We demonstrate precise control of magnetism in MnBi2Te4 thin films through careful synthesis by molecular beam epitaxy, achieving minimal defects and accurate layer thickness control. By optimizing Mn-Bi-Te ratios and growth temperatures, we minimize detrimental self-doping effects and accurately target integer-layer films. X-ray diffraction and reflectivity provide quantitative measures of film quality and thickness. When these macroscale probes of structure and thickness are integrated with magnetotransport measurements, a striking even-odd layer dependence of the anomalous Hall effect is revealed. Odd-layer films exhibit a large hysteresis up to the N & eacute;el temperature (similar to 25 K), consistent with noncompensated antiferromagnetism, while even-layer films show minimal response, as expected for an antiferromagnet. The sign of the anomalous Hall effect exhibits a sign reversal for intrinsic magnetism versus magnetism associated with defects. This work identifies critical factors for inducing pure, noncompensated ferromagnetism and reveals the characteristics of the intrinsic anomalous Hall effect in MnBi2Te4, which together is a step toward realizing the zero-field quantum anomalous Hall effect in topological materials.

Phase selecting nearly degenerate crystalline polymorphs during epitaxial growth can be challenging yet critical to targeting physical properties for specific applications. Here, we establish how phase selectivity of altermagnetic and noncentrosymmetric polymorphs of MnTe can be programmed by subtle changes to the surface of lattice-matched InP substrates in molecular beam epitaxy growth. Bulk altermagnetic MnTe is thermodynamically stable in the hexagonal NiAs-structure and is synthesized here on the polar (111)A surface (In-terminated) of InP, while the noncentrosymmetric, cubic ZnS-structure with wide band gap (>3 eV), which epitaxially matches III-V materials, is stabilized on the (111)B surface (P-terminated). Electron microscopy, X-ray photoemission spectroscopy, and reflection high-energy electron diffraction indicate that phase selection is triggered at the interface and proceeds along the growing surface. First-principles calculations suggest that interfacial termination and strain have a significant effect on the interfacial energy; stabilizing the NiAs polymorph on the In-terminated surface and the ZnS structure on the P-terminated surface. Selectively grown, high-quality, phase pure films of both MnTe polymorphs will enable our understanding of the novel properties of these materials, thereby facilitating their use in new applications ranging from spintronics to microelectronic devices.

This paper shows how data-driven machine learning approaches can improve growth control, reproducibility, and physical insight in the pulsed laser deposition (PLD) growth of correlated oxides. Despite well-known relationships between growth conditions and material properties, consistently producing high-quality films of complex materials like LaVO_3 remains difficult due to the highly non-equilibrium nature of PLD and the defects and competing phases that accumulate during growth. Here, we use an active learning framework based on Gaussian process Bayesian optimization that incorporates measured bulk and surface lattice properties along with impurity phase information to efficiently map the multidimensional growth space of LaVO_3 by PLD. By tuning the relative weighting of these properties, the model identifies an optimized region where phase-pure films of LaVO_3 exhibit two-dimensional surfaces, near-ideal lattice parameters, and minimal sub-band gap optical absorption. The trained model reveals clear competition among different defect formation mechanisms that are connected to unseen parameters like supersaturation and surface mobility, thus giving insight into the highly non-equilibrium process of PLD growth. Together, this demonstrates that property-guided machine learning can accelerate materials optimization while providing a new way to address fundamental growth mechanisms in PLD that enable understanding and utilization of quantum phenomena found in complex oxides.

The epitaxial synthesis of high‐quality 2D layered materials is an essential driver of both fundamental physics studies and technological applications. Bi 2 Se 3 , a prototypical 2D layered topological insulator, is sensitive to defects imparted during the growth, either thermodynamically or due to the film‐substrate interaction. In this study, it is shown that step‐terminated Al 2 O 3 substrates with a high miscut angle (3°) can effectively suppress a particular hard‐to‐mitigate defect, the antiphase twin. Systematic investigations across a range of growth temperatures and substrate miscut angles confirm that atomic step edges act as preferential nucleation sites, stabilizing a single twin domain. First‐principles calculations suggest that there is a significant energy barrier for twin boundary formation at step edges, supporting the experimental observations. Detailed structural characterization indicates that this twin‐selectivity is lost through the mechanism of the 2D layers overgrowing the step edges, leading to higher twin density as the thickness increases. These findings highlight the complex energy landscape unique to 2D materials that is driven by the interplay between substrate properties, nucleation dynamics, and defect formation, and overcoming and controlling these are critical to improve material quality for quantum and electronic applications.

