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Veronika Stará

Publications and source records attributed to Veronika Stará.

7 recordsLinked to original sources

Unveiling Davydov-Split Excitons in a Template-Engineered Molecular-Graphene Heterostructure

The realization of high-fidelity organic-inorganic quantum emulators is frequently hindered by the interfacial imperfections introduced during device fabrication. Here, we demonstrate a robust nanofabrication protocol that restores the atomic-scale purity of epitaxial graphene on SiC to UHV-equivalent levels, as confirmed by Low-Energy Electron Diffraction, and Microscopy. This pristine interface enables the emergence of macroscopic excitonic coherence in epitaxial overlayers of 2,3,6,7,10,11-hexamethoxytriphenylene (HMTP), a model molecular system characterized by intense electron-phonon coupling. Through a combination of high-sensitivity Fourier Transform Photo-current Spectroscopy, photoluminescence, and dynamic Raman mapping, we resolve a complex vibronic manifold governed by Davydov splitting. We show that the $P6_3/m$ crystalline symmetry of the HMTP overlayer lifts the degeneracy of the HOMO-LUMO transition, creating discrete bright and dark excitonic branches. Using an analytical tight-binding model parameterized by ARPES-derived intermolecular coupling and Raman vibrational modes validated by molecular dynamics simulations, we quantify the polarization energy, the Huang-Rhys factor, and Herzberg-Teller corrections to the Franck-Condon model. Our results reveal that the dark-state branch dominates the radiative channel, following a polaron-mediated relaxation pathway consistent with Kasha's rule. By reconciling macroscopic device architecture with UHV-level surface science, this work establishes a scalable platform for the study of dark-exciton dynamics and the development of solid-state molecular quantum memories.

cond-mat.mes-hall↗

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↗

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↗

Long distance electron-electron scattering detected with point contacts

We measure electron transport through point contacts in an electron gas in AlGaAs/GaAs heterostructures and graphene for a range of temperatures, magnetic fields and electron densities. We find a magnetoconductance peak around B = 0. With increasing temperature, the width of the peak increases monotonically, while its amplitude first increases and then decreases. For GaAs point contacts the peak is particularly sharp at relatively low temperatures $T\approx$1.5 K: the curve rounds on a scale of few tens of $μ$T hinting at length scales of several millimeters for the corresponding scattering processes. We propose a model based on the transition between different transport regimes with increasing temperature: from ballistic transport to few electron-electron scatterings to hydrodynamic superballistic flow to hydrodynamic Poiseuille-like flow. The model is in qualitative and, in many cases, quantitative agreement with the experimental observations.

cond-mat.mes-hall↗

Counting Statistics of Single Electron Transport in Bilayer Graphene Quantum Dots

We measure telegraph noise of current fluctuations in an electrostatically defined quantum dot in bilayer graphene by real-time detection of single electron tunneling with a capacitively coupled neighboring quantum dot. Suppression of the second and third cumulant (related to shot noise) in a tunable graphene quantum dot is demonstrated experimentally. With this method we demonstrate the ability to measure very low current and noise levels. Furthermore, we use this method to investigate the first spin excited state, an essential prerequisite to measure spin relaxation.

cond-mat.mes-hall↗

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↗