- Award ID(s):
- Publication Date:
- NSF-PAR ID:
- Journal Name:
- Sponsoring Org:
- National Science Foundation
More Like this
We apply the density-functional theory to study various phases (including non-magnetic (NM), anti-ferromagnetic (AFM), and ferromagnetic (FM)) in monolayer magnetic chromium triiodide (CrI 3 ), a recently fabricated 2D magnetic material. It is found that: (1) the introduction of magnetism in monolayer CrI 3 gives rise to metal-to-semiconductor transition; (2) the electronic band topologies as well as the nature of direct and indirect band gaps in either AFM or FM phases exhibit delicate dependence on the magnetic ordering and spin–orbit coupling; and (3) the phonon modes involving Cr atoms are particularly sensitive to the magnetic ordering, highlighting distinct spin–lattice and spin–phonon coupling in this magnet. First-principles simulations of the Raman spectra demonstrate that both frequencies and intensities of the Raman peaks strongly depend on the magnetic ordering. The polarization dependent A 1g modes at 77 cm −1 and 130 cm −1 along with the E g mode at about 50 cm −1 in the FM phase may offer a useful fingerprint to characterize this material. Our results not only provide a detailed guiding map for experimental characterization of CrI 3 , but also reveal how the evolution of magnetism can be tracked by its lattice dynamics and Raman response.
Abstract The emerging field of twistronics, which harnesses the twist angle between two-dimensional materials, represents a promising route for the design of quantum materials, as the twist-angle-induced superlattices offer means to control topology and strong correlations. At the small twist limit, and particularly under strain, as atomic relaxation prevails, the emergent moiré superlattice encodes elusive insights into the local interlayer interaction. Here we introduce moiré metrology as a combined experiment-theory framework to probe the stacking energy landscape of bilayer structures at the 0.1 meV/atom scale, outperforming the gold-standard of quantum chemistry. Through studying the shapes of moiré domains with numerous nano-imaging techniques, and correlating with multi-scale modelling, we assess and refine first-principle models for the interlayer interaction. We document the prowess of moiré metrology for three representative twisted systems: bilayer graphene, double bilayer graphene and H-stacked MoSe 2 /WSe 2 . Moiré metrology establishes sought after experimental benchmarks for interlayer interaction, thus enabling accurate modelling of twisted multilayers.
Moiré superlattices in van der Waals (vdW) heterostructures could trap long-lived interlayer excitons. These moiré excitons could form ordered quantum dot arrays, paving the way for unprecedented optoelectronic and quantum information applications. Here, we perform first-principles simulations to shed light on moiré excitons in twisted MoS 2 /WS 2 heterostructures. We provide direct evidence of localized interlayer moiré excitons in vdW heterostructures. The interlayer and intralayer moiré potentials are mapped out based on spatial modulations of energy gaps. Nearly flat valence bands are observed in the heterostructures. The dependence of spatial localization and binding energy of the moiré excitons on the twist angle of the heterostructures is examined. We explore how vertical electric field can be tuned to control the position, polarity, emission energy, and hybridization strength of the moiré excitons. We predict that alternating electric fields could modulate the dipole moments of hybridized moiré excitons and suppress their diffusion in moiré lattices.
Multiple flat bands and topological Hofstadter butterfly in twisted bilayer graphene close to the second magic angleMoiré superlattices in two-dimensional van der Waals heterostructures provide an efficient way to engineer electron band properties. The recent discovery of exotic quantum phases and their interplay in twisted bilayer graphene (tBLG) has made this moiré system one of the most renowned condensed matter platforms. So far studies of tBLG have been mostly focused on the lowest two flat moiré bands at the first magic angle θ m1 ∼ 1.1°, leaving high-order moiré bands and magic angles largely unexplored. Here we report an observation of multiple well-isolated flat moiré bands in tBLG close to the second magic angle θ m2 ∼ 0.5°, which cannot be explained without considering electron–election interactions. With high magnetic field magnetotransport measurements we further reveal an energetically unbound Hofstadter butterfly spectrum in which continuously extended quantized Landau level gaps cross all trivial band gaps. The connected Hofstadter butterfly strongly evidences the topologically nontrivial textures of the multiple moiré bands. Overall, our work provides a perspective for understanding the quantum phases in tBLG and the fractal Hofstadter spectra of multiple topological bands.
Moiré superlattices created by the twisted stacking of two-dimensional crystals can host electronic bands with flat energy dispersion in which enhanced interactions promote correlated electron states. The twisted double bilayer graphene (TDBG), where two Bernal bilayer graphene are stacked with a twist angle, is such a moiré system with tunable flat bands. Here, we use gate-tuned scanning tunneling spectroscopy to directly demonstrate the tunability of the band structure of TDBG with an electric field and to show spectroscopic signatures of electronic correlations and topology for its flat band. Our spectroscopic experiments are in agreement with a continuum model of TDBG band structure and reveal signatures of a correlated insulator gap at partial filling of its isolated flat band. The topological properties of this flat band are probed with the application of a magnetic field, which leads to valley polarization and the splitting of Chern bands with a large effective g-factor.