二维范德华超晶格及其层间相互作用的研究在近年来发现了许多高度可调的物质新相后受到了越来越多的关注。形成内层和外层纳米管的层

之间不同的原子注册表也可以形成一维(1D) vdW 莫尔超晶格。在这篇综述中，总结了与一维 vdW 莫尔超晶格中层间相互作用有关的实验观

察和理论观点。重点讨论了双壁碳纳米管(DWNTs)——一维 vdW 云纹模型系统，着重讨论了一维 DWNTs 中非平凡的强层间耦合效应和独
特的物理特性所产生的新的光学特性。提出并讨论了在探索一维 vdW 莫尔超晶格中引人注目的物理现象方面的未来发展方向和问题，如在
DWNTs 之外的不同一维莫尔系统中的相关物理。

PERSPECTIVE
透视图
www.advancedscience.com
Www.advancedscience. com

Interlay
Studying two-dimensional (2D) van der Waals (vdW) moiré superlattices and their

er
interlayer interactions have received surging attention after recent discoveries of
many new phases of matter that are highly tunable. Different atomistic registry

Interact
between layers forming the inner and outer nanotubes can also form one-
dimensional (1D) vdW moiré superlattices. In this review, experimental
ions in
observations and theoretical perspectives related to interlayer interactions in 1D
vdW moiré superlattices are summarized. The discussion focuses on double-
1D Van
walled carbon nanotubes (DWNTs), a model 1D vdW moiré system, and the authors
highlight the new optical features emerging from the non-trivial strong interlayer
der
coupling effect and the unique physics in 1D DWNTs. Future directions and
questions in probing the intriguing physical phenomena in 1D vdW moiré
Waals
superlattices such as, correlated physics in different 1D moiré systems beyond

Moiré
DWNTs are proposed and discussed.

Superl
attices
一维 Van der Waals Moiré 超晶格中的层间
相互作用
Sihan Zhao,* Ryo Kitaura,* Pilkyung Moon, Mikito Koshino, and Feng Wang*
赵思寒，吉田良，皮尔京月，木野三木户，王峰
1. Introduction
1、简介
interlayer interactions in layered mate-rials
Van der Waals (vdW) materials represent a large number of nat- with different stacking orders can lead to
ural and artificial layered materials in which the stacking layers profound differences in their electronic
are weakly coupled by the vdW force, yet the atoms within each properties. For example, Bernal-stacked
layer are ionically or covalently bonded.[1,2] Owing to the weak graphite[8–10] and rhombohedral
bonds between the layers, most of vdW materials can be exfo- graphite,[11–13] two stable forms of crys-
liated down to atomically-thin layers.[3–7] Remarkably, the vdW talline graphite, exhibit very different
Van der Waals (vdW)材料是大量的自然和人工层状材料，层 electronic properties. When graphite is
thinned down to the monolayer, the ab-sence
状材料中的叠加层由 vdW 力弱耦合，而每层中的原子是离子
of interlayer interactions makes electrons in
键或共价键。[1,2]由于层之间的弱键，大多数 vdW 材料可以 graphene behave as massless Dirac
被剥离到原子薄层。[3-7]显然，vdW fermions,[14–16] in sharp contrast to the
massive fermions in few layered
graphene.[8,12] Significant effect of inter-
layer interactions was also found in other
vdW layered materials such as, transition
metal dichalcogenides (TMDCs),[5,17–19]
transition metal halides,[20–22] metal phos-
phorus trichalcogenides, etc.[21–23]
不同堆积顺序的层状材料中的层间相互作
用会导致其电子性质的巨大差异。例如，
bernal 堆积石墨[8-10]和菱形石墨[11-13]
 这两种稳定形式的晶体高碳石墨，表现出 the broad exploration of novel physical phenomena in 2D vdW
非常不同的电子性质。当石墨被稀释到单 heterostructures. The formed vdW heterostructures, following the
层时，层间相互作用的消失使得石墨烯中 creation of graphene/hexagonal boron nitride (hBN) het-
的电子表现为无质量的狄拉克费米子[14- erostructures, usually do not have to satisfy the stringent lattice
16] ，这与少数层状石墨烯中的大量费米 matching requirements, and that the interfaces between the layers
can be extremely clean. Since 2018, fabricating artificial
子形成鲜明对比。[8,12]在其他 vdW 层状
二维层状材料的成功隔离以及 vdW 组装技术的发展[24,25]
材料中也发现了显著的层间相互作用效应，
使得对二维 vdW 异质结构中新物理现象的广泛探索成为可能。
如过渡金属二卤化物(TMDCs) ，[5,17-19]
随着石墨烯/六方氮化硼(hBN)热失重结构的形成，所形成的
过渡金属卤化物，[20-22]金属磷-三卤化
vdW 异质结构通常不需要满足严格的晶格匹配要求，层间界
物等[21-23]
The successful isolation of 2D layered materials together with 面可以非常干净。自 2018 年以来，人工制造
the development of vdW assembly technique[24,25] have enabled

