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Pavel Procházka

Publications and source records attributed to Pavel Procházka.

13 recordsLinked to original sources

Beliefs Beyond Posteriors: The Predictive Cost of ELBO Binding

Posterior-seeking training need not produce the best predictive distribution in its family under model misspecification. For a last-layer weight belief, we locate the restriction responsible for this gap and quantify its cost. At the last layer the negative ELBO decomposes exactly into the belief's predictive log scores, the prior KL, and a binding: a sum of per-observation Jensen gaps that constrains predictive dispersion through posterior covariance. Removing the binding gives the established KL-regularised form of predictive-score training; a parameterisation-dependent factor-normaliser form performs similarly at the last layer. At fixed predictive mean, the leading restricted direction is the variance at each input, and its local value is the classical variance-component score evaluated at the plug-in predictor. This yields both a diagnostic and a price: in the flat-leverage limit, the Gaussian cost is the Jensen gap of a representable residual-variance profile, whereas a likelihood without a dispersion parameter pays the full expressible improvement over the plug-in. Controlled experiments find typically tenths of a nat for Gaussian regression but units to tens of nats for overdispersed Poisson counts. In an exploratory, prospectively specified validation on 28 count sets, 27 unused elsewhere, a screen computed from the point-prediction head alone agreed with the measured outcome on 24 of 25 decided sets (an always-open rule: 18), and its price proxy, once fixed, was within a factor of three of the predictive-score gain of the fitted free profile on all 10 open sets tested afterwards. Score training changes the inferential target: it yields classical per-input overdispersed heads whose covariance represents residual dispersion, not posterior or epistemic uncertainty.

cs.LG↗

Fe-DCA Metal-Organic Frameworks on the Bi2Se3(0001) Topological Insulator Surface

The formation of two-dimensional metal-organic frameworks (MOFs) on an inert surface of a topological insulator (TI) is a pathway to engineer quantum materials with exotic properties. MOFs featuring ferromagnetically coupled metal atoms are theoretically predicted to induce an exchange gap in the TI surface band structure, potentially leading to a quantum anomalous Hall effect. However, achieving ordered MOFs on TI surfaces remains challenging due to the limited knowledge of self-assembly on these substrates. In this paper, we demonstrate self-assembly of Fe atoms and dicyanoanthracene (DCA) molecules into 2D MOFs on the Bi2Se3(0001) surface at room temperature, investigated via a combination of low-energy electron microscopy and diffraction (LEEM/LEED), scanning tunneling microscopy (STM), and ab initio calculations based on density functional theory (DFT). Two competing Fe-DCA phases form. The first phase corresponds to a close-packed Fe1DCA3 structure. In contrast, the second phase exhibits a larger unit cell with no match to either known or DFT-calculated systems, indicating a more complex bonding environment. These findings advance the understanding of the growth of MOFs on a strong topological insulator surface and provide insights for designing MOFs/TI interfaces with tailored electronic and magnetic properties.

cond-mat.mtrl-sci↗

Interfacial Coupling Controls Molecular Epitaxy of HMTP on Graphene/SiC

Epitaxial growth critically influences structural and electronic properties of organic semiconductors. Graphene serves as a prominent van der Waals template for molecular self-assembly; however, graphene on SiC is intrinsically heterogeneous, with decoupled monolayer graphene coexisting with residuals of a covalently bound buffer layer, which may affect molecular ordering. Here, we track the ordering of the molecular donor, 2,3,6,7,10,11-hexamethoxytriphenylene (HMTP), from the first layer to thin films, combining low-energy electron microscopy and diffraction with X-ray diffraction. HMTP forms highly ordered epitaxial layers on single-layer graphene, whereas growth on the buffer layer initiates as amorphous and evolves into polycrystalline films with weak orientation with respect to the substrate. Crucially, hydrogen intercalation decouples the buffer layer, converting it into quasi-freestanding monolayer graphene and restoring epitaxial growth. These findings demonstrate that interfacial coupling governs molecular epitaxy on graphene/SiC, and interface engineering via hydrogen intercalation provides a scalable route to control organic thin-film crystallinity on graphene.

