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L. Besombes

Publications and source records attributed to L. Besombes.

At least 19 recordsLinked to original sources

Strain-driven spin mixing and dark-exciton recombination in a neutral Ni2+ doped quantum dot

We investigate the optical properties of neutral excitons in CdTe/ZnTe quantum dots containing a single Ni2+ ion. We show that the photoluminescence spectra provide a direct spectroscopic signature of strain induced mixing of the Ni2+ spin states. A misalignment between the principal axis of the local strain tensor and the quantum dot growth direction reorients the spin quantization axis of the magnetic ion, reducing the hole Ni2+ exchange interaction at low magnetic field and giving rise to photoluminescence replicas around the partially linearly polarized bright-exciton transitions. A longitudinal magnetic field restores the circularly polarized optical selection rules, allowing the three spin projections S_z = 0, +-1 of the Ni2+ ion to be spectrally resolved. Dark exciton emission appears on the low energy side of the spectra and is dominated at low field by transitions involving spin flips of the magnetic ion. An effective spin Hamiltonian including strain orientation and valence band mixing reproduces the magnetic field evolution of both bright and dark exciton spectra. These results highlight the key role of the local strain environment in determining the spin exciton coupling of transition metal dopants in semiconductor quantum dots.

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Influence of local strain on the optical probing of a Ni$^{2+}$ spin in a charged self-assembled quantum dot

This study explores the optical properties of quantum dots doped with a Ni$^{2+}$ ion that interacts with a charged exciton. Systematic magneto-optical analysis reveals that the strain distribution at the Ni$^{2+}$ site significantly influences its spin structure. In positively charged dots dominated by in-plane biaxial strain, the three spins states of the Ni$^{2+}$ (S$_z$=0, S$_z$=$\pm$1) can be observed and the magneto-optical spectra enables a local strain anisotropy to be determined. However, in most of the dots, lower-symmetry strain mixes all the Ni$^{2+}$ spin states, thereby increasing the number of observed optical transitions. In charged dots, we identify optical transitions that share a common excited state. They form a series of $\Lambda$ levels systems that can be individually addressed optically to determine the energy level structure. Magneto-optical measurements demonstrate that the hole-Ni$^{2+}$ exchange interaction is antiferromagnetic and considerably stronger than the electron-Ni$^{2+}$ interaction. A spin-effective model that incorporates local strain orientation can successfully reproduce key experimental results. Furthermore, we demonstrate that low-symmetry terms in the hole-Ni$^{2+}$ exchange interaction must be considered in order to accurately describe the emission spectra details in a magnetic field.

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Optical probing of the carriers-mediated coupling of the spin of two Co atoms in a quantum dot

We report on the optical spectroscopy of the spin of two Co atoms in a quantum dot and interacting with a single exciton. The spectrum of quantum dots containing two Co atoms are exchange interaction and by the strain at the location of the magnetic atoms. A wide range of spectrum can be obtained depending on the relative coupling of each atom to the confined exciton. We obtained a comprehensive interpretation of the experimental data with a spin Hamiltonian model. We show that the two Co atoms spins can be orientated by the injection of spin polarized carriers at zero magnetic field. This induces a correlation between the two spins that is observed in the intensity distribution of the emission spectra. The optical absorption in the phonon sideband of quantum dots doped with two Co reveals resonant absorptions which strongly depend on a transverse magnetic field. We show that these characteristic absorptions result from an interplay between the mixing of Co spin states induced by the presence of in-plane strain anisotropy at the magnetic atoms location and the transverse field.