S. Zhao P. Moon
赵s 文p
Interdisciplinary Center for Quantum Information Arts and Sciences
量子信息跨学科中心 艺术及科学
Zhejiang Province Key Laboratory of Quantum Technology and NYU Shanghai
Device State Key Laboratory of Silicon Materials Department of 纽约大学上海分校
Physics Shanghai 200122, China
浙江省量子技术与设备重点实验室硅材料物理系国家重点实验室 上海 200122，中国
Zhejiang University P. Moon
浙江大学 文p
Hangzhou 310027, China NYU-ECNU Institute of Physics at NYU Shanghai
杭州 310027，中国 上海纽约大学 ecnu 物理研究所
E-mail: sihanzhao88@zju.edu.cn Shanghai 200062, China
邮箱: sihanzhao88@zju.edu. cn 上海 200062，中国
R. Kitaura M. Koshino Department
R. Kitaura of Physics Osaka
Department of Chemistry University Toyonaka
化学系 560-0043, Japan
Nagoya University 日本大阪大学丰中 560-
名古屋大学 0043 日本丰中 560-
Nagoya 464-8602, Japan 0043
日本名古屋 464-8602
F. Wang
E-mail: r.kitaura@nagoya-u.jp
王先生
电子邮件: r.kitaura@nagoya-u.jp
Department of Physics
物理系
University of California at Berkeley
加州大学伯克利分校
The ORCID identification number(s) for the author(s) of this article Berkeley, CA 94720, USA
can be found under https://doi.org/10.1002/advs.202103460 伯克利，加州 94720，美国
本文作者的 ORCID 标识号可以在 https://doi.org/10.1002/advs. E-mail: fengwang76@berkeley.edu
202103460 下找到 电子邮件: fengwang76@berkeley. edu
© 2021 The Authors. Advanced Science published by Wiley-VCH F. Wang
GmbH. This is an open access article under the terms of the Creative 王先生
Commons Attribution License, which permits use, distribution and Materials Science Division
reproduction in any medium, provided the original work is properly cited. 材料科学部
2021 作者。由 Wiley-VCH GmbH 出版。这是一个开放获取的条款下的 Lawrence Berkeley National
知识共享署名许可证的条款，它允许使用，分配和复制在任何媒体，只要 Laboratory Berkeley, CA USA
美国加州伯克利劳伦斯伯克利国家实
原作品被正确引用。
验室
DOI: 10.1002/advs.202103460 F. Wang
DOI: 10.1002/advs. 202103460 王先生
Kavli Energy NanoSciences Institute at University of California
Berkeley and Lawrence Berkeley National Laboratory Berkeley,
CA 94720, USA
加州大学伯克利分校 Kavli 能源纳米科学研究所和劳伦斯伯克利国
家实验室伯克利，加州 94720，美国

Adv. Sci. 2022, 9, 2103460 2103460 (1 of 15) © 2021 The Authors. Advanced Science published by Wiley-VCH GmbH
2022,9,21034602103460(1 of 15)2021 作者: Wiley-VCH GmbH
www.advancedsciencenews.com www.advancedscience.com
Www.advancedsciencenews.com www.advancedscience.com

