Transition-metal dichalcogenides hosting multiple competing structural and electronic phases are thus ideal platforms for constructing polytype heterostructures with emergent quantum properties. However, controlling phase transitions to form diverse heterostructures inside a single crystal remains challenging. In this study, we realize vertical/lateral polytype heterostructures in a hole-doped Mott insulator via thermal annealing-induced structural transitions. Raman spectroscopy, atomic force microscopy and scanning Kelvin probe force microscopy confirm the coexistence of T-H polytype heterostructures. Atomic-scale scanning tunneling microscopy/spectroscopy measurements reveal the transparent effect in 1H/1T vertical heterostructures, where positive bias voltage induces in a pronounced superposition of the 13 & times;13 CDW of the 1T-layer on the 1H-layer. By systematically comparing the 1T/1H and 1T/1T interfaces, we demonstrate that the metallic 1H-layer induces a Coulomb screening effect on the 1T-layer, suppressing the formation of CDW domain walls and forming more ordered electronic states. These results clarify the interfacial coupling between distinct quantum many-body phases and establish a controllable pathway for constructing two-dimensional polytype heterostructures with tunable electronic properties.

Magnetic anisotropy defines the easy axis of a magnetic material and governs the spatial arrangement of its domains. To date, anisotropy engineering has focused on reorienting the easy axis or tuning the anisotropy energy, both of which demand substantial energy input. Here, we demonstrate that magnetic domain textures can be switched without reorienting the easy axis, as observed in a kagome ferromagnet EuTi3Bi4 crystal. Using low-temperature magnetic force microscopy, we observe that the preferred orientation of magnetic domains switches from the a-axis to the b-axis upon temperature variation, and that this switching can also be triggered by an out-of-plane magnetic-field reset. Magnetization measurements and density functional theory calculations confirm a robust c-axis easy magnetization, ruling out a conventional spin-reorientation transition. Instead, the texture switching is governed by the temperature dependence of the in-plane variation of the Magnetic anisotropy energy landscape, which arises from two competing interactions with different decay rates: single-ion anisotropy favors a-oriented spin components, while nearest-neighbor anisotropic exchange favors b-oriented ones. Furthermore, the critical switching temperature is substantially elevated in a mechanically exfoliated EuTi3Bi4 flake. Our findings establish that macroscopic magnetic textures can be effectively manipulated by tuning the competition between in-plane anisotropic interactions, without the energy cost of reorienting the easy axis.

Two-dimensional (2D) magnets hold promise for spintronics but still face challenges regarding limited magnetic tunability and air stability. Here, we demonstrate an effective oxygen plasma treatment strategy that simultaneously modulates magnetism and enhances the air stability of 1T-CrTe2 films. Microstructural characterizations reveal a depth-dependent progressive oxygen induced reconstruction process, in which oxygen substitution induces local Cr-Te-O structural rearrangements that are more pronounced near the surface and gradually extend toward the inner layers with increasing treatment duration. Theoretical calculations combined with magnetic measurements suggest that the effective oxidation level regulates interlayer magnetic coupling, leading to an evolution from a FiM-related step-like magnetic transition behavior to a FM-dominated magnetic response. Significantly, the oxygen-doped 1T-CrTe2 exhibits robust environmental stability, retaining room-temperature magnetism even after long-term ambient exposure. This work presents a dual-purpose approach for engineering robust, tunable 2D materials for future spintronic applications.

Metallic charge transport of field-induced carriers can be observed in single-crystal silicon over a wide temperature range. Such behaviour is rare in undoped organic semiconductors but is beneficial for engineering devices with advanced performance. Here we report metallic charge transport in conjugated molecular bilayers down to 8 K with an electrical conductivity of up to 245 S cm−1 and a Hall mobility larger than 100 cm2 V−1 s−1 at 20 K. We use molecular-crystal bilayers of the organic semiconductor 2-decyl-7-phenyl-[1]benzothieno[3,2-b][1]benzothiophene. We infer that this transport behaviour originates from the phenyl bridge coupling between the two molecular layers, which suppresses molecular vibrations and weakens Coulomb interactions. We develop a controlled method for introducing defects, using which we observe a disorder-driven metal–insulator transition in the molecular crystal. Molecular bilayer crystals of an organic semiconductor can exhibit metallic charge transport down to 8 K with an electrical conductivity of up to 245 S cm−1, as well as charge carrier mobility values of more than 100 cm2 V−1 s−1 at 20 K.

