝; 杨威; 张广宇

doi:10.7498/aps.71.20220015

摘要

二硫化钼是一种层状的过渡金属硫族化合物半导体, 它在二维自旋电子学、谷电子学及光电子学领域有很多的应用. 本综述以二硫化钼为代表, 系统介绍其单层、双层及转角双层的堆垛和能带结构; 介绍了转角双层莫尔超晶格的制备方法、以及低温电学输运方面的实验进展, 例如超导和强关联现象; 分析了转角过渡金属硫化物莫尔超晶格在优化接触和样品质量等方面存在的一些挑战, 并展望该领域未来的发展.

关键词:

Molybdenum disulfide is a layered transition metal chalcogenide semiconductor. It has many applications in the fields of two-dimensional spintronics, valleytronics and optoelectronics. In this review, molybdenum disulfide is taken as a representative to systematically introduce the energy band structures of single layer, bilayer and twisted bilayer molybdenum disulfide, as well as the latest experimental progress of its realization and low-temperature electrical transport, such as superconductivity and strong correlation phenomenon. Finally, two-dimensional transition metal chalcogenide moiré superlattice’s challenges in optimizing contact and sample quality are analyzed and the future development of this field is also presented.

Keywords:

作者及机构信息

1.
中国科学院物理研究所, 北京凝聚态物理国家研究中心, 北京　100190

2.
中国科学院大学物理科学学院, 北京　100049

3.
松山湖材料实验室, 东莞　523808

通信作者: 杨威, wei.yang@iphy.ac.cn

基金项目: 国家重点研发计划(批准号: 2020YFA0309600, 2021YFA1202900)、国家自然科学基金 (批准号: 11834017, 61888102)、中国科学院战略性先导科技专项 B (批准号: XDB30000000, XDB33000000)和广东省重点领域研发计划(批准号: 2020B0101340001)资助的课题

Authors and contacts

1.
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China

2.
School of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China

3.
Songshan Lake Materials Laboratory, Dongguan 523808, China

Corresponding author: Yang Wei, wei.yang@iphy.ac.cn

Funds: Project supported by the National Key Research and Development Program of China (Grant Nos. 2020YFA0309600, 2021YFA1202900), the National Natural Science Foundation of China (Grant Nos. 11834017, 61888102), the Strategic Priority Research Program of Chinese Academy of Sciences (Grant Nos. XDB30000000, XDB33000000), and the Key-Area Research and Development Program of Guangdong Province, China (Grant No. 2020B0101340001).

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施引文献

图 1 单层二硫化钼　(a) 2H相原子结构示意图^[36]; (b) 准粒子自洽格林函数方法计算得到的能带结构^[37]; (c) 荧光谱^[42]; (d) 朗道扇形图^[58]; (e) 谷霍尔效应示意图

Fig. 1. Single layer molybdenum disulfide: (a) Schematic diagram of atomic structure of 2H phase^[36]; (b) energy band structure obtained by quasiparticle self-consistent GW (QSGW) method ^[37]; (c) photoluminescence spectra^[42]; (d) Landau fan^[58]; (e) schematic of valley hall effect.

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图 2 双层二硫化钼的能带结构与物性　(a) 本征双层二硫化钼的原子结构示意图; (b) 准粒子自洽格林函数方法计算得到的能带结构图^[37]; (c) 电场可调的谷霍尔效应^[72]; (d) 转角双层二硫化钼中的莫尔超晶格结构^[88]; (e) 2.65°转角的双层二硫化钼的价带能带结构^[88]; (f) 非平庸的拓扑子能带^[100]

Fig. 2. Bilayer molybdenum disulfide’s band structure and physical properties: (a) Atomic structure of natural double-layer molybdenum disulfide; (b) QSGW calculated band structure^[37]; (c) electric field tunable valley Hall effect^[72]; (d) moiré superlattice in twisted bilayer molybdenum disulfide^[88]; (e) valence band structure of twisted bilayer molybdenum disulfide with 2.65°^[88]; (f) non-trivial topological flat bands^[100].

