arXiv subjects

E. Courtade

Publications and source records attributed to E. Courtade.

17 recordsLinked to original sources

arXiv2019

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↗

arXiv2019

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↗

arXiv2018

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↗

arXiv2018

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↗

arXiv2018

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↗

arXiv2018

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↗

arXiv2018

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↗

arXiv2017

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↗

arXiv2017

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↗

arXiv2017

Excitonic linewidth approaching the homogeneous limit in MoS2 based van der Waals heterostructures : accessing spin-valley dynamics

The strong light matter interaction and the valley selective optical selection rules make monolayer (ML) MoS2 an exciting 2D material for fundamental physics and optoelectronics applications. But so far optical transition linewidths even at low temperature are typically as large as a few tens of meV and contain homogenous and inhomogeneous contributions. This prevented in-depth studies, in contrast to the better-characterized ML materials MoSe2 and WSe2. In this work we show that encapsulation of ML MoS2 in hexagonal boron nitride can efficiently suppress the inhomogeneous contribution to the exciton linewidth, as we measure in photoluminescence and reflectivity a FWHM down to 2 meV at T = 4K. This indicates that surface protection and substrate flatness are key ingredients for obtaining stable, high quality samples. Among the new possibilities offered by the well-defined optical transitions we measure the homogeneous broadening induced by the interaction with phonons in temperature dependent experiments. We uncover new information on spin and valley physics and present the rotation of valley coherence in applied magnetic fields perpendicular to the ML.

cond-mat.mtrl-sci↗

arXiv2017

Enabling valley selective exciton scattering in monolayer WSe$_2$ through upconversion

Excitons, Coulomb bound electron-hole pairs, are composite bosons and their interactions in traditional semiconductors lead to condensation and light amplification. The much stronger Coulomb interaction in transition metal dichalcogenides such as WSe$_2$ monolayers combined with the presence of the valley degree of freedom is expected to provide new opportunities for controlling excitonic effects. But so far the bosonic character of exciton scattering processes remains largely unexplored in these two-dimensional (2D) materials. Here we show that scattering between B-excitons and A-excitons preferably happens within the same valley in momentum space. This leads to power dependent, negative polarization of the hot B-exciton emission. We use a selective upconversion technique for efficient generation of B-excitons in the presence of resonantly excited A-excitons at lower energy, we also observe the excited A-excitons state $2s$. Detuning of the continuous wave, low power laser excitation outside the A-exciton resonance (with a full width at half maximum of 4 meV) results in vanishing upconversion signal.

cond-mat.mes-hall↗

arXiv2005

Manipulation of ultracold atomic mixtures using microwave techniques

We used microwave radiation to evaporatively cool a mixture of of 133Cs and 87Rb atoms in a magnetic trap. A mixture composed of an equal number (around 10^4) of Rb and Cs atoms in their doubly polarized states at ultracold temperatures was prepared. We also used microwaves to selectively evaporate atoms in different Zeeman states.

physics.atom-ph↗

arXiv2004

Sympathetic cooling and collisional properties of a Rb-Cs mixture

We report on measurements of the collisional properties of a mixture of $^{133}$Cs and $^{87}$Rb atoms in a magnetic trap at $μ\mathrm{K}$ temperatures. By selectively evaporating the Rb atoms using a radio-frequency field, we achieved sympathetic cooling of Cs down to a few $μ\mathrm{K}$. The inter-species collisional cross-section was determined through rethermalization measurements, leading to an estimate of $a_s=595 a_0$ for the s-wave scattering length for Rb in the $|F=2, m_F=2>$ and Cs in the $|F=4, m_F=4>$ magnetic states. We briefly speculate on the prospects for reaching Bose-Einstein condensation of Cs inside a magnetic trap through sympathetic cooling.

cond-mat.soft↗

arXiv2003

Rotational bosonic current in a quasi-condensate confined in an optical toroidal trap

We investigate the possibility of inducing a bosonic current which is rotational in a pseudo 1D quasi-condensate confined in an optical toroidal trap. The stability of such a current is also analyzed using hydrodynamics approach. We find that such a current is uniform when the circular symmetry is preserved and energetically stable when the modes of elementary excitations are restricted to one dimension. This scheme allows to distinguish between a quasi and a true condensate by measuring the rotational spectra of the sample.

cond-mat.stat-mech↗

arXiv2003

Instabilities of a Bose-Einstein condensate in a periodic potential: an experimental investigation

By accelerating a Bose-Einstein condensate in a controlled way across the edge of the Brillouin zone of a 1D optical lattice, we investigate the stability of the condensate in the vicinity of the zone edge. Through an analysis of the visibility of the interference pattern after a time-of-flight and the widths of the interference peaks, we characterize the onset of instability as the acceleration of the lattice is decreased. We briefly discuss the significance of our results with respect to recent theoretical work.

cond-mat↗

arXiv2003

Asymmetric Landau-Zener tunneling in a periodic potential

Using a simple model for nonlinear Landau-Zener tunneling between two energy bands of a Bose-Einstein condensate in a periodic potential, we find that the tunneling rates for the two directions of tunneling are not the same. Tunneling from the ground state to the excited state is enhanced by the nonlinearity, whereas in the opposite direction it is suppressed. These findings are confirmed by numerical simulations of the condensate dynamics. Measuring the tunneling rates for a condensate of rubidium atoms in an optical lattice, we have found experimental evidence for this asymmetry.

cond-mat.soft↗

arXiv2002

Magnetic Field Effects on the 1083 nm Atomic Line of Helium. Optical Pumping of Helium and Optical Polarisation Measurement in High Magnetic Field

The structure of the excited $2^{3}$S and $2^{3}$P triplet states of $^{3}$He and $^{4}$He in an applied magnetic field B is studied using different approximations of the atomic Hamiltonian. All optical transitions (line positions and intensities) of the 1083 nm $2^{3}$S-$2^{3}$P transition are computed as a function of B. The effect of metastability exchange collisions between atoms in the ground state and in the $2^{3}$S metastable state is studied, and rate equations are derived, for the populations these states in the general case of an isotopic mixture in an arbitrary field B. It is shown that the usual spin-temperature description remains valid. A simple optical pumping model based on these rate equations is used to study the B-dependence of the population couplings which result from the exchange collisions. Simple spectroscopy measurements are performed using a single-frequency laser diode on the 1083 nm transition. The accuracy of frequency scans and of measurements of transition intensities is studied. Systematic experimental verifications are made for B=0 to 1.5 T. Optical pumping effects resulting from hyperfine decoupling in high field are observed to be in good agreement with the predictions of the simple model. Based on adequately chosen absorption measurements at 1083 nm, a general optical method to measure the nuclear polarisation of the atoms in the ground state in an arbitrary field is described. It is demonstrated at $B\sim$0.1 T, a field for which the usual optical methods could not operate.

physics.atom-ph↗