116 research outputs found
Splitting between Bright and Dark excitons in Transition Metal Dichalcogenide Monolayers
The optical properties of transition metal dichalcogenide monolayers such as
the two-dimensional semiconductors MoS and WSe are dominated by
excitons, Coulomb bound electron-hole pairs. The light emission yield depends
on whether the electron-hole transitions are optically allowed (bright) or
forbidden (dark). By solving the Bethe Salpeter Equation on top of wave
functions in density functional theory calculations, we determine the sign and
amplitude of the splitting between bright and dark exciton states. We evaluate
the influence of the spin-orbit coupling on the optical spectra and clearly
demonstrate the strong impact of the intra-valley Coulomb exchange term on the
dark-bright exciton fine structure splitting.Comment: 6 pages, 2 figure
Efficient dynamical nuclear polarization in quantum dots: Temperature dependence
We investigate in micro-photoluminescence experiments the dynamical nuclear
polarization in individual InGaAs quantum dots. Experiments carried out in an
applied magnetic field of 2T show that the nuclear polarization achieved
through the optical pumping of electron spins is increasing with the sample
temperature between 2K and 55K, reaching a maximum of about 50%. Analysing the
dependence of the Overhauser shift on the spin polarization of the optically
injected electron as a function of temperature enables us to identify the main
reasons for this increase.Comment: 5 pages, 3 figure
Carrier and polarization dynamics in monolayer MoS2
In monolayer MoS2 optical transitions across the direct bandgap are governed
by chiral selection rules, allowing optical valley initialization. In time
resolved photoluminescence (PL) experiments we find that both the polarization
and emission dynamics do not change from 4K to 300K within our time resolution.
We measure a high polarization and show that under pulsed excitation the
emission polarization significantly decreases with increasing laser power. We
find a fast exciton emission decay time on the order of 4ps. The absence of a
clear PL polarization decay within our time resolution suggests that the
initially injected polarization dominates the steady state PL polarization. The
observed decrease of the initial polarization with increasing pump photon
energy hints at a possible ultrafast intervalley relaxation beyond the
experimental ps time resolution. By compensating the temperature induced change
in bandgap energy with the excitation laser energy an emission polarization of
40% is recovered at 300K, close to the maximum emission polarization for this
sample at 4K.Comment: 7 pages, 7 figures including supplementary materia
Electron spin quantum beats in positively charged quantum dots: nuclear field effects
We have studied the electron spin coherence in an ensemble of positively
charged InAs/GaAs quantum dots. In a transverse magnetic field, we show that
two main contributions must be taken into account to explain the damping of the
circular polarization oscillations. The first one is due to the nuclear field
fluctuations from dot to dot experienced by the electron spin. The second one
is due to the dispersion of the transverse electron Lande g-factor, due to the
inherent inhomogeneity of the system, and leads to a field dependent
contribution to the damping. We have developed a model taking into account both
contributions, which is in good agreement with the experimental data. This
enables us to extract the pure contribution to dephasing due to the nuclei.Comment: 10 pages, 6 figure
Bistability of the Nuclear Polarisation created through optical pumping in InGaAs Quantum Dots
We show that optical pumping of electron spins in individual InGaAs quantum
dots leads to strong nuclear polarisation that we measure via the Overhauser
shift (OHS) in magneto-photoluminescence experiments between 0 and 4T. We find
a strongly non-monotonous dependence of the OHS on the applied magnetic field,
with a maximum nuclear polarisation of 40% for intermediate magnetic fields. We
observe that the OHS is larger for nuclear fields anti-parallel to the external
field than in the parallel configuration. A bistability in the dependence of
the OHS on the spin polarization of the optically injected electrons is found.
All our findings are qualitatively understood with a model based on a simple
perturbative approach.Comment: Phys Rev B (in press
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 and MoSe 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 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.Comment: 5 pages, 3 figure
Robust optical emission polarization in MoS2 monolayers through selective valley excitation
We report polarization resolved photoluminescence from monolayer MoS2, a
two-dimensional, non-centrosymmetric crystal with direct energy gaps at two
different valleys in momentum space. The inherent chiral optical selectivity
allows exciting one of these valleys and close to 90% polarized emission at 4K
is observed with 40% polarization remaining at 300K. The high polarization
degree of the emission remains unchanged in transverse magnetic fields up to 9T
indicating robust, selective valley excitation.Comment: 5 pages, 3 figure
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 and MoTe 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 exciton below 1.5 meV and 3 meV in our MoSe and
MoTe 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 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.Comment: 14 pages, 7 figures, main text and appendi
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