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Jochen Mannhart

Publications and source records attributed to Jochen Mannhart.

At least 19 recordsLinked to original sources

Optical Signature of Moir\'e Superlattices Formed by Twisted SrTiO$_3$ Membranes

Moir\'e superlattices formed at the interfaces of mismatched lattices have attracted significant interest over the past decade due to their large tunability of band parameters and interactions among electrons, spins, and lattices. Superlattices made from twisted perovskite oxides may have strong structure and potential modulation, but evidence of such modulation over macroscopic areas, particularly at large twisting angles, has not been clearly demonstrated so far. Here, we fabricated millimeter-scale twisted oxide bilayers at $36^\circ$ angle, close to the simple coincidence site lattice condition $\Sigma5$, from freestanding SrTiO$_3$ membranes. We discovered new low-frequency vibrational modes whose Raman activity, according to molecular dynamics simulations, is greatly enhanced by an asymmetric, twisted interface between the SrO and TiO$_2$ layers. Such an interface is energetically favorable from first-principles calculations and is corroborated by the observation of strong second harmonic generation from the interface comparable to that from the SrTiO$_3$ surface throughout the bilayer region. The results are consistent with interlayer coupling enhanced by high-temperature annealing and confirmed by cross-sectional scanning transmission electron microscopy imaging. Our work sheds light on the structural behavior of twisted oxides and provides directions for tuning their phononic and nonlinear optical properties in future studies.

cond-mat.mtrl-sci

Materials Beyond Hamiltonian Limits -- Quantum Measurement as a Resource for Material Design

Recent studies have identified materials and devices whose behavior lies beyond the scope of conventional electronic-structure theory. Such theories are formulated entirely in terms of Hamiltonian evolution and therefore describe only unitary dynamics and thus only a restricted class of quantum systems. In contrast, electron systems that incorporate quantum measurement as an intrinsic dynamical element undergo Hamiltonian evolution interleaved with projection-induced state updates. This unitary-projective dynamics breaks constraints imposed by purely unitary evolution and permits stochastic population transfer between symmetry-related transport channels, thereby enabling fundamentally new material functionalities. This insight motivates the deliberate design of materials and devices that harness unitary-projective dynamics. This article explores the foundations of unitary-projective electron dynamics and charts the resulting landscape of quantum materials and their functionalities. Model calculations demonstrate passive mesoscopic structures with intrinsic nonreciprocal single-electron transmission, materials exhibiting a novel category of magnetism, and possible platforms for energy harvesting and conversion with efficiencies that exceed the standard Carnot limit.

cond-mat.stat-mech

Instability-driven mechanically locked states in functional oxide membranes

Mechanical instabilities in thin solids offer a powerful route to engineer nonlinear responses, yet their controlled use in functional crystalline oxides has remained largely unexplored. Notably, by changing the aspect ratio of solids, the energy landscape around equilibrium can be modified to induce non-linearities under lateral stresses through non-lateral deformations. These nonlinear systems can develop multiple local energy minima where the system can settle and switch between states through the application of a driving force. Crucially, recent advances in oxide thin film growth have enabled the fabrication of freestanding oxide membranes, paving a viable path for their use in bistable architecture, particularly at the nanoscale. Here, we demonstrate that freestanding oxide membranes, such as SrTiO3 (STO) and BaTiO3 (BTO), relax into well-defined metastable buckling states when transferred onto lithographically defined cavities. The membrane deformation is determined by the interplay between built-in residual strain, bending stiffness, and cavity geometry, resulting in reproducible bistable states with distinct strain distributions. Using a combination of atomic force microscopy, in-contact Kelvin probe measurements, and finite-element modelling, we reveal that these mechanically locked states directly shape the electromechanical potential landscape of ferroelectric BaTiO3. We further demonstrate reversible snapthrough transitions between mechanically degenerate states, establishing complex oxides as deterministic, geometry-tunable building blocks for nonlinear nanoelectromechanical architectures. Our results illustrate a general strategy for exploiting mechanical instabilities to encode and manipulate functional responses in ultrathin crystalline membranes.

