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B. Urbaszek

Publications and source records attributed to B. Urbaszek.

At least 19 recordsLinked to original sources

2D Excitonics with Atomically Thin Lateral Heterostructures

Semiconducting transition metal dichalcogenides (TMDs), such as MoSe$_2$ and WSe$_2$, exhibit unique optical and electronic properties. Vertical stacking of layers of one or more TMDs, to create heterostructures, has expanded the fields of moir\'e physics and twistronics. Bottom-up fabrication techniques, such as chemical vapor deposition, have advanced the creation of heterostructures beyond what was possible with mechanical exfoliation and stacking. These techniques now enable the fabrication of lateral heterostructures, where two or more monolayers are covalently bonded in the plane of their atoms. At their atomically sharp interfaces, lateral heterostructures exhibit additional phenomena, such as the formation of charge-transfer excitons, in which the electron and hole reside on opposite sides of the interface. Due to the energy landscape created by differences in the band structures of the constituent materials, unique effects such as unidirectional exciton transport and excitonic lensing can be observed in lateral heterostructures. This review outlines recent progress in exciton dynamics and spectroscopy of TMD-based lateral heterostructures and offers an outlook on future developments in excitonics in this promising system.

cond-mat.mtrl-sci

Electrostatic modulation of excitonic fluid in GaN/AlGaN quantum wells by deposition of few-layered graphene and nickel/gold films

Excitons hosted by GaN/(Al,Ga)N quantum wells (QWs) are spatially indirect due to the giant built-in electric field that separates electrons and holes along the growth direction. This electric field, and thus exciton energy, can be reduced by depositing metallic layers on the sample surface. Using spatially-resolved micro-photoluminescence spectroscopy we compare the effects of two different materials, Nickel/Gold (NiAu) and few-layered graphene (FLG), on the potential landscape experienced by the excitons. We are able to (i) determine the potential barriers imposed on QW excitons by deposition of FLG and NiAu to be $14$ and $82$~meV, respectively, and (ii) to evidence their impact on the exciton transport at appropriate densities. Optical losses and inhomogeneous broadening induced by deposition of NiAu and FLG layers are similar, and their joined implementation constitute a promising tool for electrostatic modulation of IX densities even in the absence of any applied electric bias.

cond-mat.quant-gas

Non-linear diffusion of negatively charged excitons in WSe2 monolayer

We investigate the diffusion process of negatively charged excitons (trions) in WSe2 transition metal dichalcogenide monolayer. We measure time-resolved photoluminescence spatial profiles of these excitonic complexes which exhibit a non-linear diffusion process with an effective negative diffusion behavior. Specifically, we examine the dynamics of the two negatively charged bright excitons (intervalley and intravalley trion) as well as the dark trion. The time evolution allows us to identify the interplay of different excitonic species: the trionic species appear after the neutral excitonic ones, consistent with a bimolecular formation mechanism. Using the experimental observations, we propose a phenomenological model suggesting the coexistence of two populations: a first one exhibiting a fast and efficient diffusion mechanism and a second one with a slower dynamics and a less efficient diffusion process. These two contributions could be attributed to hot and cold trion populations.

cond-mat.mtrl-sci

Spin dependent charge transfer in MoSe2/hBN/Ni hybrid structures

We present magneto-photoluminescence measurements in a hybrid 2D semiconductor/ferromagnetic structure consisting of MoSe2/hBN/Ni. When the Nickel layer is magnetized, we observe circularly polarized photoluminescence of the trion peak in MoSe2 monolayer under linearly polarized excitation. This build-up of circular polarization can reach a measured value of about 4% when the magnetization of Ni is saturated perpendicularly to the sample plane, and changes its sign when the magnetization is reversed. The circular polarization decreases when the hBN barrier thickness increases. These results are interpreted in terms of a spin-dependent charge transfer between the MoSe2 monolayer and the Nickel film. The build-up of circular polarization is observed up to 120 K, mainly limited by the trion emission that vanishes with temperature.

cond-mat.mtrl-sci

Control of the exciton valley dynamics in van der Waals heterostructures

The exciton valley dynamics in van der Waals heterostructures with transition metal dichalcogenides monolayers is driven by the long-range exchange interaction between the electron and the hole in the exciton. It couples the states active in the opposite circular polarizations resulting in the longitudinal-transverse splitting of excitons propagating in the monolayer plane. Here we study theoretically the effect of the dielectric environment on the long-range exchange interaction and demonstrate how the encapsulation in the hexagonal boron nitride modifies the exciton longitudinal-transverse splitting. We calculate the exciton spin/valley polarization relaxation due to the long-range exchange interaction and demonstrate that the variation of the monolayer environment results in significant, up to five-fold, enhancement of the exciton valley polarization lifetime.

