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Kim Kisslinger

Publications and source records attributed to Kim Kisslinger.

At least 19 recordsLinked to original sources

Surface Platinum Alloying for Passivation of Oxide Interfaces on Superconducting Niobium Films

Dielectric loss arising from two-level systems (TLS) at surfaces and interfaces remains a primary limitation to coherence in superconducting transmon qubits. Niobium (Nb), a widely used material in superconducting quantum circuits, readily forms native oxides under ambient conditions, leading to lossy dielectric interfaces that degrade device performance. Here, a robust and scalable fabrication strategy is demonstrated for chemically stabilizing Nb surfaces and mitigating further oxidation, including protection of both surface and sidewall regions. High-purity Nb films were fabricated with bulk-like superconducting transition temperatures ($T_c = 9.30\pm0.10$) K. We demonstrate that a thin Pt encapsulation layer, deposited after native oxide formation, can be transformed via thermal annealing into a Nb-Pt alloy at the surface. Spectroscopic and microscopic analyses confirm the formation of a chemically stable metallic alloy layer and its ability to suppress further oxide growth. Ab initio simulations elucidate the atomic-scale rearrangement and electronic structure evolution associated with Pt incorporation on native niobium oxide, providing insight into the stabilization mechanism of the alloyed surface. This approach offers a materials pathway for engineering chemically robust Nb interfaces, including sidewalls, toward higher-coherence superconducting qubit architectures."

cond-mat.supr-con

Temperature-Dependent Dielectric Function of Tantalum Nitride Formed by Atomic Layer Deposition for Tunnel Barriers in Josephson Junctions

We report the dielectric functions of insulating tantalum nitride (TaN) films, deposited using atomic layer deposition (ALD) on 300 mm Si/SiO2 substrates, to demonstrate their suitability as tunnel barriers in tantalum-based Josephson junctions (JJ) for superconducting quantum circuits. The temperature-dependent ellipsometric angles were measured using ALD TaN films with nominal thicknesses of 13 nm and 25 nm at an incidence angle of 70 degrees, across photon energy ranges of 0.03 eV to 0.7 eV (80-300 K) and 0.5 eV to 6.5 eV (80-600 K). This data was used to develop a dispersion model for insulating ALD TaN films that incorporates a Tauc-Lorentz oscillator with a band gap of 1.5-1.8 eV to model the interband optical transitions. The extracted dielectric function of ALD TaN films shows an insulating behavior (mid-infrared transparency) at all temperatures and for both film thicknesses tested. ALD TaN does not exhibit infrared absorption due to free carriers, even at elevated temperatures, demonstrating its insulating nature, which is required for the tunnel barrier of the JJ in quantum applications. The results of transmission electron microscopy, including selected area electron diffraction, and X-ray diffraction are also discussed. Sputter depth-profile X-ray photoelectron spectroscopy (XPS) shows an N/Ta ratio of ~1.2 throughout the film. The lower band gap, low roughness, and thermal stability of ALD TaN compared to AlOx suggest the possibility of fabricating JJs with thicker barriers while achieving critical current densities required for qubits, better control of thickness and composition, reduced topography, and resistance to aging.

cond-mat.supr-con

Polymer-Iron Oxide Hybrid Films for Controlling Electrokinetic Properties

Electrokinetic phenomena at polymer-water interfaces are central to technologies for water purification, ion separations, and energy conversion, yet the ability to systematically control polymer surface charge and associated electrokinetic processes remains limited. Here, we demonstrate a simple liquid-phase infiltration (LPI) method to synthesize polymer-metal oxide hybrid films with controllable interfacial properties. Hydroxy-terminated poly(2-vinylpyridine) (P2VP-OH) brushes grafted to silicon substrates were infiltrated with iron nitrate from ethanolic solution, followed by low-temperature thermal treatment to convert the infiltrated precursor into iron oxide. Spectroscopic ellipsometry, X-ray photoelectron spectroscopy, and thermogravimetric analysis confirmed oxide incorporation and hybrid film formation without polymer degradation. Electrokinetic flow characterization reveals that the hybrid films acquire the electrokinetic properties of the infiltrated oxide, with concentration-dependent streaming potentials and surface conductivities closely matching those of pure iron oxide films. These results establish metal oxide infiltration as a scalable and low-cost strategy for controlling interfacial charge in polymer surfaces. The approach introduces new materials and design parameters for tailoring ion selectivity, transport, and energy conversion, with broad implications for the development of advanced membranes, electrokinetic harvesting devices, and polymer-supported oxide electrodes.

