arXiv subjects

Anton Tadich

Publications and source records attributed to Anton Tadich.

At least 19 recordsLinked to original sources

arXiv2025

Selective Oxidation and Cr Segregation in High-Entropy Oxide Thin Films

High-entropy oxides (HEOs) offer exceptional compositional flexibility and structural stability, making them promising materials for energy and catalytic applications. Here, we investigate Sr doping effects on B-site cation oxidation states, local composition, and structure in epitaxial La1-xSrx(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 thin films. X-ray spectroscopies reveal that Sr doping preferentially promotes Cr oxidation from Cr3+ to Cr6+, partially oxidizes Co and Ni, while leaving Mn4+ and Fe3+ unchanged. Atomic-resolution scanning transmission electron microscopy with energy-dispersive X-ray spectroscopy shows pronounced Cr segregation, with Cr exhibiting depletion at the film-substrate interface and enrichment at the film surface, along with the formation of a partially amorphous phase in heavily Sr-doped samples. This segregation is likely driven by oxidation-induced migration of smaller, high-valence Cr cations during the growth. These findings underscore the critical interplay between charge transfer, local strain, and compositional fluctuations, providing strategies to control surface composition and electronic structure in HEOs for more robust electrocatalyst design.

cond-mat.mtrl-sci↗

arXiv2025

Spin Texture Control and Magnetic Gap Engineering in a Ferromagnetic Insulator-Topological Insulator Sandwiched Heterostructure

Quantum materials combining magnetism and topological fermions are a key platform for low-energy electronics, spintronics, and quantum phases that break time-reversal symmetry (TRS), such as the quantum anomalous Hall effect (QAHE). Coupling a topological insulator to a magnetic material allows proximity magnetization with the potential to achieve these phases at elevated temperatures. One potential architecture for realizing QAHE at elevated temperature is a heterostructure comprising two single-septuple layers (1SL) of MnBi2Te4 (a 2D ferromagnetic insulator) with four-quintuple layer (4QL) Bi2Te3 in the middle. However, the origin of this gap has not yet been explicitly determined, as there are other non-magnetic mechanisms that have been shown to produce bandgaps in similar systems. Here, through spin- and angle-resolved photoemission, the magnetic nature of the gap opening is investigated to demonstrates direct control of the spin state via small magnetic fields and confirm the magnetic origin of the gap through spin splitting and broken TRS. Furthermore, the hallmark chiral spin texture of non-magnetic topological insulators is preserved away from the {\Gamma}-point, despite the large 72+/-10 meV exchange gap at the Dirac point. The robust magnetic gap and controllable spin texture hold significant promise for future technologies requiring both magnetic properties and topological protection.

cond-mat.mtrl-sci↗

arXiv2025

Three-dimensional flat band in ultra-thin Kagome metal Mn3Sn film

Flat bands with small energy dispersion can give rise to strongly correlated electronic and topological phases, especially when located at the Fermi level. Whilst flat bands have been experimentally realized in two-dimensional (2D) twisted van der Waals heterostructures, they are highly sensitive to twist angle, necessitating complex fabrication techniques. Geometrically frustrated kagome lattices have emerged as an attractive platform as they natively host flat bands that have been observed experimentally in quasi-2D bulk-crystal kagome metals. An outstanding experimental question is whether flat bands can be realized in atomically thin metals, with opportunities for stronger electron-electron interactions through tuning of the surrounding dielectric environment. Here we use angle-resolved photoelectron spectroscopy, scanning tunnelling microscopy and band structure calculations to show that ultra-thin films of the kagome metal Mn3Sn host a robust dispersionless flat band with a bandwidth of 50 meV. Furthermore, we demonstrate chemical tuning of the flat band to near the Fermi level via manganese defect engineering. The realization of tunable kagome-derived flat bands in an ultra-thin kagome metal, represents a promising platform to study strongly correlated and topological phenomena, with applications in quantum computing, spintronics and low-energy electronics.