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图 3 精准制备不同转角的多层同质结　(a), (e)“捡起堆叠”法示意图, 红色框表示半球形基板的放大视图^[109]; (b)—(d) 示意图过程和 (f)—(h) 相应步骤的光学结果, (b) 和 (f) 表示基板和底部单层石墨烯的部分接触^[109]; (i) 利用聚二甲基硅氧烷 (PDMS) 作为媒介, 将分割好的定向单层二硫化钼堆叠成所需转角^[108]; (j) 在沉积300 nm二氧化硅的硅衬底上, 具有精确控制的转角多层MoS₂薄膜^[108]

Fig. 3. Twist angle engineering of multilayer homostructures. (a), (e) Schematic of layer pick-up. The red box represents a zoom-in view of the hemispherical handle substrate^[109]. (b)–(d) Schematics and (f)–(h) corresponding optical micrographs of successive stacking steps. Panels (b) and (f) illustrate a partial contact of the handle with the bottom graphene^[109]. (i) The water-assisted transfer process. Polydimethylsiloxane (PDMS) are used as transfer medium^[108]. (j) Image of multilayer MoS₂ films with precise-controlled twist angles on Si substrates with 300 nm SiO₂^[108].

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图 4 转角双层二硫化钼中可能存在的强关联现象　(a) 关联绝缘态, 红线代表莫特绝缘态; 蓝色区域代表电荷局域态与费米液体共存的状态, 称为轨道选择性莫特态; 黑色虚线内代表近藤晶格模型^[101]; (b) 整数填充附近的超导相变; (c)量子反常霍尔效应; (d) 魏格纳晶格态, 图(d)表示了2/3电子填充态^[123]; (e) 量子临界行为, 红色和蓝色区域表示电阻随温度的依赖关系, 其中α ≠ β

Fig. 4. Strong correlation phenomenon predicted in twisted bilayer MoS₂. (a) Schematic phase diagram. A charge localized state of one species can coexist with a Fermi liquid state of the other, which is known as the orbitally selective Mott (OSM) state. Inside the region marked by the dashed black line the essential ingredients of a Kondo lattice model are realized. The red lines indicate correlated insulating states^[101]. (b) Superconductivity in the doped Mott insulator. (c) Quantum anomalous Hall effect. (d) Wigner Crystal state. The figure shows representative 2/3 electron filling^[123]. (e) Quantum critical behaviors in which α≠β. The blue and red regions indicate the resistance dependence on temperature.

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1. 引　言

二维层状过渡金属硫族化合物(TMDs)由于其原子级厚度和合适的半导体带宽成为当下研究最热门的二维材料之一. TMDs的通用表达式为MX₂, M代表过渡金属元素包括Nb, Ta, Mo, W, Re等; X代表硫族元素包括S, Se, Te等^[1]. 其中, 以2H相的MoS₂, MoSe₂, WS₂和WSe₂ 四种半导体材料的研究居多, 它们都在空气中具有很好的稳定性^[2]. 同时, TMDs原子在层内通过强的化学键结合, 在层间通过弱的范德瓦耳斯力组合起来, 因此可通过机械剥离法得到单层样品. 除了机械剥离法, 人们还可以用化学气相沉积^[3-5]、分子束外延^[6,7]的方法获取大面积的单层样品, 甚至制备出高质量的晶圆级单层二硫化钼^[8-10].