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Coupling of the triplet states of a negatively charged exciton in a quantum dot with the spin of a magnetic atom

Two electrons in a quantum dot (QD) can form triplet states. We analyze the exchange coupling of the triplet states of the negatively charged exciton in a QD (X$^-$, two electrons and one hole) with the spin of a magnetic atom (Mn). Two techniques are used to access the spin structure of this magnetic complex: the resonant excitation of the excited states of X$^-$-Mn and the analysis of the emission of a negatively charged biexciton in a magnetic dot (XX$^-$-Mn). The photo-luminescence (PL) excitation of X$^-$-Mn reveals excited states with a circularly polarized fine structure which strongly depends on the Mn spin state S$_z$ and gives rise to negative circular polarization emission. This fine structure arises from the coupling of the triplet states of an excited charged exciton with the Mn (X$^{-*}$-Mn) and its S$_z$ dependence can be described by a spin effective model. The recombination of XX$^-$-Mn leaves in the dot a charged exciton in its excited state and the PL structure is controlled by the coupling of triplet states of X$^{-*}$ with the Mn spin. An analysis of the polarization and magneto-optic properties of this emission gives access to the electron-hole exchange interaction within the triplets states. Comparing the fine structure of the singlet X$^-$-Mn and of the triplets of X$^{-*}$-Mn we can independently study the different source of anisotropy in the QD: the valence band mixing and the exchange interaction in an anisotropic potential

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Spin dynamics of positively charged excitons in Cr$^+$-doped quantum dots probed by resonant photoluminescence

We study the dynamics of the spin system that consist of a positively charged II-VI semiconductor quantum dot doped with a single Cr$^+$ ion. The resonant photoluminescence (PL) of the positively charged exciton coupled with the Cr$^+$ spin is used to analyze the main spin relaxation channels. The intensity of the resonant PL is reduced by an optical pumping of the spin of the resident hole-Cr$^+$ complex that can be seen as a nano-magnet. The spin memory can be partially erased by a non-resonant optical excitation. This leads to an increase of the resonant PL signal. The resonant PL is co-circularly polarized and corresponds to relaxation channels that conserve the Cr$^+$ spin $\vert S_z \vert$. The observation in the resonant-PL excitation spectra of optical transitions with a change of the Cr$^+$ spin permits to determine the magnetic anisotropy of the magnetic atom. Optical pumping, auto-correlation measurements and the power dependence of the PL intensity distribution show that the effective temperature of the hole-Cr$^+$ spin system is affected by the optical excitation through the local generation of phonons.

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A hole-Cr$^{+}$ nano-magnet in a semiconductor quantum dot

We study a new diluted magnetic semiconductor system based on the spin of the ionized acceptor Cr$^+$. We show that the negatively charged Cr$^+$ ion, an excited state of the Cr in II-VI semiconductor, can be stable when inserted in a CdTe quantum dot (QD). The Cr$^+$ attracts a heavy-hole in the QD and form a stable hole-Cr$^+$ complex. Optical probing of this system reveals a ferromagnetic coupling between heavy-holes and Cr$^+$ spins. At low temperature, the thermalization on the ground state of the hole-Cr$^+$ system with parallel spins prevents the optical recombination of the excess electron on the 3$d$ shell of the atom. We study the dynamics of the nano-magnet formed by the hole-Cr$^+$ exchange interaction. The ferromagnetic ground states with M$_z$=$\pm$4 can be controlled by resonant optical pumping and a spin relaxation time in the 20 $μ$s range is obtained at T=4.2 K. This spin memory at zero magnetic field is limited by the interaction with phonons.

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Radio-frequency stress-induced modulation of CdTe/ZnTe quantum dots

We demonstrate radio-frequency tuning of the energy of individual CdTe/ZnTe quantum dots (QDs) by Surface Acoustic Waves (SAWs). Despite the very weak piezoelectric coefficient of ZnTe, SAW in the GHz range can be launched on a ZnTe surface using interdigitated transducers deposited on a c-axis oriented ZnO layer grown on ZnTe containing CdTe QDs. The photoluminescence (PL) of individual QDs is used as a nanometer-scale sensor of the acoustic strain field. The energy of QDs is modulated by SAW in the GHz range and leads to characteristic broadening of time-integrated PL spectra. The dynamic modulation of the QD PL energy can also be detected in the time domain using phase-locked time domain spectroscopy. This technique is in particular used for monitoring complex local acoustic fields resulting from the superposition of two or more SAW pulses in a cavity. Under magnetic field, the dynamic spectral tuning of a single QD by SAW can be used to generate single photons with alternating circular polarization controlled in the GHz range.

