arXiv subjects

Alexander I. Tartakovskii

Publications and source records attributed to Alexander I. Tartakovskii.

At least 19 recordsLinked to original sources

arXiv2026

Near-Field Characterisation of Guided Modes in WS2 Nanobeams and Quasi-Bulk Crystals

The exceptionally high in-plane refractive index, low sub-bandgap absorption, and strong optical anisotropy of WS2 make it a promising material platform for next-generation integrated circuits for nanophotonics. Its layered van der Waals structure further enables heterogeneous integration with silicon photonics and emerging two-dimensional optoelectronic materials. However, despite increasing interest in the waveguiding properties of WS2, experimental studies of wavelength-dependent modal confinement and attenuation remain limited. Additionally, though the extinction coefficient of WS2 is expected to be near-negligible beneath the bandgap, reported values span orders of magnitude, leading to large uncertainty in predicted modal decay lengths and wafer-scale integration feasibility. To resolve these ambiguities we perform hyperspectral cavity-enhanced imaging, determining high-resolution upper and lower bounds on the extinction coefficient of WS2 within the visible-NIR edge. We further employ scattering-type scanning near-field optical microscopy (s-SNOM) to probe TE0, TM0, and higher-order modes in both quasi-bulk and nanobeam WS2 waveguides across the 800-1400 nm spectral range, enabling identification of mode-specific trends in wavevector dispersion and loss. This work simultaneously assesses s-SNOM as a probe of waveguide performance, and we find that while absolute loss values depend on measurement geometry, s-SNOM reliably captures relative modal trends and provides upper bounds on propagation loss, supporting its use as a diagnostic tool for anisotropic waveguides. We further identify significant artefacts in nanobeam measurements arising from transverse interference and spatial sampling effects when the structure size approaches the excitation wavelength, which can shift extracted effective indices by up to 0.25.

physics.optics↗

arXiv2026

Magnetic switching of exciton lifetime in CrSBr

Exciton dynamics in layered magnetic semiconductors provide a sensitive probe of the interplay between spin order and light-matter interaction. Here, we study thin CrSBr layers using time-resolved photoluminescence spectroscopy in an external magnetic field, revealing a step-like reduction in the exciton lifetime from 11 to 7 ps, during the magnetization flip from the antiferromagnetic to the ferromagnetic phase. The reduction of the exciton lifetime in the ferromagnetic phase persists below the Néel temperature, as evidenced by its strong magnetic-field dependence that disappears in the paramagnetic phase. Ab initio calculations reveal a one-dimensional nature of free excitons accompanied by a pronounced change in the oscillator strength across the magnetic phase transition predicting a shorter radiative lifetime of free excitons in the antiferromagnetic phase of CrSBr contradicting the experimental observations. This discrepancy is explained by strong localization of excitons at low tempature. We show both experimentally and theoretically that the observed magnetic switching of the exciton lifetime is attributed to a larger exciton localization volume leading to a larger oscillator strength in the ferromagnetic phase. The results show that disorder-induced localization effects play a key role in exciton dynamics in CrSBr.

cond-mat.mes-hall↗

arXiv2025

Polarization- and time-resolved nonlinear multi-photon spectroscopy for confocal microscopy of semiconductor nanostructures

We present a versatile confocal microscopy setup for optical second harmonic generation (SHG) and multi-photon spectroscopy that enables polarization-resolved studies of semiconductor bulk crystals and low-dimensional structures. The system offers full polarization control in both excitation and detection, spatial scanning with micrometer resolution, and spectrally tunable excitation over a broad energy range from 0.5 to 4.0 eV, using femtosecond and picosecond laser pulses. Samples are mounted in a helium-flow cryostat, allowing temperature control from 4 to 300 K. Magnetic fields up to 0.625 T can be applied in the Voigt geometry via an electromagnet. The nonlinear optical signals are analyzed using a high-resolution spectrometer with a spectral resolution of 60 $μ$eV. We demonstrate the potential of the setup by means of SHG polarization tomography measurements on a Cu$_2$O crystal as well as through a SHG spectral scan of a ZnSe crystal over a wide energy range from 1.4 to 3.1 eV. Polarization-resolved confocal SHG mapping of various twisted mono- and bilayer MoS$_2$ structures is also presented. In addition, time-resolved two-color pump-probe experiments are shown for a Cs$_2$AgBiBr$_6$ crystal, illustrating the potential of the system for investigating coherent exciton and phonon dynamics.

