arXiv subjects

Diana Vaclavkova

Publications and source records attributed to Diana Vaclavkova.

11 recordsLinked to original sources

arXiv2026

Magnetic-Field-Induced Darkening of Bright Excitons in a MoWSe$_2$ Monolayer Alloy

Magnetic fields are widely used to brighten spin-forbidden dark excitons, but the inverse effect on an optically bright exciton has remained largely unexplored. We demonstrate the complementary phenomenon of magnetic-field-induced darkening of a bright exciton in Mo$_{0.68}$W$_{0.32}$Se$_2$. At 4.2 K, an in-plane magnetic field up to 25 T activates a dark-exciton line 14.2$\pm$1.3 meV below the bright exciton while suppressing the bright-exciton emission by about 85\%. A bright-dark mixing model quantitatively captures the coupled energy and intensity evolution with an effective in-plane $g$ factor of $|g_{\parallel}|=5.2\pm0.2$. Alloying is crucial to the effect, as it brings the system close to the bright-dark crossover, where a small bright-dark splitting is combined with unusually strong in-plane magnetic coupling. This places the system in a regime where field-induced level repulsion raises the bright-like branch and strongly depletes its thermal population. These results identify a general route to magnetic control of exciton populations through engineering of the bright-dark hierarchy.

cond-mat.mes-hall↗

arXiv2025

Extremely high excitonic $g$-factors in 2D crystals by alloy-induced admixing of band states

Monolayers (MLs) of semiconducting transition metal dichalcogenides (\mbox{S-TMDs}) emit light very efficiently and display rich spin-valley physics, with gyromagnetic ($g$-) factors of about -4. Here, we investigate how these properties can be tailored by alloying. Magneto-optical spectroscopy is used to reveal the peculiar properties of excitonic complexes in Mo$_{x}$W$_{1-x}$Se$_2$ MLs with different Mo and W concentrations. We show that the alloys feature extremely high $g$-factors for neutral excitons, that change gradually with the composition up to reaching values of the order of -10 for $x \approx 0.2$. First-principles calculations corroborate the experimental findings and provide evidence that alloying in S-TMDs results in a non-trivial band structure engineering, being at the origin of the high $g$-factors. The theoretical framework also suggests a higher strain sensitivity of the alloys, making them promising candidates for tailor-made optoelectronic devices.

cond-mat.mtrl-sci↗

arXiv2025

Strong and selective magnon-phonon coupling in van der Waals antiferromagnet CoPS$_3$

The Raman scattering response of the biaxial antiferromagnet CoPS$_3$ has been investigated as a function of both magnetic field and temperature. The peaks observed in the low-frequency spectral range (90--200~cm$^{-1}$) have been identified as hybrid magnon--phonon excitations. The energies of the bare magnon and phonon modes, as well as the effective coupling strengths between different excitation pairs, have been determined. The strong and selective magnon--phonon interaction largely accounts for the pronounced splitting of two phonon-like modes observed at 152~cm$^{-1}$ and 158~cm$^{-1}$ in the antiferromagnetic phase of CoPS$_3$. Based on the identification of bare magnon excitations and their magnetic-field dependence, we propose an updated set of parameters for the effective exchange ($J_{\mathrm{eff}} = 9.9$~meV) and biaxial magnetic anisotropy ($D = 4.3$~meV and $E = -0.7$~meV) and advocate for an apparent anisotropic $g$-factor ($g_x = g_y = 2$, $g_z = 4$) in the CoPS$_3$ antiferromagnet.

cond-mat.mes-hall↗

arXiv2024

Orientation-Driven Large Magnetic Hysteresis of Er(III) Cyclooctatetraenide-Based Single-Ion Magnets Adsorbed on Ag(100)