cond-mat.mtrl-sci

Adsorption-controlled Growth of Homoepitaxial c-plane Sapphire Films

Sapphire is a technologically highly relevant material, but it poses many challenges to performing epitaxial thin-film deposition. We have identified and applied the conditions for adsorption-controlled homoepitaxial growth of c-plane sapphire. The films thus grown are atomically smooth, have a controlled termination, and are of outstanding crystallinity. Their chemical purity exceeds that of the substrates. The films exhibit exceptional optical properties such as a single-crystal-like bandgap and a low density of F+ centers.

cond-mat.mtrl-sci

alpha-Ta Films on c-plane Sapphire with Enhanced Microstructure

Superconducting films of alpha-Ta are promising candidates for the fabrication of advanced superconducting qubits. However, alpha-Ta films suffer from many growth-induced structural inadequacies that negatively affect their performance. We have therefore explored a new synthesis method for alpha-Ta films which allows the growth of these films with unprecedented quality. Using this method, high quality alpha-Ta films are deposited at a comparably high substrate temperature of 1150 C. They are single-phase alpha-Ta and have a single out-of-plane (110) orientation. They consist of grains above 2 um that have one of three possible in-plane orientations. As shown by scanning transmission electron microscopy and electron energy loss studies the substrate-film interfaces are sharp with no observable intermixing. The obtained insights into the epitaxial growth of body-centered-cubic films on quasi-hexagonal substrates lay the basis for harnessing the high structural coherence of such films in various applications.

cond-mat.supr-con

Vector-substrate-based Josephson junctions

We present a way to We present a way to fabricate bicrystal Josephson junctions of high-Tc cuprate superconductors that does not require bulk bicrystalline substrates. Based on vector substrate technology, this novel approach makes use of a few tens-of-nanometers-thick bicrystalline membranes transferred onto conventional substrates.We demonstrate 24° YBa2Cu3O7-x Josephson junctions fabricated on sapphire single crystals by utilizing 10-nm-thick bicrystalline membranes of SrTiO3. This technique allows one to manufacture bicrystalline Josephson junctions of high-Tc superconductors on a large variety of bulk substrate materials, providing novel degrees of freedom in designing the junctions and their electronic properties. It furthermore offers the capability to replace the fabrication of bulk bicrystalline substrates with thin-film growth methods

cond-mat.supr-con

Magnetotransport Properties of Epitaxial Films and Hall Bar Devices of the Correlated Layered Ruthenate Sr$_3$Ru$_2$O$_7$

For epitaxial Sr$_3$Ru$_2$O$_7$ films grown by pulsed laser deposition, we report a combined structural and magnetotransport study of thin films and Hall bar devices patterned side-by-side on the same film. Structural properties of these films are investigated using X-ray diffraction and high-resolution transmission electron microscopy, and confirm that these films are epitaxially oriented and nearly phase pure. For magnetic fields applied along the $c-$axis, a positive magnetoresistance of 10\% is measured for unpatterned Sr$_3$Ru$_2$O$_7$ films, whereas for patterned Hall bar devices of channel widths of $10$ and $5\, μ$m, magnetoresistance values of 40\% and 140\% are found, respectively. These films show switching behaviors from positive to negative magnetoresistance that are controlled by the direction of the applied magnetic field. The present results provide a promising route for achieving stable epitaxial synthesis of intermediate members of correlated layered strontium ruthenates, and for the exploration of device physics in thin films of these compounds.

physics.app-ph

Interface Design Beyond Epitaxy: Oxide Heterostructures Comprising Symmetry-forbidden Interfaces

Epitaxial growth of thin-film heterostructures is generally considered the most successful procedure to obtain interfaces of excellent structural and electronic quality between three-dimensional materials. However, these interfaces can only join material systems with crystal lattices of matching symmetries and lattice constants. We present a novel category of interfaces, the fabrication of which is membrane-based and does not require epitaxial growth. These interfaces therefore overcome limitations imposed by epitaxy. Leveraging the additional degrees of freedom gained, we demonstrate atomically clean interfaces between three-fold symmetric sapphire and four-fold symmetric SrTiO3. Atomic-resolution imaging reveals structurally well-defined interfaces with a novel moiré-type reconstruction.

cond-mat.mtrl-sci

Exact description of transport and non-reciprocity in monitored quantum devices

We study non-interacting fermionic systems undergoing continuous monitoring and driven by biased reservoirs. Averaging over the measurement outcomes, we derive exact formulas for the particle and heat flows in the system. We show that these currents feature competing elastic and inelastic components, which depend non-trivially on the monitoring strength $γ$. We highlight that monitor-induced inelastic processes lead to non-reciprocal currents, allowing to extract work from measurements without active feedback control. We illustrate our formalism with two distinct monitoring schemes providing measurement-induced power or cooling.~Optimal performances are found for values of the monitoring strength $γ$ which are hard to address with perturbative approaches.