cond-mat.mtrl-sci↗

arXiv2025

Exciton-polaritons in a monolayer semiconductor coupled to van der Waals dielectric nanoantennas on a metallic mirror

Polaritons in nanophotonic structures have attracted long-standing interest owing to their fundamental importance and potential for applications in nonlinear and quantum optics. Nanoantennas (NAs) made from high refractive index dielectrics offer a suitable platform for polariton physics thanks to the strongly confined optical Mie resonances and low optical losses in contrast to metallic NAs. However, Mie modes are mainly confined within the NA, making inefficient their coupling with excitons in materials deposited externally. Here, we overcome this limitation by using a high-refractive index van der Waals material WS$_2$, which allows straightforward fabrication of NAs on gold. The combination of a 27 nm tall WS$_2$ NA and a gold substrate enables strong modification of the Mie mode distribution and field enhancement inside and in the vicinity of the NA. This allows observation of room-temperature Mie-polaritons (with a Rabi splitting above 80 meV) arising from the strong coupling between Mie modes and the exciton in a monolayer WSe$_2$ placed on WS$_2$/gold NAs. We demonstrate strong nonlinearity of Mie-polaritons, one order of magnitude higher than for excitons in monolayer WSe$_2$ on gold. Our results highlight applicability of van der Waals materials for the realisation of hybrid dielectric-metallic nanophotonics for the study of the strong light-matter interaction.

physics.optics↗

arXiv2025

Topological Jackiw-Rebbi States in Photonic Van der Waals Heterostructures

Topological phenomena, first studied in solid state physics, have seen increased interest for applications in nanophotonics owing to highly controllable light confinement with inherent robustness to defects. Photonic crystals can be designed to host topologically protected interface states for directional light transport, localization and robust lasing via tuning of the bulk topological invariant. At the same time, van der Waals (vdW) materials, in both their monolayer and quasi-bulk forms, are emerging as exciting additions to the field of nanophotonics, with a range of unique optoelectronic properties and intrinsic adherence to any type of host material, allowing fabrication of complex multi-layer structures. We present here a 1D topological photonic platform made from stacked nanostructured and planar layers of quasi-bulk WS$_2$ to achieve Jackiw-Rebbi (JR) interface states between two topologically distinct gratings in the near-infrared range around 750 nm. Such states are measured in the far-field with angle-resolved reflectance contrast measurements, exhibiting linewidth of 10 meV and highly directional emission with an angular bandwidth of 8.0$^\circ$. Subsequent local mapping of the structure via sub-wavelength resolution scattering-type scanning near-field optical microscopy (s-SNOM) reveals strong spatial confinement of the JR state to the grating interface region. Finally, we couple in the JR state the photoluminescence of monolayer WSe$_2$ incorporated in a five-layer vdW grating heterostructure, giving rise to directional enhancement of the excitonic emission of up to 22 times that of uncoupled monolayer, thus demonstrating the potential of the topological interface states for highly directional light emission in addition to light scattering.

physics.optics↗

arXiv2025

Fabrication of ultra-smooth, high-aspect ratio, sub-10 nanometer nanostructures

Deterministic and versatile approaches to sample preparation on nanoscopic scales are important in many fields including photonics, electronics, biology and material science. However, challenges exist in meeting many nanostructuring demands--particularly in emerging optical materials and component architectures. Here, we report a nanofabrication workflow that overcomes long-standing challenges in deterministic and top-down sample preparation procedures. The salient feature is a carbon mask with a low sputter yield that can be readily shaped using high resolution electron beam processing techniques. When combined with focused ion beam processing, the masking technique yields structures with ultra-smooth, near-vertical side walls. We target different material platforms to showcase the broad utility of the technique. As a first test case, we prepared nanometric gaps in evaporated Au. Gap widths of 7 plus/minus 2 nm, aspect ratios of 17, and line edge roughness values of 3sigma = 2.04 nm are achieved. Furthermore, the gap widths represent an order of magnitude improvement on system resolution limits. As a second test case, we designed and fabricated dielectric resonators in the ternary compounds MnPSe3 and NiPS3; a class of van der Waals material resistant to chemical etch approaches. Nanoantenna arrays with incrementally increasing diameter were fabricated in crystalline, exfoliated flakes. The optical response was measured by dark field spectroscopy and is in agreement with simulations. The workflow reported here leverages established techniques in material processing without the need for custom or specialized hardware. It is broadly applicable to functional materials and devices, and extends high speed focused ion beam milling to true sub-10 nm length scales.

