Ghost anti-crossings caused by interlayer umklapp hybridization of bands in 2D heterostructures
Abigail J. Graham, Johanna Zultak, Matthew J. Hamer, Viktor Zolyomi, Samuel Magorrian, Alexei Barinov, Viktor Kandyba, Alessio Giampietri, Andrea Locatelli, Fra… 展开作者
Abigail J. Graham, Johanna Zultak, Matthew J. Hamer, Viktor Zolyomi, Samuel Magorrian, Alexei Barinov, Viktor Kandyba, Alessio Giampietri, Andrea Locatelli, Francesca Genuzio, Natalie C. Teutsch, Temok Salazar, Nicholas D. M. Hine, Vladimir I. Fal'ko, Roman V. Gorbachev, Neil R. Wilson
In two-dimensional heterostructures, crystalline atomic layers with differing lattice parameters can stack directly one on another. The resultant close proximity of atomic lattices with differing periodicity can lead to new phenomena. For umklapp processes, this opens the possibility for interlayer umklapp scattering, where interactions are mediated by the transfer of momenta to or from the lattice in the neighbouring layer. Using angle-resolved photoemission spectroscopy to study a graphene on InSe heterostructure, we present evidence that interlayer umklapp processes can cause hybridization between bands from neighbouring layers in regions of the Brillouin zone where bands from only one layer are expected, despite no evidence for moir/'e-induced replica bands. This phenomenon manifests itself as 'ghost' anti-crossings in the InSe electronic dispersion. Applied to a range of suitable 2DM pairs, this phenomenon of interlayer umklapp hybridization can be used to create strong mixing of their electronic states, giving a new tool for twist-controlled band structure engineering.
Umklapp-Enhanced Interlayer Valley Drag in Moiré Bilayers
Institute of Mathematical Sciences（数学科学研究所）；Tata Institute of Fundamental Research（塔塔基础研究所）；Indiana University（印第安纳大学）；Indian Institute of Technology - Kanpur（坎普尔印度理工学院）
Geometrical moiré patterns, generic for almost aligned bilayers of two-dimensional (2D) crystals with similar lattice structure but slightly different lattice constants, lead to zone folding and miniband formation for electronic states. Here, we show that moiré superlattice (mSL) effects in $\mathrm{MoSe}_2/\mathrm{WS}_2$ and $\mathrm{MoTe}_2/\mathrm{MoSe}_2$ heterobilayers that feature alignment of the band edges are enhanced by resonant interlayer hybridization, and anticipate similar features in twisted homobilayers of TMDs, including examples of narrow minibands close to the actual band ed…
The incommensurate 30$^{\circ}$ twisted bilayer graphene (BG) possesses both relativistic Dirac fermions and quasiperiodicity with 12-fold rotational symmetry arising from the interlayer interaction [\href{https://science.sciencemag.org/content/361/6404/782}{Ahn et al., Science \textbf{361}, 782 (2018)} and \href{https://www.pnas.org/content/115/27/6928}{Yao et al., Proc. Natl. Acad. Sci. \textbf{115}, 6928 (2018)}]. Understanding how the interlayer states interact with each other is of vital importance for identifying and subsequently engineering the quasicrystalline order in the layered stru…
Excitons in bilayer transition metal dichalcogenides (2L-TMDs) are Coulomb-bound electron/hole pairs that can be viewed as broadly tunable analogs of atomic or molecular systems. Here, we study the properties of 2L-TMD excitons under strong electric field. To overcome the field limit, reached in previous experiments, we developed a new organic/inorganic molecular gating technique. Our approach allows reaching the field > 0.27 V nm-1, about twice higher than previously available. Under this field inter and intra-layer excitonic are brought into an energetic resonance, allowing us to discover ne…
Layered two-dimensional materials exhibit rich transport and optical phenomena in twisted or lattice-incommensurate heterostructures with spatial variations of interlayer hybridization arising from moiré interference effects. Here, we report experimental and theoretical studies of excitons in twisted heterobilayers and heterotrilayers of transition metal dichalcogenides. Using MoSe$_2$-WSe$_2$ stacks as representative realizations of twisted van der Waals bilayer and trilayer heterostructures, we observe contrasting optical signatures and interpret them in the theoretical framework of interlay…