quant-ph

Employing High-temperature-grown SrZrO$_3$ Buffer to Enhance the Electron Mobility in La:BaSnO$_3$-based Heterostructures

We report a synthetic route to achieve high electron mobility at room temperature in epitaxial La:BaSnO$_3$/SrZrO$_3$ heterostructures prepared on several oxide substrates. Room-temperature mobilities of 157, 145, and 143 cm$^2$V$^{-1}$s$^{-1}$ are achieved for heterostructures grown on DyScO$_3$ (110), MgO (001), and TbScO$_3$ (110) crystalline substrates, respectively. This is realized by first employing pulsed laser deposition to grow at very high temperature the SrZrO$_3$ buffer layer to reduce dislocation density in the active layer, then followed by the epitaxial growth of an overlaying La:BaSnO$_3$ active layer by molecular-beam epitaxy. Structural properties of these heterostructures are investigated, and the extracted upper limit of threading dislocations is well below $1.0\times 10^{10}$cm$^{-2}$ for buffered films on DyScO$_3$, MgO, and TbScO$_3$ substrates. The present results provide a promising route towards achieving high mobility in buffered La:BaSnO$_3$ films prepared on most, if not all, oxide substrates with large compressive or tensile lattice mismatches to the film.

cond-mat.mtrl-sci

Combined Spectroscopy and Electrical Characterization of La:BaSnO$_\text{3}$ Thin Films and Heterostructures

For La-doped BaSnO$_\text{3}$ thin films grown by pulsed laser deposition, we combine chemical surface characterization and electronic transport studies to probe the evolution of electronic states in the band structure for different La-doping content. Systematic analyses of spectroscopic data based on fitting the core electron line shapes help to unravel the composition of the surface as well as the dynamics associated with increasing doping. This dynamics is observed with a more pronounced signature in the Sn 3d core level, which exhibits an increasing asymmetry to the high binding energy side of the peak with increasing electron density. The present results expand the current understanding of the interplay between the doping concentration, electronic band structure and transport properties of epitaxial La:BaSnO$_\text{3}$ films.

cond-mat.mtrl-sci

Tunable Magnetic Anisotropy in Patterned SrRuO3 Quantum Structures: Competition between Lattice Anisotropy and Oxygen Octahedral Rotation

Artificial perovskite-oxide nanostructures possess intriguing magnetic properties due to their tailorable electron-electron interactions, which are extremely sensitive to the oxygen coordination environment. To date, perovskite-oxide nanodots with sizes below 50 nm have rarely been reported. Furthermore, the oxygen octahedral distortion and its relation to magnetic properties in perovskite oxide nanodots remain unexplored yet. Here, we have studied the magnetic anisotropy in patterned SrRuO3 (SRO) nanodots as small as 30 nm while performing atomic-resolution electron microscopy and spectroscopy to directly visualize the constituent elements, in particular oxygen ions. We observe that the magnetic anisotropy and RuO6 octahedra distortion in SRO nanodots are both nanodots' size-dependent but remain unchanged in the first 3-unit-cell interfacial SRO monolayers regardless of the dots' size. Combined with the first principle calculations, we unravel a unique structural mechanism behind the nanodots' size-dependent magnetic anisotropy in SRO nanodots, sugguesting that the competition between lattice anisotropy and oxygen octahedral rotation mediates anisotropic exchange interactions in SRO nanodots. These findings demonstrate a new avenue towards tuning magnetic properties of correlated perovskite oxides and imply that patterned nanodots could be a promising playground for engineering emergent functional behaviors.