physics.optics↗

arXiv2024

Simultaneous observation of bright and dark polariton states in subwavelength gratings made from quasi-bulk WS$_2$

Over the last decade, layered crystals, dubbed van der Waals (vdW) materials, have attracted tremendous interest due to their unique properties in their single and few layer regimes. Their bulk counterparts, however, have only been recently explored as building blocks for nanophotonics as they offer promising properties such as high refractive indices and adherence to any type of substrates. We present here a variety of 1D grating structures composed of bulk transition metal dichalcogenide (TMD) WS$_2$ as a highly tunable and versatile platform for observation of multi-level polaritonic system. The WS$_2$ excitons are simultaneously strongly coupled with the two grating photonic modes including the Bound State in the Continuum (BIC) of the lower energetic mode giving rise to polariton-BICs (pol-BICs). The polaritonic dispersion shapes can be varied in a straightforward fashion by choosing WS$_2$ films of different thicknesses and by changing the period of the grating.

physics.optics↗

arXiv2024

Singlet fission contributes to solar energy harvesting in photosynthesis

Singlet fission (SF), the spin-allowed conversion of one singlet exciton into two triplet excitons, offers a promising strategy for enhancing the efficiency of photovoltaic devices. However, realising this potential necessitates materials capable of ultrafast (sub-picosecond) SF and the generation of long-lived (> microsecond) triplet excitons, a synthetic challenge. Some photosynthetic organisms have evolved sophisticated molecular architectures that demonstrate these criteria, but despite 40 years of study, the underlying SF mechanisms and its functional significance in these organisms remain unclear. Here, we use a suite of ultrafast and magneto-optical spectroscopic techniques to understand the mechanism of SF within light-harvesting 1 (LH1) complexes from wild-type and genetically modified photosynthetic bacteria. Our findings reveal a SF process, termed "heterofission", wherein singlet excitons are transformed into triplet excitons localised on adjacent carotenoid (Crt) and bacteriochlorophyll (BChl) molecules. We also uncover an unexpected functional role for SF in augmenting Crt-to-BChl photosynthetic energy transfer efficiency. By transiently storing electronic excitation within the SF-generated triplet pair, the system circumvents rapid thermalisation of Crt excitations, thereby enhancing energy transfer efficiency to the BChl Qy state, and enabling the organism to usefully harvest more sunlight.

physics.bio-ph↗

arXiv2024

Single photon emitters in monolayer semiconductors coupled to transition metal dichalcogenide nanoantennas on silica and gold substrates

Transition metal dichalcogenide (TMD) single photon emitters (SPEs) offer numerous advantages to quantum information applications, such as high single photon purity and deterministic positioning. Strain in the host monolayer, induced by underlying dielectric Mie resonators, is known to localize their formation to positions co-located with near-field photonic hotspots providing further control over their optical properties. However, traditional materials used for the fabrication of nanoresonators, such as silicon or gallium phosphide (GaP), often require a high refractive index substrate resulting in losses of the emitted light and limited photonic enhancement. Here, we use nanoantennas (NAs) fabricated from multilayer TMDs, which allow complete flexibility with the choice of substrate due to the adhesive van der Waals forces, enabling high refractive index contrast or the use of highly reflective metallic surfaces. We demonstrate the localized formation of SPEs in WSe$_2$ monolayers transferred onto WS$_2$ NAs on both SiO$_2$ and Au substrates, enabling strong photonic enhancements and increased single photon collection. We provide evidence for enhanced quantum efficiencies (QE) reaching an average value of 43% (7%) for SPEs on WS$_2$ NAs on a SiO$_2$ (Au) substrate. We further combine the advantages offered by both dielectric and metallic substrates to numerically simulate an optimized NA geometry for maximum WSe$_2$ single photon excitation, emission, collection. Thus, the fluorescence is enhanced by a factor of over 4 orders of magnitude compared to vacuum and 5 orders of magnitude compared to a flat SiO$_2$/Si surface. Our work showcases the advantages offered by employing TMD material nanoresonators on various substrates for SPE formation and photonic enhancement.

