arXiv subjects

Georgy Ermolaev

Publications and source records attributed to Georgy Ermolaev.

14 recordsLinked to original sources

arXiv2026

Hyperbolic-enhanced Raman scattering in van der Waals MoOCl2: from Fano resonances to picomolar detection

Natural van der Waals (vdW) crystals with hyperbolic dispersion challenge artificial metamaterials but remain confined to the mid-infrared. The emergence of MoOCl2, a quasi-one-dimensional metal with in-plane hyperbolicity, overcomes this spectral limit, shifting the focus to the practical visible range. Here, using angle-resolved polarized Raman spectroscopy, we uncover pronounced polarization-dependent Fano lineshapes that reveal coupling between phonons and the anisotropic metallic continuum, together with strong wavelength-dependent reshaping of the Raman polarization patterns governed by the anisotropic optical response of MoOCl2. Harnessing this optical anisotropy, we demonstrate "Hyperbolic-Enhanced Raman" (HypER) scattering, where MoOCl2 provides polarization-tunable analytical enhancement factors exceeding 10^7 and picomolar-level detection of Rhodamine 6G down to 100 pM, without deliberate surface nanostructuring. These results establish air-stable MoOCl2 as a simple, wafer-compatible platform for visible-range hyperbolic nanophotonics and lithography-free sensing.

physics.optics↗

arXiv2026

Deep-Subwavelength and Broadband Quarter-Wave Retardation in Ultrathin Hyperbolic MoOCl2

The miniaturization of polarization-controlling optical components is one of the central pursuits in nanophotonics. While traditional anisotropic materials require large propagation lengths to achieve the desired phase shifts, metasurfaces mitigate this size constraint but often introduce narrow operational bandwidths and high fabrication complexities. To bridge this gap, we introduce MoOCl2 as a promising material for ultracompact and broadband phase retardation. Building on its giant optical anisotropy, we experimentally demonstrate MoOCl2 quarter-wave plates with thicknesses of 77 nm and 98 nm. These flakes exhibit achromatic quarter-wave retardation across broad visible (445 - 525 nm) and near-infrared (730 - 945 nm) spectral windows, surpassing the fundamental thickness and bandwidth limitations of both conventional optical materials and artificial nanostructures. Moreover, MoOCl2 waveplates demonstrate up to lambda/4500 retardance tolerance at central wavelengths. As a result, this study establishes MoOCl2 as a building block for ultracompact polarization optics.

physics.optics↗

arXiv2025

Giant exciton binding energy in bulk CrCl3

Van der Waals (vdW) materials, with their unique combination of electronic, optical, and magnetic properties, are emerging as promising platforms for exploring excitonic phenomena. Thus far, the choice of materials with exceptional excitonic response has been limited to two-dimensional (2D) configurations of vdW materials. At the same time, large interlayer distance and the possibility to create a variety of heterostructures offers an opportunity to control the dielectric screening in van der Waals heterostructures and van der Waals 3D materials, thus engineering the excitonic properties. Here, we reveal that bulk vdW crystal CrCl3 answers this quest with a record exciton binding energy of 1.64 eV owing to a delicate interplay of quasi-2D electronic confinement and local magnetic correlations. We also suggest that the non-local magnetic correlations play an important role in the temperature dependence of photoluminescence intensity. Furthermore, we observe colossal binding energies in vdW crystals NbOCl2 (0.66 eV) and MoCl3 (0.35 eV) and formulate a universal exciton binding energy dependence on bandgap for 2D and 3D vdW materials. Hence, our findings establish a fundamental link between the layered structure of vdW materials and their excitonic properties.

cond-mat.mtrl-sci↗

arXiv2025

Scalable van der Waals Photonics: High-Refractive-Index Gallium Sulfide Films with Single-Crystal Optical Properties