cond-mat.mtrl-sci

Hydrazine-Free Precursor for Solution-Processed All-Inorganic Se and Se1-xTex Photovoltaics

Selenium (Se) has reemerged as a promising absorber material for indoor and tandem photovoltaics (PVs), and its alloys with Te (Se1-xTex) offer a widely tunable bandgap. Solution processing of this materials system offers a route to low-cost fabrication. However, solution processing of Se has, thus far, only used hydrazine, which is an extremely hazardous solvent. In this work, we prepare and isolate propylammonium poly-Se and poly-Se-Te precursors from a safer thiol-amine solvent system. We formulate molecular inks by dissolving the precursor n,n-dimethylformamide (DMF) with a monoethanolamine (EA) additive and process high-quality Se and Se1-xTex films with bandgaps ranging from 1.20 eV to 1.86 eV. We fabricate PVs from these films using TiO2 and MoO3 charge transport layers (CTLs) to achieve power conversion efficiencies as high as 2.73% for Se and 2.33% for Se0.7Te0.3 under solar simulation. Se devices show excellent stability with no degradation after 1 month in air, enabled by the excellent stability of Se and the use of inorganic CTLs. This work represents an important step towards low-cost solution-phase processing of Se and Se1-xTex alloys for PVs and photodetectors with low toxicity and high bandgap tunability.

cond-mat.mtrl-sci

Observing Differential Spin Currents by Resonant Inelastic X-ray Scattering

Controlling spin currents, i.e., the flow of spin angular momentum, in small magnetic devices is the principal objective of spin electronics, a main contender for future energy efficient information technologies. Surprisingly, a pure spin current has never been measured directly since the associated electric stray fields and/or shifts in the non-equilibrium spin-dependent distribution functions are too small for conventional experimental detection methods optimized for charge transport. Here we report that resonant inelastic x-ray scattering (RIXS) can bridge this gap by measuring the spin current carried by magnons -- the quanta of the spin wave excitations of the magnetic order -- in the presence of temperature gradients across a magnetic insulator. This is possible due to the sensitivity of the momentum- and energy-resolved RIXS intensity to minute changes in the magnon distribution under non-equilibrium conditions. We use the Boltzmann equation in the relaxation time approximation to extract transport parameters, such as the magnon lifetime at finite momentum, essential for the realization of magnon spintronics.

cond-mat.mes-hall

Single crystalline orthorhombic GdAlGe as a rare earth magnetic Dirac nodal-line metal

Crystal engineering is a method for discovering new quantum materials and phases, which may be achieved by external pressure or strain. Chemical pressure is unique in that it generates internal pressure perpetually to the lattice. As an example, GdAlSi from the rare-earth ($R$) $R$Al$X$ ($X =$ Si or Ge) family of Weyl semimetals is considered. Replacing Si with the larger isovalent element Ge creates sufficiently large chemical pressure to induce a structural transition from the tetragonal structure of GdAlSi, compatible with a Weyl semimetallic state, to an orthorhombic phase in GdAlGe, resulting in an inversion-symmetry-protected nodal-line metal. We find that GdAlGe hosts an antiferromagnetic ground state with two successive orderings, at $T_\mathrm{N1}$ = 35 K and $T_\mathrm{N2}$ = 30 K. In-plane isothermal magnetization shows a magnetic field induced metamagnetic transition at 6.2 T for 2 K. Furthermore, electron-hole compensation gives rise to a large magnetoresistance of $\sim 100\%$ at 2 K and 14 T. Angle-resolved photoemission spectroscopy measurements and density functional theory calculations reveal a Dirac-like linear band dispersion over an exceptionally large energy range of $\sim$ 1.5 eV with a high Fermi velocity of $\sim 10^6$ m/s, a rare feature not observed in any magnetic topological materials.

cond-mat.mtrl-sci

Nucleation and Antiphase Twin Control in Bi$_2$Se$_3$ via Step-Terminated Al$_2$O$_3$ Substrates

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{\deg}) 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.

cond-mat.mtrl-sci

Single-layer magnet phase in intrinsic magnetic topological insulators, $[\mathrm{MnTe}][\mathrm{Bi}_{2}\mathrm{Te}_{3}]_{\mathrm{n}}$, far beyond the thermodynamic limit

