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Daniel Paget

Publications and source records attributed to Daniel Paget.

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Imaging Seebeck drift of excitons and trions in MoSe2 monolayers

Hyperspectral imaging at cryogenic temperatures is used to investigate exciton and trion propagation in MoSe$_2$ monolayers encapsulated with hexagonal boron nitride (hBN). Under a tightly focused, continuous-wave laser excitation, the spatial distribution of neutral excitons and charged trions strongly differ at high excitation densities. Remarkably, in this regime the trion distribution develops a halo shape, similar to that previously observed in WS2 monolayers at room temperature and under pulsed excitation. In contrast, the exciton distribution only presents a moderate broadening without the appereance of a halo. Spatially and spectrally resolved luminescence spectra reveal the buildup of a significant temperature gradient at high excitation power, that is attributed to the energy relaxation of photoinduced hot carriers. We show, via a numerical resolution of the transport equations for excitons and trions, that the halo can be interpreted as thermal drift of trions due to a Seebeck term in the particle current. The model shows that the difference between trion and exciton profiles is simply understood in terms of the very different lifetimes of these two quasiparticles.

cond-mat.mtrl-sci

Spin/Valley pumping of resident electrons in WSe2 and WS2 monolayers

Monolayers of transition metal dichalcogenides are ideal materials to control both spin and valley degrees of freedom either electrically or optically. Nevertheless, optical excitation mostly generates excitons species with inherently short lifetime and spin/valley relaxation time. Here we demonstrate a very efficient spin/valley optical pumping of resident electrons in n-doped WSe2 and WS2 monolayers. We observe that, using a continuous wave laser and appropriate doping and excitation densities, negative trion doublet lines exhibit circular polarization of opposite sign and the photoluminescence intensity of the triplet trion is more than four times larger with circular excitation than with linear excitation. We interpret our results as a consequence of a large dynamic polarization of resident electrons using circular light.

cond-mat.mes-hall

Charge and spin transport over record distances in GaAs metallic n-type nanowires : I photocarrier transport in a dense Fermi sea

We have investigated charge and spin transport in n-type metallic GaAs nanowires (~ 10^17 cm^-3 doping level), grown by hydride vapor phase epitaxy (HVPE) on Si substrates. This was done by exciting the nanowire by tightly-focussed circularly-polarized light and by monitoring the intensity and circular polarization spectrum as a function of distance from the excitation spot. The spin-polarized photoelectrons give rise to a well-defined feature in the nearbandgap spectrum, distinct from the main line due to recombination of the spin-unpolarized electrons of the Fermi sea with the same minority photoholes. At a distance of 2 (micro)m, only the main line remains, implying that photoelectrons have reached a charge thermodynamic equilibrium with the Fermi sea. However, although no line is present in the intensity spectrum at the corresponding energy, the circular polarization is still observed at the same energy in the spectrum, implying that photoelectrons have preserved their spin orientation and that the two spin reservoirs remain distinct. Investigations as a function of distance to the excitation spot show that, depending on excitation power, a photoelectron spin polarization of 20% can be transported over a record distance of more than 20 (micro)m. This finding has potential applications for long distance spin transport in n-type doped nanowires.

cond-mat.mes-hall

VLS-HVPE growth of ultra-long and defect-free GaAs nanowires investigated by ab initio simulation coupled to near-field microscopy

High aspect ratio, rod-like and single crystal phase GaAs nanowires (NWs) were grown by gold catalyst-assisted hydride vapor phase epitaxy (HVPE). High resolution transmission electron microscopy (HRTEM) and micro-Raman spectroscopy revealed polytypism-free zinc blende NWs over lengths of several tens of micrometers for diameters ranging between 50 and 150 nm. Micro-photoluminescence studies of individual NWs showed linewidths smaller than those reported elsewhere which is consistent with the crystalline quality of the NWs. HVPE makes use of chloride growth precursors of which high decomposition frequency, after adsorption onto the catalyst particle, favors a direct and rapid introduction of the Ga atoms from the vapor phase into the catalyst liquid droplet. This yields high axial growth rate (more than 100 micron/h) of NWs. The fast diffusion of the Ga atoms in the droplet towards the interface between the liquid and the solid nanowire was investigated by using density functional theory calculations. The diffusion coefficient of Ga atoms was estimated to be 3x10-9 m2/s, which matches the experimental observations.

cond-mat.mes-hall

Imaging ambipolar diffusion of photocarriers in GaAs thin films

Images of the steady-state luminescence of passivated GaAs self-standing films under excitation by a tightly-focussed laser are analyzed as a function of light excitation power. While unipolar diffusion of photoelectrons is dominant at very low light excitation power, an increased power results in a decrease of the diffusion constant near the center of the image due to the onset of ambipolar diffusion. The results are in agreement with a numerical solution of the diffusion equations and with a physical analysis of the luminescence intensity at the centre of the image, which permits the determination of the ambipolar diffusion constant as a function of electron concentration.

cond-mat.mes-hall

Light-induced nuclear quadrupolar relaxation in semiconductors

Light excitation of a semiconductor, known to dynamically-polarize the nuclear spins by hyperfine contact interaction with the photoelectrons, also generates an intrinsic nuclear depolarization mechanism. This novel relaxation process arises from the modulation of the nuclear quadrupolar Hamiltonian by photoelectron trapping and recombination at nearby localized states. For nuclei near shallow donors, the usual diffusion radius is replaced by a smaller, quadrupolar, radius. If the light excitation conditions correspond to partial donor occupation by photoelectrons, the nuclear magnetization and the nuclear field can be decreased by more than one order of magnitude.

quant-ph