The integration of high-refractive-index dielectrics into scalable photonic architectures is foundational to advancing integrated circuits and augmented reality (AR) displays. Van der Waals (vdW) materials offer exceptional optical properties, including high refractive indices and giant anisotropy, but their implementation is constrained by the small area and uncontrolled thickness of mechanically exfoliated flakes. Here, we demonstrate that atomic layer deposition (ALD) grown gallium sulfide (GaS) overcomes the trade-off between high optical performance and manufacturability, emerging as a large-scale vdW dielectric platform. Through rigorous optical and structural benchmarking against pristine single crystals, we establish that the optical constants (n, k) of ALD-GaS are virtually indistinguishable from single-crystal counterparts. By leveraging the retained out-of-plane anisotropy, we demonstrate that ALD-GaS enables superior suppression of crosstalk in densely integrated waveguides compared to conventional scalable high-index platforms. Our findings establish ALD-GaS as a technologically viable pathway for implementing anisotropic vdW materials in visible-spectrum photonics.

physics.optics↗

arXiv2025

Giant optical anisotropy and visible-frequency epsilon-near-zero in hyperbolic van der Waals MoOCl2

The realization of extreme optical anisotropy is foundational to nanoscale light manipulation. Van der Waals (vdW) crystal MoOCl2 has emerged as a promising candidate for this quest, hosting hyperbolic plasmon polaritons in the visible and near-infrared wavelengths. However, the fundamental anisotropic dielectric tensor governing this behavior has remained elusive. Here, we resolve this problem by providing the first experimental determination of the full dielectric tensor of hyperbolic vdW MoOCl2. Via spectroscopic ellipsometry, Mueller matrix, and reflectance measurements, we quantify the material's optical duality: a metallic optical response (ε_1 < 0) along the crystallographic a-axis and a dielectric response (ε_1 > 0) along the orthogonal directions. This dichotomy drives an epsilon-near-zero (ENZ) condition at \approx 512 nm and results in giant in-plane birefringence of δn \approx 2.2 for MoOCl2. As a result, our work provides the critical missing experimental parameters for MoOCl2, establishing it as a benchmark hyperbolic and ENZ material.

physics.optics↗

arXiv2025

Giant optical anisotropy in CrSBr from giant exciton oscillator strength

The interplay between dimensionality and electronic correlations in van der Waals (vdW) materials offers a powerful toolkit for engineering light-matter interactions at the nanoscale. Excitons, bound electron-hole pairs, are central to this endeavor, yet maximizing their oscillator strength, which dictates the interaction cross-section, remains a challenge. Conventional wisdom suggests a trade-off, where the observable oscillator strength often decreases in strongly bound systems due to population dynamics. Here, we unveil a colossal oscillator strength associated with the quasi-one-dimensional (quasi-1D) excitons in the layered magnetic semiconductor CrSBr, which fundamentally defies this established scaling law. Through comprehensive optical characterization and ab initio calculations, we establish that this anomalous enhancement originates directly from the reduced dimensionality, which enforces an increased electron-hole wavefunction overlap. Moreover, we find a close connection between fundamental exciton and local spin fluctuations that contribute to the opening of the gap in the electronic spectrum. The resulting optical anisotropy shows a giant in-plane birefringence (Delta_n = 1.45) and profoundly anisotropic waveguiding, which we directly visualize using nano-optical imaging. Leveraging this extreme response, we realize a true zero-order quarter-wave plate with an unprecedented wavelength-to-thickness ratio (lambda/t) exceeding 3.4, surpassing the limits of current miniaturization technologies, including state-of-the-art metasurfaces. Our findings underscore the profound impact of dimensionality engineering in magnetic vdW materials for realizing novel regimes of light-matter coupling and developing next-generation ultracompact photonic architectures.

cond-mat.mtrl-sci↗

arXiv2025

Laser-Synthesized Amorphous PdSe$_{\mathrm{2-x}}$ Nanoparticles: A Defect-Rich Platform for High-Efficiency SERS, Photocatalysis, and Photothermal Conversion