Interlayer coupling between twisted graphenes through atomically-precise barriers
The University of Hong Kong（香港大学）；State Key Laboratory of Optical Quantum Materials, The University of Hong Kong（香港大学光学量子材料国家重点实验室）；National Graphene Institute, University of Manchester（曼彻斯特大学国家石墨烯研究所）；Department of Physics and Astronomy, University of Manchester（曼彻斯特大学物理与天文学系）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（物质材料研究机构电子与光学材料研究中心）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（物质材料研究机构材料纳米结构研究中心）
Theory of In-Plane Orbital Magnetization with Layer Hybridization
The Hong Kong University of Science and Technology（香港科技大学）；RIKEN Center for Emergent Matter Science (CEMS)（理化学研究所新兴物质科学中心）；Beijing Institute of Technology（北京理工大学）
Interlayer Coupling and Floquet-Driven Topological Phases in Bilayer Haldane Lattices
Zhejiang Normal University（浙江师范大学）；Khazar University（哈扎尔大学）；Quaid-I Azam University Islamabad（巴基斯坦奎德-阿扎姆大学伊斯兰堡分校）；Institute for Research in Fundamental Sciences (IPM)（伊朗基础科学研究院）
In van der Waals heterostructures, the relative alignment of bands between layers, and the resulting band hybridisation, are key factors in determining a range of electronic properties. This work examines these effects for heterostructures of transition metal dichalcogenides (TMDs) and hexagonal boron nitride (hBN), an ubiquitous combination given the role of hBN as an encapsulating material. By comparing results of density functional calculations with experimental angle-resolved photoemission spectroscopy (ARPES) results, we explore the hybridisation between the valence states of the TMD and …
The large surface-to-volume ratio in atomically thin 2D materials allows to efficiently tune their properties through modifications of their environment. Artificial stacking of two monolayers into a bilayer leads to an overlap of layer-localized wave functions giving rise to a twist angle-dependent hybridization of excitonic states. In this joint theory-experiment study, we demonstrate the impact of interlayer hybridization on bright and momentum-dark excitons in twisted WSe$_2$ bilayers. In particular, we show that the strong hybridization of electrons at the $Λ$ point leads to a drastic reds…
Hybridisation of electronic bands of two-dimensional materials, assembled into twistronic heterostructures, enables one to tune their optoelectronic properties by selecting conditions for resonant interlayer hybridisation. Resonant interlayer hybridisation qualitatively modifies the excitons in such heterostructures, transforming these optically active modes into superposition states of interlayer and intralayer excitons. For MoSe$_2$/WSe$_2$ heterostructures, strong hybridization occurs between the holes in the spin-split valence band of WSe$_2$ and in the top valence band of MoSe$_2$, especi…
Monolayers and multilayers of semiconducting transition metal dichalcogenides (TMDCs) offer an ideal platform to explore valley-selective physics with promising applications in valleytronics and information processing. Here we manipulate the energetic degeneracy of the $\mathrm{K}^+$ and $\mathrm{K}^-$ valleys in few-layer TMDCs. We perform high-field magneto-reflectance spectroscopy on WSe$_2$, MoSe$_2$, and MoTe$_2$ crystals of thickness from monolayer to the bulk limit under magnetic fields up to 30 T applied perpendicular to the sample plane. Because of a strong spin-layer locking, the gro…
Layer-Hybridized Wigner Crystals in MoSe2/WS2 Moiré Superlattice
Carnegie Mellon University（卡内基梅隆大学）；Arizona State University（亚利桑那州立大学）；National Institute for Materials Science（国立材料研究所）；The University of Texas at Dallas（德克萨斯大学达拉斯分校）；University of California at Riverside（加州大学河滨分校）