The intrinsic magnetic topological insulator (IMTI) family $[\mathrm{MnTe}][\mathrm{Bi}_{2}\mathrm{Te}_{3}]_{\mathrm{n}}$ has demonstrated magneto-topological properties dependent on $n$, making it a promising platform for advanced electronics and spintronics. However, due to technical barriers in sample synthesis, their properties in the large $n$ limit remain unknown. To overcome this, we utilized the atomic layer-by-layer molecular beam epitaxy (ALL-MBE) technique and achieved IMTIs with $n$ as large as 15, far beyond the previously reported in bulk crystals or thin films. Then, we discover that the "single-layer magnet (SLM)" phase, primarily determined by intralayer ferromagnetic coupling, emerges for $n >$ $\sim 4$ and remains little affected up to $n = 15$. Nonetheless, still, non-zero, interlayer ferromagnetic coupling is necessary to stabilize the SLM phase, suggesting that the SLM phase eventually disappears in the $n\to\infty$ limit. This study uncovers the secrets of IMTIs beyond the thermodynamic limit and opens a door to diverse magneto-topological applications.

cond-mat.mes-hall

Universal Superconductivity in FeTe and All-Iron-Based Ferromagnetic Superconductor Heterostructures

Ferromagnetism (FM) and superconductivity (SC) are two of the most famous macroscopic quantum phenomena. However, nature normally does not allow SC and FM to coexist without significant degradation. Here, we introduce the first fully iron-based SC/FM heterostructures, composed of Fe(Te,Se) and Fe3GeTe2, and show that in this platform strong FM and high-temperature SC robustly coexist. We subsequently discover that chemical proximity effect from neighboring layers can universally drive the otherwise non-superconducting FeTe films into a SC state. This suggests that the ground state of FeTe is so close to the SC state that it could be driven in and out of the SC state with various other perturbations. Altogether, this shows that Fe-Te-based heterostructures provide a unique opportunity to manipulate magnetism, superconductivity and topological physics, paving the way toward new superconducting technologies.

cond-mat.supr-con

Revealing the Origin and Nature of the Buried Metal-Substrate Interface Layer in Ta/Sapphire Superconducting Films

Despite constituting a smaller fraction of the qubits electromagnetic mode, surfaces and interfaces can exert significant influence as sources of high-loss tangents, which brings forward the need to reveal properties of these extended defects and identify routes to their control. Here, we examine the structure and composition of the metal-substrate interfacial layer that exists in Ta/sapphire-based superconducting films. Synchrotron-based X-ray reflectivity measurements of Ta films, commonly used in these qubits, reveal an unexplored interface layer at the metal-substrate interface. Scanning transmission electron microscopy and core-level electron energy loss spectroscopy identified an approximately 0.65 \ \text{nm} \pm 0.05 \ \text{nm} thick intermixing layer at the metal-substrate interface containing Al, O, and Ta atoms. Density functional theory (DFT) modeling reveals that the structure and properties of the Ta/sapphire heterojunctions are determined by the oxygen content on the sapphire surface prior to Ta deposition, as discussed for the limiting cases of Ta films on the O-rich versus Al-rich Al2O3 (0001) surface. By using a multimodal approach, integrating various material characterization techniques and DFT modeling, we have gained deeper insights into the interface layer between the metal and substrate. This intermixing at the metal-substrate interface influences their thermodynamic stability and electronic behavior, which may affect qubit performance.

cond-mat.mtrl-sci

Eliminating Surface Oxides of Superconducting Circuits with Noble Metal Encapsulation

The lifetime of superconducting qubits is limited by dielectric loss, and a major source of dielectric loss is the native oxide present at the surface of the superconducting metal. Specifically, tantalum-based superconducting qubits have been demonstrated with record lifetimes, but a major source of loss is the presence of two-level systems (TLSs) in the surface tantalum oxide. Here, we demonstrate a strategy for avoiding oxide formation by encapsulating the tantalum with noble metals that do not form native oxide. By depositing a few nanometers of Au or AuPd alloy before breaking vacuum, we completely suppress tantalum oxide formation. Microwave loss measurements of superconducting resonators reveal that the noble metal is proximitized, with a superconducting gap over 80% of the bare tantalum at thicknesses where the oxide is fully suppressed. We find that losses in resonators fabricated by subtractive etching are dominated by oxides on the sidewalls, suggesting total surface encapsulation by additive fabrication as a promising strategy for eliminating surface oxide TLS loss in superconducting qubits.