cond-mat.mes-hall

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

Revealing exciton masses and dielectric properties of monolayer semiconductors with high magnetic fields

In semiconductor physics, many essential optoelectronic material parameters can be experimentally revealed via optical spectroscopy in sufficiently large magnetic fields. For monolayer transition-metal dichalcogenide semiconductors, this field scale is substantial --tens of teslas or more-- due to heavy carrier masses and huge exciton binding energies. Here we report absorption spectroscopy of monolayer MoS$_2$, MoSe$_2$, MoTe$_2$, and WS$_2$ in very high magnetic fields to 91~T. We follow the diamagnetic shifts and valley Zeeman splittings of not only the exciton's $1s$ ground state but also its excited $2s$, $3s$, ..., $ns$ Rydberg states. This provides a direct experimental measure of the effective (reduced) exciton masses and dielectric properties. Exciton binding energies, exciton radii, and free-particle bandgaps are also determined. The measured exciton masses are heavier than theoretically predicted, especially for Mo-based monolayers. These results provide essential and quantitative parameters for the rational design of opto-electronic van der Waals heterostructures incorporating 2D semiconductors.

cond-mat.mes-hall

Control of the Exciton Radiative Lifetime in van der Waals Heterostructures

Optical properties of atomically thin transition metal dichalcogenides are controlled by robust excitons characterized by a very large oscillator strength. Encapsulation of monolayers such as MoSe$_2$ in hexagonal boron nitride (hBN) yields narrow optical transitions approaching the homogenous exciton linewidth. We demonstrate that the exciton radiative rate in these van der Waals heterostructures can be tailored by a simple change of the hBN encapsulation layer thickness as a consequence of the Purcell effect. The time-resolved photoluminescence measurements together with cw reflectivity and photoluminescence experiments show that the neutral exciton spontaneous emission time can be tuned by one order of magnitude depending on the thickness of the surrounding hBN layers. The inhibition of the radiative recombination can yield spontaneous emission time up to $10$~ps. These results are in very good agreement with the calculated recombination rate in the weak exciton-photon coupling regime. The analysis shows that we are also able to observe a sizeable enhancement of the exciton radiative decay rate. Understanding the role of these electrodynamical effects allow us to elucidate the complex dynamics of relaxation and recombination for both neutral and charged excitons.

cond-mat.mes-hall

Intervalley Polaron in Atomically Thin Transition Metal Dichalcogenides

We study theoretically intervalley coupling in transition-metal dichalcogenide monolayers due to electron interaction with short-wavelength phonons. We demonstrate that this intervalley polaron coupling results in (i) a renormalization of the conduction band spin splitting and (ii) an increase of the electron effective masses. We also calculate the renormalization of the cyclotron energy and the Landau level splitting in the presence of an external magnetic field. An inter-valley magneto-phonon resonance is uncovered. Similar, but much weaker effects are also expected for the valence band holes. These results might help to resolve the discrepancy between ab initio values of the electron effective masses and the ones deduced from magneto-transport measurements.

cond-mat.mes-hall

Exciton states in monolayer MoSe2 and MoTe2 probed by upconversion spectroscopy

Transitions metal dichalcogenides (TMDs) are direct semiconductors in the atomic monolayer (ML) limit with fascinating optical and spin-valley properties. The strong optical absorption of up to 20 % for a single ML is governed by excitons, electron-hole pairs bound by Coulomb attraction. Excited exciton states in MoSe$_2$ and MoTe$_2$ monolayers have so far been elusive due to their low oscillator strength and strong inhomogeneous broadening. Here we show that encapsulation in hexagonal boron nitride results in emission line width of the A:1$s$ exciton below 1.5 meV and 3 meV in our MoSe$_2$ and MoTe$_2$ monolayer samples, respectively. This allows us to investigate the excited exciton states by photoluminescence upconversion spectroscopy for both monolayer materials. The excitation laser is tuned into resonance with the A:1$s$ transition and we observe emission of excited exciton states up to 200 meV above the laser energy. We demonstrate bias control of the efficiency of this non-linear optical process. At the origin of upconversion our model calculations suggest an exciton-exciton (Auger) scattering mechanism specific to TMD MLs involving an excited conduction band thus generating high energy excitons with small wave-vectors. The optical transitions are further investigated by white light reflectivity, photoluminescence excitation and resonant Raman scattering confirming their origin as excited excitonic states in monolayer thin semiconductors.

