1. School of Physics and Wuhan National High Magnetic Field Center, Huazhong University of Science and Technology, Wuhan 430074, China
2. International Center for Quantum Materials, School of Physics, Peking University, Beijing 100871, China
3. Beijing Academy of Quantum Information Sciences, Beijing 100193, China
4. CAS Center for Excellence in Topological Quantum Computation, University of Chinese Academy of Sciences, Beijing 100190, China
5. Center for Advanced Quantum Studies, Department of Physics, Beijing Normal University, Beijing 100875, China
jinhua@hust.edu.cn
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Received
Accepted
Published
2022-08-16
2022-10-19
2023-02-15
Issue Date
Revised Date
2022-11-15
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Abstract
We report that the twisted few layer graphite (tFL-graphite) is a new family of moiré heterostructures (MHSs), which has richer and highly tunable moiré flat band structures entirely distinct from all the known MHSs. A tFL-graphite is composed of two few-layer graphite (Bernal stacked multilayer graphene), which are stacked on each other with a small twisted angle. The moiré band structure of the tFL-graphite strongly depends on the layer number of its composed two van der Waals layers. Near the magic angle, a tFL-graphite always has two nearly flat bands coexisting with a few pairs of narrowed dispersive (parabolic or linear) bands at the Fermi level, thus, enhances the DOS at EF . This coexistence property may also enhance the possible superconductivity as been demonstrated in other multiband superconductivity systems. Therefore, we expect strong multiband correlation effects in tFL-graphite. Meanwhile, a proper perpendicular electric field can induce several isolated nearly flat bands with nonzero valley Chern number in some simple tFL-graphites, indicating that tFL-graphite is also a novel topological flat band system.
Moiré heterostructures (MHSs) have drawn great research interest recently [1-8]. The celebrated example is the twisted bilayer graphene (TBG), in which two atomically thin van der Waals (vdW) layers, i.e., graphene monolayers here, are stacked with a controlled twist angle . A small twist angle results in a long period moiré superlattice. Most importantly, the moiré interlayer hopping (MIH) will give rise to two nearly flat bands, when approaches the so-called magic angles [9-14]. Due to the divergent DOS of the moiré flat bands, exotic correlation phenomena, e.g., superconductivity and Mott insulator, have been observed in experiments [1-7], and intensively studied with various theoretical methods [15-28].
Further studies indicate that the moiré flat bands exist in a variety of MHSs, such as twisted double bilayer graphene [29-39], twisted trilayer graphene [40-47], twisted rhombohedral (ABC) multilayer graphene [48], trilayer graphene on boron nitride [49-51] and transition metal dichalcogenide heterostructures [52-57]. Note that, in all the above-mentioned MHSs, the low energy moiré band structures are in some sense similar, i.e., two moiré flat bands at Dirac Point isolated from other high energy bands. This is because that their vdW layers, like graphene monolayer, bilayer, ABC stacked multilayer, etc., just happen to have two low energy bands near the Fermi level , which are hybridized by the MIH to form the two flat bands. In this work, we report a new family of moiré flat band systems, twisted few-layer graphite (tFL-graphite), which have richer and highly controllable moiré flat band structures entirely distinct from all the known MHSs. It is noteworthy that tFL-graphite has a similar band structure to double twisted trilayer garphene, which has been paid special attention to in recent experiments and was reported that unconventional superconductivity [58-60].
Typical tFL-graphites are shown in Fig.1. Here, few layer graphite (FL-graphite) refers to multilayer graphene with Bernal (AB) stacking, in contrast to that with rhombohedral one. Generally, an M + N tFL-graphite is composed of two FL-graphites (red and green in Fig.1) stacked on top of each other with a twist angle , where M (N) is the layer number of the top (bottom) FL-graphite. We assume that N ≥ M without loss of generality, and only focus on the cases with N ≥ 3. So, the simplest tFL-graphite here is the A + ABA (or 1 + 3) configuration, where A is the top monolayer (red) and ABA is the bottom ABA stacked trilayer (green) [see Fig.1 (c)].
The distinct moiré band structure of tFL-graphite mainly results from the richer electronic structure of FL-graphite. It is known that an N-layer FL-graphite has electron-like bands and hole-like bands touching at the Dirac points if is even, while an additional pair of linear bands appears for an odd N [62-64]. Thus, it is natural to expect a rather different moiré band structure in the tFL-graphite. And, as we will see later, twist actually has different influences on the bands of FL-graphite.
