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Mykhailo Shestopalov

Publications and source records attributed to Mykhailo Shestopalov.

5 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

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

Investigation of internal electric fields in graphene/6H-SiC under illumination by Pockels effect

In this paper, we introduce a method for mapping profiles of internal electric fields in birefringent crystals based on the electro-optic Pockels effect and measuring phase differences of low-intensity polarized light. In the case of the studied 6H-SiC crystal with graphene electrodes, the experiment is significantly affected by birefringence at zero bias voltage applied to the crystal and a strong thermo-optical effect. We dealt with these phenomena by adding a Soleil-Babinet compensator and using considerations based on measurements of crystal heating under laser illumination. The method can be generalized and adapted to any Pockels crystal that can withstand sufficiently high voltages. We demonstrate the significant formation of space charge in semi-insulating 6H-SiC under illumination by above-bandgap light.

physics.optics

Plasmon-plasmon interaction and the role of buffer in epitaxial graphene micro-flakes

We investigate the origin of the translational symmetry breaking in epitaxially grown single-layer graphene. Despite the surface morphology of homogeneous graphene films influenced by the presence of mutually parallel SiC surface terraces, the far-infrared magneto-plasmon absorption is almost independent of the angle between the probing light polarization and the orientation of terraces. Based on a detailed analysis of the plasmon absorption lineshape and its behavior in the magnetic field, supported by confocal Raman mapping and atomic force microscopy, we explain this discrepancy by spontaneously formed graphene micro flakes. We further support our conclusions using data collected on artificially created graphene nanoribbons: we recognize similar plasmon origin in artificial ribbons and naturally formed grains. An unexpectedly large plasmon resonance redshift was observed in nanoribbons. In a hydrogen-intercalated sample (which does not contain the buffer), this redshift is quantitatively taken into account by a plasmon-plasmon interaction. In non-intercalated samples featuring a buffer layer, this redshift is due to an interplay between the plasmon-plasmon coupling and Coulomb screening by the buffer-induced interface states. This model determines the density of interface states in good agreement with experimentally reported values.

cond-mat.mes-hall

Spectral Current Density and Responsivity Scaling for Fourier Transform Photocurrent Spectroscopy

We propose and experimentally verify two methods to scale arbitrary units to photocurrent spectral density (A/eV) in Fourier Transform Photocurrent (FTPC) spectroscopy. We also propose the FTPC scaling to responsivity (A/W), provided a narrow-band optical power measurement is available. The constant background of the interferogram provides a precise determination of the photocurrent spectral density. The second method relies on the scaled amplitude of the interferogram. Although the latter method leads to more significant errors, it still provides good order of magnitude estimates of the total photocurrent. We demonstrate the technique on a calibrated InGaAs diode and weak responsivity SiC interdigital sensors. We identify a series of impurity-band and interband transitions in the SiC sensors.

cond-mat.mtrl-sci