cond-mat.str-el↗

arXiv2024

Reversal of charge transfer doping on the negative electronic compressibility surface of MoS2

The strong electron-electron interaction in transition metal dichalcogenides (TMDs) gives rise to phenomena such as strong exciton and trion binding and excitonic condensation, as well as large negative exchange and correlation contributions to the electron energies, resulting in negative electronic compressibility. Here we use angle-resolved photoemission spectroscopy to demonstrate a striking effect of negative electronic compressibility in semiconducting TMD MoS2 on the charge transfer to and from a partial overlayer of monolayer semimetallic WTe2. We track the changes in binding energy of the valence bands of both WTe2 and MoS2 as a function of surface transfer doping with donor (K) and acceptor (F4-TCNQ) species. Donor doping increases the binding energy of the MoS2 valence band, as expected, while counterintuitively reducing the binding energy of the WTe2 valence bands and core levels. The inverse effect is observed for acceptor doping, where a typical reduction in the MoS2 binding energies is accopanied by an unexpected increase in those of WTe2. The observations imply a reversal of the expected charge transfer; donor (acceptor) deposition decreases (increases) the carrier density in the WTe2 adlayer. The charge transfer reversal is a direct consequence of the negative electronic compressibility of the MoS2 surface layer, for which addition (subtraction) of charge leads to attraction (repulsion) of further charge from neighbouring layers. These findings highlight the importance of many-body interactions for the electrons in transition metal dichalcogenides and underscore the potential for exploring strongly correlated quantum states in two-dimensional semiconductors.

cond-mat.str-el↗

arXiv2024

The submonolayer assembly of C60F48 surface acceptors on the hydrogen-terminated (100) diamond surface

We have characterised the submonolayer assembly of C60F48 molecular surface acceptors on the hydrogen terminated (100) diamond surface using scanning tunneling microscopy and X-ray photoelectron spectroscopy, and explored the influence this assembly has on the energy level alignment which governs surface transfer doping. Following deposition, disordered multilayered islands are observed. Annealing to 90$^{\circ} \rm{C}$ causes a transition from dewetting multi-layered islands to a single wetting layer at sufficiently high coverage, accompanied by a change in the energy alignment between the C60F48 and the diamond surface which consequently decreased the carrier density induced by transfer doping by 20%.

cond-mat.mtrl-sci↗

arXiv2024

Reactivity of ultra-thin Kagome Metal FeSn towards Oxygen and Water

The kagome metal FeSn, consists of alternating layers of kagome-lattice Fe3Sn and honeycomb Sn2, and exhibits great potential for applications in future low energy electronics and spintronics because of an ideal combination of novel topological phases and high-temperature magnetic ordering. Robust synthesis methods for ultra-thin FeSn films, as well as an understanding of their air stability is crucial for its development and long-term operation in future devices. In this work, we realize large area, sub-10 nm epitaxial FeSn thin films, and explore the oxidation process via synchrotron-based photoelectron spectroscopy using in-situ oxygen and water dosing, as well as ex-situ air exposure. Upon exposure to atmosphere the FeSn films are shown to be highly reactive, with a stable ~3 nm thick oxide layer forming at the surface within 10 minutes. Notably the surface Fe remains largely unoxidized when compared to Sn, which undergoes near-complete oxidation. This is further confirmed with controlled in-situ dosing of O2 and H2O where only the Sn2 (stanene) inter-layers within the FeSn lattice oxidize, suggesting the Fe3Sn kagome layers remain almost pristine. These results are in excellent agreement with first principles calculations, which show Fe-O bonds to the Fe3Sn layer are energetically unfavorable, and furthermore, a large formation energy preference of 1.37 eV for Sn-O bonds in the stanene Sn2 layer over Sn-O bonds in the kagome Fe3Sn layer. The demonstration that oxidation only occurs within the stanene layers may provide new avenues in how to engineer, handle and prepare future kagome metal devices.