The integration of monolayer (ML) two-dimensional (2D) materials into next-generation microelectronics, optoelectronics, and sensors is hindered by their sensitivity to environmental exposure. Deposition of additional layers for encapsulation or growth on ML 2D materials by versatile but energetic plasma techniques such as pulsed laser deposition (PLD) has not been considered at the monolayer level because of potential damage caused by hyperthermal species with kinetic energies (KEs) exceeding the threshold displacement energy (TDE) of the ML. Here, we describe a general strategy to understand and mitigate damage during PLD by reducing the incident KE of ablated species below the TDE of the 2D monolayer using background gas collisions. Ion flux diagnostics, combined with in situ Raman spectroscopy of monolayer graphene during PLD of amorphous boron nitride (a-BN) as a dielectric encapsulation layer, show that damage is primarily correlated with fast ions that penetrate the background gas in accordance with Beer's Law and are often overlooked in ICCD imaging due to the dominance of the bright, delayed plasma luminescence. Significantly, if fast ions are eliminated and a ∼2 nm-thick a-BN layer is "soft landed", the monolayer graphene is effectively protected from damage by high KE species in the boron nitride plasma plume. Deposited a-BN films display a characteristic dielectric constant of 3.6 at 100 kHz and tunable charge injection properties. Our results enable PLD as a viable option for encapsulation and thin film growth onto ML 2D materials, with implications for both fundamental research and device integration.

The epitaxial synthesis of high-quality 2D layered materials is an essential driver of both fundamental physics studies and technological applications. Bi$_2$Se$_3$, a prototypical 2D layered topological insulator, is sensitive to defects imparted during the growth, either thermodynamically or due to the film-substrates interaction. In this study, we demonstrate that step-terminated Al$_2$O$_3$ substrates with a high miscut angle (3$^\circ$) can effectively suppress a particular hard-to-mitigate defect, the antiphase twin. Systematic investigations across a range of growth temperatures and substrate miscut angles confirm that atomic step edges act as preferential nucleation sites, stabilizing a single twin domain. First principles calculations suggest that there is a significant energy barrier for twin boundary formation at step edges, supporting the experimental observations. Detailed structural characterization indicates that this twin-selectivity is lost through the mechanism of the 2D layers overgrowing the step edges, leading to higher twin density as the thickness increases. These findings highlight the complex energy landscape unique to 2D materials that is driven by the interplay between substrate topology, nucleation dynamics, and defect formation, and overcoming and controlling these are critical to improve material quality for quantum and electronic applications.

Superconductor-normal-superconductor (SC-N-SC) weak links enable Cooper-pair tunneling and serve as Josephson junctions (JJs) used in modern superconducting qubits. Conventional JJs rely on vertically stacked Al-AlOx-Al trilayers that are difficult to fabricate and are sensitive to ambient exposure. Here, we demonstrate an all-in-plane alternative by "nanosculpting" 100 nm-wide channels into thin films of FeTe0.75Se0.25/Bi2Te3 (FTS/BT), a candidate topological superconductor, with a Si++ focusses ion beam (FIB). Systematic irradiation shows that increasing the ion dose, while keeping the beam energy constant, progressively suppresses both the critical temperature (Tc) and critical current (Ic), confirming the creation of a controllable weak link even though a Fraunhofer interference pattern is not observed. Kelvin prove force microscopy , atomic force microscopy and scanning electron microscopy corroborate the structural and electronic modification of the irradiated region. Ic (B) measurements reveal a slower field-induced decay of Ic at higher doses, indicating that irradiation-induced defects act as vortex-pinning centers that mitigate vortex motion and associated dissipation, By tuning beam energy and dose, the process shifts from SC-N-SC regime toward a superconductor-insulator-superconductor (SC-I-SC) geometry, offering a simple scalable pathway to JJ fabrication. These results established FIB pattering as a versatile platform for engineering robust, scalable fault-tolerant qubits.

The epitaxial synthesis of high-quality 2D layered materials is an essential driver of both fundamental physics studies and technological applications. Bi_2Se_3, a prototypical 2D layered topological insulator, is sensitive to defects imparted during the growth, either thermodynamically or due to the film-substrate interaction. In this study, it is shown that step-terminated Al_2O_3 substrates with a high miscut angle (3°) can effectively suppress a particular hard-to-mitigate defect, the antiphase twin. Systematic investigations across a range of growth temperatures and substrate miscut angles confirm that atomic step edges act as preferential nucleation sites, stabilizing a single twin domain. First-principles calculations suggest that there is a significant energy barrier for twin boundary formation at step edges, supporting the experimental observations. Detailed structural characterization indicates that this twin-selectivity is lost through the mechanism of the 2D layers overgrowing the step edges, leading to higher twin density as the thickness increases. These findings highlight the complex energy landscape unique to 2D materials that is driven by the interplay between substrate properties, nucleation dynamics, and defect formation, and overcoming and controlling these are critical to improve material quality for quantum and electronic applications.

