arXiv subjects

Georgy Gordeev

Publications and source records attributed to Georgy Gordeev.

12 recordsLinked to original sources

arXiv2026

Cross-Dimensional Exciton Coupling in Quantum Dot - Carbon Nanotube Hybrid Thin Films

Dipole-dipole interactions provide a route to couple excitons across materials of different dimensionality. Here, we introduce hybrid films as a cross-dimensional excitonic platform and develop a theory of resonant Raman scattering in the presence of dipolar exciton coupling. Combining a coupled-oscillator model with perturbation theory, we show that coupling renormalizes the exciton-photon matrix elements and modifies nanotube Raman excitation profiles. We test this framework in vacuum-filtered films containing InP/ZnS quantum dots and mixed chirality metallic single-walled carbon nanotubes. The quantum-dot exciton remains near 1.83 eV, while chirality-dependent nanotube excitons span 1.7-1.93 eV, enabling systematic control of excitonic detuning. Relative to pristine nanotube films, the hybrids exhibit detuning-dependent redshifts and blueshifts, Raman intensity enhancement, reduced effective linewidths, and near-resonant two-branch profiles. The model yields an effective splitting of approximately 110 meV. Resonant Raman scattering thus provides component-selective access to dipolar interactions that are only weakly apparent in ensemble absorption spectra.

cond-mat.mes-hall↗

arXiv2026

Raman resonances mediated by excitonic polarons in BiVO$_4$

Excitonic polarons are quasiparticles formed by a Coulomb-bound electron-hole pair with strong coupling to lattice vibrations. Despite high fundamental interest in excitonic polarons, the experimental investigation of these particles remains challenging. In this work, we exploit the resonant Raman effect to probe the excitonic polarons in bismuth vanadate. We track enhancement of Raman modes as a function of excitation energy and reveal two optical resonances: one inside the band gap at 1.94 eV and another one near the optical absorption edge at 2.45 eV. The high-energy resonance originates from free excitons, which exhibit a characteristic 40 meV anisotropy between polarizations parallel and perpendicular to the c axis. Remarkably, the low-energy resonance shows no contrast in the optical absorption spectra. We attribute this resonance to an excitonic polaron formed through strong exciton-phonon coupling, making excitonic and excitonic polaron Raman resonances similar in strength. We probe the energy level of the excitonic polaron and compare its coupling strength to the different vibrational modes. Our results establish resonant Raman spectroscopy as a unique and powerful tool for probing quasiparticles of polaronic and excitonic nature in oxide materials.

cond-mat.mtrl-sci↗

arXiv2024

Dielectric Screening Inside Carbon Nanotubes

Dielectric screening plays a vital role for the physical properties in the nanoscale and also alters our ability to detect and characterize nanomaterials by optical techniques. We study the dielectric screening inside of carbon nanotubes and how it changes electromagnetic fields and many-body effects for encapsulated nanostructures. First, we show that the local electric field inside a nanotube is altered by one-dimensional screening with dramatic effects on the effective Raman scattering efficiency of the encapsulated species for metallic walls. The scattering intensity of the inner tube is two orders of magnitude weaker than for the tube in air, which is nicely reproduced by local field calculations. Secondly, we find that the optical transition energies of the inner nanotubes shift to lower energies compared to a single-walled carbon nanotubes of the same chirality. The shift is higher if the outer tube is metallic than when it is semiconducting. The magnitude of the shift suggests that the excitons of small diameter inner metallic tubes are thermally dissociated at room temperate if the outer tube is also metallic and in essence we observe band-to-band transitions.

cond-mat.mes-hall↗

arXiv2023

Excitonic Resonances in Coherent Anti-Stokes Raman Scattering from Single Wall Carbon Nanotubes

