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M. Potemski

Publications and source records attributed to M. Potemski.

At least 37 records · Page 2Linked to original sources

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↗

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.

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Flipping exciton angular momentum with chiral phonons in MoSe$_2$/WSe$_2$ heterobilayers

Identifying quantum numbers to label elementary excitations is essential for the correct description of light-matter interaction in solids. In monolayer semiconducting transition metal dichalcogenides (TMDs) such as MoSe$_2$ or WSe$_2$, most optoelectronic phenomena are described well by labelling electron and hole states with the spin projection along the normal to the layer (S$_z$). In contrast, for WSe$_2$/MoSe$_2$ interfaces recent experiments show that taking S$_z$ as quantum number is not a good approximation, and spin mixing needs to be always considered. Here we argue that the correct quantum number for these systems is not S$_z$, but the $z$-component of the total angular momentum -- J$_z$ = L$_z$ + S$_z$ -- associated to the C$_3$ rotational lattice symmetry, which assumes half-integer values corresponding modulo 3 to distinct states. We validate this conclusion experimentally through the observation of strong intervalley scattering mediated by chiral optical phonons that -- despite carrying angular momentum 1 -- cause resonant intervalley transitions of excitons, with an angular momentum difference of 2.

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Measurement of the Spin-Forbidden Dark Excitons in MoS2 and MoSe2 monolayers

Excitons with binding energies of a few hundreds of meV control the optical properties of transition metal dichalcogenide monolayers. Knowledge of the fine structure of these excitons is therefore essential to understand the optoelectronic properties of these 2D materials. Here we measure the exciton fine structure of MoS2 and MoSe2 monolayers encapsulated in boron nitride by magneto-photoluminescence spectroscopy in magnetic fields up to 30 T. The experiments performed in transverse magnetic field reveal a brightening of the spin-forbidden dark excitons in MoS2 monolayer: we find that the dark excitons appear at 14 meV below the bright ones. Measurements performed in tilted magnetic field provide a conceivable description of the neutral exciton fine structure. The experimental results are in agreement with a model taking into account the effect of the exchange interaction on both the bright and dark exciton states as well as the interaction with the magnetic field.

cond-mat.mtrl-sci↗

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.

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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.

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Energy spectrum of two-dimensional excitons in a non-uniform dielectric medium

We demonstrate that, in monolayers (MLs) of semiconducting transition metal dichalcogenides, the $s$-type Rydberg series of excitonic states follows a simple energy ladder: $ε_n=-Ry^*/(n+δ)^2$, $n$=1,2,\ldots, in which $Ry^*$ is very close to the Rydberg energy scaled by the dielectric constant of the medium surrounding the ML and by the reduced effective electron-hole mass, whereas the ML polarizability is only accounted for by $δ$. This is justified by the analysis of experimental data on excitonic resonances, as extracted from magneto-optical measurements of a high-quality WSe$_2$ ML encapsulated in hexagonal boron nitride (hBN), and well reproduced with an analytically solvable Schrödinger equation when approximating the electron-hole potential in the form of a modified Kratzer potential. Applying our convention to other, MoSe$_2$, WS$_2$, MoS$_2$ MLs encapsulated in hBN, we estimate an apparent magnitude of $δ$ for each of the studied structures. Intriguingly, $δ$ is found to be close to zero for WSe$_2$ as well as for MoS$_2$ monolayers, what implies that the energy ladder of excitonic states in these two-dimensional structures resembles that of Rydberg states of a three-dimensional hydrogen atom.

cond-mat.mes-hall↗

Probing and manipulating valley coherence of dark excitons in monolayer WSe$_2$

Monolayers of semiconducting transition metal dichalcogenides are two-dimensional direct-gap systems which host tightly-bound excitons with an internal degree of freedom corresponding to the valley of the constituting carriers. Strong spin-orbit interaction and the resulting ordering of the spin-split subbands in the valence and conduction bands makes the lowest-lying excitons in WX$_2$ (X~being S or Se) spin-forbidden and optically dark. With polarization-resolved photoluminescence experiments performed on a WSe$_2$ monolayer encapsulated in a hexagonal boron nitride, we show how the intrinsic exchange interaction in combination with the applied in-plane and/or out-of-plane magnetic fields enables one to probe and manipulate the valley degree of freedom of the dark excitons.