Combinatorial magnetron sputtering and electrical characterization were used to systematically study the impact of compositional changes in the resistive switching of transition metal oxides, specifically the ZrxTa1-xOy system. Current-voltage behavior across a range of temperatures provided insights into the mechanisms that contribute to differences in the electrical conductivity of the pristine Ta2O5 and ZrO2, and mixed ZrxTa1-xOy devices. The underlying conductive mechanism was found to be a mixture of charge trapping and ionic motion, where charge trapping/emission dictated the short-term cycling behavior while ion motion contributed to changes in the conduction with increased cycling number. ToF-SIMS was used to identify the origin of the "wake-up" behavior of the devices, revealing an ionic motion contribution. This understanding of how cation concentration affects conduction in mixed valence systems helps provide a foundation for a new approach toward manipulating resistive switching in these active layer materials.

As Moore’s law approaches its limits, chalcogenides offer a promising route to next-generation computing and sensing, thanks to their topological, magnetoelectric, excitonic, and spintronic properties. Yet the same traits that make them appealing, e.g., exotic properties at monolayer thickness, clean van der Waals interfaces, and strong many-body effects, also heighten sensitivity to fabrication, hindering translation into scalable devices. Progress is further constrained by fragmented knowledge across synthesis, processing, and integration, and by the lack of systematic links between fabrication parameters and performance metrics. This Perspective examines key obstacles in controlling chalcogenide heterostructures and stresses the need for an integrated co-design framework, uniting materials growth, processing, and device architecture to accelerate practical technologies.

Quantum materials with novel spin textures from strong spin-orbit coupling (SOC) are essential components for a wide array of proposed spintronic devices. Topological insulators have a necessary strong SOC that imposes a unique spin texture on topological states and Rashba states that arise on the boundary, but there is no established methodology to control the spin texture reversibly. Here, it is demonstrated that functionalizing Bi2Se3 films by altering the step-edge termination directly changes the strength of SOC and thereby modifies the Rashba strength of 1D edge states. Scanning tunneling microscopy/spectroscopy shows that these Rashba edge states arise and subsequently vanish through the Se functionalization and reduction process of the step edges. The observations are corroborated by density functional theory calculations, which show that a subtle chemical change of edge termination fundamentally alters the underlying electronic structure. Importantly, fully reversible and repeatable switching of Rashba edge states across multiple cycles at room temperature is experimentally demonstrated. The results imply Se functionalization as a practical method to control SOC and spin texture of quantum states in topological insulators.

The epitaxial synthesis of high-quality 2D layered materials is an essential driver of both fundamental physics studies and technological applications. Bi2Se3, a prototypical 2D layered topological insulator, is sensitive to defects imparted during the growth, either thermodynamically or due to the film-substrate interaction. In this study, it is shown that step-terminated Al2O3 substrates with a high miscut angle (3 degrees) can effectively suppress a particular hard-to-mitigate defect, the antiphase twin. Systematic investigations across a range of growth temperatures and substrate miscut angles confirm that atomic step edges act as preferential nucleation sites, stabilizing a single twin domain. First-principles calculations suggest that there is a significant energy barrier for twin boundary formation at step edges, supporting the experimental observations. Detailed structural characterization indicates that this twin-selectivity is lost through the mechanism of the 2D layers overgrowing the step edges, leading to higher twin density as the thickness increases. These findings highlight the complex energy landscape unique to 2D materials that is driven by the interplay between substrate properties, nucleation dynamics, and defect formation, and overcoming and controlling these are critical to improve material quality for quantum and electronic applications.