Figure 1. Strongly correlated phenomena induced by interlayer coupling in 2D moiré superlattices. a) Twisted bilayer graphene (TBG) near the magic
angle (i.e., MATBG) has a triangular lattice with alternating AA and AB/BA stacking orders in the moiré supercell. AA sites appear higher in the STM
topology and hold large local density of states (DOS). b) Phase diagram of MATBG. Correlated states (CS) appear at all the integer fillings of the
moiré band, which are accompanied by superconducting (SC) phases. Two green arrows indicate the integer fillings at v = ±2. c) Quantum
anomalous Hall (QAH) showing quantized Hall resistance in MATBG aligned with hBN at an integer filling v = 3. The observed quantized Hall signal
at B = 0 comes from a pure orbital magnetism and indicates an incipient topological Chern insulator as a result of interaction -induced spontaneous
time-reversal symmetry breaking. d) Mott insulating states (half-filling of the moiré hole band at v = −1) and generalized Wigner crystal insulating
states (fractional fillings at v = −1/3 and v = −2/3) were observed in angle-aligned TMDC (WS2/WSe2) moiré superlattices by an effective capacitance
measurement. Insets show the localized hole positions (red balls) on the moiré superlattice at v = −1 and v = −1/3. e) A diverse set of Wigner crystal
[42]
states beyond 1/3 and 2/3 fillings also exist in the WS 2/WSe2 moiré system. a) Reproduced with permission. Copyright 2019, Springer Nature
[41] [61]
Limited. b) Reproduced with permission. Copyright 2019, Springer Nature Limited. c) Reproduced with permission. Copyright 2020, American
[49]
Association for the Advancement of Science. d) Reproduced with permission. Copyright 2020, Springer Nature Limited. e) Reproduced with
[51]
permission. Copyright 2020, Springer Nature Limited.
图 1。二维莫尔超晶格中层间耦合引起的强相关现象。A)双层扭曲石墨烯(TBG)在莫尔超单元中具有交替的 AA 级和 AB/BA 级的三角晶格。AA 位点
在 STM 拓扑结构中显得更高，并且具有较大的局域态密度(DOS)。B) MATBG 的相图。相关态(CS)出现在莫尔带的所有整数填充物上，并伴随着超导
(SC)相。两个绿色箭头表示 v = ± 2 的整数填充。C)显示在整数填充 v = 3 时与 hBN 对齐的 MATBG 中的量子化 Hall 电阻的量子异常 Hall (QAH)。观
察到的 b = 0 的量子化 Hall 信号来源于纯轨道磁性，表明由于相互作用诱导的自发时间反转对称性破缺，产生了一个早期的拓扑 Chern 绝缘子。D)采
用有效电容测量方法，在角排列的 TMDC (WS2/WSe2)云纹超晶格中观察到 Mott 绝缘态(v =-1 的云纹空穴带的半填充)和广义 Wigner 晶体绝缘态(v
=-1/3 和 v =-2/3 的分数填充)。Insets 显示在 v =-1 和 v =-1/3 处莫尔超晶格上的局部空穴位置(红球)。E)在 WS2/wse2 莫尔系统中也存在超过 1/3 和
2/3 填充的多种 Wigner 晶体状态。A)经许可复制。版权所有 2019，Springer Nature Limited。B)经许可转载。版权所有 2019，Springer Nature
Limited。C)经许可转载。版权所有 2020 年，美国科学进步协会。D)转载许可。[49]版权 2020，Springer Nature Limited。E)经许可转载。版权所有
2020，Springer Nature Limited。
systems of MATBG (Figure 1a–c) and TMDC (Figure 1d,e) vdW
heterostructures.
moiré superlattices has provided a powerful tool to engineer the 莫尔超晶格为二维材料的电子能带结构和性质的设计提供了强有
electronic band structures and properties of 2D materials that are 力的工具。[26-39]在二维莫尔超晶格中发现了许多有趣的新物质
otherwise difficult by conventional techniques in bulk materials. [26–39] 相，包括魔角扭曲双层石墨烯(MATBG)中的 Mott 和超导现象，
Many fascinating new phases of matter have been discovered in 2D 以及与 hBN 对齐的 ABC 三层石墨烯，TMDC 莫尔超晶格中的莫
moiré superlattices,[32,33,40–64] including Mott and superconductivity 尔激子[45-48]和 Wigner 晶体状态[49-52]。莫尔超晶格中的层间
ground states in magic-angle twisted bilayer graphene 电子耦合导致莫尔平坦微带的形成。[29,53-59]因此，现场和/或
(MATBG)[32,33,40,41] and ABC trilayer graphene aligned with 远程库仑相互作用可以成为主导的动能和导致强相关的电子态。
二维 vdW 莫尔超晶格还为研究强相关电子系统中的非平凡拓扑
hBN,[43,44] and moiré excitons[45–48] and Wigner crys-tal states[49–52]
性质提供了一个独特的场所，在这个系统中，多体电子-电子库仑
in TMDC moiré superlattices, which are achieved by a delicate control
of doping and/or bandwidth in a single bench-top device. Interlayer 相互作用可以引起对称破缺。[60-64]在工作装置中实现强磁状态
electronic coupling in moiré super-lattices leads to the formation of (纯轨道磁性)[60-62]和超导开关[65-67]的电气控制，有望在利用
moiré flat minibands.[29,53–59] Consequently, the on-site and/or long- 可调超导电路实现电可写磁存储器和量子信息计算方面提供强相
range coulomb interac-tions can become dominant over the kinetic 关的二维莫尔超晶格。图 1 中展示的作品概括了最近在 MATBG
energy and lead to strongly correlated electronic states. 2D vdW moiré (图 1a-c)和 TMDC (图 1d，e) vdW 异质结构系统中云纹图诱导的
superlattices also provide a unique playground for studying the non- 相关物理现象的实验结果。
trivial topological properties in a strongly correlated electronic system
in which many-body electron-electron Coulomb interactions can
induce symmetry-breakings.[60–64] Realization of an electrical control
of robust magnetic states (pure orbital magnetism)[60–62] and
superconducting switches in working devices [65–67] delivers promise
of strongly correlated 2D moiré superlattices in the ap-plication of
electrically-writable magnetic memory and quantum information
computing using tunable superconducting circuits. The works
displayed in Figure 1 represent a summary of recent experimental
findings of moiré pattern-induced correlated phys-ical phenomena in