cond-mat.mes-hall

Optical control of an individual Cr spin in a semiconductor quantum dot

We demonstrate that the spin of a Cr atom in a quantum dot (QD) can be controlled optically and we discuss the main properties of this single spin system. The photoluminescence of individual Cr-doped QDs and their evolution in magnetic field reveal a large magnetic anisotropy of the Cr spin induced by local strain. This results in a splitting of the Cr spin states and in a thermalization on the lower energy states states S$_z$=0 and S$_z$=$\pm$1. The magneto-optical properties of Cr-doped QDs can be modelled by an effective spin Hamiltonian including the spin to strain coupling and the influence of the QD symmetry. We also show that a single Cr spin can be prepared by resonant optical pumping. Monitoring the intensity of the resonant fluorescence of the QD during this process permits to probe the dynamics of the optical initialization of the spin. Hole-Cr flip-flops induced by an interplay of the hole-Cr exchange interaction and the coupling with acoustic phonons are the main source of relaxation that explains the efficient resonant optical pumping. The Cr spin relaxation time is measured in the $μs$ range. We evidence that a Cr spin couples to non-equilibrium acoustic phonons generated during the optical excitation inside or near the QD). Finally we show that the energy of any spin state of an individual Cr atom can be independently tuned by a resonant single mode laser through the optical Stark effect. All these properties make Cr-doped QDs very promising for the development of hybrid spin-mechanical systems where a coherent mechanical driving of an individual spin in an oscillator is required.

cond-mat.mes-hall

Influence of non-equilibrium phonons on the spin dynamics of a single Cr atom

We analyse the influence of optically generated non-equilibrium phonons on the spin relaxation and effective spin temperature of an individual Cr atom inserted in a quantum dot. Using a three pulses pump-probe technique, we show that the spin relaxation measured in resonant optical pumping experiments strongly depends on the optical excitation conditions. We observe for an isolated Cr in the dark a heating time shorter than a few hundreds $ns$ after an initial high power non-resonant excitation pulse. A cooling time larger than a few tens of $μs$, independent on the excitation, is obtained in the same experimental conditions. We show that a tunable spin-lattice coupling dependent on the density of non-equilibrium phonons can explain the observed dynamics. Low energy excitation conditions are found where the Cr spin states S$_z$=$\pm$1 can be efficiently populated by a non-resonant optical excitation, prepared and read-out by resonant optical pumping and conserved in the dark during a few $μ$s.

cond-mat.mes-hall

Charge fluctuations of a Cr atom probed in the optical spectra of a quantum dot

We study the emission of individual quantum dots in CdTe/ZnTe samples doped with a low concentration of Cr. In addition to dots with a photoluminescence (PL) split by the exchange interaction with a magnetic Cr atom, we observe another type of dots with a complex PL structure composed of a minimum of six lines on the exciton and biexciton and three lines on the charged excitons. In these dots, the linear polarization dependence and the magnetic field dependence of the PL behave like three similar quantum dots emitting at slightly different energies. Cross-correlation intensity measurements show that these emission lines are not independent but exchange intensities in a time scale of a few hundred nanoseconds depending on the optical excitation power. We attribute this PL structure to charge fluctuations of a Cr atom located in the vicinity the CdTe dots in the ZnTe barrier. We present a model which confirms that the presence of a single charge fluctuating between -e (Cr$^{+}$), 0 (Cr$^{2+}$) and +e (Cr$^{3+}$) and located a few nm away from the dot explains the observation of three emission energies. We finally show that the interaction between the confined carriers and the nearby fluctuating localized charge can be modified by an applied static electric field which modulates the splitting of the emission lines.