The chromium-based kagome metal CsCr3Sb5 has garnered broad interest owing to its strong electron correlations, intertwined orders and potential for unconventional superconductivity under high pressure. The evolution of magnetic and superconducting interactions as the more frequently studied CsV3Sb5 is doped to CsCr3Sb5 remains poorly understood. Here we demonstrate the emergence of a spatially anisotropic Kondo resonance intertwined with the superconducting gap, enabled by introducing magnetic Cr impurities into the kagome superconductor CsV3Sb5. The addition of dilute Cr impurities not only weakens the long-range charge density wave order but also produces local magnetic moments, which leads to Kondo resonances. We show that the Kondo resonance forms anisotropic, ripple-like spatial patterns around individual Cr atoms, breaking all local mirror symmetries. We further reveal that, with the emergence of Kondo screening, the coherence peak and depth of the superconducting gap with finite zero-energy conductance are enhanced. This suggests that non-superconducting carriers at the Fermi surface in the parent compound participate in the Kondo effect, simultaneously screening Cr magnetic moments and increasing the superfluid density. Our findings offer an opportunity to study the interplay between superconductivity and local magnetism in kagome materials.

Inverse materials design starts from target functionality and searches for structures that can realize it. Its value in closed-loop discovery depends not only on prediction performance, but also on whether expensive first-principles results are independently validated, provenance-recorded, and admitted as feedback only when evidence is sufficient. This is especially important for composite properties such as carrier mobility, where a final scalar value hides intermediate quantities, fit quality, convergence history, and workflow assumptions. Here we present InvDesMobility, a reliability-gated first-principles feedback framework that integrates multi-agent automated DFT, evidence stratification, generative structure proposal, acquisition ranking, and auditable release. Using 516 2DMatPedia-derived candidates, the workflow produced 280 QC-passed materials and 573 retained carrier-direction seed channels after channel-level reliability gating. These records were split into two feedback objects: relaxed structures updated the generative model, while retained mobility channels trained the acquisition model and set validation priority. Over multiple iterations, InvDesMobility screened 2.4 x 10^6 structures, submitted 102 candidates for DFT validation, and retained 86 reliability-gated generated channels across 41 formulas. Overall, the main contribution is not a fixed list of high-mobility materials, but a transferable feedback contract that makes closed-loop inverse design both useful and auditable when learning from expensive calculated properties. All source data, retained feedback records, and workflows are available at https://github.com/DreamLufei/invDesMobility, with an accompanying evidence website at https://dreamlufei.github.io/invDesMobility/.

Controlling mesoscale and nanoscale material structures and properties through self-organized atomic behavior is essential for atomic-scale manufacturing. However, direct and visual studies of the cross-scale effects of such atomic self-organization on mesoscopic structures remain scarce. Herein, we report the intertwined atomic-nanoscale-mesoscale structures via the intralayer Fe-chains in the sandwich-like layered FePd2Te2 crystal by scanning tunneling microscopy (STM) and atomic force microscopy (AFM). The hierarchical orthogonal corrugated morphologies are directly revealed and attributed to their chain-orientation-determined twinning-domain effect. Both Fe-chains of the middle-sublayer and two kinds of Te atoms of the top-sublayer are further atomically resolved, indicating the critical effects of Pd atoms/voids on the intralayer anisotropic Fe-chains and the interlayer structural alignment. The thermally induced and strain-related structural transitions of the surface layer are further investigated and discussed based on the proposed filling model of Pd-voids by the intralayer Pd atoms. Our work not only provides a deep understanding of this exotic layered magnetic material but also will inspire more perspectives for tailoring its anisotropic atomic-to-mesoscale structures and properties.

Information units are progressively approaching the fundamental physical limits of integration density, including in terms of extremely small sizes, multistates and probabilistic traversal. However, simultaneously encompassing all of these characteristics in a unit remains elusive. Here, via real-time in situ electrical monitoring, we clearly observed stochastic alterations of multiple conductance states in Sc2C2@C88. The true random bit sequence generated exhibited an autocorrelation function whose confidence interval fell within ±0.02, demonstrating high-quality randomness. The alterations of multiple conductance states are controllable, that is, whose probability distributions could traverse from 0 to 1, enabling us to factorize 551 into its prime factors. Furthermore, we proposed a matrix-chain multiplication scheme and experimentally verified the multiplication of two 4 × 4 state-transition matrices with a small maximum error of <0.05. Combined with theoretical calculations, the stochastic but controllable multistates are probably attributed to the rich energy landscape, which could be stepwise changed by the electric field. Our findings reveal extremely small multilevel probabilistic bit for matrix multiplication, which pave the way for ultra-compact intelligent electronic devices.