The molecular self-assembly and the magnetic properties of two cyclooctatetraenide (COT) - based single-ion magnets (SIM) adsorbed on Ag(100) in the sub-monolayer range are reported. Our study combines scanning-tunneling microscopy, X-ray photoemission spectroscopy and polarized X-ray absorption spectroscopy to show that Cp*ErCOT (Cp* = 1,2,3,4,5-pentamethylcyclopentadienide anion) SIMs self-assemble as alternating compact parallel rows including standing-up and lying-down conformations, following the main crystallographic directions of the substrate. Conversely, K[Er(COT)$_2$], obtained from subliming the [K(18-c-6)][Er(COT)$_2$]$\cdot$ 2THF salt, forms uniaxially ordered domains with the (COT)$^{2-}$ rings perpendicular to the substrate plane. The polarization-dependent X-ray absorption spectra reproduced by the multiX simulations suggest that the strong in-plane magnetic anisotropy of K[Er(COT)$_2$]/Ag(100) and the weak out-of-plane anisotropy of Cp*ErCOT/Ag(100) can be attributed to the strikingly different surface ordering of these two complexes. Compared to the bulk phase, surface-supported K[Er(COT)$_2$] exhibits a similarly large hysteresis opening, while the Cp*ErCOT shows a rather small opening. This result reveals that despite structural similarities, the two organometallic SMMs have strongly different magnetic properties when adsorbed on the metal substrate, attributed to the different orientations and the resulting interactions of the ligand rings with the surface.

cond-mat.mtrl-sci↗

arXiv2022

High-angular momentum excitations in collinear antiferromagnet FePS$_3$

We report on magneto-optical studies of the quasi-two-dimensional van der Waals antiferromagnet FePS$_3$. Our measurements reveal an excitation that closely resembles the antiferromagnetic resonance mode typical of easy-axis antiferromagnets, nevertheless, it displays an unusual, four-times larger Zeeman splitting in an applied magnetic field. We identify this excitation with an $|S_z|=4$ multipolar magnon -- a single-ion 4-magnon bound state -- that corresponds to a full reversal of a single magnetic moment of the Fe$^{2+}$ ion. We argue that condensation of multipolar magnons in large-spin materials with a strong magnetic anisotropy can produce new exotic states.

cond-mat.str-el↗

arXiv2022

Excitons and trions in WSSe monolayers

The possibility of almost linear tuning of the band gap and of the electrical and optical properties in monolayers (MLs) of semiconducting transition metal dichalcogenide (S-TMD) alloys opens up the way to fabricate materials with on-demand characteristics. By making use of photoluminescence spectroscopy, we investigate optical properties of WSSe MLs with a S/Se ratio of 57/43 deposited on SiO$_2$/Si substrate and encapsulated in hexagonal BN flakes. Similarly to the $"parent"$ WS$_2$ and WSe$_2$ MLs, we assign the WSSe MLs to the ML family with the dark ground exciton state. We find that, in addition to the neutral bright A exciton line, three observed emission lines are associated with negatively charged excitons. The application of in-plane and out-of-plane magnetic fields allows us to assign undeniably the bright and dark (spin- and momentum-forbidden) negative trions as well as the phonon replica of the dark spin-forbidden complex. Furthermore, the existence of the single photon emitters in the WSSe ML is also demonstrated, thus prompting the opportunity to enlarge the wavelength range for potential future quantum applications of S-TMDs.

cond-mat.mes-hall↗

arXiv2022

High pressure tuning of magnon-polarons in the layered antiferromagnet FePS$_3$

Magnetic layered materials have emerged recently as promising systems to introduce magnetism in structures based on two-dimensional (2D) materials and to investigate exotic magnetic ground states in the 2D limit. In this work, we apply high hydrostatic pressures up to P = 8.7 GPa to the bulk layered antiferromagnet FePS$_3$ to tune the collective lattice excitations (phonons) in resonance with magnetic excitations (magnons). Close to P = 4 GPa, the magnon-phonon resonance is achieved and the strong coupling between these collective modes leads to the formation of new quasi-particles, the magnon-polarons, evidenced in our low temperature Raman scattering experiments by a particular avoided crossing behavior between the phonon and the doubly degenerate antiferromagnetic magnon. At the pressure-induced magnon-phonon resonance, three distinct coupled modes emerge. As it is mainly defined by intralayer properties, we show that the energy of the magnon is nearly pressure independent. We additionally apply high magnetic fields up to B = 30 T to fully identify and characterize the magnon excitations, and to explore the different magnon-polaron regimes for which the phonon has an energy lower-, equal to-, or higher- than the magnon energy. The description of our experimental data requires introducing a phonon-phonon coupling not taken into account in actual calculations.