cond-mat.supr-con

Evolution of the Fermi surface of 1T-VSe$_2$ across a structural phase transition

The electronic origin of the structural transition in 1T-VSe$_2$ is re-evaluated through an extensive angle-resolved photoemission spectroscopy experiment. The components of the band structure, missing in previous reports, are revealed. Earlier observations, shown to be temperature independent and therefore not correlated with the phase transition, are explained in terms of the increased complexity of the band structure close to the Fermi level. Only the overall size of the Fermi surface is found to be positively correlated with the phase transition at 110 K. These observations, quite distant from the charge density wave scenario commonly considered for 1T-VSe$_2$, bring fresh perspectives toward the correct description of structural transitions in dichalcogenides materials.

cond-mat.mtrl-sci

Atomic-Layer-Controlled Magnetic Orders in MnBi2Te4-Bi2Te3 Topological Heterostructures

The natural van der Waals superlattice MnBi2Te4-(Bi2Te3)m provides an optimal platform to combine topology and magnetism in one system with minimal structural disorder. Here, we show that this system can harbor both ferromagnetic (FM) and antiferromagnetic (AFM) orders and that these magnetic orders can be controlled in two different ways by either varying the Mn-Mn distance while keeping the Bi2Te3/MnBi2Te4 ratio constant or vice versa. We achieve this by creating atomically engineered sandwich structures composed of Bi2Te3 and MnBi2Te4 layers. We show that the AFM order is exclusively determined by the Mn-Mn distance whereas the FM order depends only on the overall Bi2Te3/MnBi2Te4 ratio regardless of the distance between the MnBi2Te4 layers. Our results shed light on the origins of the AFM and FM orders and provide insights into how to manipulate magnetic orders not only for the MnBi2Te4-Bi2Te3 system but also for other magneto-topological materials.

cond-mat.mtrl-sci

Buffer-layer-controlled Nickeline vs Zinc-Blende/Wurtzite-type MnTe growths on c-plane Al2O3 substrates

In the recent past, MnTe has proven to be a crucial component of the intrinsic magnetic topological insulator (IMTI) family [MnTe]m[Bi2Te3]n, which hosts a wide range of magneto-topological properties depending on the choice of m and n. However, bulk crystal growth allows only a few combinations of m and n for these IMTIs due to the strict limitations of the thermodynamic growth conditions. One way to overcome this challenge is to utilize atomic layer-by-layer molecular beam epitaxy (MBE) technique, which allows arbitrary sequences of [MnTe]m and [Bi2Te3]n to be formed beyond the thermodynamic limit. For such MBE growth, finding optimal growth templates and conditions for the parent building block, MnTe, is a key requirement. Here, we report that two different hexagonal phases of MnTe-nickeline (NC) and zinc-blende/wurtzite (ZB-WZ) structures, with distinct in-plane lattice constants of 4.20 +/- 0.04 A and 4.39 +/- 0.04 A, respectively-can be selectively grown on c-plane Al2O3 substrates using different buffer layers and growth temperatures. Moreover, we provide the first comparative studies of different MnTe phases using atomic-resolution scanning transmission electron microscopy and show that ZB and WZ-like stacking sequences can easily alternate between the two. Surprisingly, In2Se3 buffer layer, despite its lattice constant (4.02 A) being closer to that of the NC phase, fosters the ZB-WZ instead, whereas Bi2Te3, sharing the same lattice constant (4.39 A) with the ZB-WZ phase, fosters the NC phase. These discoveries suggest that lattice matching is not always the most critical factor determining the preferred phase during epitaxial growth. Overall, this will deepen our understanding of epitaxial growth modes for chalcogenide materials and accelerate progress toward new IMTI phases as well as other magneto-topological applications.

cond-mat.mtrl-sci

Ultrathin Magnesium-based Coating as an Efficient Oxygen Barrier for Superconducting Circuit Materials

