Two-dimensional (2D) ferroelectrics with robust polarization down to atomic thicknesses provide building blocks for functional heterostructures. Experimental realization remains challenging because of the requirement of a layered polar crystal. Here, we demonstrate a rational design approach to engineering 2D ferroelectrics from a nonferroelectric parent compound by using van der Waals assembly. Parallel-stacked bilayer boron nitride exhibits out-of-plane electric polarization that reverses depending on the stacking order. The polarization switching is probed through the resistance of an adjacently stacked graphene sheet. Twisting the boron nitride sheets by a small angle changes the dynamics of switching because of the formation of moiré ferroelectricity with staggered polarization. The ferroelectricity persists to room temperature while keeping the high mobility of graphene, paving the way for potential ultrathin nonvolatile memory applications.
Sliding ferroelectricity in 2D van der Waals materials: Related physics and future opportunities
Near the 100th anniversary of the discovery of ferroelectricity, so-called sliding ferroelectricity has been proposed and confirmed recently in a series of experiments that have stimulated remarkable interest. Such ferroelectricity exists widely and exists only in two-dimensional (2D) van der Waals stacked layers, where the vertical electric polarization is switched by in-plane interlayer sliding. Reciprocally, interlayer sliding and the “ripplocation” domain wall can be driven by an external vertical electric field. The unique combination of intralayer stiffness and interlayer slipperiness of 2D van der Waals layers greatly facilitates such switching while still maintaining environmental and mechanical robustness at ambient conditions. In this perspective, we discuss the progress and future opportunities in this behavior. The origin of such ferroelectricity as well as a general rule for judging its existence are summarized, where the vertical stacking sequence is crucial for its formation. This discovery broadens 2D ferroelectrics from very few material candidates to most of the known 2D materials. Their low switching barriers enable high-speed data writing with low energy cost. Related physics like Moiré ferroelectricity, the ferroelectric nonlinear anomalous Hall effect, and multiferroic coupling are discussed. For 2D valleytronics, nontrivial band topology and superconductivity, their possible couplings with sliding ferroelectricity via certain stacking or Moiré ferroelectricity also deserve interest. We provide critical reviews on the current challenges in this emerging area.
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- Award ID(s):
- 1923976
- NSF-PAR ID:
- 10326015
- Date Published:
- Journal Name:
- Proceedings of the National Academy of Sciences
- Volume:
- 118
- Issue:
- 50
- ISSN:
- 0027-8424
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Twisting or sliding two-dimensional crystals with respect to each other gives rise to moiré patterns determined by the difference in their periodicities. Such lattice mismatches can exist for several reasons: differences between the intrinsic lattice constants of the two layers, as is the case for graphene on BN; rotations between the two lattices, as is the case for twisted bilayer graphene; and strains between two identical layers in a bilayer. Moiré patterns are responsible for a number of new electronic phenomena observed in recent years in van der Waals heterostructures, including the observation of superlattice Dirac points for graphene on BN, collective electronic phases in twisted bilayers and twisted double bilayers, and trapping of excitons in the moiré potential. An open question is whether we can use moiré potentials to achieve strong trapping potentials for electrons. Here, we report a technique to achieve deep, deterministic trapping potentials via strain-based moiré engineering in van der Waals materials. We use strain engineering to create on-demand soliton networks in transition metal dichalcogenides. Intersecting solitons form a honeycomb-like network resulting from the three-fold symmetry of the adhesion potential between layers. The vertices of this network occur in bound pairs with different interlayer stacking arrangements. One vertex of the pair is found to be an efficient trap for electrons, displaying two states that are deeply confined within the semiconductor gap and have a spatial extent of 2 nm. Soliton networks thus provide a path to engineer deeply confined states with a strain-dependent tunable spatial separation, without the necessity of introducing chemical defects into the host materials.more » « less
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The discovery of ferroelectricity marks its 100th anniversary this year ( 1 ), and this phenomenon continues to enrich our understanding of many fields of physics and material science, as well as creating subfields on its own. All of the ferroelectrics discovered have been limited to those exhibiting a polar space group of the bulk crystal that supports two or more topologically equivalent variants with different orientations of electric polarization. On pages 1458 and 1462 of this issue, Yasuda et al. ( 2 ) and Vizner Stern et al. ( 3 ), respectively, show that ferroelectricity can be engineered by artificially stacking a nonpolar in bulk, two-dimensional (2D) material, boron nitride (BN). A relatively weak van der Waals (vdW) coupling between the adjacent BN monolayers allows their parallel alignment in a metastable non-centrosymmetric coordination supporting 2D ferroelectricity with an out-of-plane electric polarization. These findings open opportunities to design 2D ferroelectrics out of parent nonpolar compounds.more » « less
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Van der Waals heterojunctions of two-dimensional transition-metal dichalcogenides are intensely investigated for multiple optoelectronics applications. Strong and adjustable interactions between layers can influence the charge and energy flow that govern material performance. We report ab initio quantum molecular dynamics investigation of the influence of the bilayer twist angle on charge transfer and recombination in MoS 2 /WS 2 heterojunctions, including high-symmetry 0° and 60° configurations, and low symmetry 9.43° and 50.57° structures with Moiré patterns. The twist angle modulates interlayer coupling, as evidenced by changes in the interlayer distance, electron-vibrational interactions, and spectral shifts in the out-of-plane vibrational frequencies. Occurring on a femtosecond timescale, the hole transfer depends weakly on the twist angle and is ultrafast due to high density of acceptor states and large nonadiabatic coupling. In contrast, the electron–hole recombination takes nanoseconds and varies by an order of magnitude depending on the twist angle. The recombination is slow because it occurs across a large energy gap. It depends on the twist angle because the nonadiabatic coupling is sensitive to the interlayer distance and overlap of electron and hole wavefunctions. The Moiré pattern systems exhibit weaker interlayer interaction, generating longer-lived charges. Both charge separation and recombination are driven by out-of-plane vibrational motions. The simulations rationalize the experimental results on the influence of the bilayer twist angle on the charge separation and recombination. The atomistic insights provide theoretical guidance for design of high-performance optoelectronic devices based on 2D van der Waals heterostructures.more » « less
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1073/pnas.2115703118