Moiré superlattices formed in van der Waals bilayers have enabled the creation and manipulation of new quantum states, as is exemplified by the discovery of superconducting and correlated insulating states in twisted bilayer graphene near the magic angle. Twisted bilayer semiconductors may lead to tunable exciton lattices and topological states, yet signatures of moiré excitons have been reported only in closely angularly-aligned bilayers. Here we report tuning of moiré lattice in WS$_{2}$ /MoSe$_{2}$ bilayers over a wide range of twist angles, leading to the continuous tuning of moiré lattice…
Nearly localized moire flat bands in momentum space, arising at particular twist angles, are the key to achieve correlated effects in transition-metal dichalcogenides. Here, we use angle-resolved photoemission spectroscopy (ARPES) to visualize the presence of a flat band near the Fermi level of van der Waals (vdW) WSe2/MoSe2 heterobilayer grown by molecular beam epitaxy. This flat band is localized near the K point of the Brillouin zone and has a width of several hundred meVs. By combining ARPES measurements with density functional theory (DFT) calculations, we confirm the coexistence of diffe…
Valley selective hybridization and residual coupling of electronic states in commensurate van der Waals heterobilayers enable the control of the orbital character of interlayer excitons. We demonstrate electric field control of layer index, orbital character, lifetime and emission energy of indirect excitons in MoS2/WS2 heterobilayers embedded in an vdW field effect structure. Different excitonic dipoles normal to the layers are found to stem from bound electrons and holes located in different valleys of MoS2/WS2 with a valley selective degree of hybridization. For the energetically lowest emi…
Moire superlattices in van der Waals (vdW) heterostructures could trap strongly bonded and long lived interlayer excitons. Assumed to be localized, these moire excitons could form ordered quantum dot arrays, paving the way for novel optoelectronic and quantum information applications. Here we perform first principles simulations to shed light on moire excitons in twisted MoS2/WS2 heterostructures. We provide the direct evidence of localized interlayer moire excitons in vdW heterostructures. The moire potentials are mapped out based on spatial modulations of energy gaps. Nearly flat valence ban…
Excitons in monolayer semiconductors have large optical transition dipole for strong coupling with light field. Interlayer excitons in heterobilayers, with layer separation of electron and hole components, feature large electric dipole that enables strong coupling with electric field and exciton-exciton interaction, at the cost that the optical dipole is substantially quenched (by several orders of magnitude). In this letter, we demonstrate the ability to create a new class of excitons in transition metal dichalcogenide (TMD) hetero- and homo-bilayers that combines the advantages of monolayer-…
University of Maryland, College Park（马里兰大学帕克分校）；Universität Heidelberg（海德堡大学）；Laboratory for Physical Sciences（物理科学实验室）；Brookhaven National Laboratory（布鲁海文国家实验室）；National Institute for Materials Science（物质材料研究机构）
Materials with high thermal conductivities (k) is valuable to solve the challenge of waste heat dissipation in highly integrated and miniaturized modern devices. Herein, we report the first synthesis of atomically thin isotopically pure hexagonal boron nitride (BN) and its one of the highest k among all semiconductors and electric insulators. Single atomic layer (1L) BN enriched with 11B has a k up to 1009 W/mK at room temperature. We find that the isotope engineering mainly suppresses the out-of-plane optical (ZO) phonon scatterings in BN, which subsequently reduces acoustic-optical scatterin…
Twistronic assembly of 2D materials employs the twist angle between adjacent layers as a tuning parameter for designing the electronic and optical properties of van der Waals heterostructures. Here, we study how interlayer hybridization, weak ferroelectric charge transfer between layers, and piezoelectric response to deformations set the valence and conduction band edges across the moir{é} supercell in twistronic homobilayers of MoS$_2$, MoSe$_2$, WS$_2$ and WSe$_2$. We show that, due to the lack of inversion symmetry in the monolayer crystals, bilayers with parallel (P) and anti-parallel (AP)…