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Upconverted electroluminescence via Auger scattering of interlayer excitons in van der Waals heterostructures

The intriguing physics of carrier-carrier interactions, which likewise affect the operation of light emitting devices, stimulate the research on semiconductor structures at high densities of excited carriers, a limit reachable at large pumping rates or in systems with long-lived electron-hole pairs. By electrically injecting carriers into WSe$_2$/MoS$_2$ type-II heterostructures which are indirect in real and k-space, we establish a large population of typical optically silent interlayer excitons. Here, we reveal their emission spectra and show that the emission energy is tunable by an applied electric field. When the population is further increased by suppressing the radiative recombination rate with the introduction of an hBN spacer between WSe$_2$ and MoS$_2$, Auger-type and exciton-exciton annihilation processes become important. These processes are traced by the observation of an up-converted emission demonstrating that excitons gaining energy in non-radiative Auger processes can be recovered and recombine radiatively.

cond-mat.mes-hall↗

Dimensional crossover of acoustic phonon lifetime in $2H$-MoSe$_2$

A time-resolved observation of coherent interlayer longitudinal acoustic phonons in 2$H$-MoSe$_2$ is reported. A femtosecond pump-probe technique is used to investigate the evolution of the energy loss of these vibrational modes in a wide selection of MoSe$_2$ flakes with different thicknesses ranging from bilayer up to the bulk limit. By directly analysing the temporal decay of the modes, we can clearly distinguish an abrupt crossover related to the acoustic mean free path of the phonons in a layered system, and the constraints imposed to the acoustic decay channels when reducing the dimensionality. Loses intrinsic to the low dimensionality of single or few layer materials impose critical limitations for their use in optomechanical and optoelectronic devices.

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Fine structure of $\mathrm{K}$-excitons in multilayers of transition metal dichalcogenides

Reflectance and magneto-reflectance experiments together with theoretical modelling based on the $\mathbf{k\cdot p}$ approach have been employed to study the evolution of direct bandgap excitons in MoS$_2$ layers with a thickness ranging from mono- to trilayer. The extra excitonic resonances observed in MoS$_2$ multilayers emerge as a result of the hybridization of Bloch states of each sub-layer due to the interlayer coupling. The properties of such excitons in bi- and trilayers are classified by the symmetry of corresponding crystals. The inter- and intralayer character of the reported excitonic resonances is fingerprinted with the magneto-optical measurements: the excitonic $g$-factors of opposite sign and of different amplitude are revealed for these two types of resonances. The parameters describing the strength of the spin-orbit interaction are estimated for bi- and trilayer MoS$_2$.

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Valley polarization of exciton-polaritons in monolayer WSe2 in a tunable microcavity

Monolayer transition metal dichalcogenides, known for exhibiting strong excitonic resonances, constitute a very interesting and versatile platform for investigation of light-matter interactions. In this work we report on a strong coupling regime between excitons in monolayer WSe2 and photons confined in an open, voltage-tunable dielectric microcavity. The tunability of our system allows us to extend the exciton-polariton state over a wide energy range and, in particular, to bring the excitonic component of the lower polariton mode into resonance with other excitonic transitions in monolayer WSe2. With selective excitation of spin-polarized exciton-polaritons we demonstrate the valley polarization when the polaritons from the lower branch come into resonance with a bright trion state in monolayer WSe2 and valley depolarization when they are in resonance with a dark trion state.

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Raman scattering from the bulk inactive out-of-plane B$^{1}_{2\text{g}}$ mode in few-layer MoTe$_{2}$

Raman scattering from the out-of-plane vibrational modes (A$_{1\text{g}}$/A'$_{1}$), which originate from the bulk-inactive out-of-plane B$^{1}_{2\text{g}}$ mode, are studied in few-layer MoTe$_{2}$. Temperature-dependent measurements reveal a doublet structure of the corresponding peaks in the Raman scattering spectra of tetralayer and pentalayer samples. A strong enhancement of their lower energy components is recorded at low temperature for 1.91 eV and 1.96 eV laser excitation. We discuss the attribution of the peaks to the inner modes of the respective Raman-active vibrations. The temperature evolution of their intensity strongly suggests a resonant character of the employed excitation, which leads to the mode enhancement at low temperature. The resonance of the laser light with the singularity of the electronic density of states at the $M$ point of the Brillouin zone in MoTe$_{2}$ is proposed to be responsible for the observed effects.