Compared with the exciting developments in 2D vdW moiré
superlattices, 1D moiré superlattices have been little explored. In
the following, we first introduce 1D moiré superlattices and the
interlayer interactions using a representative vdW material in 1D,
double-walled carbon nanotubes (DWNTs). Then we briefly re-
view previous results on the mechanical and transport properties
of structure-identified DWNTs. We then focus on the optical spec-
troscopy studies of interlayer interactions in structure-identified
DWNTs, which revealed new insights of the interlayer interac-
tions in 1D moiré systems, with highlighting the unique physics of
1D moiré systems. Finally, we will discuss the future directions
and outlook of studying the 1D moiré superlattices and 1D moiré
physics.
与 2d vdW 莫尔超晶格的令人兴奋的发展相比，1D 莫尔超
晶格几乎没有被探索。在下文中，我们首先介绍了一维莫尔
超晶格和层间相互作用的代表性材料 vdW 在一维，双壁碳纳
米管(DWNTs)。然后，我们简要回顾以前关于结构识别的
DWNTs 的力学和输运性质的结果。然后重点研究了结构识别
的 DWNTs 中层间相互作用的光谱学研究，揭示了一维云纹
系统中层间相互作用的新见解，突出了一维云纹系统的独特
物理特性。最后，我们将讨论研究一维莫尔超晶格和一维莫
尔物理的未来方向和前景。
Adv. Sci. 2022, 9, 2103460 2103460
科学期刊 2022,9,21034602103460(2 of 15)2021 作者: Wiley-VCH GmbH
2. Interlayer Interactions in 1D Moiré Superlattices
2. 一维莫尔超晶格中的层间相互作用
When two or more vdW layered materials are concentrically
rolled up, they form 1D moiré superlattices. Double-walled and
multi-walled carbon,[68–72] boron nitride,[73,74] TMDC [75] nan-
otubes and their heterostructures[76,77] are among the available
material list of 1D vdW moiré superlattices.
当两个或两个以上的 vdW 层状材料同心卷起时，它们就形成
了一维莫尔超晶格。双壁和多壁碳，[68-72]氮化硼，[73,74]
TMDC [75]纳米管及其异质结构[76,77]是一维 vdW 莫尔超晶
格的可用材料列表。
2.1. A Model System of 1D Moiré Superlattices:
Double-Walled Carbon Nanotubes
2.1. 一维莫尔超晶格模型体系: 双壁碳纳米管
DWNTs provide one of the ideal model systems to study the in-
terlayer interactions in 1D moiré superlattices because the phys-
ical properties of a DWNT depend on the combination of the
DWNT 是研究一维莫尔超晶格层间相互作用的理想模型系统
之一，因为 DWNT 的物理性质取决于层间相互作用的组合
(2 of 15) © 2021 The Authors. Advanced Science published by Wiley-VCH GmbH
www.advancedsciencenews.com www.advancedscience.com
Www.advancedsciencenews.com www.advancedscience.com