The field of spintronics has seen a surge of interest in altermagnetism due to novel predictions and many possible applications. MnTe is a leading altermagnetic candidate that is of significant interest across spintronics due to its layered antiferromagnetic structure, high Neel temperature (TN approximate to 310 K) and semiconducting properties. The results on molecular beam epitaxy (MBE) grown MnTe/InP(111) films are presented. Here, it is found that the electronic and magnetic properties are driven by the natural stoichiometry of MnTe. Electronic transport and in situ angle-resolved photoemission spectroscopy show the films are natively metallic with the Fermi level in the valence band and the band structure is in good agreement with first-principles calculations for altermagnetic spin-splitting. Neutron diffraction confirms that the film is antiferromagnetic with planar anisotropy and polarized neutron reflectometry indicates weak ferromagnetism, which is linked to a slight Mn-richness that is intrinsic to the MBE-grown samples. When combined with the anomalous Hall effect, this work shows that the electronic response is strongly affected by the ferromagnetic moment. Altogether, this highlights potential mechanisms for controlling altermagnetic ordering for diverse spintronic applications. Seeking to understand recent predictions of the exotic state known as "altermagnetism". The study reports that even when high-quality samples are grown by molecular beam epitaxy, altermagnetic candidates may exhibit richer phenomena than anticipated, which highlights new routes to take advantage of these novel magnetic materials for new applications. image

Realizing topological superconductivity by integrating high-transition-temperature (TC) superconductors with topological insulators can open new paths for quantum computing applications. Here, a new approach is reported for increasing the superconducting transition temperature ( T C onset ) $( {T_{\mathrm{C}}^{{\mathrm{onset}}}} )$ by interfacing the unconventional superconductor Fe(Te,Se) with the topological insulator Bi-Te system in the low-Se doping regime, near where superconductivity vanishes in the bulk. The critical finding is that the T C onset $T_{\mathrm{C}}^{{\mathrm{onset}}}$ of Fe(Te,Se) increases from nominally non-superconducting to as high as 12.5 K when Bi2Te3 is replaced with the topological phase Bi4Te3. Interfacing Fe(Te,Se) with Bi4Te3 is also found to be critical for stabilizing superconductivity in monolayer films where T C onset $T_{\mathrm{C}}^{{\mathrm{onset}}}$ can be as high as 6 K. Measurements of the electronic and crystalline structure of the Bi4Te3 layer reveal that a large electron transfer, epitaxial strain, and novel chemical reduction processes are critical factors for the enhancement of superconductivity. This novel route for enhancing TC in an important epitaxial system provides new insight on the nature of interfacial superconductivity and a platform to identify and utilize new electronic phases.

Automated platforms for synthesis are a necessity to increase the rate of discovery, synthesis, and optimization of materials to match the accelerating pace of theoretical predictions. Here, we introduce a novel pulsed laser deposition (PLD) platform that combines in situ Raman, photoluminescence, and white light reflectance spectroscopies as a material probe with intensified CCD (ICCD) imaging/spectroscopy and ion probe gas-phase PLD plume diagnostics. These diagnostics together with full automation and high-throughput synthesis schemes enable rapid synthesis and characterization with a Python-based dataflow for seamless integration with machine learning algorithms. Examples of in situ spectroscopy of 2D materials during growth and modification will be discussed.

Boron-doped carbon nanostructures have attracted great interest recently because of their remarkable electrocatalytic performance comparable to or better than that of conventional metal catalysts. In a previous work (Carbon 123, 605 (2017)), we reported that along with significant performance improvement, B doping enhances the oxidation resistance of few-layer graphene (FLG) that provides increased structural stability for intermediate-temperature fuel-cell electrodes. In general, detailed characterization of the atomic and electronic structure transformations that occur in B-doped carbon nanostructures during fuel-cell operation is lacking. In this work, we use aberration-corrected scanning transmission electron microscopy, nanobeam electron diffraction, and electron energy-loss spectroscopy (EELS) to characterize the atomic and electronic structures of B-doped FLG before and after fuel-cell operation. These data point to the nanoscale corrugation of B-doped FLGs as the key factor responsible for increased stability and high corrosion resistance. The similarity of the 1s to π* and σ* transition features in the B K-edge EELS to those in B-doped carbon nanotubes provides an estimate for the curvature of nanocorrugation in B-FLG.

The current challenge to realizing continuously tunablemagnetismlies in our inability to systematically change properties, such asvalence, spin, and orbital degrees of freedom, as well as crystallographicgeometry. Here, we demonstrate that ferromagnetism can be externallyturned on with the application of low-energy helium implantation andcan be subsequently erased and returned to the pristine state viaannealing. This high level of continuous control is made possibleby targeting magnetic metastability in the ultrahigh-conductivity,nonmagnetic layered oxide PdCoO2 where local lattice distortionsgenerated by helium implantation induce the emergence of a net momenton the surrounding transition metal octahedral sites. These highlylocalized moments communicate through the itinerant metal states,which trigger the onset of percolated long-range ferromagnetism. Theability to continuously tune competing interactions enables tailoringprecise magnetic and magnetotransport responses in an ultrahigh-conductivityfilm and will be critical to applications across spintronics.