Scaling up superconducting quantum circuits based on transmon qubits necessitates substantial enhancements in qubit coherence time. Among the materials considered for transmon qubits, tantalum (Ta) has emerged as a promising candidate, surpassing conventional counterparts in terms of coherence time. However, the presence of an amorphous surface Ta oxide layer introduces dielectric loss, ultimately placing a limit on the coherence time. In this study, we present a novel approach for suppressing the formation of tantalum oxide using an ultrathin magnesium (Mg) capping layer deposited on top of tantalum. Synchrotron-based X-ray photoelectron spectroscopy (XPS) studies demonstrate that oxide is confined to an extremely thin region directly beneath the Mg/Ta interface. Additionally, we demonstrate that the superconducting properties of thin Ta films are improved following the Mg capping, exhibiting sharper and higher-temperature transitions to superconductive and magnetically ordered states. Based on the experimental data and computational modeling, we establish an atomic-scale mechanistic understanding of the role of the capping layer in protecting Ta from oxidation. This work provides valuable insights into the formation mechanism and functionality of surface tantalum oxide, as well as a new materials design principle with the potential to reduce dielectric loss in superconducting quantum materials. Ultimately, our findings pave the way for the realization of large-scale, high-performance quantum computing systems.

cond-mat.mtrl-sci

Anisotropy of Antiferromagnetic Domains in a Spin-orbit Mott Insulator

The temperature-dependent behavior of magnetic domains plays an essential role in the magnetic properties of materials, leading to widespread applications. However, experimental methods to access the three-dimensional (3D) magnetic domain structures are very limited, especially for antiferromagnets. Over the past decades, the spin-orbit Mott insulator iridate $Sr_2IrO_4$ has attracted particular attention because of its interesting magnetic structure and analogy to superconducting cuprates. Here, we apply resonant x-ray magnetic Bragg coherent diffraction imaging to track the real-space 3D evolution of antiferromagnetic ordering inside a $Sr_2IrO_4$ single crystal as a function of temperature, finding that the antiferromagnetic domain shows anisotropic changes. The anisotropy of the domain shape reveals the underlying anisotropy of the antiferromagnetic coupling strength within $Sr_2IrO_4$. These results demonstrate the high potential significance of 3D domain imaging in magnetism research.

cond-mat.str-el

Surpassing millisecond coherence times in on-chip superconducting quantum memories by optimizing materials, processes, and circuit design

The performance of superconducting quantum circuits for quantum computing has advanced tremendously in recent decades; however, a comprehensive understanding of relaxation mechanisms does not yet exist. In this work, we utilize a multimode approach to characterizing energy losses in superconducting quantum circuits, with the goals of predicting device performance and improving coherence through materials, process, and circuit design optimization. Using this approach, we measure significant reductions in surface and bulk dielectric losses by employing a tantalum-based materials platform and annealed sapphire substrates. With this knowledge we predict and experimentally verify the relaxation times of aluminum- and tantalum-based transmon qubits. We additionally optimize device geometry to maximize coherence within a coaxial tunnel architecture, and realize on-chip quantum memories with single-photon Ramsey times of 2.0$-$2.7 ms, limited by their energy relaxation times of 1.0$-$1.4 ms. To our knowledge this is the highest coherence achieved in an on-chip quantum memory, and demonstrates an advancement towards a more modular and compact coaxial circuit architecture for bosonic qubits with reproducibly high coherence.

quant-ph

Microwave loss characterization using multi-mode superconducting resonators

Measuring the losses arising from different materials and interfaces is crucial to improving the coherence of superconducting quantum circuits. Although this has been of interest for a long time, current studies can either only provide bounds to those losses, or require several devices for a complete characterization. In this work, we introduce a method to measure the microwave losses of materials and interfaces with a single multi-mode superconducting resonator. We demonstrate a formalism for analyzing the loss sensitivity of multi-mode systems and discuss the design strategies of multi-mode resonators for material loss studies. We present two types of multi-mode superconducting resonators for the study of bulk superconductors: the forky whispering-gallery-mode resonator (FWGMR) and the ellipsoidal cavity. We use these resonators to measure the surface dielectric, conductor, and seam losses of high-purity (5N5) aluminum and aluminum alloy (6061), as well as how they are affected by chemical etching, diamond turning, and thin-film coating. We find that chemical etching and diamond turning reduce both the surface dielectric and conductive losses of high-purity aluminum, but provide no appreciable improvement to the seam. Coating the surfaces of diamond-turned aluminum alloys with e-beam evaporated or sputtered aluminum thin-films significantly reduces all three losses under study. In addition, we study the effect of chemical etching on the surface of high-purity aluminum using transmission electron microscopy (TEM) and find that the chemical etching process creates a thinner and more uniform oxide layer, consistent with the observed improvement in the surface dielectric loss.

quant-ph