cond-mat.mtrl-sci↗

arXiv2024

2024 roadmap on 2D topological insulators

2D topological insulators promise novel approaches towards electronic, spintronic, and quantum device applications. This is owing to unique features of their electronic band structure, in which bulk-boundary correspondences enforces the existence of 1D spin-momentum locked metallic edge states - both helical and chiral - surrounding an electrically insulating bulk. Forty years since the first discoveries of topological phases in condensed matter, the abstract concept of band topology has sprung into realization with several materials now available in which sizable bulk energy gaps - up to a few hundred meV - promise to enable topology for applications even at room-temperature. Further, the possibility of combining 2D TIs in heterostructures with functional materials such as multiferroics, ferromagnets, and superconductors, vastly extends the range of applicability beyond their intrinsic properties. While 2D TIs remain a unique testbed for questions of fundamental condensed matter physics, proposals seek to control the topologically protected bulk or boundary states electrically, or even induce topological phase transitions to engender switching functionality. Induction of superconducting pairing in 2D TIs strives to realize non-Abelian quasiparticles, promising avenues towards fault-tolerant topological quantum computing. This roadmap aims to present a status update of the field, reviewing recent advances and remaining challenges in theoretical understanding, materials synthesis, physical characterization and, ultimately, device perspectives.

cond-mat.mes-hall↗

arXiv2024

Formation of a boron-oxide termination for the (100) diamond surface

A boron-oxide termination of the diamond (100) surface has been formed by depositing molecular boron oxide $\rm{B_2O_3}$ onto the hydrogen-terminated (100) diamond surface under ultrahigh vacuum conditions and annealing to $\rm{950^{\circ} C}$. The resulting termination was highly oriented and chemically homogeneous, although further optimisation is required to increase the surface coverage beyond the 0.4 ML achieved here. This work demonstrates the possibility of using molecular deposition under ultrahigh vacuum conditions for complex surface engineering of the diamond surface, and may be a first step in an alternative approach to fabricating boron doped delta layers in diamond.

cond-mat.mtrl-sci↗

arXiv2023

Quasi-free-standing AA-stacked bilayer graphene induced by calcium intercalation of the graphene-silicon carbide interface

We study quasi-freestanding bilayer graphene on silicon carbide intercalated by calcium. The intercalation, and subsequent changes to the system, were investigated by low-energy electron diffraction, angle-resolved photoemission spectroscopy (ARPES) and density-functional theory (DFT). Calcium is found to intercalate only at the graphene-SiC interface, completely displacing the hydrogen terminating SiC. As a consequence, the system becomes highly n-doped. Comparison to DFT calculations shows that the band dispersion, as determined by ARPES, deviates from the band structure expected for Bernal-stacked bilayer graphene. Instead, the electronic structure closely matches AA-stacked bilayer graphene on Ca-terminated SiC, indicating a spontaneous transition from AB- to AA-stacked bilayer graphene following calcium intercalation of the underlying graphene-SiC interface.

cond-mat.mtrl-sci↗

arXiv2023

Increasing the Rate of Magnesium Intercalation Underneath Epitaxial Graphene on 6H-SiC(0001)

Magnesium intercalated 'quasi-freestanding' bilayer graphene on 6H-SiC(0001) (Mg-QFSBLG) has many favorable properties (e.g., highly n-type doped, relatively stable in ambient conditions). However, intercalation of Mg underneath monolayer graphene is challenging, requiring multiple intercalation steps. Here, we overcome these challenges and subsequently increase the rate of Mg intercalation by laser patterning (ablating) the graphene to form micron-sized discontinuities. We then use low energy electron diffraction to verify Mg-intercalation and conversion to Mg-QFSBLG, and X-ray photoelectron spectroscopy to determine the Mg intercalation rate for patterned and non-patterned samples. By modeling Mg intercalation with the Verhulst equation, we find that the intercalation rate increase for the patterned sample is 4.5$\pm$1.7. Since the edge length of the patterned sample is $\approx$5.2 times that of the non-patterned sample, the model implies that the increased intercalation rate is proportional to the increase in edge length. Moreover, Mg intercalation likely begins at graphene discontinuities in pristine samples (not step edges or flat terraces), where the 2D-like crystal growth of Mg-silicide proceeds. Our laser patterning technique may enable the rapid intercalation of other atomic or molecular species, thereby expanding upon the library of intercalants used to modify the characteristics of graphene, or other 2D materials and heterostructures.