由于这些二维半导体材料的带隙分布非常广, 从近红外波段到可见光波段, 因此具有丰富的电学和光学性能^[11]. 以二硫化钼为代表的单层TMDs中具有许多与电子自由度相关的独特性质. 单层的二硫化钼作为一个直接带隙的半导体, 其导带和价带的极值均位于六方布里渊区的K和–K点, 因此主要由K谷和–K谷电子决定了它的电学和光学性质^[12,13]. 单层TMDs中一个最重要的性质是激子的光学跃迁遵循与谷有关的选择定则^[14,15]: K谷的激子只和右旋极化光耦合, –K谷只和左旋极化光耦合, 因此材料的能谷信息可以和不同手性的光对应起来, 从而实现谷赝自旋的量子调控^[16,17]. 不同于单层的过渡金属硫族化合物, 双层及以上的TMDs材料一般都是间接带隙半导体, 带隙大小随着层数增加呈减小趋势, 导带的底部从K谷转移到了Q谷, 价带顶从K谷转移到Γ谷^[18,19]. 一方面, TMDs的载流子迁移率普遍比单层石墨烯低很多, 主要是和其抛物线型的能带结构(较大的电子有效质量)以及较大的带隙有关^[20]. 另一方面, TMDs载流子很高的电子有效质量^[21-23]和面内电荷的屏蔽降低^[24], 意味着其中电子相互作用会很强^[25], 因此是研究复杂的量子多体相互作用的一个很好的平台. 除了值得探究的输运性质以外, TMDs材料特殊的能带结构使得它具有有趣的激子行为. 激子作为固体中的一种元激发, 其状态与材料的电子能带结构和外场作用有关. 光学实验证明了在单层TMDs中存在与直接跃迁相关的激子, 而且由于存在强大的库仑相互作用, 它们的激子束缚能高达几百个毫电子伏特^[26,27]. 同时, 由于直接跃迁不需要声子辅助, 单层TMDs发光跃迁的概率很大, 可以成为很强的发光中心. TMDs的荧光发射还容易受到电场调控, 尤其是层间激子在空间电场的调控下形成荧光峰位随电场移动的量子限制斯塔克效应^[28]. 激子效应对半导体中光吸收、光学非线性作用等物理过程具有重要影响. 在实际应用中, 基于单层TMDs的p-n结可实现高效的电致发光^[29,30]. 最近热门的“魔角石墨烯”推动了对转角TMDs体系的研究, 莫尔超晶格是能够调节电子的动能和势能比, 为研究强关联物理现象提供了一个方便的平台. TMDs转角体系中发现了关联绝缘态、超导、相变与量子临界行为、量子反常霍尔效应等诸多有趣的现象^[31-34], 涵盖了凝聚态物理中几个最热门的方向. 同时, 由于简单的结构, TMDs莫尔超晶格有望成为三角晶格上哈伯德模型的量子模拟器^[35]. 综上所述, TMDs的这些独特性质可以让它们在场效应晶体管、光电器件、电子自旋、低温强关联量子现象等多方面大展身手. 本文主要综述了单双层及转角双层二硫化钼中的新奇电子能带特性和有关的实验进展.

5. 总　结

单层二硫化钼具有很新奇的电学性质包括带边载流子的谷赝自旋, 谷相关贝利曲率, 强自旋-轨道耦合导致的自旋谷锁定效应, 强库仑相互作用等. 虽然二硫化钼的晶格结构复杂, 但是其输运和光学性质主要由带边的K谷来决定, 是一个相对简单的有质量的费米子模型. 双层二硫化钼的性质很容易受到电场调控, 可以用来调控自旋和谷电子学并实现一些应用. 二硫化钼具备较大的载流子有效质量和强电子相互作用, 具备成为强关联体系的要素. 通过构建合适的莫尔超晶格结构, 人们在输运上可以看到例如超导、关联绝缘态、铁磁态等有意思的物理现象. 最近两年这一领域的研究刚热门起来, 无论是理论还有实验均不完善, 意味着我们有很多机会去探索新的基础物理现象以及潜在的应用.

随着对二硫化钼内在输运物理的理解, 制备出的器件迁移率越来越高, 工艺经验不断积累, 包括保持干净的接触界面、功函数匹配、六方氮化硼封装、石墨烯接触等. 但是在满足强关联物理所需的较低掺杂浓度范围内, 目前的器件接触还有待提高. 最近报道称利用铋金属作为二硫化钼的接触电极会达到零肖特基势垒^[124], 这对二硫化钼的低温电输运研究提供了一个可行的方案. 但是如何兼容目前的诸多工艺并提高样品与器件的质量依然存在挑战^[125], 仍需多个领域的学者共同努力. 可以预见, 二硫化钼的研究和应用依然是一个未来活跃的领域.

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二硫化钼的电子能带结构和低温输运实验进展