In this work we investigate the role of exciton resonances in coherent anti-Stokes Raman scattering (er-CARS) in single walled carbon nanotubes (SWCNTs). We drive the nanotube system in simultaneous phonon and excitonic resonances, where we observe a superior enhancement by orders of magnitude exceeding non-resonant cases. We investigated the resonant effects in five $(n,m)$ chiralities and find that the er-CARS intensity varies drastically between different nanotube species. The experimental results are compared with a perturbation theory model. Finally, we show that such giant resonant non-linear signals enable rapid mapping and local heating of individualized CNTs, suggesting easy tracking of CNTs for future nanotoxology studies and therapeutic application in biological tissues.

cond-mat.mes-hall↗

arXiv2023

Phonon-phonon coupling in bismuth vanadate over a large temperature range across the monoclinic phase

In this work we study phonon-phonon coupling in bismuth vanadate (BiVO4), known for its second-order transition involving a variety of coupling mechanisms. Using Raman spectroscopy as a probe, we identify two optical coupled phonon modes of the VO4 tetrahedron and study them by varying light polarization and temperature. The coupling manifests in non-Lorentzian line-shapes of Raman peaks and frequency shifts. We use theoretical framework of coupled damped harmonic oscillators to model the coupling and capture the phenomena in the temperature evolution of the coupling parameters. The coupling is negligible at temperatures below 100 K and later increases in magnitude with temperature until 400 K. The sign of the coupling parameter depends on the light polarization direction, causing either phonon attraction or repulsion. After 400 K the phonon-phonon coupling diminishes when approaching phase transition at which the phonon modes change their symmetry and the coupling is no longer allowed.

cond-mat.mtrl-sci↗

arXiv2022

Nanomechanical spectroscopy of 2D materials

We introduce a nanomechanical platform for fast and sensitive measurements of the spectrally-resolved optical dielectric function of 2D materials. At the heart of our approach is a suspended 2D material integrated into a nanomechanical resonator illuminated by a wavelength-tunable laser source. From the heating-related frequency shift of the resonator as well as its optical reflection measured as a function of photon energy, we obtain the real and imaginary parts of the dielectric function. Our measurements are unaffected by substrate-related screening and do not require any assumptions on the underling optical constants. This fast ($τ_{rise}$ $\sim$ 135 ns), sensitive (noise-equivalent power = 90 $\frac{pW}{\sqrt{Hz}}$ ), and broadband (1.2 $-$ 3.1 eV, extendable to UV-THz) method provides an attractive alternative to spectroscopic or ellipsometric characterisation techniques.

cond-mat.mes-hall↗

arXiv2022

Light Control over Chirality Selective Functionalization of Substrate Supported Carbon Nanotubes

Diazonium reactions with carbon nanotubes form optical $sp^3$ defects that can be used in optical and electrical circuits. We investigate a direct on-device reaction supported by confined laser irradiation and present a technique where an arbitrary carbon nanotube can be preferentially functionalized within a device by matching the light frequency with its transition energy. An exemplary reaction was carried out between (9,7) nanotube and 4-bromobenzenediazonium tetrafluoroborate. The substrate supported nanotubes of multiple semiconducting chiralities were locally exposed to laser light while monitoring the reaction kinetics in-situ via Raman spectroscopy. The chiral selectivity of the reaction was confirmed by resonant Raman spectroscopy, reporting a 10 meV $E_{22}$ transition energy red-shift only of the targeted species. We further demonstrated this method on a single tube (9,7) electroluminescent device and show a 25 meV red-shifted emission of the ground state $E_{11}$ compared to the emission from the pristine tubes.

cond-mat.mes-hall↗

arXiv2021

Moiré-induced Vibrational Coupling in Double Walled Carbon Nanotubes

Moiré patterns are additional, long-range periodicities in twisted crystalline bilayers. They are known to fundamentally change the electronic states of the layers, but similar effects on their mechanical and vibrational properties have not been discussed so far. Here we show that the Moiré potential shifts the radial breathing mode in double walled carbon nanotubes (DWCNTs). The change of frequency is expected to be proportional to the shift in optical transition energies, which are induced by the Moiré patterns. To verify our model we performed resonant Raman scattering on purified and sorted semiconducting DWCNTs. We find that the radial breathing mode shifts up to 14 cm$^{-1}$ higher in energy followed by optical transitions energies displacement up to 200 meV to lower energies, compared to the single-walled tubes. We show how to identify the strong coupling condition in DWCNTs from their phonon frequencies and construct a Kataura plot to aid their future experimental assignment.