Breathing kagome materials Nb3X8 (X = F, Cl, Br, I) have attracted broad interest owing to their Mott insulating behavior and stacking-dependent magnetic ground states. However, the role of interlayer coupling in modulating these properties remains underexplored. Here, using density functional theory with Hubbard U corrections, we systematically investigated how interlayer coupling affects the Mott insulating states and magnetic ground states across 24 bilayer stacking configurations for each compound. We found that all bilayers remain Mott insulators, demonstrating robust Mottness. Driven by the competition between interlayer Pauli repulsion and hopping, most stackings favor interlayer AFM order, including conventional and compensated AFM, while some exhibit AFM-FM degeneracy or stabilize interlayer FM. This robustness of Mott states coexisting with tunable interlayer magnetism provides novel analysis and insights for research on breathing kagome Mott insulators.

The charge states of metal adatoms on surfaces play a crucial role in controlling adsorption and interaction behaviors that underpin surface chemistry and catalysis, yet the atomically precise synthesis of negatively charged metal atoms remains a significant challenge. Here, we report negatively charged Ag dimer (Ag2δ-) arrays assembled on Ag(100) surface through coordination with a polycyclic aromatic hydrocarbon, 8,9-diaza-8a-borabenzo[fg]tetracene (DBT), featuring a doping moiety with N-B-N bonds at zigzag edge. The Ag dimers are stabilized by two DBT monomers through N-Ag-N coordination bonding. In contrast to surface Ag atoms, the coordinated dimers display anionic character, as demonstrated by noncontact atomic force microscopy, Kelvin probe force microscopy, X-ray photoelectron spectroscopy, and density functional theory calculations. Neutral dimers Ag20 can be converted from the coordinated complex by tip-induced detachment of one DBT monomer and showed markedly higher affinity for CO adsorption, a process that is suppressed on Ag2δ-. These findings establish an atomically defined platform for stabilizing and controlling anionic metal centers on metallic surfaces, providing a model system for exploring charge-state effects in surface chemistry.

Luttinger compensated antiferromagnets (LcAFMs), combining spin polarization with vanishing net magnetization, offer distinct advantages for next-generation spintronic applications. Using first-principles calculations, we demonstrate that conventional antiferromagnetic CrCl2 double chains can be transformed into one-dimensional LcAFMs under an external electric field, exhibiting pronounced isotropic spin splitting. The magnitude of the splitting, as well as the bandgap, can be effectively tuned by both in-plane and out-of-plane fields, thereby providing greater controllability than in two-dimensional counterparts. To further enhance the tunability, we design a nearly lattice-matched CrCl2/MoTe2 heterostructure and uncover that interfacial charge transfer generates a built-in electric field, inducing spin splitting comparable to that driven by external fields. These results establish interfacial engineering as a highly efficient route to realize and manipulate LcAFM states in low-dimensional magnets, expanding the design principles for spintronic functionalities at the nanoscale.

Atomically thin InTe, a III-VI analogue of InSe, has recently emerged as a promising two-dimensional semiconductor for nanoelectronics, yet the nature of its two-dimensional electron gas (2DEG) has remained experimentally elusive. Here, using scanning tunneling microscopy (STM) combined with quasiparticle interference (QPI) imaging, we present direct evidence of the existence of a 2DEG in monolayer and bilayer InTe. Bias-dependent standing-wave patterns reveal a parabolic conduction-band dispersion in both thicknesses. Quantitative analysis yields a low electron effective mass of 0.241me in monolayer InTe, smaller than that of monolayer InSe/BLG (∼0.27me). In bilayer InTe, interlayer coupling lifts the conduction-band-edge degeneracy, and produces two subbands with effective masses of 0.197me and 0.802me. Density functional theory calculations are in good agreement with the experimental observations. These results establish atomically thin InTe as a promising platform for low-dimensional electronic physics and nanoelectronic applications.

Correlated and topological phases often coexist or compete in van der Waals materials, yet achieving an electrically switchable and reversible conversion between them remains a substantial challenge. Such control is crucial for understanding their interplay and enabling nonvolatile, low-power topological electronics. Here, we propose and demonstrate a polarization-controlled route to switch between Mott insulator and topological metal in ferroelectric-Mott heterostructures. In α-In2Se3/1T-NbSe2, polarization reversal modulates interlayer coupling through out-of-plane orbital alignment. Downward polarization stabilizes Mott-insulating states with type-I band alignment, whereas upward polarization enhances interfacial hybridization, forms interlayer covalent-like quasi-bonding, and drives Γ-point band inversions. The resulting spin-split hybridized valleys penetrate the valence band, inducing a nontrivial topological state with intrinsic anomalous Hall conductivity of ∼102 siemens per centimeter. The comparison with α-In2Se3/1T-TaSe2 and α-In2Se3/1T-TaS2 further identifies Γ-centered valleys and out-of-plane [Formula: see text]-orbital coupling as key ingredients for polarization-switchable topology, providing a general design framework for electrically programmable correlated-topological integration in two-dimensional heterostructures.

