arXiv subjects

M. R. Molas

Publications and source records attributed to M. R. Molas.

At least 37 records · Page 2Linked to original sources

arXiv2019

Magneto-spectroscopy of exciton Rydberg states in a CVD grown WSe2 monolayer

The results of magneto-optical spectroscopy investigations of excitons in a CVD grown monolayer of WSe2 encapsulated in hexagonal boron nitride are presented. The emission linewidth for the 1s state is of 4:7 meV, close to the narrowest emissions observed in monolayers exfoliated from bulk material. The 2s excitonic state is also observed at higher energies in the photoluminescence spectrum. Magneto-optical spectroscopy allows for the determination of the g-factors and of the spatial extent of the excitonic wave functions associated with these emissions. Our work establishes CVD grown monolayers of transition metal dichalcogenides as a mature technology for optoelectronic applications.

cond-mat.mes-hall↗

arXiv2019

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↗

arXiv2018

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$_2$.

cond-mat.mes-hall↗

arXiv2018

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.

cond-mat.mes-hall↗

arXiv2018

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↗

arXiv2018

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.

cond-mat.mes-hall↗

arXiv2018

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↗

arXiv2017

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.

cond-mat.mes-hall↗

arXiv2017

2s exciton-polariton revealed in an external magnetic field

We demonstrate the existence of the excited state of an exciton-polariton in a semiconductor microcavity. The strong coupling of the quantum well heavy-hole exciton in an excited 2s state to the cavity photon is observed in non-zero magnetic field due to surprisingly fast increase of Rabi energy of the 2s exciton-polariton in magnetic field. This effect is explained by a strong modification of the wave-function of the relative electron-hole motion for the 2s exciton state.

cond-mat.quant-gas↗

arXiv2017

Sub-bandgap voltage electroluminescence and magneto-oscillations in a WSe2 light-emitting van der Waals heterostructure

We report on experimental investigations of an electrically driven WSe2 based light-emitting van der Waals heterostructure. We observe a threshold voltage for electroluminescence significantly lower than the corresponding single particle band gap of monolayer WSe2. This observation can be interpreted by considering the Coulomb interaction and a tunneling process involving excitons, well beyond the picture of independent charge carriers. An applied magnetic field reveals pronounced magneto-oscillations in the electroluminescence of the free exciton emission intensity with a 1/B-periodicity. This effect is ascribed to a modulation of the tunneling probability resulting from the Landau quantization in the graphene electrodes. A sharp feature in the differential conductance indicates that the Fermi level is pinned and allows for an estimation of the acceptor binding energy.

cond-mat.mes-hall↗

arXiv2016

Optical properties of atomically thin transition metal dichalcogenides: Observations and puzzles

Recent results on the optical properties of mono- and few-layers of semiconducting transition metal dichalcogenides are reviewed. Experimental observations are presented and discussed in the frame of existing models, highlighting the limits of our understanding in this emerging field of research. We first introduce the representative band structure of these systems and their interband optical transitions. The effect of an external magnetic field is then considered to discuss Zeeman spectroscopy and optical pumping experiments, both revealing phenomena related to the valley degree of freedom. Finally, we discuss the observation of single photon emitters in different types of layered materials, including wide band gap hexagonal boron nitride. While going through these topics, we try to focus on open questions and on experimental observations, which do not yet have a clear explanation.

cond-mat.mes-hall↗

arXiv2016

Brightening of dark excitons in monolayers of semiconducting transition metal dichalcogenides

We present low temperature magneto-photoluminescence experiments which demonstrate the brightening of dark excitons by an in-plane magnetic field $B$ applied to monolayers of different semiconducting transition metal dichalcogenides. For both WSe$_2$ and WS$_2$ monolayers, the dark exciton emission is observed at $\sim$50 meV below the bright exciton peak and displays a characteristic doublet structure which intensity is growing with $B^2$, while no magnetic field induced emission peaks appear for MoSe$_2$ monolayer. Our experiments also show that the MoS$_2$ monolayer has a dark exciton ground state with a dark-bright exciton splitting energy of $\sim$100 meV.

cond-mat.mes-hall↗

arXiv2016

Resonant quenching of Raman scattering due to out-of-plane A$_{1g}$/A'$_1$ modes in few-layer MoTe$_2$

Temperature-dependent (5 K to 300 K) Raman scattering study of A$_{1g}$/A'$_1$ phonon modes in mono-layer (1L), bilayer (2L), trilayer (3L), and tetralayer (4L) MoTe$_2$ is reported. The temperature evolution of the modes' intensity critically depends on the flake thickness. In particular with $λ$=632.8 nm light excitation, a strongly non-monotonic dependence of the A$_{1g}$ mode intensity is observed in 2L MoTe$_2$. The intensity decreases with decreasing temperature down to 220 K and the A$_{1g}$ mode almost completely vanishes from the Stokes scattering spectrum in the temperature range between 160 K and 220 K. The peak recovers at lower temperatures and at T=5 K it becomes three times more intense that at room temperature. Similar non-monotonic intensity evolution is observed for the out-of-plane mode in 3L MoTe$_2$ in which tellurium atoms in all three layers vibrate in-phase. The intensity of the other out-of-plane Raman-active mode, (with vibrations of tellurium atoms in the central layer shifted by 180$^o$ with respect to the vibrations in outer layers), only weakly depends on temperature. The observed quenching of the Raman scattering in 2L and 3L MoTe$_2$ is attributed to a destructive interference between the resonant and non-resonant contributions to the Raman scattering amplitude. The observed "antiresonance" is related to the electronic excitation at the M point of the Brillouin zone in few-layer MoTe$_2$.