cond-mat.mtrl-sci↗

Low-energy electron microscopy as a tool for analysis of self-assembled molecular layers on surfaces

Low-energy electron microscopy (LEEM) is a surface science method that works primarily in the UHV environment. It provides information complementary to the other established techniques: it extends the limited view of scanning probe microscopies from nanometers to micrometers and measurement time down to tens of milliseconds, enabling to visualize the changes during sample treatment, e.g., annealing, deposition, and gas or light exposure. From the point of structural analysis, it allows the measurement of diffraction patterns from an area of diameter below 200 nm and imaging of phase distribution on the surfaces either through dark-filed imaging or LEEM-I(V) fingerprinting. The advanced modes provide local angle-resolved photoelectron spectra and surface potential distribution. In this review, we aim to describe the utilization of LEEM to study self-assembled molecular structures on solid surfaces. We present the LEEM instrumentation and analysis of measured data in a tutorial way to provide the necessary background knowledge to enter the field. In the second part, we summarize the knowledge obtained by LEEM for several selected systems, which points to the strength of LEEM in understanding the self-assembled molecular systems and its synergy with other surface science techniques.

cond-mat.mes-hall↗

Convolutional Signal Propagation: A Simple Scalable Algorithm for Hypergraphs

Last decade has seen the emergence of numerous methods for learning on graphs, particularly Graph Neural Networks (GNNs). These methods, however, are often not directly applicable to more complex structures like bipartite graphs (equivalent to hypergraphs), which represent interactions among two entity types (e.g. a user liking a movie). This paper proposes Convolutional Signal Propagation (CSP), a non-parametric simple and scalable method that natively operates on bipartite graphs (hypergraphs) and can be implemented with just a few lines of code. After defining CSP, we demonstrate its relationship with well-established methods like label propagation, Naive Bayes, and Hypergraph Convolutional Networks. We evaluate CSP against several reference methods on real-world datasets from multiple domains, focusing on retrieval and classification tasks. Our results show that CSP offers competitive performance while maintaining low computational complexity, making it an ideal first choice as a baseline for hypergraph node classification and retrieval. Moreover, despite operating on hypergraphs, CSP achieves good results in tasks typically not associated with hypergraphs, such as natural language processing.

cs.LG↗

Direct observation of structural phase transformations during continuous phosphorus deposition on Cu(111)

Blue phosphorene -- two-dimensional, hexagonal-structured, semiconducting phosphorus -- has gained attention as it is considered easier to synthesize on metal surfaces than its allotrope, black phosphorene. Recent studies report different structures of phosphorene, for example, on Cu(111), but the underlying mechanisms of their formation are not known. Here, using a combination of in situ ultrahigh vacuum low-energy electron microscopy and in vacuo scanning tunneling microscopy, we determine the time-evolution of the surface structure and morphology during the deposition of phosphorus on single-crystalline Cu(111). We find that during early stages of deposition, phosphorus intermixes with Cu, resulting in copper phosphide structures. With increasing surface concentration of phosphorus, the phosphide phase disappears and a blue phosphorene layer forms, followed by self-assembly of highly ordered phosphorus clusters that eventually grow into multilayer islands. We attribute the unexpected transformation of stable phosphide to a phosphorene layer, and the previously unreported multilayer growth, to the presence of a large concentration of P2 dimers on the surface. Our results constitute direct evidence for a new growth mode leading to a phosphorene layer via an intermediary phase, which could underpin the growth of other 2D materials on strongly interacting substrates.

cond-mat.mtrl-sci↗

Robust Dipolar Layers between Organic Semiconductors and Silver for Energy-Level Alignment