cond-mat.mtrl-sci↗

arXiv2022

Giant gate-tunable renormalization of spin-correlated flat-band states and bandgap in a 2D magnetic insulator

Emergent quantum phenomena in two-dimensional van der Waal (vdW) magnets are largely governed by the interplay between the exchange and Coulomb interactions. The ability to tune the Coulomb interaction in such strongly correlated materials enables the precise control of spin-correlated flat-band states, bandgap (Eg) and unconventional magnetism, all of which are crucial for next-generation spintronics and magnonics applications. Here, we demonstrate a giant gate-tunable renormalization of spin-correlated flat-band states and bandgap in magnetic chromium tribromide (CrBr3) monolayers grown on graphene. Our gate-dependent scanning tunneling spectroscopy (STS) studies reveal that the inter-flat-band spacing and bandgap of CrBr3 can be continuously tuned by 120 meV and 240 meV respectively via electrostatic injection of carriers into the hybrid CrBr3/graphene system, equivalent to the modulation of the Cr on-site Coulomb repulsion energy by 500 meV. This can be attributed to the self-screening of CrBr3 arising from the gate-induced carriers injected into CrBr3, which dominates over the opposite trend from the remote screening of the graphene substrate. Precise tuning of the spin-correlated flat-band states and bandgap in 2D magnets via electrostatic modulation of Coulomb interactions not only provides new strategies for optimizing the spin transport channels but also may exert a crucial influence on the exchange energy and spin-wave gap, which could raise the critical temperature for magnetic order.

cond-mat.mes-hall↗

arXiv2021

Formation of a stable surface oxide in MnBi$_2$Te$_4$ thin films

Understanding the air-stability of MnBi$_2$Te$_4$ thin films is crucial for the development and long-term operation of electronic devices based around magnetic topological insulators. In the present work, we study MnBi$_2$Te$_4$ thin films upon exposure to atmosphere using a combination of synchrotron-based photoelectron spectroscopy, room temperature electrical transport and atomic force microscopy to determine the oxidation process. After 2 days air exposure a 2 nm thick oxide passivates the surface, corresponding to oxidation of only the top two surface layers, with the underlying layers preserved. This protective oxide layer results in samples that still exhibit metallic conduction even after several days air exposure. Furthermore, the work function decreases from 4.4 eV for pristine MnBi$_2$Te$_4$ to 4.0 eV after the formation of the oxide, along with only a small shift in the core levels indicating minimal doping as a result of air exposure. With the oxide confined to the top surface layers, and the underlying layers preserved, it may be possible to explore new avenues in how to handle, prepare and passivate future MnBi$_2$Te$_4$ devices.

cond-mat.mtrl-sci↗

arXiv2021

Crossover from 2D ferromagnetic insulator to wide bandgap quantum anomalous Hall insulator in ultra-thin MnBi2Te4

Intrinsic magnetic topological insulators offer low disorder and large magnetic bandgaps for robust magnetic topological phases operating at higher temperatures. By controlling the layer thickness, emergent phenomena such as the Quantum Anomalous Hall (QAH) effect and axion insulator phases have been realised. These observations occur at temperatures significantly lower than the Neel temperature of bulk MnBi2Te4, and measurement of the magnetic energy gap at the Dirac point in ultra-thin MnBi2Te4 has yet to be achieved. Critical to achieving the promise of this system is a direct measurement of the layer-dependent energy gap and verifying whether the gap is magnetic in the QAH phase. Here we utilise temperature dependent angle-resolved photoemission spectroscopy to study epitaxial ultra-thin MnBi2Te4. We directly observe a layer dependent crossover from a 2D ferromagnetic insulator with a bandgap greater than 780 meV in one septuple layer (1 SL) to a QAH insulator with a large energy gap (>100 meV) at 8 K in 3 and 5 SL MnBi2Te4. The QAH gap is confirmed to be magnetic in origin, as it abruptly diminishes with increasing temperature above 8 K. The direct observation of a large magnetic energy gap in the QAH phase of few-SL MnBi2Te4 is promising for further increasing the operating temperature of QAH materials.