cond-mat.mes-hall

Charged excitons in monolayer WSe$_2$: experiment and theory

Charged excitons, or X$^{\pm}$-trions, in monolayer transition metal dichalcogenides have binding energies of several tens of meV. Together with the neutral exciton X$^0$ they dominate the emission spectrum at low and elevated temperatures. We use charge tunable devices based on WSe$_2$ monolayers encapsulated in hexagonal boron nitride, to investigate the difference in binding energy between X$^+$ and X$^-$ and the X$^-$ fine structure. We find in the charge neutral regime, the X$^0$ emission accompanied at lower energy by a strong peak close to the longitudinal optical (LO) phonon energy. This peak is absent in reflectivity measurements, where only the X$^0$ and an excited state of the X$^0$ are visible. In the $n$-doped regime, we find a closer correspondence between emission and reflectivity as the trion transition with a well-resolved fine-structure splitting of 6~meV for X$^-$ is observed. We present a symmetry analysis of the different X$^+$ and X$^-$ trion states and results of the binding energy calculations. We compare the trion binding energy for the $n$-and $p$-doped regimes with our model calculations for low carrier concentrations. We demonstrate that the splitting between the X$^+$ and X$^-$ trions as well as the fine structure of the X$^-$ state can be related to the short-range Coulomb exchange interaction between the charge carriers.

cond-mat.mes-hall

Spectrally narrow exciton luminescence from monolayer MoS2 exfoliated onto epitaxially grown hexagonal BN

The strong light-matter interaction in transition Metal dichalcogenides (TMDs) monolayers (MLs) is governed by robust excitons. Important progress has been made to control the dielectric environment surrounding the MLs, especially through hexagonal boron nitride (hBN) encapsulation, which drastically reduces the inhomogeneous contribution to the exciton linewidth. Most studies use exfoliated hBN from high quality flakes grown under high pressure. In this work, we show that hBN grown by molecular beam epitaxy (MBE) over a large surface area substrate has a similarly positive impact on the optical emission from TMD MLs. We deposit MoS$_2$ and MoSe$_2$ MLs on ultrathin hBN films (few MLs thick) grown on Ni/MgO(111) by MBE. Then we cover them with exfoliated hBN to finally obtain an encapsulated sample : exfoliated hBN/TMD ML/MBE hBN. We observe an improved optical quality of our samples compared to TMD MLs exfoliated directly on SiO$_2$ substrates. Our results suggest that hBN grown by MBE could be used as a flat and charge free substrate for fabricating TMD-based heterostructures on a larger scale.

cond-mat.mtrl-sci

Exciton-phonon coupling in MoSe2 monolayers

We study experimentally and theoretically the exciton-phonon interaction in MoSe2 monolayers encapsulated in hexagonal BN, which has an important impact on both optical absorption and emission processes. The exciton transition linewidth down to 1 meV at low temperatures makes it possible to observe high energy tails in absorption and emission extending over several meV, not masked by inhomogeneous broadening. We develop an analytical theory of the exciton-phonon interaction accounting for the deformation potential induced by the longitudinal acoustic phonons, which plays an important role in exciton formation. The theory allows fitting absorption and emission spectra and permits estimating the deformation potential in MoSe2 monolayers. We underline the reasons why exciton-phonon coupling is much stronger in two-dimensional transition metal dichalcodenides as compared to conventional quantum well structures. The importance of exciton-phonon interactions is further highlighted by the observation of a multitude of Raman features in the photoluminescence excitation experiments.

cond-mat.mtrl-sci

Electrically tunable dynamic nuclear spin polarization in GaAs quantum dots at zero magnetic field

In III-V semiconductor nano-structures the electron and nuclear spin dynamics are strongly coupled. Both spin systems can be controlled optically. The nuclear spin dynamics is widely studied, but little is known about the initialization mechanisms. Here we investigate optical pumping of carrier and nuclear spins in charge tunable GaAs dots grown on 111A substrates. We demonstrate dynamic nuclear polarization (DNP) at zero magnetic field in a single quantum dot for the positively charged exciton X$^+$ state transition. We tune the DNP in both amplitude and sign by variation of an applied bias voltage V$_g$. Variation of $Δ$V$_g$ of the order of 100 mV changes the Overhauser splitting (nuclear spin polarization) from -30 $μ$eV (-22 %) to +10 $μ$eV (+7 %), although the X$^+$ photoluminescence polarization does not change sign over this voltage range. This indicates that absorption in the structure and energy relaxation towards the X$^+$ ground state might provide favourable scenarios for efficient electron-nuclear spin flip-flops, generating DNP during the first tens of ps of the X$^+$ lifetime which is of the order of hundreds of ps. Voltage control of DNP is further confirmed in Hanle experiments.

