arXiv subjects

M. Grzeszczyk

Publications and source records attributed to M. Grzeszczyk.

At least 19 recordsLinked to original sources

arXiv2024

The temperature influence on the brightening of neutral and charged dark excitons in WSe$_2$ monolayer

The optically dark states play an important role in the electronic and optical properties of monolayers (MLs) of semiconducting transition metal dichalcogenides. The effect of temperature on the in-plane-field activation of the neutral and charged dark excitons is investigated in a WSe$_2$ ML encapsulated in hexagonal BN flakes. The brightening rates of the neutral dark (X$^D$) and grey (X$^G$) excitons and the negative dark trion (T$^D$) differ substantially at a particular temperature. More importantly, they vanish considerably by about 3 -- 4 orders of magnitude with the temperature increased from 4.2 K to 100 K. The quenching of the dark-related emissions is accompanied by the two-order-of-magnitude increase in the emissions of their neutral bright counterparts, $i.e.$ neutral bright exciton (X$^B$) and spin-singlet (T$^S$) and spin-triplet (T$^T$) negative trions, due to the thermal activations of dark states. Furthermore, the energy splittings between the dark X$^D$ and T$^D$ complexes and the corresponding bright X$^B$, T$^S$, and T$^T$ ones vary with temperature rises from 4.2 K to 100 K. This can be explained in terms of the different exciton-phonon couplings for the bright and dark excitons stemming from their distinct symmetry properties.

cond-mat.mes-hall↗

arXiv2024

Atomic and electronic structure of defects in hBN: enhancing single-defect functionalities

Defect centers in insulators play a critical role in creating important functionalities in materials: prototype qubits, single-photon sources, magnetic field probes, and pressure sensors. These functionalities are highly dependent on their mid-gap electronic structure and orbital/spin wave-function contributions. However, in most cases, these fundamental properties remain unknown or speculative due to the defects being deeply embedded beneath the surface of highly resistive host crystals, thus impeding access through surface probes. Here, we directly inspected the atomic and electronic structures of defects in thin carbon-doped hexagonal boron nitride (hBN:C) using scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS). Such investigation adds direct information about the electronic mid-gap states to the well-established photoluminescence response (including single photon emission) of intentionally created carbon defects in the most commonly investigated van der Waals insulator. Our joint atomic-scale experimental and theoretical investigations reveal two main categories of defects: 1) single-site defects manifesting as donor-like states with atomically resolved structures observable via STM, and 2) multi-site defect complexes exhibiting a ladder of empty and occupied mid-gap states characterized by distinct spatial geometries. Combining direct probing of mid-gap states through tunneling spectroscopy with the inspection of the optical response of insulators hosting specific defect structures holds promise for creating and enhancing functionalities realized with individual defects in the quantum limit. These findings underscore not only the versatility of hBN:C as a platform for quantum defect engineering but also its potential to drive advancements in atomic-scale optoelectronics.

cond-mat.mtrl-sci↗

arXiv2023

Raman scattering excitation in monolayers of semiconducting transition metal dichalcogenides

Raman scattering excitation (RSE) is an experimental technique in which the spectrum is made up by sweeping the excitation energy when the detection energy is fixed. We study the low-temperature ($T$=5~K) RSE spectra measured on four high quality monolayers (ML) of semiconducting transition metal dichalcogenides (S-TMDs), $i.e.$ MoS$_2$, MoSe$_2$, WS$_2$, and WSe$_2$, encapsulated in hexagonal BN. The outgoing resonant conditions of Raman scattering reveal an extraordinary intensity enhancement of the phonon modes, which results in extremely rich RSE spectra. The obtained spectra are composed not only of Raman-active peaks, $i.e.$ in-plane E$'$ and out-of-plane A$'_1$, but the appearance of 1$^{st}$, 2$^{nd}$, and higher-order phonon modes is recognised. The intensity profiles of the A$'_1$ modes in the investigated MLs resemble the emissions due to neutral excitons measured in the corresponding PL spectra for the outgoing type of resonant Raman scattering conditions. Furthermore, for the WSe$_2$ ML, the A$'_1$ mode was observed when the incoming light was in resonance with the neutral exciton line. The strength of the exciton-phonon coupling (EPC) in S-TMD MLs strongly depends on the type of their ground excitonic state, $i.e.$ bright or dark, resulting in different shapes of the RSE spectra. Our results demonstrate that RSE spectroscopy is a powerful technique for studying EPC in S-TMD MLs.

cond-mat.mes-hall↗

arXiv2023

Electrical excitation of carbon centers in hexagonal boron nitride with tuneable quantum efficiency