cond-mat.mtrl-sci↗

arXiv2020

Low Temperature Growth of Graphene on Semiconductor

The industrial realization of graphene has so far been limited by challenges related to the quality, reproducibility, and high process temperatures required to manufacture graphene on suitable substrates. We demonstrate that epitaxial graphene can be grown on transition metal treated 6H-SiC(0001) surfaces, with an onset of graphitization starting around $450-500^\circ\text{C}$. From the chemical reaction between SiC and thin films of Fe or Ru, $\text{sp}^{3}$ carbon is liberated from the SiC crystal and converted to $\text{sp}^{2}$ carbon at the surface. The quality of the graphene is demonstrated using angle-resolved photoemission spectroscopy and low-energy electron diffraction. Furthermore, the orientation and placement of the graphene layers relative to the SiC substrate is verified using angle-resolved absorption spectroscopy and energy-dependent photoelectron spectroscopy, respectively. With subsequent thermal treatments to higher temperatures, a steerable diffusion of the metal layers into the bulk SiC is achieved. The result is graphene supported on magnetic silicide or optionally, directly on semiconductor, at temperatures ideal for further large-scale processing into graphene based device structures.

cond-mat.mtrl-sci↗

arXiv2020

Magnesium-intercalated graphene on SiC: highly n-doped air-stable bilayer graphene at extreme displacement fields

We use angle-resolved photoemission spectroscopy to investigate the electronic structure of bilayer graphene at high n-doping and extreme displacement fields, created by intercalating epitaxial monolayer graphene on silicon carbide with magnesium to form quasi-freestanding bilayer graphene on magnesium-terminated silicon carbide. Angle-resolved photoemission spectroscopy reveals that upon magnesium intercalation, the single massless Dirac band of epitaxial monolayer graphene is transformed into the characteristic massive double-band Dirac spectrum of quasi-freestanding bilayer graphene. Analysis of the spectrum using a simple tight binding model indicates that magnesium intercalation results in an n-type doping of 2.1 $\times$ 10$^{14}$ cm$^{-2}$, creates an extremely high displacement field of 2.6 V/nm, opening a considerable gap of 0.36 eV at the Dirac point. This is further confirmed by density-functional theory calculations for quasi-freestanding bilayer graphene on magnesium-terminated silicon carbide, which show a similar doping level, displacement field and bandgap. Finally, magnesium-intercalated samples are surprisingly robust to ambient conditions; no significant changes in the electronic structure are observed after 30 minutes exposure in air.

cond-mat.mes-hall↗

arXiv2020

Freestanding n-Doped Graphene via Intercalation of Calcium and Magnesium into the Buffer Layer - SiC(0001) Interface