cond-mat.mes-hall↗

arXiv2024

Femtosecond switching of strong light-matter interactions in microcavities with two-dimensional semiconductors

Ultrafast all-optical logic devices based on nonlinear light-matter interactions hold the promise to overcome the speed limitations of conventional electronic devices. Strong coupling of excitons and photons inside an optical resonator enhances such interactions and generates new polariton states which give access to unique nonlinear phenomena, such as Bose-Einstein condensation, used for all-optical ultrafast polariton transistors. However, the pulse energies required to pump such devices range from tens to hundreds of pJ, making them not competitive with electronic transistors. Here we introduce a new paradigm for all-optical switching based on the ultrafast transition from the strong to the weak coupling regime in microcavities embedding atomically thin transition metal dichalcogenides. Employing single and double stacks of hBN-encapsulated MoS$_2$ homobilayers with high optical nonlinearities and fast exciton relaxation times, we observe a collapse of the 55-meV polariton gap and its revival in less than one picosecond, lowering the threshold for optical switching below 4 pJ per pulse, while retaining ultrahigh switching frequencies. As an additional degree of freedom, the switching can be triggered pumping either the intra- or the interlayer excitons of the bilayers at different wavelengths, speeding up the polariton dynamics, owing to unique interspecies excitonic interactions. Our approach will enable the development of compact ultrafast all-optical logical circuits and neural networks, showcasing a new platform for polaritonic information processing based on manipulating the light-matter coupling.

physics.optics↗

arXiv2024

Realization of Z$_2$ topological photonic insulators made from multilayer transition metal dichalcogenides

Monolayers of semiconducting transition metal dichalcogenides (TMDs) have long attracted interest for their intriguing optical and electronic properties. Recently TMDs in their quasi-bulk form have started to show considerable promise for nanophotonics thanks to their high refractive indices, large optical anisotropy, wide transparency windows reaching to the visible, and robust room temperature excitons promising for nonlinear optics. Adherence of TMD layers to any substrate via van der Waals forces is a further key enabler for nanofabrication of sophisticated photonic structures requiring heterointegration. Here, we capitalize on these attractive properties and realize topological spin-Hall photonic lattices made of arrays of triangular nanoholes in 50 to 100 nm thick WS$_2$ flakes exfoliated on SiO$_2$/Si substrates. High quality structures are achieved taking advantage of anisotropic dry etching dictated by the crystal axes of WS$_2$. Reflectance measurements at room temperature show a photonic gap opening in the near-infrared in trivial and topological phases. Unidirectional propagation along the domain interface is demonstrated in real space via circularly polarized laser excitation in samples with both zigzag and armchair domain boundaries. Finite-difference time-domain simulations are used to interpret optical spectroscopy results. Our work opens the way for future sophisticated nanophotonic devices based on the layered (van der Waals) materials platform.

physics.optics↗

arXiv2024

Spin relaxation of localized electrons in monolayer MoSe$_2$: importance of random effective magnetic fields

We study the Hanle and spin polarization recovery effects on resident electrons in a monolayer MoSe$_2$ on EuS. We demonstrate that localized electrons provide the main contribution to the spin dynamics signal at low temperatures below 15~K for small magnetic fields of only a few mT. The spin relaxation of these electrons is determined by random effective magnetic fields due to a contact spin interaction, namely the hyperfine interaction with the nuclei in MoSe$_2$ or the exchange interaction with the magnetic ions of the EuS film. From the magnetic field angular dependence of the spin polarization we evaluate the anisotropy of the intervalley electron $g$-factor and the spin relaxation time. The non-zero in-plane $g$-factor $|g_x|\approx 0.1$, the value of which is comparable to its dispersion, is attributed to randomly localized electrons in the MoSe$_2$ layer.