Figure 2. VdW-coupled 1D DWNT moiré superlattice. a) Structure model of a DWNT composed of two vdW-coupled SWNTs. b) STM topology image
of an isolated DWNT showing a spatially-modulated moiré pattern. c) The rigid lattice model of a DWNT reproducing the observed moiré pattern in b).
SWNTs (25,20) and (21,32) are used in panel c) for the inner and outer nanotubes. d) Electron diffraction pattern of an DWNT with chirality
(16,6)@(22,11). There are total 4 sets of hexagons in its diffraction pattern, two each belonging to each nanotube. The equatorial line oscillates in
intensity with E and e representing the long and short periods. Distances for features outside the equatorial line to the equatorial line (e.g., do2 and
do3 for the outer SWNT and di2 and di3 for the inner SWNT) are used to uniquely determine the DWNT chirality in conjunction with the measured E
and e. b,c) Reproduced with permission.[85] Copyright 2013, ELSEVIER. d) Reproduced with permission.[86] Copyright 2014, Springer.
图 2。Vdw 耦合的一维 DWNT 莫尔超晶格。A)由两个 vdw 耦合的 SWNTs 组成的 DWNT 的结构模型。B)显示空间调制的莫尔模式的孤立 DWNT 的
STM 拓扑图像。C) DWNT 的刚性格子模型在 b 中重现观察到的莫尔模式)。图 c 中使用 SWNTs (25,20)和(21,32)作为内部和外部纳米管。D)具有手性
(16,6)@(22,11)的 DWNT 的电子衍射图案。衍射图案中共有 4 组六边形，每个六边形属于一个纳米管。赤道线的振荡强度为 e，e 代表长周期和短周期。
赤道线以外的特征与赤道线的距离(例如，外部 SWNT 的 do2 和 do3，以及内部 SWNT 的 di2 和 di3)是用来独特地确定 DWNT 的手征性，并结合所
测量的 e 和 e，b，c)经许可复制。[85]版权 2013，ELSEVIER。D)经许可转载。版权所有 2014，Springer。

