Moiré superlattices are emerging as a new route for engineering strongly correlated electronic states in two-dimensional van der Waals heterostructures, as recently demonstrated in the correlated insulating and superconducting states in magic-angle twisted bilayer graphene and ABC trilayer graphene/boron nitride moiré superlattices 1-4 . Transition metal dichalcogenide (TMDC) moiré heterostructures provide another exciting model system to explore correlated quantum phenomena 5 , with the addition of strong light-matter interactions and large spin-orbital coupling. Here we report the optical detection of strongly correlated phases in semiconducting WSe2/WS2 moiré superlattices. Our sensitive optical detection technique reveals a Mott insulator state at one hole per superlattice site (ν = 1), and surprising insulating phases at fractional filling factors ν = 1/3 and 2/3, which we assign to generalized Wigner crystallization on an underlying lattice 6-9 . Furthermore, the unique spin-valley optical selection rules 10-12 of TMDC heterostructures allow us to optically create and investigate low-energy spin excited states in the Mott insulator. We reveal an especially slow spin relaxation lifetime of many microseconds in the Mott insulating state, orders-of-magnitude longer than that of charge excitations. Our studies highlight novel correlated physics that can emerge in moiré superlattices beyond graphene.
The ability to detect linearly polarized light is central to practical applications in polarized optical and optoelectronic fields and has been successfully demonstrated with polarized photodetection of in-plane anisotropic two-dimensional (2D) materials. Here, we report the anisotropic optical characterization of a group IV–V compound-2D germanium arsenic (GeAs) with anisotropic monoclinic structures. High-quality 2D GeAs crystals show the representative angle-resolved Raman property. The in-plane anisotropic optical nature of the GeAs crystal is further investigated by polarization-resolved absorption spectra (400–2000 nm) and polarization-sensitive photodetectors. From the visible to the near-infrared range, 2D GeAs nanoflakes demonstrate the distinct perpendicular optical reversal with a 75–80° angle on both the linear dichroism and polarization-sensitive photodetection. Obvious anisotropic features and the high dichroic ratio of I pmax /I pmin ∼ 1.49 at 520 nm and I pmax /I pmin ∼ 4.4 at 830 nm are achieved by the polarization-sensitive photodetection. The polarization-dependent photocurrent mapping implied that the polarized photocurrent mainly occurred at the Schottky photodiodes between electrode/GeAs interface. These experimental results are consistent with the theoretical calculation of band structure and band realignment. Besides the excellent polarization-sensitive photoresponse properties, GeAs-based photodetectors also exhibit rapid on/off response. These results demonstrate that the 2D GeAs crystals have promising potential for polarization optical applications.
Tungsten-based monolayer transition metal dichalcogenides host a long-lived “dark” exciton, an electron-hole pair in a spin-triplet configuration. The long lifetime and unique spin properties of the dark exciton provide exciting opportunities to explore light-matter interactions beyond electric dipole transitions. Here we demonstrate that the coupling of the dark exciton and an optically silent chiral phonon enables the intrinsic photoluminescence of the dark-exciton replica in monolayer WSe 2 . Gate and magnetic-field dependent PL measurements unveil a circularly-polarized replica peak located below the dark exciton by 21.6 meV, equal to E″ phonon energy from Se vibrations. First-principles calculations show that the exciton-phonon interaction selectively couples the spin-forbidden dark exciton to the intravalley spin-allowed bright exciton, permitting the simultaneous emission of a chiral phonon and a circularly-polarized photon. Our discovery and understanding of the phonon replica reveals a chirality dictated emission channel of the phonons and photons, unveiling a new route of manipulating valley-spin.
Magnetism in two-dimensional (2D) van der Waals (vdW) materials has recently emerged as one of the most promising areas in condensed matter research, with many exciting emerging properties and significant potential for applications ranging from topological magnonics to low-power spintronics, quantum computing, and optical communications. In the brief time after their discovery, 2D magnets have blossomed into a rich area for investigation, where fundamental concepts in magnetism are challenged by the behavior of spins that can develop at the single layer limit. However, much effort is still needed in multiple fronts before 2D magnets can be routinely used for practical implementations. In this comprehensive review, prominent authors with expertise in complementary fields of 2D magnetism ( i.e. , synthesis, device engineering, magneto-optics, imaging, transport, mechanics, spin excitations, and theory and simulations) have joined together to provide a genome of current knowledge and a guideline for future developments in 2D magnetic materials research.
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