cond-mat.mes-hall↗

arXiv2021

Destructive photon echo formation in six-wave mixing signals of a MoSe$_2$ monolayer

Monolayers of transition metal dichalcogenides display a strong excitonic optical response. Additionally encapsulating the monolayer with hexagonal boron nitride allows to reach the limit of a purely homogeneously broadened exciton system. On such a MoSe$_{2}$-based system we perform ultrafast six-wave mixing spectroscopy and find a novel destructive photon echo effect. This process manifests as a characteristic depression of the nonlinear signal dynamics when scanning the delay between the applied laser pulses. By theoretically describing the process within a local field model we reach an excellent agreement with the experiment. We develop an effective Bloch vector representation and thereby demonstrate that the destructive photon echo stems from a destructive interference of successive repetitions of the heterodyning experiment.

cond-mat.mes-hall↗

arXiv2021

Rydberg series of dark excitons and the conduction band spin-orbit splitting in monolayer WSe$_2$

Strong Coulomb correlations together with multi-valley electronic bands in the presence of spin-orbit interaction and possible new optoelectronic applications are at the heart of studies of the rich physics of excitons in semiconductor structures made of monolayers of transition metal dichalcogenides (TMD). In intrinsic TMD monolayers the basic, intravalley excitons are formed by a hole from the top of the valence band and an electron either from the lower or upper spin-orbit-split conduction band subbands: one of these excitons is optically active, the second one is "dark", although possibly observed under special conditions. Here we demonstrate the s-series of Rydberg dark exciton states in monolayer WSe$_2$, which appears in addition to a conventional bright exciton series in photoluminescence spectra measured in high in-plane magnetic fields. The comparison of energy ladders of bright and dark Rydberg excitons is shown to be a method to experimentally evaluate one of the missing band parameters in TMD monolayers: the amplitude of the spin-orbit splitting of the conduction band.

cond-mat.mes-hall↗

arXiv2020

Magnetoelastic interaction in the two-dimensional magnetic material MnPS$_3$ studied by first principles calculations and Raman experiments

We report experimental and theoretical studies on the magnetoelastic interactions in MnPS$_3$. Raman scattering response measured as a function of temperature shows a blue shift of the Raman active modes at 120.2 and 155.1 cm$^{-1}$, when the temperature is raised across the antiferromagnetic-paramagnetic transition. Density functional theory (DFT) calculations have been performed to estimate the effective exchange interactions and calculate the Raman active phonon modes. The calculations lead to the conclusion that the peculiar behavior with temperature of the two low energy phonon modes can be explained by the symmetry of their corresponding normal coordinates which involve the virtual modification of the super-exchange angles associated with the leading antiferromagnetic (AFM) interactions.

cond-mat.mes-hall↗

arXiv2020

Coherent dynamics and mapping of excitons in single-layer MoSe$_2$ and WSe$_2$ at the homogeneous limit

We perform coherent nonlinear spectroscopy of excitons in single-layers of MoSe$_2$ and WSe$_2$ encapsulated between thin films of hexagonal boron nitride. Employing four-wave mixing microscopy we identify virtually disorder free areas, generating exciton optical response at the homogeneous limit. Focussing on such areas, we measure exciton homogeneous broadening as a function of environmental factors, namely temperature and exciton density. Exploiting FWM imaging, we find that at such locations, nonlinear absorption of the exciton excited states and their coherent couplings can be observed. Using the WSe$_2$ heterostructure, we infer coherence and density dynamics of the exciton 2S state. Owing to its increased radiative lifetime, at low temperatures, the dephasing of the 2S state is longer than of the 1S transition. While scanning various heterostructures across tens of micrometers, we conclude that the disorder, principally induced by strain variations, remain to be present creating spatially varying inhomogeneous broadening.

cond-mat.mtrl-sci↗