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Resonant photoluminescence and dynamics of a hybrid Mn-hole spin in a positively charged magnetic quantum dot

We analyze, through resonant photoluminescence, the spin dynamics of an individual magnetic atom (Mn) coupled to a hole in a semiconductor quantum dot. The hybrid Mn-hole spin and the positively charged exciton in a CdTe/ZnTe quantum dot forms an ensemble of $Λ$ systems which can be addressed optically. Auto-correlation of the resonant photoluminescence and resonant optical pumping experiments are used to study the spin relaxation channels in this multilevel spin system. We identified for the hybrid Mn-hole spin an efficient relaxation channel driven by the interplay of the Mn-hole exchange interaction and the coupling to acoustic phonons. We also show that the optical $Λ$ systems are connected through inefficient spin-flips than can be enhanced under weak transverse magnetic field. The dynamics of the resonant photoluminescence in a p-doped magnetic quantum dot is well described by a complete rate equation model. Our results suggest that long lived hybrid Mn-hole spin could be obtained in quantum dot systems with large heavy-hole/light-hole splitting.

cond-mat.mes-hall

Resonant optical control of the spin of a single Cr atom in a quantum dot

A Cr atom in a semiconductor host carries a localized spin with an intrinsic large spin to strain coupling particularly promising for the development of hybrid spin-mechanical systems and coherent mechanical spin driving. We demonstrate here that the spin of an individual Cr atom inserted in a semiconductor quantum dot can be controlled optically. We first show that a Cr spin can be prepared by resonant optical pumping. Monitoring the time dependence of the intensity of the resonant fluorescence of the quantum dot during this process permits to probe the dynamics of the optical initialization of the Cr spin. Using this initialization and read-out technique we measured a Cr spin relaxation time at T=5 K of about 2 microseconds. We finally demonstrate that, under a resonant single mode laser field, the energy of any spin state of an individual Cr atom can be independently tuned by using the optical Stark effect.

cond-mat.mes-hall

Spin dynamics of an individual Cr atom in a semiconductor quantum dot under optical excitation

We studied the spin dynamics of a Cr atom incorporated in a II-VI semiconductor quantum dot using photon correlation techniques. We used recently developed singly Cr-doped CdTe/ZnTe quantum dots (A. Lafuente-Sampietro {\it et al.}, [1]) to access the spin of an individual magnetic atom. Auto-correlation of the photons emitted by the quantum dot under continuous wave optical excitation reveals fluctuations of the localized spin with a timescale in the 10 ns range. Cross-correlation gives quantitative transfer time between Cr spin states. A calculation of the time dependence of the spin levels population in Cr-doped quantum dots shows that the observed spin dynamics is controlled by the exciton-Cr interaction. These measurements also provide a lower bound in the 20 ns range for the intrinsic Cr spin relaxation time.

cond-mat.mes-hall

Individual Cr atom in a semiconductor quantum dot: optical addressability and spin-strain coupling

We demonstrate the optical addressability of the spin of an individual Chromium atom (Cr) embedded in a semiconductor quantum dot. The emission of Cr-doped quantum dots and their evolution in magnetic field reveal a large magnetic anisotropy of the Cr spin induced by local strain. This results in the zero field splitting of the 0, +-1 and +-2 Cr spin states and in a thermalization on the magnetic ground states 0 and +-1. The observed strong spin to strain coupling of Cr is of particular interest for the development of hybrid spin-mechanical devices where coherent mechanical driving of an individual spin in an oscillator is needed. The magneto-optical properties of Cr-doped quantum dots are modelled by a spin Hamiltonian including the sensitivity of the Cr spin to the strain and the influence of the quantum dot symmetry on the carrier-Cr spin coupling.

cond-mat.mes-hall

Strain induced coherent dynamics of coupled carriers and Mn spins in a quantum dot