cond-mat.mes-hall↗

arXiv2021

Synthesis of Multifunctional Charge Transfer Agents: Towards Single Walled Carbon Nanotubes with Defined Covalent Functionality and Preserved π System

The attachment of well-defined charge transfer agents to the surface of nanomaterials is an efficient strategy to control their charge density and also to tune their optical, electrical, and physicochemical properties. Particularly interesting are charge transfer agents that either donate or withdraw electrons depending on the arrangements of their building units and that promise a non-destructive attachment to delicate nanomaterials like sp$^2$ compounds. In this work, we rationally synthesize molecular moieties with versatile functionalities. A reactive anchor group allows to attach them to carbon nanotubes as defined charge transfer agents while preserving the tube $π$-conjugation. The charge transfer agents were synthesized through the stepwise nucleophilic substitution of either one (monosubstituted series) or two chlorine (disubstituted series) atoms of cyanuric chloride by aniline derivatives containing one, two or three methoxy groups in the para and meta positions. Variation in the number and position of methoxy as an electron transferring group help us to manipulate the electronic and optical properties of the molecular probes and their charge transfer to the SWNTs systematically. The correlation between the optical properties of these molecular probes and their functionality was investigated by experiments and quantum chemical calculations. While the optoelectronic properties of the conjugated charge transfer agents were dominated by the aniline segments, the triazine warrants the ability to nondestructively attach to the surface of SWNTs. This study is one step ahead towards the production of SWNTs with desired optical and electrical properties by covalent $π$-preserving functionalization.

cond-mat.mes-hall↗

arXiv2021

Raman Sideband Thermometry of Single Carbyne Chains

We demonstrate Raman sideband thermometry of single carbyne chains confined in double-walled carbon nanotubes. Our results show that carbyne's record-high Raman scattering cross section enables anti-Stokes Raman measurements at the single chain level. Using laser irradiation as a heating source, we exploit the temperature dependence of the anti-Stokes/Stokes ratio for local temperature sensing. Due to its molecular size and its large Raman cross section carbyne is an efficient probe for local temperature monitoring, with applications ranging from nanoelectronics to biology.

cond-mat.mes-hall↗

arXiv2020

Raman Scattering Cross Section of Confined Carbyne

We experimentally quantify the Raman scattering from individual carbyne chains confined in double-walled carbon nanotubes. We find that the resonant differential Raman cross section of confined carbyne is on the order of $10^{-22}$ cm$^{2}\,$sr$^{-1}$ per atom, making it the strongest Raman scatterer ever reported.

cond-mat.mes-hall↗

arXiv2019

Atomic-Resolution Visualization and Doping Effects of Complex Structures in Intercalated Bilayer Graphene

Molecules intercalating two-dimensional (2D) materials form complex structures that have been mostly characterized by spatially averaged techniques. Here we use aberration-corrected scanning transmission electron microscopy and density-functional-theory (DFT) calculations to study the atomic structure of bilayer graphene (BLG) and few-layer graphene (FLG) intercalated with FeCl$_3$. In BLG we discover two distinct intercalated structures that we identify as monolayer-FeCl$_3$ and monolayer-FeCl$_2$. The two structures are separated by atomically sharp boundaries and induce large but different free-carrier densities in the graphene layers, $7.1\times10^{13}$ cm$^{-2}$ and $7.1\times10^{13}$ cm$^{-2}$ respectively. In FLG, we observe multiple FeCl$_3$ layers stacked in a variety of possible configurations with respect to one another. Finally, we find that the microscope's electron beam can convert the FeCl$_3$ monolayer into FeOCl monolayers in a rectangular lattice. These results reveal the need for a combination of atomically-resolved microscopy, spectroscopy, and DFT calculations to identify intercalated structures and study their properties.

cond-mat.mtrl-sci↗