two components,[78–81] non-interacting single-walled carbon nan- slow ones (with period E). This originates from the interference of
otubes (SWNTs). The electronic property of each SWNT is physi- electron waves scattered by two nanotubes in the radial direc-tion.
cally determined by a chiral vector with two integer components Because of the high sensitivity of the wave interference to
(also known as chirality). Conventionally, the two chiral vectors diameter and/or chirality of each nanotube, the equatorial line
for inner and outer SWNTs in a DWNT are represented by C and profile serves as a decisive feature for the unambiguous determi-
nation of the DWNT structure. By measuring the distances from
C′,[78] respectively, where
features outside the equatorial line to the equatorial line, for ex-
两个组件，[78-81]非相互作用的单壁碳纳米管(SWNTs)。每
ample, do2 and do3 from outer SWNT and di2 and di3 from inner
个 SWNT 的电子性质是由具有两个整数分量(也称为手性)的
SWNT, the DWNT physical structure can be fully obtained by us-
手性向量物理确定的。传统上，DWNT 中内部和外部 SWNTs
ing a set of equations:[89]
的两个手性载体分别由 c 和 c’表示[78] ，其中
缓慢的(e 期)。这起源于两个纳米管在径向上散射的电子波的
( )
C = n1a1 + n2 a2 = n1, n2 干涉。由于波干涉对每个纳米管的直径和/或手性的高度敏感
C = n1a1 + n2a2 = n1， n2 性，赤道线轮廓是确定 DWNT 结构的决定性因素。通过测量
从赤道线以外的地物到赤道线的距离，例如外部 SWNT 的
and
do2 和 do3 以及内部 SWNT 的 di2 和 di3，可以通过一组方程
和
式完全得到 DWNT 的物理结构: [89]
(1) n 2di −E), (2di2 −
(1) 1 3 − di2) n2 di3) ( e −
C′ = n1′ a1 + n2′ a2 = (n1′, n2′) N 2di ( e - e) ， (2di2- E ) ,
C ′ = n1′ a1 + n2′ a2 = (n1′ ，n2′) - di2)(e) n2 = 3 di3) (e-e)、,
1 = 3 1 1 1 1
with a1 and a2 denoting the unit lattice vectors of 2D √3 √

graphene n ), (2do2 − (
A1 和 a2 表示二维石墨烯的单位晶格矢量 √3 (
1′ 2d −
sheet. The chiral angle of a specific SWNT is ) n2 do3 e
N o3 do2
defined as 1 2d ( e+ E) ， (2do2- (e + E )
Do
特定单壁碳纳米管的手征角定义为 ’ =3 (o3 2 )(e + e n2 = 3 do3 ) ) + e)
= cos−1 2n1 + n2 (2) 1 1 ′ 1 1
= cos-1 2n1 + n2 (2) √ (3)
n12 + n22 + √ (3)
n1n2
N12 + n22 +
2 √ n1n2

constrained within 0° ≤ ≤ 30°. The physical structure of a DWNT is denoted as C@C′. In a DWNT, the inner and outer SWNTs are
coupled by vdW interactions (Figure 2a) with inter-layer distance ranging from 0.30–0.40 nm.[82,83] It is still debat-able if there is any
correlation of chiral angles between the inner and outer SWNTs,[82–84] and the answer may depend on the syn-thesis method by which
the DWNT samples are produced. The DWNT forms a generic 1D moiré superlattice in analogy with the 2D counterpart. Formation of
1D moiré superlattices has been clearly observed in real space by scanning tunneling microscopy (STM) (Figure 2b,c).[85]
约束在 0 ° ≤≤30 ° 。DWNT 的物理结构表示为 c@C’。在 DWNT 中，内部和外部 SWNTs 通过 vdW 相互作用耦合(图 2a) ，层
间距离为 0.30-0.40 nm。[82,83]内外单壁碳纳米管之间是否存在手性角的相关性仍然存在争议[82-84] ，其答案可能取决于生产
双壁碳纳米管样品的合成方法。DWNT 形成类似于 2d 对应物的通用 1d 莫尔超晶格。通过扫描隧道显微镜(STM)在实际空间中
清楚地观察到一维莫尔超晶格的形成(图 2b，c)。[85]
The physical structure (i.e., moiré superlattice) of an individual DWNT so far can only be unequivocally determined by electron beam
diffractions.[82–84,86–89]Figure 2d shows a typical diffraction pattern of an isolated DWNT and illustrates how the chirality of two constituent
SWNTs are determined.[86] The diffraction pat-tern of a DWNT typically exhibits two sets of mutually twisted hexagonal patterns belonging to
two constituent SWNTs.[90–92] The equatorial line in the DWNT diffraction pattern (perpendic-ular to the DWNT axis in real space) exhibits a
“beating-like” be-havior with the fast oscillations (with period e) modulated by the
 The determined structure of Figure 2d using Equation (3) is (16,6)@(22,11),[86] whose result is further compared and corrob-orated
by simulations.