We report on the coherent dynamics of the spin of an individual magnetic atom coupled to carriers in a semiconductor quantum dot which has been investigated by resonant photoluminescence of the positively charged exciton (X+). We demonstrate that a positively charged CdTe/ZnTe quantum dot doped with a single Mn atom forms an ensemble of optical Lambda systems which can be addressed independently. We show that the spin dynamics of the X+Mn complex is dominated by the electron-Mn exchange interaction and report on the coherent dynamics of the electron-Mn spin system that is directly observed in the time domain. Quantum beats reflecting the coherent transfer of population between electron-Mn spin states, which are mixed by an anisotropic strain in the plane of the quantum dot, are clearly observed. We finally highlight that this strain induced coherent coupling is tunable with an external magnetic field.

cond-mat.mes-hall

Dynamics of a Mn spin coupled to a single hole confined in a quantum dot

Using the emission of the positively charged exciton as a probe, we analyze the dynamics of the optical pumping and the dynamics of the relaxation of a Mn spin exchange-coupled with a confined hole spin in a II-VI semiconductor quantum dot. The hole-Mn spin can be efficiently initialized in a few tens of $ns$ under optical injection of spin polarized carriers. We show that this optical pumping process and its dynamics are controlled by electron-Mn flip-flops within the positively charged exciton-Mn complex. The pumping mechanism and its magnetic field dependence are theoretically described by a model including the dynamics of the electron-Mn complex in the excited state and the dynamics of the hole-Mn complex in the ground state of the positively charged quantum dot. We measure at zero magnetic field a spin relaxation time of the hole-Mn spin in the $μs$ range or shorter. This hole-Mn spin relaxation is induced by the presence of valence band mixing in self-assembled quantum dots.

cond-mat.mes-hall

Resonant optical pumping of a Mn spin in a strain free quantum dot

We report on the spin properties of individual Mn atoms in II-VI semiconductor strain free quantum dots. Strain free Mn-doped CdTe quantum dots are formed by width fluctuations in thin quantum wells lattice matched on a CdTe substrate. These quantum dots permit to optically probe and address any spin state of a Mn atom in a controlled strain environment. The absence of strain induced magnetic anisotropy prevents an optical pumping of the Mn spin at zero magnetic field. Thus, a large photoluminescence is obtained under resonant optical excitation of the exciton-Mn complex. An efficient optical pumping of the coupled electronic and nuclear spins of the Mn is restored under a weak magnetic field. The observed reduction of the resonant photoluminescence intensity under magnetic field is well described by a model including the hyperfine coupling and a residual crystal field splitting of the Mn atom. Finally, we show that the second order correlation function of the resonant photoluminescence presents a large photon bunching at short delay which is a probe of the dynamics of coupled electronic and nuclear spins of the Mn atom.

cond-mat.mes-hall

Phase diagrams of magnetopolariton gases

The magnetic field effect on phase transitions in electrically neutral bosonic systems is much less studied than those in fermionic systems, such as superconducting or ferromagnetic phase transitions. Nevertheless, composite bosons are strongly sensitive to magnetic fields: both their internal structure and motion as whole particles may be affected. A joint effort of ten laboratories has been focused on studies of polariton lasers, where non-equilibrium Bose-Einstein condensates of bosonic quasiparticles, exciton-polaritons, may appear or disappear under an effect of applied magnetic fields. Polariton lasers based on pillar or planar microcavities were excited both optically and electrically. In all cases a pronounced dependence of the onset to lasing on the magnetic field has been observed. For the sake of comparison, photon lasing (lasing by an electron-hole plasma) in the presence of a magnetic field has been studied on the same samples as polariton lasing. The threshold to photon lasing is essentially governed by the excitonic Mott transition which appears to be sensitive to magnetic fields too. All the observed experimental features are qualitatively described within a uniform model based on coupled diffusion equations for electrons, holes and excitons and the Gross-Pitaevskii equation for exciton-polariton condensates. Our research sheds more light on the physics of non-equilibrium Bose-Einstein condensates and the results manifest high potentiality of polariton lasers for spin-based quantum logic applications.

cond-mat.mes-hall