We theoretically calculate the electronic structures of tFL-graphites based on a continuum model. Our results show that the electronic structure of a tFL-graphite strongly depends on the layer number of its composed vdW layers, which always has two moiré flat bands coexisting with a few pair of parabolic (or linear) narrow bands near the magic angle. For an M + N tFL-graphite, the main characteristics of its moiré band structures are summarized as follows: (i) The number of the moiré bands at is determined by N, i.e., the layer number of the thicker vdW layer, where it has N (N + 1) moiré bands if N is even (odd). (ii) Near the magic angle (about ), two of these moiré bands become flat, while others are still parabolic or linear at the Dirac points with narrowed bandwidth. (iii) We can get four isolated nearly flat bands with various nonzero valley Chern number by applying a proper electric field in the N = 3 cases.
Due to the unique electronic structures, the tFL-graphite has several great advantages as an intriguing MHS. (i) It has a richer and more flexible moiré band structure than the known MHSs, which can be dramatically changed by choosing different layer number. (ii) The coexistence of flat bands and other dispersive bands will not only enhance the density of states (DOS) at , but also may meet the demand for the enhancement of superconductivity according to the steep band/flat band scenario [65, 66]. Both these two points imply that stronger multiband correlation effects, e.g., superconductivity at higher temperature, may occur in the tFL-graphite. (iii) It is a promising platform to study correlation effects in topological bands. (iv) The sample preparation of tFL-graphite may not be too challenging [67]. Note that natural graphite is Bernal stacked (more stable than the ABC graphene multilayers), and FL-graphite can be directly obtained by mechanical exfoliation.
2 Continuum model
Similar as the TBG, the required in the commensurate cases is determined by an integer , where . The corresponding lattice vectors of the moiré supercell are and , while and are the lattice vectors of graphene with lattice constant . The moiré Brillouin zone (BZ) is given in Fig.1(b) (black), which is determined by the BZ of the top vdW layer (red) and that of the bottom layer (green). The reciprocal lattice vectors can be obtained from , and () is the Dirac point corresponding to the top (bottom) layer [see Fig.1 (b)].
The effective continuum model is used to describe the tFL-graphite [10-12]. For an M + N tFL-graphite, the Hamiltonian is
where , and is the rotation matrix. () is the Hamiltonian of M-layer (N-layer) FL-graphite [62-64, 68]. For example, is the Hamiltonian of the ABA trilayer
where is the low-energy effective Hamiltonian for graphene monolayer and is the interlayer hopping
Here, , with for the two different valley in multilayer graphene. is the vertical hopping and (i = 3, 4). and are the remote interlayer hoppings, which stand for the trigonal warping and electron-hole asymmetry, respectively. The moiré interlayer coupling is , where
Here, is an matrix with only one nonzero matrix element , , . At last, in Eq. (1) is a diagonal matrix denoting the perpendicular electric field induced potential in layers, where we set the potential difference between adjacent two layers is [61].
3 Moiré bands of the simplest tFL-graphite
Most of the moiré band characteristics of tFL-graphite can be seen from the simplest tFL-graphites, i.e., N = 3 and M = (1, 2, 3). The calculated moiré bands are given in Fig.2, each row of which corresponds to one structure of tFL-graphite. Here, we use a minimal model, only including the dominating interlayer hopping in Eq. (3), to illustrate the ideal flat bands at the magic angle. We also use a full parameter model to account for the realistic situations, where the influence of and are considered [61]. The first to fourth columns in Fig.2 are the moiré bands with , , and , respectively. Corresponding DOS is also plotted.
First of all, tFL-graphite has more moiré bands than all the known MHSs at . For example, all the cases (N = 3) in Fig.2 have four moiré bands at , instead of two like in TBG. It is because that the low energy moiré bands of a tFL-grapite are constructed by hybridizing the bands of top and bottom vdW layers near the Dirac points via the MIH. In TBG, each vdW layer has two linear bands near the Dirac point. But in the A + ABA tFL-graphite, the top vdW layer (monolayer) has two linear bands, while the bottom vdW layer (ABA-trilayer) has four bands, i.e., a parabolic electron band, a parabolic hole band and a pair of linear bands. As shown in Fig.2(a)−(d), the MIH hybridizes the two parabolic bands of the bottom ABA-trilayer with the two linear bands of the top monolayer (red lines), while the remaining two linear bands of the ABA-trilayer are modified into two other moiré bands at (blue lines). Thus, there are four moiré bands near in the A + ABA tFL-graphite. The moiré bands of BA + ABA [Fig.2(e)−(h)] and ABA+ABA [Fig.2(i)−(l)] tFL-graphites can be understood in a similar way. Generally, for an M + N tFL-graphite, the number of moiré bands at is equal to that of the thicker vdW layer, i.e., it has moiré bands () if N is even (odd) when N ≥ M. Half of the moiré bands are electron-like and the others are hole-like.