cond-mat.mes-hall↗

arXiv2024

Spin-order-dependent magneto-elastic coupling in two dimensional antiferromagnetic MnPSe$_3$ observed through Raman spectroscopy

Layered antiferromagnetic materials have emerged as a novel subset of the two-dimensional family providing a highly accessible regime with prospects for layer-number-dependent magnetism. Furthermore, transition metal phosphorous trichalcogenides, MPX3 (M = transition metal; X = chalcogen) provide a platform for investigating fundamental interactions between magnetic and lattice degrees of freedom providing new insights for developing fields of spintronics and magnonics. Here, we use a combination of temperature dependent Raman spectroscopy and density functional theory to explore magnetic-ordering-dependent interactions between the manganese spin degree of freedom and lattice vibrations of the non-magnetic sub-lattice via a Kramers-Anderson super-exchange pathway in both bulk, and few-layer, manganese phosphorous triselenide (MnPSe$_3$). We observe a nonlinear temperature dependent shift of phonon modes predominantly associated with the non-magnetic sub-lattice, revealing their non-trivial spin-phonon coupling below the N{é}el temperature at 74 K, allowing us to extract mode-specific spin-phonon coupling constants.

cond-mat.mtrl-sci↗

arXiv2023

Resonant band hybridization in alloyed transition metal dichalcogenide heterobilayers

Bandstructure engineering using alloying is widely utilised for achieving optimised performance in modern semiconductor devices. While alloying has been studied in monolayer transition metal dichalcogenides, its application in van der Waals heterostructures built from atomically thin layers is largely unexplored. Here, we fabricate heterobilayers made from monolayers of WSe$_2$ (or MoSe$_2$) and Mo$_x$W$_{1-x}$Se$_2$ alloy and observe nontrivial tuning of the resultant bandstructure as a function of concentration $x$. We monitor this evolution by measuring the energy of photoluminescence (PL) of the interlayer exciton (IX) composed of an electron and hole residing in different monolayers. In Mo$_x$W$_{1-x}$Se$_2$/WSe$_2$, we observe a strong IX energy shift of $\approx$100 meV for $x$ varied from 1 to 0.6. However, for $x<0.6$ this shift saturates and the IX PL energy asymptotically approaches that of the indirect bandgap in bilayer WSe$_2$. We theoretically interpret this observation as the strong variation of the conduction band K valley for $x>0.6$, with IX PL arising from the K-K transition, while for $x<0.6$, the bandstructure hybridization becomes prevalent leading to the dominating momentum-indirect K-Q transition. This bandstructure hybridization is accompanied with strong modification of IX PL dynamics and nonlinear exciton properties. Our work provides foundation for bandstructure engineering in van der Waals heterostructures highlighting the importance of hybridization effects and opening a way to devices with accurately tailored electronic properties.

cond-mat.mtrl-sci↗

arXiv2023

Van der Waals Nanoantennas on Gold as Hosts for Hybrid Mie-Plasmonic Resonances

Dielectric nanoresonators have been shown to circumvent the heavy optical losses associated with plasmonic devices, however they suffer from less confined resonances. By constructing a hybrid system of both dielectric and metallic materials, one can retain the low losses of dielectric resonances, whilst gaining additional control over the tuning of the modes with the metal, and achieving stronger mode confinement. In particular, multi-layered van der Waals materials are emerging as promising candidates for integration with metals owing to their weak attractive forces, which enable deposition onto such substrates without the requirement of lattice matching. Here we use layered, high refractive index WS$_2$ exfoliated on gold, to fabricate and optically characterize a hybrid nanoantenna-on-gold system. We experimentally observe a hybridization of Mie resonances, Fabry-Pérot modes, and surface plasmon-polaritons launched from the nanoantennas into the substrate. We achieve experimental quality factors of Mie-plasmonic modes of up to 20 times that of Mie resonances in nanoantennas on silica, and observe signatures of a supercavity mode with a Q factor of 263 $\pm$ 28, resulting from strong mode coupling between a higher-order anapole and Fabry-Pérot-plasmonic mode. We further simulate WS$_2$ nanoantennas on gold with an hBN spacer, resulting in calculated electric field enhancements exceeding 2600, and a Purcell factor of 713. Our results demonstrate dramatic changes in the optical response of dielectric nanophotonic structures placed on gold, opening new possibilities for nanophotonics and sensing with simple-to-fabricate devices.