Defect centers in wide-band-gap crystals attracted considerable attention due to the realisations of qubits, sensors, or single photon emitters at room temperature. The family of these centers is constantly growing, including well-known examples such as nitrogen-vacancy centers in diamond, silicon-vacancy in silicon carbide, chromium substitutions in aluminium oxide, and many others. Unfortunately, such defect centers embedded in highly insulating crystals have been notoriously difficult to excite electrically. Herewith, we present a realisation of insulating light-emitting diodes based on carbon centers in hexagonal boron nitride. The rational design of the vertical tunnelling devices via van der Waals technology enabled us to control the charge dynamics related to non-radiative tunelling, defect-to-band electroluminescence, and intradefect electroluminescence. The fundamental understanding of the tunnelling events enabled us to achieve high efficiency of electrical excitation, which exceeded by a few orders of magnitude the efficiency of optical excitation in the sub-band-gap regime. A combination of a Stark effect and screening by band electrons provide a control knob for tuning the energy of emission. With this work, we solve an outstanding problem of creating electrically driven devices realised with defect centers in wide-band-gap crystals, which are relevant in the domain of optoelectronics, telecommunication, computation, or sensing.

cond-mat.mes-hall↗

arXiv2023

Excitonic luminescence of iodine-intercalated HfS$_2$

Photoluminescence from bulk HfS$_2$ grown by the chemical vapor transport method is reported. A series of emission lines is apparent at low temperature in the energy range of 1.4 - 1.5 eV. Two groups of the observed excitonic transitions followed by their replicas involving acoustic and optical phonons are distinguished using classical intensity correlation analysis. The emission is attributed to the recombination of excitons bound to iodine (I$_2$) molecules intercalated between layers of HfS$_2$. The I$_2$ molecules are introduced to the crystal during the growth as halogen transport agents in the growth process. Their presence in the crystal is confirmed by secondary ion mass spectroscopy.

cond-mat.mtrl-sci↗

arXiv2021

Carbon and vacancy centers in hexagonal boron nitride

Creation of defect with predetermined optical, chemical and other characteristics is a powerful tool to enhance the functionalities of materials. Herewith, we utilize density functional theory to understand the microscopic mechanisms of formation of defects in hexagonal boron nitride based on vacancies and substitutional atoms. Through in-depth analysis of the defect-induced band structure and formation energy in varying growth conditions, we uncovered a dominant role of interdefect electron paring in stabilization of defect complexes. The electron reorganization modifies the exchange component of the electronic interactions which dominates over direct Coulomb repulsion or structural relaxation effects making the combination of acceptor- and donor-type defect centers energetically favorable. Based on an analysis of a large number of defect complexes we develop a simple picture of the inheritance of electronic properties when individual defects are combined together to form more complex centers.

cond-mat.mtrl-sci↗

arXiv2021

ZnPSe$_3$ as ultrabright indirect bandgap system with microsecond excitonic lifetimes

We report an optical characterization of ZnPSe$_3$ crystals that demonstrates indirect band gap characteristics in combination with unusually strong photoluminescence. We found evidence of interband recombination from excitonic states with microsecond lifetimes. Through optical characterization, we reconstructed the electronic band scheme relevant for fundamental processes of light absorption, carrier relaxation and radiative recombination. The investigation of the radiative processes in the presence of magnetic field revealed spin polarization of fundamental electronic states. This observation opens a pathway towards controlling the spin of excitonic states in technologically relevant microsecond timescales.

cond-mat.mes-hall↗

arXiv2021

Pressure-driven phase transitions in bulk HfS$_2$

The effect of hydrostatic pressure up to 27 GPa on the Raman scattering (RS) in bulk HfS$_2$ is investigated. There are two transformations of RS spectra, which take place during compression at pressure between 5.7 GPa and 9.8 GPa as well as between 12.8 GPa and 15.2 GPa. Seven vibrational modes can be observed after the transformation, as compared to four modes before the transformation. The observed change suggests structural change in the material of yet unknown nature. The frequencies of the RS modes observed above the transformation change linearly with pressure and corresponding pressure coefficients have been determined. The other transition manifests itself as a change in the RS lineshape. While a series of well-defined RS modes are observed under pressure below the transition, broad spectral bands can be seen at higher pressure. The overall lineshape of the spectra resembles that of disordered materials. The lineshape does not change during decompression, which suggests permanent nature of the high-pressure transition.