The interface between a metal electrode and an organic semiconductor (OS) layer has a defining role in the properties of the resulting device. To obtain a desired performance, interlayers are introduced to modify the adhesion and growth of OS and enhance the efficiency of charge transport through the interface. However, the employed interlayers face common challenges, including a lack of electric dipoles to tune the mutual position of energy levels, being too thick for efficient electronic transport, or being prone to intermixing with subsequently deposited OS layers. Here, we show that monolayers of 1,3,5-tris(4 carboxyphenyl)benzene (BTB) with fully deprotonated carboxyl groups on silver substrates form a compact layer resistant to intermixing while mediating energy level alignment and showing a large insensitivity to substrate termination. Employing a combination of surface-sensitive techniques, i.e., low-energy electron microscopy and diffraction, X-ray photoelectron spectroscopy, and scanning tunneling microscopy, we have comprehensively characterized the compact layer and proven its robustness against mixing with the subsequently deposited organic semiconductor layer. DFT calculations show that the robustness arises from a strong interaction of carboxylate groups with the Ag surface, and thus, the BTB in the first layer is energetically favored. Synchrotron radiation photoelectron spectroscopy shows that this layer displays considerable electrical dipoles that can be utilized for work function engineering and electronic alignment of molecular frontier orbitals with respect to the substrate Fermi level. Our work thus provides a widely applicable molecular interlayer and general insights necessary for engineering of charge injection layers for efficient organic electronics.

cond-mat.mtrl-sci↗

Tunable Energy Level Alignment in the Multilayers of Carboxylic Acids on Silver

The precise energy level alignment between a metal electrode and an organic semiconductor is required to reduce contact resistance and enhance the efficiency of organic-semiconductor-based devices. One of the ways is to include interlayers that mediate the energy level alignment, i.e., charge injection layers (CILs). Here we introduce the monolayer thick CILs based on the aromatic carboxylic acids that can induce the energy level shift in the subsequent layers by up to 0.8 eV. By gradual chemical transformation of the as-deposited molecules, we achieve a highly tunable energy level shift in the range of 0.5 eV. We reveal that the position of both the work function and energy-level position in the CIL increases linearly with the density of induced dipoles. The energy level position of subsequent layers changes in the same way as the CIL. Our results thus connect the energy alignment quantities, i.e., energy level positions of both CIL and subsequent layers and sample work function. The high tunability would allow precise tuning of the active layers deposited on the CIL, which marks the path towards efficient charge injection layers on metal electrodes.

cond-mat.mtrl-sci↗

The Role of Phase Stabilization and Surface Orientation in 4,4'-Biphenyl-Dicarboxylic Acid Self-Assembly and Transformation on Silver Substrates

Molecular functionalization of nanoparticles and metallic substrates can be used to tune their properties for specific applications. However, polycrystalline substrates and nanoparticles exhibit surface planes with distinct crystallographic orientations. Therefore, the development of reliable strategies for molecular functionalization requires knowledge of the role of the surface plane orientation in the growth kinetics, structure, and properties of the molecular layer. Here, we apply a multiscale analysis to investigate the self-assembly of 4,4'-biphenyl-dicarboxylic acid (BDA) on Ag(111) and critically discuss the difference to Ag(100). Whereas the structural motifs for intact and fully deprotonated BDA are similar on both surfaces, the intermediate phases comprising partially deprotonated BDA differ in the structure and chemical composition. A real-time view of the phase transformations enables us to present a generalized picture of the phase transformations between the self-assembled molecular phases on the surfaces and underline important features such as the phase stabilization of the chemical composition and the mechanism of the related burst transformation. The influence of the substrate orientation on the structure of molecular layers and phase transformations provides the necessary background for developing functionalization strategies of the substrates displaying multiple surface planes and kinetic models for the growth near thermodynamic equilibrium.

cond-mat.mtrl-sci↗

Secondary frequency control stabilizing voltage dynamics

The ongoing energy transition challenges the stability of the electrical power system. Stable operation of the electrical power grid requires both the voltage (amplitude) and the frequency to stay within operational bounds. While much research has focused on frequency dynamics and stability, the voltage dynamics has been neglected. Here, we study frequency and voltage stability in the case of simple networks via linear stability and bulk analysis. In particular, our linear stability analysis of the network shows that the frequency secondary control guarantees the stability of a particular electric network. Even more interesting, while we only consider secondary frequency control, we observe a stabilizing effect on the voltage dynamics, especially in our numerical bulk analysis.