The control of material properties at the atomic scale remains a central challenge in materials science. Transition metal dichalcogenides (TMDCs) offer remarkable electronic and optical properties, but their functionality is largely dictated by their stable crystalline phases. Here we demonstrate a single-step, ligand-free strategy using femtosecond laser ablation in liquid to transform crystalline, stoichiometric palladium diselenide (PdSe$_{\mathrm{2}}$) into highly stable, amorphous, and non-stoichiometric nanoparticles (PdSe$_{\mathrm{2-x}}$, with x$\approx$1). This laser-driven amorphization creates a high density of selenium vacancies and coordinatively unsaturated sites, which unlock a range of emergent functions absent in the crystalline precursor, including plasmon-free surface-enhanced Raman scattering with an enhancement factor exceeding 10$^\mathrm{6}$, a 50-fold increase in photocatalytic activity, and near-infrared photothermal conversion efficiency reaching 83$\%$. Our findings establish laser-induced amorphization as a powerful top-down approach for defect-engineered TMDCs and advances their practical usage in optics, catalysis, and nanomedicine.

cond-mat.mtrl-sci↗

arXiv2025

The influence of shot noise on the performance of phase singularity-based refractometric sensors

Topological singularities of optical response functions -- such as reflection amplitudes -- enable elegant practical applications ranging from analog signal processing to novel molecular sensing approaches. A phase singularity-based refractometric sensor monitors the rapidly evolving argument of the optical field near the point of phase singularity, in contrast to the reflection zero in traditional surface plasmon polariton sensors. This raises a natural question: What happens with the sensitivity and resolution of such a sensor when it operates close to a zero of the response function, where the detected signal may be greatly influenced by various noise sources? In this paper, we systematically study the effect of the shot noise on the performance of a generic phase singularity-based refractometric sensor. We develop a theoretical model of a spectroscopic ellipsometry-based system operating near a phase singularity and couple the macroscopic optical picture of the detection with a quantum shot noise model. Within the developed model, we illustrate how the shot noise of the detector comes into play and study its effect on the sensitivity and resolution of the refractometric sensor. Our results suggest that such an ellipsometry-based phase singularity sensor remains stable even in the presence of shot noise near the point of zero reflection.

physics.optics↗

arXiv2025

Computational discovery of high-refractive-index van der Waals materials: The case of HfS$_2$

New high-refractive-index dielectric materials may enhance many optical technologies by enabling efficient manipulation of light in waveguides, metasurfaces, and nanoscale resonators. Van der Waals materials are particularly promising due to their excitonic response and strong in-plane polarizability. Here we combine ab initio calculations and experiments to discover new high-refractive-index materials. Our screening highlights both known and new promising optical materials, including hafnium disulfide (HfS$_2$), which shows an in-plane refractive index above 3 and large anisotropy in the visible range. We confirm these theoretical predictions through ellipsometry measurements and investigate the photonic potential of HfS$_2$ by fabricating nanodisk resonators, observing optical Mie resonances in the visible spectrum. Over the course of seven days, we observe a structural change in HfS$_2$, which we show can be mitigated by storage in either argon-rich or humidity-reduced environments. This work provides a comparative overview of high-index van der Waals materials and showcases the potential of HfS$_2$ for photonic applications in the visible spectrum.

physics.optics↗

arXiv2024

Tunable Nanostructuring for van der Waals Materials

Van der Waals (vdW) materials are becoming increasingly popular in scientific and industrial applications because of their unique mixture of record electronic, optical, and mechanical properties. However, nanostructuring of vdW materials is still in its infancy and strongly depends on the specific vdW crystal. As a result, the universal self-assembled technology of vdW materials nanostructuring opens vast technological prospects. This work demonstrates an express and universal synthesis method of vdW nanoparticles with well-defined geometry using femtosecond laser ablation and fragmentation. The disarming simplicity of the technique allows us to create nanoparticles from over 50 vdW precursor materials covering transition metal chalcogenides, MXenes, and other vdW materials. Obtained nanoparticles manifest perfectly defined crystalline structures and diverse shapes, from nanospheres to nanocubes and nanotetrahedrons. Thus, our work provides a new paradigm for vdW nanostructuring with a vast potential of tunability for size, shape, and materials specific to the particular application.

physics.app-ph↗

arXiv2024

Anisotropic van der Waals Crystal with High Refractive Index and Transparency for UV-Visible Range Applications