cond-mat.mtrl-sci↗

arXiv2021

Magnon-polarons in van der Waals antiferromagnet FePS3

The hybridization of magnons (spin waves) with phonons, if sufficiently strong and comprising long wavelength excitations, may offer a new playground when manipulating the magnetically ordered systems with light. Applying a magnetic field to a quasi-2D antiferromagnet, FePS3, we tune the magnon-gap excitation towards coincidence with the initially lower-in-energy phonon modes. Hybrid magnon-phonon modes, the magnon polarons are unveiled with demonstration of a pronounced avoided crossing between the otherwise bare magnon and phonon excitations. The magnon polarons in FePS3 are primary traced with Raman scattering experiments, but, as we show, they also couple directly to terahertz photons, what evokes their further explorations in the domain of antiferromagnetic optospintronics.

cond-mat.mtrl-sci↗

arXiv2021

The optical response of artificially twisted MoS$_2$ bilayers

Two-dimensional layered materials offer the possibility to create artificial vertically stacked structures possessing an additional degree of freedom - $the$ $interlayer$ $twist$. We present a comprehensive optical study of artificially stacked bilayers (BLs) MoS$_2$ encapsulated in hexagonal BN with interlayer twist angle ranging from 0 to 60 degrees using Raman scattering and photoluminescence spectroscopies. It is found that the strength of the interlayer coupling in the studied BLs can be estimated using the energy dependence of indirect emission versus the A$_\textrm{1g}$-E$_\textrm{2g}^1$ energy separation. Due to the hybridization of electronic states in the valence band, the emission line related to the interlayer exciton is apparent in both the natural (2H) and artificial (62$^\circ$) MoS$_2$ BLs, while it is absent in the structures with other twist angles. The interlayer coupling energy is estimated to be of about 50 meV. The effect of temperature on energies and intensities of the direct and indirect emission lines in MoS$_2$ bilayers is also quantified.

cond-mat.mes-hall↗

arXiv2020

Excitonic complexes in $n$-doped WS$_2$ monolayer

We investigate the origin of emission lines apparent in the low-temperature photoluminescence spectra of $n$-doped WS$_2$ monolayer embedded in hexagonal BN layers using external magnetic fields and first-principles calculations. Apart from the neutral A exciton line, all observed emission lines are related to the negatively charged excitons. Consequently, we identify emissions due to both the bright (singlet and triplet) and dark (spin- and momentum-forbidden) negative trions as well as the phonon replicas of the latter optically-inactive complexes. The semi-dark trions and negative biexcitons are distinguished. Based on their experimentally extracted and theoretically calculated $g$-factors, we identify three distinct families of emissions due to exciton complexes in WS$_2$: bright, intravalley and intervalley dark. The $g$-factors of the spin-split subbands in both the conduction and valence bands are also determined.

cond-mat.mes-hall↗

arXiv2020

Resonance and antiresonance in Raman scattering in GaSe and InSe crystals

The temperature effect on the Raman scattering efficiency is investigated in $\varepsilon$-GaSe and $γ$-InSe crystals. We found that varying the temperature over a broad range from 5 K to 350 K permits to achieve both the resonant conditions and the antiresonance behaviour in Raman scattering of the studied materials. The resonant conditions of Raman scattering are observed at about 270 K under the 1.96 eV excitation for GaSe due to the energy proximity of the optical band gap. In the case of InSe, the resonant Raman spectra are apparent at about 50 K and 270 K under correspondingly the 2.41 eV and 2.54 eV excitations as a result of the energy proximity of the \mbox{so-called} B transition. Interestingly, the observed resonances for both materials are followed by an antiresonance behaviour noticeable at higher temperatures than the detected resonances. The significant variations of phonon-modes intensities can be explained in terms of electron-phonon coupling and quantum interference of contributions from different points of the Brillouin zone

cond-mat.mtrl-sci↗

arXiv2020

The optical signature of few-layer ReSe$_2$

Optical properties of thin layers of rhenium diselenide (ReSe$_2$) with thickness ranging from mono- (1 ML) to nona-layer (9 MLs) are demonstrated. The photoluminescence (PL) and Raman scattering were measured at low ($T$=5 K) and room ($T$=300 K) temperature, respectively. The PL spectra of ReSe$_2$ layers display two well-resolved emission lines, which blueshift by about 120 meV when the layer thickness decreases from 9 MLs to a monolayer. A rich structure of the observed low-energy Raman scattering modes can be explained within a linear chain model. The two phonon modes of intralayer vibrations, observed in Raman scattering spectra at about 120 cm$^{-1}$, exhibit very sensitive and opposite evolution as a function of layer thickness. It is shown that their energy difference can serve as a convenient and reliable tool to determine the thickness of ReSe$_2$ flakes in the few-layer limit.