cond-mat.mes-hall↗

arXiv2016

Raman scattering in few-layer MoTe$_{2}$

We report on room-temperature Raman scattering measurements in few-layer crystals of exfoliated molybdenum ditelluride (MoTe$_{2}$) performed with the use of 632.8 nm (1.96 eV) laser light excitation. In agreement with recent study reported by G. Froehlicher et al, (2015 $Nano$ $Lett.$ 15 6481) we observe a complex structure of the out-of-plane vibrational modes (A$_{1g}$/A$^{'}_{1}$), which can be explained in terms of interlayer interactions between single atomic planes of MoTe$_{2}$. In the case of low-energy shear and breathing modes of rigid interlayer vibrations it is shown that their energy evolution with the number of layers can be well reproduced within a linear chain model with only the nearest neighbor interaction taken into account. Based on this model the corresponding in-plane and out-of-plane force constants are determined. We also show that the Raman scattering in MoTe$_{2}$ measured using 514.5 nm (2.41 eV) laser light excitation results in much simpler spectra. We argue that the rich structure of the out-of-plane vibrational modes observed in Raman scattering spectra excited with the use of 632.8 nm laser light results from its resonance with the electronic transition at the M or K points of the MoTe$_{2}$ first Brillouin zone.

cond-mat.mtrl-sci↗

arXiv2016

Experimental approval of the extended flat bands and gapped subbands in rhombohedral multilayer graphene

Graphene layers are known to stack in two stable configurations, namely ABA or ABC stacking, with drastically distinct electronic properties. Unlike the ABA stacking, little has been done to experimentally investigate the electronic properties of ABC graphene multilayers. Here, we report the first magneto optical study of a large ABC domain in a graphene multilayers flake, with ABC sequences exceeding 17 graphene sheets. The ABC-stacked multilayers can be fingerprinted with a characteristic electronic Raman scattering response, which persists even at room temperatures. Tracing the magnetic field evolution of the inter Landau level excitations from this domain gives strong evidence to the existence of a dispersionless electronic band near the Fermi level, characteristic of such stacking. Our findings present a simple yet powerful approach to probe ABC stacking in graphene multilayer flakes, where this highly degenerated band appears as an appealing candidate to host strongly correlated states.

cond-mat.mes-hall↗

arXiv2016

Energy spectrum of confined positively charged excitons in single quantum dots

A theoretical model, which relates the binding energy of a positively charged exciton in a quantum dot with the confinement energy is presented. It is shown that the binding energy, defined as the energy difference between the corresponding charged and neutral complexes confined on the same excitonic shell strongly depends on the shell index. Moreover, it is shown that the ratio of the binding energy for positively charged excitons from the $p$- and $s$-shells of a dot depends mainly on the nearly perfect confinement in the dot, which is due to the "hidden symmetry" of the multi-electron-hole system. We applied the theory to the excitons confined to a single GaAlAs/AlAs quantum dots. The relevant binding energy was determined using the micro-photoluminescence and micro-photoluminescence excitation magneto-spectroscopy. We show that within our theory, the confinement energy determined using the ratio of the binding energy corresponds well to the actual confinement energy of the investigated dot.

cond-mat.mes-hall↗

arXiv2016

The excited spin-triplet state of a charged exciton in quantum dots

We report on single-object spectroscopic studies of a characteristic set of three resonances which appear in GaAlAs/AlAs quantum dot structures. The experiments included the photoluminescence (PL) and photoluminescence excitation (PLE) spectroscopy, photon-correlation measurements, analysis of the linear polarization of the emission spectra as well as the PL and PLE spectroscopy performed as a function of magnetic field. The investigated resonances are assigned to three different states of a positively charged exciton: a singlet ground state, a conventional triplet state (involving an electron from the ground state electronic $s$-shell), and additionally, a highly excited triplet state (involving the electron from the excited electronic $p$-shell). Advantageously (due to partially suppressed relaxation efficiency), the emission due to the highly excited triplet can seen in the spectra which allows us to scrupulously determine its properties and compare them to those of the conventional triplet state. Whereas both triplet states show similar patterns of the fine structure and Zeeman splitting, the splitting amplitudes are found to be significantly different for these two states. The presented results emphasize the role of the symmetry of the electronic state on the properties of the triplet states of the two holes + electron excitonic complex.

cond-mat.mes-hall↗

arXiv2015

Quadexciton cascade and fine structure splitting of the triexciton in a single quantum dot

We report the properties of emission lines associated with the cascaded recombination of a quadexciton in single GaAlAs/AlAs quantum dots, studied by means of polarization-resolved photoluminescence and single-photon correlation experiments. It is found that photons which are emitted in a double-step 4X-3X process preserve their linear polarization, similarly to the case of conserved polarization of correlated photons in the 2X-X cascade. In contrast, an emission of either co-linear or cross-linear pairs of photons is observed for the 3X-2X cascade. Each emission line associated with the quadexciton cascade shows doublet structure in the polarization-resolved photoluminescence experiment. The maximum splitting is seen when the polarization axis is chosen along and perpendicular to the [110] crystallographic direction. This effect is ascribed to the fine structure splitting of the exciton and triexciton states in the presence of an anisotropic confining potential of ae dot. We also show that the splitting in the triexciton state surpasses that in the exciton state by a factor up to eight and their ratio scales with the energy distance between the 3X and X emission lines, thus, very likely, with a lateral size and/or a composition of the dot.

cond-mat.mes-hall↗