cond-mat.mtrl-sci

An optimized TEM specimen preparation method of quantum nanostructures

Electron transparent TEM lamella with unaltered microstructure and chemistry is the prerequisite for successful TEM explorations. Currently, TEM specimen preparation of quantum nanostructures, such as quantum dots (QDs), remains a challenge. In this work, we optimize the sample-preparation routine for achieving high-quality TEM specimens consisting of SrRuO3 (SRO) QDs grown on SrTiO3 (STO) substrates. We demonstrate that a combination of ion-beam-milling techniques can produce higher-quality specimens of quantum nanostructures compared to TEM specimens prepared by a combination of tripod polishing followed by Ar+ ion milling. In the proposed method, simultaneous imaging in a focused ion-beam device enables accurate positioning of the QD regions and assures the presence of dots in the thin lamella by cutting the sample inclined by 5° relative to the dots array. Furthermore, the preparation of TEM lamellae with several large electron-transparent regions that are separated by thicker walls effectively reduces the bending of the specimen and offers broad thin areas. The final use of a NanoMill efficiently removes the amorphous layer without introducing any additional damage.

cond-mat.mes-hall

Thermal laser evaporation of elements from across the periodic table

We propose and demonstrate that thermal laser evaporation can be applied to all solid, non-radioactive elements in the periodic table. By depositing thin films, we achieve growth rates exceeding 1 angstrom/s with output laser powers less than 500 W, using identical beam parameters for many different elements. The source temperature is found to vary linearly with laser power within the examined power range. High growth rates are possible using free-standing sources for most of the elements tested, eliminating the need for crucibles.

cond-mat.mtrl-sci

Inelastic Electron Tunneling Spectroscopy at High-Temperatures

Ion conducting materials are critical components of batteries, fuel cells, and devices such as memristive switches. Analytical tools are therefore sought that allow the behavior of ions in solids to be monitored and analyzed with high spatial resolution and in real time. In principle, inelastic tunneling spectroscopy offers these capabilities. However, as its spectral resolution is limited by thermal softening of the Fermi-Dirac distribution, tunneling spectroscopy is usually constrained to cryogenic temperatures. This constraint would seem to render tunneling spectroscopy useless for studying ions in motion. We report here the first inelastic tunneling spectroscopy studies above room temperature. For these measurements, we have developed high-temperature-stable tunnel junctions that incorporate within the tunnel barrier ultrathin layers for efficient proton conduction. By analyzing the vibrational modes of O-H bonds in BaZrO3-based heterostructures, we demonstrate the detection of protons with a spectral resolution of 20 meV at 400 K (FWHM). Overturning the hitherto existing prediction for the spectral resolution limit of 186 meV (5.4 kBT at 400 K), this resolution enables high-temperature tunneling spectroscopy of ion conductors. With these advances, inelastic tunneling spectroscopy constitutes a novel, valuable analytical tool for solid-state ionics.

cond-mat.mtrl-sci

Fermi's golden rule and the second law of thermodynamics

We present a Gedankenexperiment that leads to a violation of detailed balance if quantum mechanical transition probabilities are treated in the usual way by applying Fermi's "golden rule". This Gedankenexperiment introduces a collection of two-level systems that absorb and emit radiation randomly through non-reciprocal coupling to a waveguide, as realized in specific chiral quantum optical systems. The non-reciprocal coupling is modeled by a hermitean Hamiltonian and is compatible with the time-reversal invariance of unitary quantum dynamics. Surprisingly, the combination of non-reciprocity with probabilistic radiation processes entails negative entropy production. Although the considered system appears to fulfill all conditions for Markovian stochastic dynamics, such a dynamics violates the Clausius inequality, a formulation of the second law of thermodynamics. Several implications concerning the interpretation of the quantum mechanical formalism are discussed.

quant-ph

Beyond Superconductivity

We present a novel device concept that utilizes the fascinating transition regime between quantum mechanics and classical physics. The devices operate by using a small number of individual quantum mechanical collapse events to interrupt the unitary evolution of quantum states represented by wave packets. Exceeding the constraints of the unitary evolution of quantum mechanics given by the Schroedinger equation and of classical Hamiltonian physics, these devices display a surprising behavior.

cond-mat.mes-hall

Bio-inspired Synthetic Ivory as a Sustainable Material for Piano Keys

Natural ivory is no longer readily or legally available, as it is obtained primarily from elephant tusks, which now enjoy international protection. Ivory, however, is the best material known for piano keys. We present a hydroxylapatite-gelatin biocomposite that is chemically identical to natural ivory but with functional properties optimized to replace it. As this biocomposite is fabricated from abundant materials in an environmentally friendly process and is furthermore biodegradable, it is a sustainable solution for piano keys with the ideal functional properties of natural ivory.

physics.app-ph