cond-mat.mes-hall↗

arXiv2020

Neutral and charged dark excitons in monolayer WS$_2$

Low temperature and polarization resolved magneto-photoluminescence experiments are used to investigate the properties of dark excitons and dark trions in a monolayer of WS$_2$ encapsulated in hexagonal BN (hBN). We find that this system is an $n$-type doped semiconductor and that dark trions dominate the emission spectrum. In line with previous studies on WSe$_2$, we identify the Coulomb exchange interaction coupled neutral dark and grey excitons through their polarization properties, while an analogous effect is not observed for dark trions. Applying the magnetic field in both perpendicular and parallel configurations with respect to the monolayer plane, we determine the g-factor of dark trions to be $g\sim$-8.6. Their decay rate is close to 0.5 ns, more than 2 orders of magnitude longer than that of bright excitons.

cond-mat.mes-hall↗

arXiv2020

Valley polarization of singlet and triplet trions in WS$_2$ monolayer in magnetic fields

The spectral signatures associated with different negatively charged exciton complexes (trions) in a WS$_2$ monolayer encapsulated in hBN, are analyzed from low temperature and polarization resolved reflectance contrast (RC) and photoluminescence (PL) experiments, with an applied magnetic field. Based on results obtained from the RC experiment, we show that the valley Zeeman effect affects the optical response of both the singlet and the triplet trion species through the evolution of their energy and of their relative intensity, when applying an external magnetic field. Our analysis allows us to estimate a free electron concentration of $\sim 1.3 \cdot 10^{11}$ cm$^{-2}$. The observed evolutions based on PL experiments on the same sample are different and can hardly be understood within the same simple frame highlighting the complexity of relaxation processes involved in the PL response.

cond-mat.mes-hall↗

arXiv2020

Breathing modes in few-layer MoTe$_2$ activated by h-BN encapsulation

The encapsulation of few-layer transition metal dichalcogenides (TMDs) in hexagonal boron nitride (h-BN) is known to improve significantly their optical and electronic properties. However, it may be expected that the h-BN encapsulation may affect also vibration properties of TMDs due to an atomically flat surface of h-BN layers. In order to study its effect on interlayer interactions in few-layer TMDs, we investigate low-energy Raman scattering spectra of bi- and trilayer MoTe$_2$. Surprisingly, three breathing modes are observed in the Raman spectra of the structures deposited on or encapsulated in h-BN as compared to a single breathing mode for the flakes deposited on a SiO$_2$/Si substrate. The shear mode is not affected by changing the MoTe$_2$ environment. The emerged structure of breathing modes is ascribed to the apparent interaction between the MoTe$_2$ layer and the bottom h-BN flake. The structure becomes visible due to a high-quality surface of the former flake. Consequently, the observed triple structure of breathing modes originates from the combination modes due to interlayer and layer-substrate interactions. Our results confirm that the h-BN encapsulation affects substantially vibration properties of layered materials.

cond-mat.mes-hall↗

arXiv2019

The effect of metallic substrates on the optical properties of monolayer MoSe$_{2}$

Atomically thin materials, like semiconducting transition metal dichalcogenides (S-TMDs), are highly sensitive to the environment. This opens up an opportunity to externally control their properties by changing their surroundings. We investigate the effect of several metallic substrates on the optical properties of MoSe$_2$ monolayer (ML) deposited on top of them with photoluminescence and reflectance contrast techniques. The optical spectra of MoSe$_{2}$ MLs deposited on Pt, Au, Mo and Zr have distinctive metal-related lineshapes. In particular, a substantial variation in the intensity ratio and the energy separation between a negative trion and a neutral exciton is observed. It is shown that using metals as substrates affects the doping of S-TMD MLs. The explanation of the effect involves the Schottky barrier formation at the interface between the MoSe$_{2}$ ML and the metallic substrates. The alignment of energy levels at the metal/semiconductor junction allows for the transfer of charge carriers between them. We argue that a proper selection of metallic substrates can be a way to inject appropriate types of carriers into the respective bands of S-TMDs.

cond-mat.mes-hall↗

arXiv2019

Exciton-polaritons in multilayer WSe$_2$ in a planar microcavity

Due to high binding energy and oscillator strength, excitons in thin flakes of transition metal dichalcogenides constitute a perfect foundation for realizing a strongly coupled light-matter system. In this paper we investigate mono- and few-layer WSe$_2$ flakes encapsulated in hexagonal boron nitride and incorporated into a planar dielectric cavity. We use an open cavity design which provides tunability of the cavity mode energy by as much as 150 meV. We observe a strong coupling regime between the cavity photons and the neutral excitons in direct-bandgap monolayer WSe$_2$, as well as in few-layer WSe$_2$ flakes exhibiting indirect bandgap. We discuss the dependence of the exciton's oscillator strength and resonance linewidth on the number of layers and predict the exciton-photon coupling strength.

cond-mat.mes-hall↗