Two-dimensional electron gas or hole gas (2DEG or 2DHG) and their functionalities at artificial heterostructure interfaces have attracted extensive attention in recent years. Many theoretical calculations and recent experimental studies have shown the formation of alternating 2DEG and 2DHG at ferroelectric/insulator interfaces, such as BiFeO3/TbScO3, depending on the different polarization states. However, a direct observation based on the local charge distribution at the BiFeO3/TbScO3interface has yet to be explored. Herein we demonstrate the direct observation of 2DHG and 2DEG at BiFeO3/TbScO3interface using four-dimensional scanning transmission electron microscopy and Bader charge analysis. The results show that the measured charge state of each Fe/O columns at the interface undergoes a significant increase/reduction for the polarization state pointing away/toward the interface, indicating the existence of 2DHG/2DEG. This method opens up a path of directly observing charge at atomic scale and provides new insights into the design of future electronic nanodevices.
The atomic structure at the interface between two-dimensional (2D) and three-dimensional (3D) materials influences properties such as contact resistance, photo-response, and high-frequency electrical performance. Moiré engineering is yet to be utilized for tailoring this 2D/3D interface, despite its success in enabling correlated physics at 2D/2D interfaces. Using epitaxially aligned MoS2/Au{111} as a model system, we demonstrate the use of advanced scanning transmission electron microscopy (STEM) combined with a geometric convolution technique in imaging the crystallographic 32 Å moiré pattern at the 2D/3D interface. This moiré period is often hidden in conventional electron microscopy, where the Au structure is seen in projection. We show, via ab initio electronic structure calculations, that charge density is modulated according to the moiré period, illustrating the potential for (opto-)electronic moiré engineering at the 2D/3D interface. Our work presents a general pathway to directly image periodic modulation at interfaces using this combination of emerging microscopy techniques.
more » « less- NSF-PAR ID:
- 10215323
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 12
- Issue:
- 1
- ISSN:
- 2041-1723
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
more » « less
Abstract -
more » « less
Abstract Lattice reconstruction and corresponding strain accumulation plays a key role in defining the electronic structure of two-dimensional moiré superlattices, including those of transition metal dichalcogenides (TMDs). Imaging of TMD moirés has so far provided a qualitative understanding of this relaxation process in terms of interlayer stacking energy, while models of the underlying deformation mechanisms have relied on simulations. Here, we use interferometric four-dimensional scanning transmission electron microscopy to quantitatively map the mechanical deformations through which reconstruction occurs in small-angle twisted bilayer MoS2and WSe2/MoS2heterobilayers. We provide direct evidence that local rotations govern relaxation for twisted homobilayers, while local dilations are prominent in heterobilayers possessing a sufficiently large lattice mismatch. Encapsulation of the moiré layers in hBN further localizes and enhances these in-plane reconstruction pathways by suppressing out-of-plane corrugation. We also find that extrinsic uniaxial heterostrain, which introduces a lattice constant difference in twisted homobilayers, leads to accumulation and redistribution of reconstruction strain, demonstrating another route to modify the moiré potential.
-
more » « less
Abstract Moiré patterns at van der Waals interfaces between twisted 2D crystals give rise to distinct optoelectronic excitations, as well as, narrowly dispersive bands responsible for correlated electron phenomena. Contrasting with the conventional, mechanically stacked planar twist moirés, recent work shows twisted van der Waals interfaces spontaneously formed in nanowires of layered crystals, where Eshelby twist due to axial screw dislocations stabilizes a chiral structure with small interlayer rotation. Here, the realization of tunable twist in germanium(II) sulfide (GeS) van der Waals nanowires is reported. Tapered nanowires host continuously variable interlayer twist. Homojunctions between dislocated (chiral) and defect‐free (achiral) segments are obtained by triggering the emission of axial dislocations during growth. Measurements across such junctions, implemented here using local absorption and luminescence spectroscopy, provide a convenient tool for detecting twist effects. The results identify a versatile system for 3D twistronics, probing moiré physics, and for realizing moiré architectures without equivalent in planar systems.
-
more » « less
Abstract Two key interfaces in flexible perovskite solar cells (f‐PSCs) are mechanically reinforced simultaneously: one between the electron‐transport layer (ETL) and the 3D metal‐halide perovskite (MHP) thin film using self‐assembled monolayer (SAM), and the other between the 3D‐MHP thin film and the hole‐transport layer (HTL) using an in situ grown low‐dimensional (LD) MHP capping layer. The interfacial mechanical properties are measured and modeled. This rational interface engineering results in the enhancement of not only the mechanical properties of both interfaces but also their optoelectronic properties holistically. As a result, the new class of dual‐interface‐reinforced f‐PSCs has an unprecedented combination of the following three important performance parameters: high power‐conversion efficiency (PCE) of 21.03% (with reduced hysteresis), improved operational stability of 1000 h
T 90(duration at 90% initial PCE retained), and enhanced mechanical reliability of 10 000 cyclesn 88(number of bending cycles at 88% initial PCE retained). The scientific underpinnings of these synergistic enhancements are elucidated. -
more » « less
Abstract Due to the coexistence of many emergent phenomena, including 2D superconductivity and a large Rashba spin‐orbit coupling, 5d transition metal oxides‐based two‐dimensional electron systems (2DESs) have been prospected as one of the potential intrants for modern electronics. However, despite the lighter electron mass, the mobility of carriers, a key requisite for high‐performance devices, in 5d‐oxides devices remains far behind their 3d‐oxides analogs. The carriers’ mobility in these oxides is significantly hampered by the inevitable presence of defects. Here, very high mobility (≈22 650 cm2V−1s−1) of 5d‐2DES confined at the LaAlO3/KTaO3interface is reported. The high mobility, which is beyond the values observed in SrTiO32DESs in the same carrier‐density range, is achieved using the ionic‐liquid gating at room temperature. The authors postulate that the ionic‐liquid gating affects the oxygen vacancies and efficiently reduces any disorder at the interface. Investigating density and mobility in a broad range of back‐gate voltage, the authors reveal that the mobility follows the power‐law
µ ∝n 1.2, indicating the very high quality of ionic‐liquid‐gated LaAlO3/KTaO3devices, consistent with the postulate. Furthermore, the analysis of the quantum oscillations confirms that the high‐mobility electrons occupy the electronic sub‐bands emerging from the Ta:5d orbitals of KTaO3.
