Charge carrier densities in electronic heterostructures are typically responsive to external electric fields or chemical doping but rarely to their magnetization history. Here, we demonstrate that magnetization acts as a non-volatile control parameter for the density of states in bilayer graphene (BLG) interfaced with the antiferromagnetic insulator chromium oxychloride (COC). Using capacitance measurements, we observe a hysteretic behavior in the density of states of BLG on a COC substrate in response to an external magnetic field, which is unrelated to the history of electrostatic gating. First-principles calculations revealed that such hysteresis arises from the magnetic-field-controlled charge transfer between BLG and COC during the antiferromagnetic (AFM) to ferrimagnetic-like (FiM) state phase transition of COC. Our work demonstrates that interfacial charging states can be effectively controlled magnetically, and it also shows that capacitance measurement is a suitable technique for detecting subtle changes not detectable via conventional resistivity measurements. These findings broaden the scope of proximity effects and open new possibilities for nanoelectronics applications.
The generation of pseudo-magnetic fields in strained graphene leads to quantized Landau levels in the absence of an external magnetic field, providing the potential to achieve a zero-magnetic-field analogue of quantum Hall effect. Here, we report the realization of pseudo-magnetic field in epitaxial graphene by building monolayer CrCl2/graphene heterointerface. The CrCl2 crystal structure exhibits spontaneous breaking of three-fold rotational symmetry, yielding anisotropic displacement field at the interface. Using scanning tunneling spectroscopy, we have discovered a sequence of pseudo-Landau levels associated with massless Dirac fermions. A control experiment performed on CrCl2/NbSe2 interface confirms the origin as the pseudo-magnetic field in the graphene layer that strongly interacts with the CrCl2. More interestingly, the strength of the pseudo-magnetic fields can be tuned by the twist angle between the monolayer CrCl2 and graphene, with a variation of up to threefold, depending on the twist angle of 0° to 30°. This work presents a rare 2D heterojunction for exploring PMF-related physics, such as valley Hall effect, with the advantage of easy and flexible implementation.
Scanning tunneling microscopy (STM) vibronic spectroscopy, which has provided submolecular insights into electron-vibration (vibronic) coupling, faces challenges when probing the pivotal low-frequency vibronic excitations. Because of eigenstate broadening on solid substrates, resolving low-frequency vibronic states demands strong decoupling. This work designs a type II band alignment in STM junction to achieve effective charge-transfer state decoupling. This strategy enables the successful identification of the lowest-frequency Hg(ω1) (Raman-active Hg mode) vibronic excitation within single C60 molecules, which, despite being notably pronounced in electron transport of C60 single-molecule transistors, has remained hidden at submolecular level. Our results show that the observed Hg(ω1) excitation is “anchored” to all molecules, irrespective of local geometry, challenging common understanding of structural definition of vibronic excitation governed by Franck-Condon principle. Density functional theory calculations reveal existence of molecule-substrate interfacial charge-transfer dipole, which, although overlooked previously, drives the dominant Hg(ω1) excitation. This charge-transfer dipole is not specific but must be general at interfaces, influencing vibronic coupling in charge transport.
Yangliu Wu, Zhaozhuo Zeng, Haipeng Lu, Xiaocang Han, Chendi Yang, Nanshu Liu, Xiaoxu Zhao, Liang Qiao, Wei Ji*, Renchao Che, Longjiang Deng*, Peng Yan* and Bo Peng*
Abstract:
Multiferroic materials have been intensively pursued to achieve the mutual control of electric and magnetic properties. The breakthrough progress in 2D magnets and ferroelectrics encourages the exploration of low-dimensional multiferroics, which holds the promise of understanding inscrutable magnetoelectric coupling and inventing advanced spintronic devices. However, confirming ferroelectricity with optical techniques is challenging in 2D materials, particularly in conjunction with antiferromagnetic orders in single- and few-layer multiferroics. Here, we report the discovery of 2D vdW multiferroic with out-of plane ferroelectric polarization in trilayer NiI2 device, as revealed by scanning reflective magnetic circular dichroism microscopy and ferroelectric hysteresis loops. The evolution between ferroelectric and antiferroelectric phases has been unambiguously observed. Moreover, the magnetoelectric interaction is directly probed by magnetic control of the multiferroic domain switching. This work opens up opportunities for exploring new multiferroic orders and multiferroic physics at the limit of single or few atomic layers, and for creating advanced magnetoelectronic devices.
Zhihong Zhang, Linwei Zhou, Zhaoxi Chen* , Antonín Jaroš, Miroslav Kolíbal, Petr Bábor, Quanzhen Zhang, Changlin Yan, Ruixi Qiao, Qing Zhang, Teng Zhang, Wei Wei, Yi Cui, Jingsi Qiao, Liwei Liu, Lihong Bao, Haitao Yang, Zhihai Cheng, Yeliang Wang, Enge Wang, Zhi Liu, Marc Willinger, Hong-Jun Gao, Kaihui Liu*, Wei Ji*, and Zhu-Jun Wang*
Abstract:
Direct growth of large-area vertically stacked two-dimensional (2D) van der Waal (vdW) materials is a prerequisite for their high-end applications in integrated electronics, optoelectronics and photovoltaics. Currently, centimetre- to even metre-scale monolayers of single-crystal graphene (MLG) and hexagonal boron nitride (h-BN) have been achieved by epitaxial growth on various single-crystalline substrates. However, in principle, this success in monolayer epitaxy seems extremely difficult to be replicated to bi- or few-layer growth, as the full coverage of the first layer was believed to terminate the reactivity of those adopting catalytic metal surfaces. Here, we report an exceptional layer-by-layer chemical vapour deposition (CVD) growth of large size bi-layer graphene single-crystals, enabled by proximity catalytic activity from platinum (Pt) surfaces to the outermost graphene layers. In-situ growth and real-time surveillance experiments, under well-controlled environments, unambiguously verify that the growth does follow the layer-by-layer mode on open surfaces of MLG/Pt(111). First-principles calculations indicate that the transmittal of catalytic activity is allowed by an appreciable electronic hybridisation between graphene overlayers and Pt surfaces, enabling catalytic dissociation of hydrocarbons and subsequently direct graphitisation of their radicals on the outermost sp2 carbon surface. This proximity catalytic activity is also proven to be robust for tube-furnace CVD in fabricating single-crystalline graphene bi-, tri- and tetra-layers, as well as h-BN few-layers. Our findings offer an exceptional strategy for potential controllable, layer-by-layer and wafer-scale growth of vertically stacked few-layered 2D single crystals.
