Each atomic layer in van der Waals heterostructures possesses a distinct electronic band structure that can be manipulated for unique device operations. In the precise device architecture, the subtle but critical band splits by the giant Stark effect between atomic layers, varied by the momentum of electrons and external electric fields in device operation, has not yet been demonstrated or applied to design original devices with the full potential of atomically thin materials. Here, resonant tunneling spectroscopy based on the negligible quantum capacitance of 2D semiconductors in resonant tunneling transistors is reported. The bandgaps and sub‐band structures of various channel materials could be demonstrated by the new conceptual spectroscopy at the device scale without debatable quasiparticle effects. Moreover, the band splits by the giant Stark effect in the channel materials could be probed, overcoming the limitations of conventional optical, photoemission, and tunneling spectroscopy. The resonant tunneling spectroscopy reveals essential and practical information for novel device applications.

The emergence of a triple phase point in a two-dimensional parameter space (such as pressure and temperature) can offer unforeseen opportunities for the coupling of two seemingly independent order parameters. On the basis of this, we demonstrate the electric control of magnetic order by manipulating chemical pressure: lanthanum substitution in the antiferromagnetic ferroelectric BiFeO3. Our demonstration relies on the finding that a multiferroic triple phase point of a single spin-disordered phase and two spin-ordered phases emerges near room temperature in Bi0.9La0.1FeO3 ferroelectric thin films. By using spatially resolved X-ray absorption spectroscopy, we provide direct evidence that the electric poling of a particular region of the compound near the triple phase point results in an antiferromagnetic phase while adjacent unpoled regions remain magnetically disordered, opening a promising avenue for magnetoelectric applications at room temperature

Polymorphism allows the symmetry of the lattice and spatial charge distributions of atomically thin materials to be designed. While various polymorphs for superconducting, magnetic, and topological states have been extensively studied, polymorphic control is a challenge for robust ferroelectricity in atomically thin geometries. Here, the atomic and electric manipulation of ferroelectric polymorphs in Mo1−xWxTe2 is reported. Atomic manipulation for polymorphic control via chemical pressure (substituting tungsten for molybdenum atoms) and charge density modulation can realize tunable polar lattice structures and robust ferroelectricity up to T = 400 K with a constant coercive field in an atomically thin material. Owing to the effective inversion symmetry breaking, the ferroelectric switching withstands a charge carrier density of up to 1.1 × 1013 cm−2, developing an original diagram for ferroelectric switching in atomically thin materials.

The massless nature of Dirac Fermions produces large energy gaps between Landau levels (LLs), which is promising for topological devices. While the energy gap between the zeroth and first LLs reaches 36 meV in a magnetic field of 1 T in graphene, exploiting the quantum Hall effect at room temperature requires large magnetic fields (∼30 T) to overcome the energy level broadening induced by charge inhomogeneities in the device. Here, we report a way to use the robust quantum oscillations of Dirac Fermions in a single-defect resonant transistor, which is based on local tunneling through a thin (∼1.4 nm) hexagonal boron nitride (h-BN) between lattice-orientation-aligned graphene layers. A single point defect in the h-BN, selected by the orientation-tuned graphene layers, probes local LLs in its proximity, minimizing the energy broadening of the LLs by charge inhomogeneity at a moderate magnetic field and ambient conditions. Thus, the resonant tunneling between lattice-orientation-aligned graphene layers highlights the potential to spectroscopically locate the atomic defects in the h-BN, which contributes to the study on electrically tunable single photon source via defect states in h-BN.

Layered semimetals such as monoclinic MoTe2 and WTe2 demonstrate superconducting, topological insulating, and Weyl semimetallic states based on their unique electronic band topology. While doping concentration, lattice constants, and spin–orbit coupling can largely modulate the quantum states of the semimetals, a puzzling issue is that their functional carrier density and magnetoresistance for practical applications critically vary by temperature, which cannot be explained by the conventional phonon effect or a structural phase transition. Here, a native doping‐mediated thermomechanical manipulation of electric transport in semimetallic MoTe2 is reported, where effective transport is controlled by temperature in an equivalent manner to electric gating. Combining X‐ray diffraction, scanning tunneling microscopy, transport measurements, and first‐principles calculations, a Fermi level shift and subsequent changes in electronic structures are revealed as the origins of the practical transport changes in MoTe2. Moreover, the initial doping state of the MoTe2, determined by the Te vacancy density in two different growth methods, reciprocally affects the thermomechanical lattice and band structure changes, which is promising for novel electronic applications such as magnetic sensors and memory devices with layered semimetals.