cond-mat.mtrl-sci↗

Singlet and triplet trions in WS$_2$ monolayer encapsulated in hexagonal boron nitride

Embedding a WS$_2$ monolayer in flakes of hexagonal boron nitride allowed us to resolve and study the photoluminescence response due to both singlet and triplet states of negatively charged excitons (trions) in this atomically thin semiconductor. The energy separation between the singlet and triplet states has been found to be relatively small reflecting rather weak effects of the electron-electron exchange interaction for the trion triplet in a WS$_2$ monolayer, which involves two electrons with the same spin but from different valleys. Polarization-resolved experiments demonstrate that the helicity of the excitation light is better preserved in the emission spectrum of the triplet trion than in that of the singlet trion. Finally, the singlet (intravalley) trions are found to be observable even at ambient conditions whereas the emission due to the triplet (intervalley) trions is only efficient at low temperatures.

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Landau level spectroscopy of valence bands in HgTe quantum wells: Effects of symmetry lowering

Landau level spectroscopy has been employed to probe the electronic structure of the valence band in a series of p-type HgTe/HgCdTe quantum wells with both normal and inverted ordering of bands. We find that the standard axial-symmetric 4-band Kane model, which is nowadays widely applied in physics of HgTe-based topological materials, does not fully account for the complex magneto-optical response observed in our experiments - notably, for the unexpected avoided crossings of excitations and for the appearance of transitions that are electric-dipole forbidden within this model. Nevertheless, reasonable agreement with experiments is achieved when the standard model is expanded to include effects of bulk and interface inversion asymmetries. These remove the axial symmetry, and among other, profoundly modify the shape of valence bands.

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The energy scale of Dirac electrons in Cd3As2

Cadmium arsenide (Cd3As2) has recently became conspicuous in solid-state physics due to several reports proposing that it hosts a pair of symmetry-protected 3D Dirac cones. Despite vast investigations, a solid experimental insight into the band structure of this material is still missing. Here we fill one of the existing gaps in our understanding of Cd3As2, and based on our Landau level spectroscopy study, we provide an estimate for the energy scale of 3D Dirac electrons in this system. We find that the appearance of such charge carriers is limited - contrary to a widespread belief in the solid-state community - to a relatively small energy scale (below 40 meV).

cond-mat.mes-hall↗

Orbital, spin and valley contributions to Zeeman splitting of excitonic resonances in MoSe$_2$, WSe$_2$ and WS$_2$ monolayers

We present a comprehensive optical study of the excitonic Zeeman effects in transition metal dichalcogenide monolayers, which are discussed comparatively for selected materials: MoSe$_2$, WSe$_2$ and WS$_2$. We introduce a simple semi-phenomenological description of the magnetic field evolution of individual electronic states in fundamental sub-bands by considering three additive components: valley, spin and orbital terms. We corroborate the validity of the proposed description by inspecting the Zeeman-like splitting of neutral and charged excitonic resonances in absorption-type spectra. The values of all three terms are estimated based on the experimental data, demonstrating the significance of the valley term for a consistent description of magnetic field evolution of optical resonances, particularly those corresponding to charged states. The established model is further exploited for discussion of magneto-luminescence data. We propose an interpretation of the observed large g-factor values of low energy emission lines, due to so-called bound/localized excitons in tungsten based compounds, based on the brightening mechanisms of dark excitonic states.

cond-mat.mes-hall↗

Impact of environment on dynamics of exciton complexes in a WS$_2$ monolayer

Scientific curiosity to uncover original optical properties and functionalities of atomically thin semiconductors, stemming from unusual Coulomb interactions in the two-dimensional geometry and multi-valley band structure, drives the research on monolayers of transition metal dichalcogenides (TMDs). While recent works ascertained the exotic energetic schemes of exciton complexes in TMDs, we here employ four-wave mixing microscopy to indicate that their subpicosecond dynamics is determined by the surrounding disorder. Focusing on a monolayer WS$_2$, we observe that exciton coherence is lost primarily due to interaction with phonons and relaxation processes towards optically dark excitonic states. Notably, when temperature is low and disorder weak excitons large coherence volume results in huge oscillator strength, allowing to reach the regime of radiatively limited dephasing and we observe long valley coherence. We thus elucidate the crucial role of exciton environment in the TMDs on its dynamics and show that revealed mechanisms are ubiquitous within that family.

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