As a fundamental phenomenon in nature, chirality has been extensively studied in molecular structures; however, it remains underexplored at the electronic level. Understanding how structural chirality transfers into electronic states is crucial for uncovering the essence of many chiral effects. In this study, we report the engineering and direct visualization of chiral electronic states within an otherwise planar, achiral hexa-peri-hexabenzocoronene (HBC) framework. By employing atomically precise asymmetric nitrogen doping of HBC through on-surface synthesis, we fabricate a C3-symmetric triaza-HBC on Au(111). Utilizing high-resolution scanning tunneling microscopy and non-contact atomic force microscopy, we resolve the chiral molecular structure of triaza-HBC confined to the surface, as well as the chiral texture of the resulting interfacial electronic states and its evolution at different energies. Density functional theory calculations reveal that these electronic chiral features arise from the molecule's intrinsic chiral orbitals, which hybridize strongly with the metal substrate while still retaining their chiral character. This study not only demonstrates a clear transfer of chirality from molecular structure to the electronic landscape but also provides a versatile platform for the rational design of chiral electronic molecules and materials.

In the field of low-energy-consumption applications, electrical control of magnetism has attracted considerable research attention. Here, we report that the Janus Cr2S2Se monolayer, where Se atoms substitute the upper S layer in the Cr2S3 monolayer, is structural stable. We find that the Janus Cr2S2Se monolayer favors the ferromagnetic configuration with a high Curie temperature of 279 K, and shows semiconducting characteristics with an indirect band gap of 0.44 eV and a valley splitting of 33 meV. By constructing a van der Waals multiferroic heterostructure combined with alpha-In2Se3 monolayer, its interlayer magnetism can be switched between two types of magnetic coupling via nonvolatile manipulation of the ferroelectric polarization. Our study reveals the switchable magnetism of the Janus Cr2S2Se monolayer, making it promising candidates for use in next-generation low-dimensional spintronics applications.

The research about two-dimensional van der Waals magnetic materials has advanced the breakthroughs in ultrathin magnetic devices. We experimentally demonstrate that a single-crystal N-face AlN polar substrate can program layer-number-parity-dependent magnetic multistates and their evolution sequence in few-layer CrI3. In odd-layer samples, as 5L-CrI3/AlN, when μ0H sweeps from 3 to -3 T, the reflective magnetic circular dichroism signal evolves through distinct magnetic multistates (+ 5 → -1 → +1 → -5), where +1 corresponds to the moment of a spin-up monolayer. Thereby, we vertically program novel magnetic ground states and their evolution sequence via a simplified heterointerface. Our first-principles calculations attribute this effect to interfacial hole doping: it globally reconfigures the magnetic ground state of odd-layer CrI3 to a novel ferrimagnetic order, and spatially differentiates the interlayer exchange coupling and magnetic anisotropy between the surface/interfacial and interior layers. Our work advances the practical integration and design of two-dimensional magnetic devices with tailored functionalities.

Strongly correlated quantum states, such as charge density waves (CDWs), are exquisitely sensitive to Fermi surface topology and lattice symmetry, and are typically quenched by heavy carrier doping. In two-dimensional (2D) systems, however, macroscopic geometric curvature emerges as a novel structural degree of freedom to modulate microscopic quantum coherence. This raises a compelling physical question: can non-Euclidean geometric deformations compete with extreme electronic perturbations to reshape, or even revive, a quenched macroscopic quantum order? Here, by constructing monolayer TiSe_2-NbSe_2 heterostructure on a BLG/SiC substrate for the first time, we report the curvature-driven revival of a frustrated charge order in a non-Euclidean space. Low-temperature angle-resolved photoemission spectroscopy (ARPES) reveals a massive interfacial charge transfer, which destroys the global Fermi surface nesting and completely suppresses the long-range CDW order in Euclidean flat regions. Strikingly, high-resolution scanning tunneling microscopy (STM) reveals that a novel, non-linear CDW state miraculously survives, remaining strictly localized within morphologically distorted, non-Euclidean nanoscale curved regions. Atomistic simulations unravel the structural origin of this phenomenon, demonstrating that interfacial twist and lattice mismatch spontaneously generate a corrugated superlattice.