The intercalation of epitaxial graphene on SiC(0001) with Ca has been studied extensively, yet precisely where the Ca resides remains elusive. Furthermore, the intercalation of Mg underneath epitaxial graphene on SiC(0001) has not been reported. Here, we use low energy electron diffraction, x-ray photoelectron spectroscopy, secondary electron cut-off photoemission and scanning tunneling microscopy to elucidate the physical and electronic structure of both Ca- and Mg-intercalated epitaxial graphene on 6H-SiC(0001). We find that Ca intercalates underneath the buffer layer and bonds to the Si-terminated SiC surface, breaking the C-Si bonds of the buffer layer i.e. 'freestanding' the buffer layer to form Ca-intercalated quasi-freestanding bilayer graphene (Ca-QFSBLG). The situation is similar for the Mg-intercalation of epitaxial graphene on SiC(0001), where an ordered Mg-terminated reconstruction at the SiC surface and Mg bonds to the Si-terminated SiC surface are formed, resulting in Mg-intercalated quasi-freestanding bilayer graphene (Mg-QFSBLG). Ca-intercalation underneath the buffer layer has not been considered in previous studies of Ca-intercalated epitaxial graphene. Furthermore, we find no evidence that either Ca or Mg intercalates between graphene layers. However, we do find that both Ca-QFSBLG and Mg-QFSBLG exhibit very low workfunctions of 3.68 and 3.78 eV, respectively, indicating high n-type doping. Upon exposure to ambient conditions, we find Ca-QFSBLG degrades rapidly, whereas Mg-QFSBLG remains remarkably stable.

cond-mat.mtrl-sci↗

arXiv2020

Electronic bandstructure of in-plane ferroelectric van der Waals $β'-In_{2}Se_{3}$

Layered indium selenides ($In_{2}Se_{3}$) have recently been discovered to host robust out-of-plane and in-plane ferroelectricity in the $α$ and $β$' phases, respectively. In this work, we utilise angle-resolved photoelectron spectroscopy to directly measure the electronic bandstructure of $β'-In_{2}Se_{3}$, and compare to hybrid density functional theory (DFT) calculations. In agreement with DFT, we find the band structure is highly two-dimensional, with negligible dispersion along the c-axis. Due to n-type doping we are able to observe the conduction band minima, and directly measure the minimum indirect (0.97 eV) and direct (1.46 eV) bandgaps. We find the Fermi surface in the conduction band is characterized by anisotropic electron pockets with sharp in-plane dispersion about the $\overline{M}$ points, yielding effective masses of 0.21 $m_{0}$ along $\overline{KM}$ and 0.33 $m_{0}$ along $\overline{ΓM}$. The measured band structure is well supported by hybrid density functional theory calculations. The highly two-dimensional (2D) bandstructure with moderate bandgap and small effective mass suggest that $β'-In_{2}Se_{3}$ is a potentially useful new van der Waals semiconductor. This together with its ferroelectricity makes it a viable material for high-mobility ferroelectric-photovoltaic devices, with applications in non-volatile memory switching and renewable energy technologies.

cond-mat.mtrl-sci↗

arXiv2019

Electric Field-Tuned Topological Phase Transition in Ultra-Thin Na3Bi - Towards a Topological Transistor

The electric field induced quantum phase transition from topological to conventional insulator has been proposed as the basis of a topological field effect transistor [1-4]. In this scheme an electric field can switch 'on' the ballistic flow of charge and spin along dissipationless edges of the two-dimensional (2D) quantum spin Hall insulator [5-9], and when 'off' is a conventional insulator with no conductive channels. Such as topological transistor is promising for low-energy logic circuits [4], which would necessitate electric field-switched materials with conventional and topological bandgaps much greater than room temperature, significantly greater than proposed to date [6-8]. Topological Dirac semimetals(TDS) are promising systems in which to look for topological field-effect switching, as they lie at the boundary between conventional and topological phases [3,10-16]. Here we use scanning probe microscopy/spectroscopy (STM/STS) and angle-resolved photoelectron spectroscopy (ARPES) to show that mono- and bilayer films of TDS Na3Bi [3,17] are 2D topological insulators with bulk bandgaps >400 meV in the absence of electric field. Upon application of electric field by doping with potassium or by close approach of the STM tip, the bandgap can be completely closed then re-opened with conventional gap greater than 100 meV. The large bandgaps in both the conventional and quantum spin Hall phases, much greater than the thermal energy kT = 25 meV at room temperature, suggest that ultrathin Na3Bi is suitable for room temperature topological transistor operation.

cond-mat.mtrl-sci↗