cond-mat.mes-hall

Electrical initialization of electron and nuclear spins in a single quantum dot at zero magnetic field

The emission of circularly polarized light from a single quantum dot relies on the injection of carriers with well-defined spin polarization. Here we demonstrate single dot electroluminescence (EL) with a circular polarization degree up to 35% at zero applied magnetic field. The injection of spin polarized electrons is achieved by combining ultrathin CoFeB electrodes on top of a spin-LED device with p-type InGaAs quantum dots in the active region. We measure an Overhauser shift of several $μ$eV at zero magnetic field for the positively charged exciton (trion X$^+$) EL emission, which changes sign as we reverse the injected electron spin orientation. This is a signature of dynamic polarization of the nuclear spins in the quantum dot induced by the hyperfine interaction with the electrically injected electron spin. This study paves the way for electrical control of nuclear spin polarization in a single quantum dot without any external magnetic field.

cond-mat.mes-hall

Exciton diffusion in WSe2 monolayers embedded in a van der Waals heterostructure

We have combined spatially-resolved steady-state micro-photoluminescence ($μ$PL) with time-resolved photoluminescence (TRPL) to investigate the exciton diffusion in a WSe$_2$ monolayer encapsulated with hexagonal boron nitride (hBN). At 300 K, we extract an exciton diffusion length $L_X= 0.36\pm 0.02 \; μ$m and an exciton diffusion coefficient of $D_X=14.5 \pm 2\;\mbox{cm}^2$/s. This represents a nearly 10-fold increase in the effective mobility of excitons with respect to several previously reported values on nonencapsulated samples. At cryogenic temperatures, the high optical quality of these samples has allowed us to discriminate the diffusion of the different exciton species : bright and dark neutral excitons, as well as charged excitons. The longer lifetime of dark neutral excitons yields a larger diffusion length of $L_{X^D}=1.5\pm 0.02 \;μ$m.

cond-mat.mes-hall

Optical spectroscopy of excited exciton states in MoS2 monolayers in van der Waals heterostructures

The optical properties of MoS2 monolayers are dominated by excitons, but for spectrally broad optical transitions in monolayers exfoliated directly onto SiO2 substrates detailed information on excited exciton states is inaccessible. Encapsulation in hexagonal boron nitride (hBN) allows approaching the homogenous exciton linewidth, but interferences in the van der Waals heterostructures make direct comparison between transitions in optical spectra with different oscillator strength more challenging. Here we reveal in reflectivity and in photoluminescence excitation spectroscopy the presence of excited states of the A-exciton in MoS2 monolayers encapsulated in hBN layers of calibrated thickness, allowing to extrapolate an exciton binding energy of about 220 meV. We theoretically reproduce the energy separations and oscillator strengths measured in reflectivity by combining the exciton resonances calculated for a screened two-dimensional Coulomb potential with transfer matrix calculations of the reflectivity for the van der Waals structure. Our analysis shows a very different evolution of the exciton oscillator strength with principal quantum number for the screened Coulomb potential as compared to the ideal two-dimensional hydrogen model.

cond-mat.mtrl-sci

In-plane Propagation of Light in Transition Metal Dichalcogenide Monolayers: Optical Selection Rules

The optical selection rules for inter-band transitions in WSe2, WS2 and MoSe2 transition metal dichalcogenide monolayers are investigated by polarization-resolved photoluminescence experiments with a signal collection from the sample edge. These measurements reveal a strong polarization-dependence of the emission lines. We see clear signatures of the emitted light with the electric field oriented perpendicular to the monolayer plane, corresponding to an inter-band optical transition forbidden at normal incidence used in standard optical spectroscopy measurements. The experimental results are in agreement with the optical selection rules deduced from group theory analysis, highlighting the key role played by the different symmetries of the conduction and valence bands split by the spin-orbit interaction. These studies yield a direct determination on the bright-dark exciton splitting, for which we measure 40 $\pm 1$ meV and 55 $\pm 2$ meV for WSe2 and WS2 monolayer, respectively.

cond-mat.mtrl-sci