cond-mat.mes-hall↗

arXiv2022

Van der Waals Materials for Applications in Nanophotonics

Numerous optical phenomena and applications have been enabled by nanophotonic structures. Their current fabrication from high refractive index dielectrics, such as silicon or gallium phosphide, pose restricting fabrication challenges, while metals, relying on plasmons and thus exhibiting high ohmic losses, limit the achievable applications. Here, we present an emerging class of layered so-called van der Waals (vdW) crystals as a viable nanophotonics platform. We extract the dielectric response of 11 mechanically exfoliated thin-film (20-200 nm) van der Waals crystals, revealing high refractive indices up to n = 5, pronounced birefringence up to $Δ$n = 3, sharp absorption resonances, and a range of transparency windows from ultraviolet to near-infrared. We then fabricate nanoantennas on SiO$_2$ and gold utilizing the compatibility of vdW thin films with a variety of substrates. We observe pronounced Mie resonances due to the high refractive index contrast on SiO$_2$ leading to a strong exciton-photon coupling regime as well as largely unexplored high-quality-factor, hybrid Mie-plasmon modes on gold. We demonstrate further vdW-material-specific degrees of freedom in fabrication by realizing nanoantennas from stacked twisted crystalline thin-films, enabling control of nonlinear optical properties, and post-fabrication nanostructure transfer, important for nano-optics with sensitive materials.

physics.optics↗

arXiv2022

Understanding the impact of heavy ions and tailoring the optical properties of large-area Monolayer WS2 using Focused Ion Beam

Focused ion beam (FIB) has been used as an effective tool for precise nanoscale fabrication. It has recently been employed to tailor defect engineering in functional nanomaterials such as two-dimensional transition metal dichalcogenides (TMDCs), providing desirable properties in TMDC-based optoelectronic devices. However, the damage caused by the FIB irradiation and milling process to these delicate atomically thin materials, especially in the extended area, has not yet been elaboratively characterised. Understanding the correlation between lateral ion beam effects and optical properties of 2D TMDCs is crucial in designing and fabricating high-performance optoelectronic devices. In this work, we investigate lateral damage in large-area monolayer WS2 caused by the gallium focused ion beam milling process. Three distinct zones away from the milling location are identified and characterised via steady-state photoluminescence (PL) and Raman spectroscopy. An unexpected bright ring-shaped emission around the milled location has been revealed by time-resolved PL spectroscopy with high spatial resolution. Our finding opens new avenues for tailoring the optical properties of TMDCs by charge and defect engineering via focused ion beam lithography. Furthermore, our study provides evidence that while some localised damage is inevitable, distant destruction can be eliminated by reducing the ion beam current. It paves the way for the use of FIB to create nanostructures in 2D TMDCs, as well as the design and realisation of optoelectrical devices on a wafer scale.

physics.app-ph↗

arXiv2022

Nonlinear interactions of dipolar excitons and polaritons in MoS2 bilayers

Nonlinear interactions between excitons strongly coupled to light are key for accessing quantum many-body phenomena in polariton systems. Atomically-thin two-dimensional semiconductors provide an attractive platform for strong light-matter coupling owing to many controllable excitonic degrees of freedom. Among these, the recently emerged exciton hybridization opens access to unexplored excitonic species, with a promise of enhanced interactions. Here, we employ hybridized interlayer excitons (hIX) in bilayer MoS2 to achieve highly nonlinear excitonic and polaritonic effects. Such interlayer excitons possess an out-of-plane electric dipole as well as an unusually large oscillator strength allowing observation of dipolar polaritons(dipolaritons) in bilayers in optical microcavities. Compared to excitons and polaritons in MoS2 monolayers, both hIX and dipolaritons exhibit about 8 times higher nonlinearity, which is further strongly enhanced when hIX and intralayer excitons, sharing the same valence band, are excited simultaneously. This gives rise to a highly nonlinear regime which we describe theoretically by introducing a concept of hole crowding. The presented insight into many-body interactions provides new tools for accessing few-polariton quantum correlations.

cond-mat.mes-hall↗