The magic angle of the tFL-graphite is about , the same as that of TBG. However, only two of these morié bands in tFL-graphite can be transformed into flat bands at the magnic angle, while others are still dispersive but their bandwidth are greatly narrowed. This is shown clearly in Fig.2(c), (g) and (k), which are calculated with based on the minimal model. Increasing , the bandwidth of the moiré bands becomes larger, and the the flat bands become dispersive [see Fig.2(b), (f), (j) with ]. With a twist angle smaller than the magic angle [e.g., in Fig.2(d), (h) and (l)], the flat band [red lines] will become slightly dispersive while the bandwidth of the other two moiré bands [blue lines] are reduced further [smaller than 10 meV in Fig.2(l)]. It suggests that the correlation in such narrow dispersive bands may be also very strong with small . At large twist angle [e.g., Fig.2(a), (e) and (i) with ], the shape of the bands near () points recovers to that of the isolated top (bottom) vdW layer. In order to figure out exactly where the flat bands distribute. we plot the wave functions of the flat band in A+ABA tFL-graphite at the Supplement [61]. The wave functions mainly distribute on both sides of the twisted interface (twisted layers), and there is almost no distribution far away from the twisted layers. Note that the A+ABA [Fig.2(c)] and BA+ABA [Fig.2(g)] both host flat bands coexisting with a single Dirac cone (), while ABA+ABA [Fig.2(k)] have two Dirac cones. This coexistence feature is very interesting because that the simultaneous occurrence of flat and steep bands is a favorable condition to enhance superconductivity, according to the “steep band/flat band” scenario of superconductivity [65, 66]. Note that coexistence of flat band with linear bands at was also noticed in some multi-twist MHSs very recently [43, 44, 69], while only one twist is required here. Due to existence of flat band and steep band, we believe tFL-graphite system will have the strongly correlated physics such as superconducting or correlated insulating states.
The low energy moiré bands of tFL-graphite also exhibit exotic topological properties, the valley Chern number of which can be nonzero. In Fig.3, we consider two example, i.e., ABA + ABA and BAB + ABA. We first see that the four moiré bands at can be isolated by a proper perpendicular electric field, while their bandwidth are still small. For these isolated moiré bands, we calculate their valley Chern numbers with the standard formula [61], which are indicated by black numbers in Fig.3. The first interesting issue is that tFL-graphite here have four moiré bands with nonzero valley Chern number, while other known MHSs only have two [33, 34, 40, 48, 49]. Furthermore, despite that ABA + ABA and BAB+ABA differ only in the relative orientation and have very similar band structure [61], their moiré bands have different valley Chern number. The cases of AB + ABA and BA + ABA are similar, and the valley Chern number is controllable by the twist angle and perpendicular electric field [61].
4 Moiré bands of thicker tFL-graphite
Now we study the moiré bands of thicker tFG-graphites. Several typical examples are given in Fig.4. These thicker tFL-graphites have various moiré bands near the , depending on their own layer numbers. For example, with N = 4 (BA + ABAB, BABA + ABAB), there exists a pair of flat bands (red lines) coexisting with a parabolic electron and a parabolic hole bands (blue lines), as shown in Fig.4(a, b) and (e, f). Compared with the N = 3 cases in Fig.2, the parabolic bands here can obviously enhance the DOS at . In general, higher DOS can always induce stronger correlation effects. It implies that correlation effects in thicker tFL-graphite may be stronger. However, more realistic facts should be considered for correlation effects in experiment. A detailed calculations (mean field for example) may be needed in future works. Increasing the layer number further, it is able to induce more moiré bands near the . An N = 5 example is given in Fig.4(i−j), which has six moiré bands including a pair of flat bands, two parabolic bands and two linear bands (green lines).
Note that the influence of the remote hopping and is critical, and different on various moiré bands, as illustrated by the full parameter model calculations in Fig.4(c, d), (g, h) and (k, l). The remote hopping always separates the the flat bands in energy (red lines) and make them dispersive. But it does not significantly modify the parabolic bands near the Dirac points (blue lines). Meanwhile, a gap at the Dirac points is induced to the linear bands in N = 5 case [see in Fig.4(k, l), green lines].
5 Summary
Our numerical calculations reveal and give some intuitive understanding about the unique, richer and highly controllable the moiré flat band structure in tFL-graphite, which may be directly verified by the nano-ARPES technique [70-73]. However, the research on the moiré bands in tFL-graphite is still at early stage, though the FL-graphite has been studied for rather a long time [67, 74-77]. Many basic problems are still unknown. For example, why does twist have different influences on the bands of FL-graphite? Whether can the multiband feature here significantly enhance the superconductivity? We hope our study will stimulate further interest on this promising system with moiré multiband correlations.
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