Thanks to their record high refractive index and giant optical anisotropy, van der Waals (vdW) materials have accelerated the development of nanophotonics. However, traditional high refractive index materials, such as titanium dioxide (TiO2), still dominate in the most important visible range. This is due to the current lack of transparent vdW materials across the entire visible spectrum. In this context, we propose that germanium disulfide (GeS2) could offer a significant breakthrough. With its high refractive index, negligible losses, and biaxial optical anisotropy across the whole visible range, GeS2 has the potential to complement TiO2 and close the application gap of vdW materials in the visible spectrum. The addition of GeS2 could have a profound impact on the design of van der Waals nanophotonic circuits for any operation wavelength from ultraviolet to infrared, emphasizing the significance of the potential impact of GeS2 on the field of nanophotonics.

physics.optics↗

arXiv2022

Anomalous optical response of graphene on hexagonal boron nitride substrates

Graphene/hBN heterostructures can be considered as one of the basic building blocks for the next-generation optoelectronics mostly owing to the record-high electron mobilities. However, currently, the studies of the intrinsic optical properties of graphene are limited to the standard substrates (SiO2/Si, glass, quartz) despite the growing interest in graphene/hBN heterostructures. This can be attributed to a challenging task of the determination of hBN's strongly anisotropic dielectric tensor in the total optical response. In this study, we overcome this issue through imaging spectroscopic ellipsometry utilizing simultaneous analysis of hBN's optical response with and without graphene monolayers. Our technique allowed us to retrieve the optical constants of graphene from graphene/hBN heterostructures in a broad spectral range of 250-950 nm. Our results suggest that graphene's absorption on hBN may exceed the one of graphene on SiO2/Si by about 60 %.

cond-mat.mes-hall↗

arXiv2021

Topological phase singularities in atomically thin high-refractive-index materials

Atomically thin transition metal dichalcogenides (TMDCs) present a promising platform for numerous photonic applications due to excitonic spectral features, possibility to tune their constants by external gating, doping, or light, and mechanical stability. Utilization of such materials for sensing or optical modulation purposes would require a clever optical design, as by itself the 2D materials can offer only a small optical phase delay - consequence of the atomic thickness. To address this issue, we combine films of 2D semiconductors which exhibit excitonic lines with the Fabry-Perot resonators of the standard commercial SiO$_2$/Si substrate, in order to realize topological phase singularities in reflection. Around these singularities, reflection spectra demonstrate rapid phase changes while the structure behaves as a perfect absorber. Furthermore, we demonstrate that such topological phase singularities are ubiquitous for the entire class of atomically thin TMDCs and other high-refractive-index materials, making it a powerful tool for phase engineering in flat optics. As a practical demonstration, we employ PdSe$_2$ topological phase singularities for a refractive index sensor and demonstrate its superior phase sensitivity compared to typical surface plasmon resonance sensors.

physics.optics↗

arXiv2020

Densification of Single-Walled Carbon Nanotube Films: Mesoscopic Distinct Element Method Simulations and Experimental Validation

Nanometer thin single-walled carbon nanotube (CNT) films collected from the aerosol chemical deposition reactors have gathered attention for their promising applications. Densification of these pristine films provides an important way to manipulate the mechanical, electronic, and optical properties. To elucidate the underlying microstructural level restructuring, which is ultimately responsible for the change in properties, we perform large scale vector-based mesoscopic distinct element method simulations in conjunction with electron microscopy and spectroscopic ellipsometry characterization of pristine and densified films by drop-cast volatile liquid processing. Matching the microscopy observations, pristine CNT films with finite thickness are modeled as self-assembled CNT networks comprising entangled dendritic bundles with branches extending down to individual CNTs. Simulations of the film under uniaxial compression uncover an ultra-soft densification regime extending to a ~75% strain, which is likely accessible with the surface tensional forces arising from liquid surface tension during the evaporation. When removing the loads, the pre-compressed samples evolve into homogeneously densified films with thickness values depending on both the pre-compression level and the sample microstructure. The significant reduction in thickness, confirmed by our spectroscopic ellipsometry, is attributed to the underlying structural changes occurring at the 100 nm scale, including the zipping of the thinnest dendritic branches.

cond-mat.mtrl-sci↗