eess.SY↗

Single-layer graphene on epitaxial FeRh thin films

Graphene is a 2D material that displays excellent electronic transport properties with prospective applications in many fields. Inducing and controlling magnetism in the graphene layer, for instance by proximity of magnetic materials, may enable its utilization in spintronic devices. This paper presents fabrication and detailed characterization of single-layer graphene formed on the surface of epitaxial FeRh thin films. The magnetic state of the FeRh surface can be controlled by temperature, magnetic field or strain due to interconnected order parameters. Characterization of graphene layers by X-ray Photoemission and X-ray Absorption Spectroscopy, Low-Energy Ion Scattering, Scanning Tunneling Microscopy, and Low-Energy Electron Microscopy shows that graphene is single-layer, polycrystalline and covers more than 97% of the substrate. Graphene displays several preferential orientations on the FeRh(001) surface with unit vectors of graphene rotated by 30°, 15°, 11°, and 19° with respect to FeRh substrate unit vectors. In addition, the graphene layer is capable to protect the films from oxidation when exposed to air for several months. Therefore, it can be also used as a protective layer during fabrication of magnetic elements or as an atomically thin spacer, which enables incorporation of switchable magnetic layers within stacks of 2D materials in advanced devices.

cond-mat.mtrl-sci↗

Step-edge assisted large scale FeSe monolayer growth on epitaxial Bi2Se3 thin films

The interest in Fe-chalcogenide unconventional superconductors is intense after the critical temperature of FeSe was reported enhanced by more than one order of magnitude in the monolayer limit at the interface to an insulating oxide substrate. In heterostructures comprising interfaces of FeSe with topological insulators, additional interesting physical phenomena is predicted to arise e.g. in form of {\it topological superconductivity}. So far superconductive properties of Fe-chalcogenide monolayers were mostly studied by local scanning tunneling spectroscopy experiments, which can detect pseudo-gaps in the density of states as an indicator for Cooper pairing. Direct macroscopic transport properties which can prove or falsify a superconducting phase were rarely reported due to the difficulty to grow films with homogeneous material properties. Here we report on a promising growth method to fabricate continuous carpets of monolayer thick FeSe on molecular beam epitaxy grown Bi$_2$Se$_3$ topological insulator thin films. In contrast to previous works using atomically flat cleaved bulk Bi$_2$Se$_3$ crystal surfaces we observe a strong influence of the high step-edge density (terrace width about 10~nm) on MBE-grown Bi$_2$Se$_3$ substrates, which significantly promotes the growth of coalescing FeSe domains with small tetragonal crystal distortion without compromising the underlying Bi$_2$Se$_3$ crystal structure.

cond-mat.mtrl-sci↗

Identification of two-dimensional $FeO_2$ termination of hematite $α-Fe_2O_3(0001)$ surface

Iron oxides are among the most abundant compounds on Earth and have consequently been studied and used extensively in industrial processes. Despite these efforts, concrete understanding of some of their surface phase structures has remained elusive, in particular the oxidized $α-Fe_2O_3(0001)$ hematite surface. We detail an optimized recipe to produce this phase over the entire hematite surface and study the geometrical parameters and composition of its complex structure by means of atomically resolved microscopy, electron diffraction and surface-sensitive spectroscopies. We conclude that the oxidized $α-Fe_2O_3(0001)$ surface is terminated by a two-dimensional iron oxide with structure, lattice parameters, and orientation different from the bulk substrate. Using total-energy density functional theory for simulation of a large-scale atomic model, we identify the structure of the surface layer as antiferromagnetic, conductive $1T-FeO_2$ attached on half-metal terminated bulk. The model succeeds in reproducing the characteristic modulations observed in the atomically resolved images and electron diffraction patterns.

cond-mat.mtrl-sci↗