Optical properties of individual manganese-doped quantum dots

The magnetic state of a single magnetic ion (Mn²⁺) embedded in an individual quantum dot is optically probed using micro-spectroscopy. The fine structure of a confined exciton in the exchange field of a single Mn²⁺ ion (S=) is analyzed in detail. The exciton–Mn²⁺ exchange interaction shifts the energy of the exciton depending on the Mn²⁺ spin component and six emission lines are observed at zero magnetic field. The emission spectra of individual quantum dots containing a single magnetic Mn atom differ strongly from dot to dot. The differences are explained by the influence of the system geometry, specifically the in-plane asymmetry of the quantum dot and the position of the Mn atom. Depending on both these parameters, one has different characteristic emission features which either reveal or hide the spin state of the magnetic atom. The observed behavior in both zero field and under magnetic field can be explained quantitatively by the interplay between the exciton–Mn²⁺ exchange interaction (dependent on the Mn position) and the anisotropic part of the electron–hole exchange interaction (related to the asymmetry of the quantum dot).     

Probing the spin state of a single magnetic ion in an individual quantum dot

The magnetic state of a single magnetic ion (Mn2+) embedded in an individual quantum dot is optically probed using microspectroscopy. The fine structure of a confined exciton in the exchange field of a single Mn2+ ion (S=5/2) is analyzed in detail. The exciton-Mn2+ exchange interaction shifts the energy of the exciton depending on the Mn2+ spin component and six emission lines are observed at zero magnetic field. Magneto-optic measurements reveal that the emission intensities in both circular polarizations are controlled by the Mn2+ spin distribution imposed by the exchange interaction with the exciton, the magnetic field, and an effective manganese temperature which depends on both the lattice temperature and the density of photocreated carriers. Under magnetic field, the electron-Mn interaction induces a mixing of the bright and dark exciton states.     

Optical spin orientation of a single manganese atom in a quantum dot

The magnetic state of a single magnetic atom (Mn) embedded in an individual semiconductor quantum dot is optically probed using micro-spectroscopy. A high degree of spin polarization can be achieved for an individual Mn atom localized in a quantum dot using quasi-resonant or fully-resonant optical excitation at zero magnetic field. Optically created spin polarized carriers generate an energy splitting of the Mn spin and enable magnetic moment orientation controlled by the photon helicity and energy. The dynamics and the magnetic field dependence of the optical pumping mechanism shows that the spin lifetime of an isolated Mn atom at zero magnetic field is controlled by a magnetic anisotropy induced by the built-in strain in the quantum dots. The Mn spin distribution prepared by optical pumping is fully conserved for a few microseconds. This opens the way to full optical control of the spin state of an individual magnetic atom in a solid state environment.     

Optically probing the fine structure of a single Mn atom in an InAs quantum dot

We report on the optical spectroscopy of a single InAs/GaAs quantum dot doped with a single Mn atom in a longitudinal magnetic field of a few Tesla. Our findings show that the Mn impurity is a neutral acceptor state A0 whose effective spin J=1 is significantly perturbed by the quantum dot potential and its associated strain field. The spin interaction with photocarriers injected in the quantum dot is shown to be ferromagnetic for holes, with an effective coupling constant of a few hundreds of mueV, but vanishingly small for electrons.     

Electron states in diluted magnetic semiconductors

One of the remarkable properties of the II–VI diluted magnetic semiconductor (DMS) quantum dot (QD) is the giant Zeeman splitting of the carrier states under application of a magnetic field. This splitting reveals strong exchange interaction between the magnetic ion moment and electronic spins in the QD. A theoretical study of the electron spectrum and of its relaxation to the ground state via the emission of a longitudinal optical (LO) phonon, in a CdSe/ZnMnSe self-assembled quantum dot, is proposed in this work. Numerical calculations showed that the strength of this interaction increases as a function of the magnetic field to become more than 30 meV and allows some level crossings. We have also shown that the electron is more localized in this DMS QD and its relaxation to the ground state via the emission of one LO phonon is allowed.     

Quantum interference in exciton-Mn spin interactions in a CdTe semiconductor quantum dot

We show theoretically and experimentally the existence of a new quantum-interference effect between the electron-hole interactions and the scattering by a single Mn impurity. The theoretical model, including electron-valence-hole correlations, the short- and long-range exchange interaction of a Mn ion with the heavy hole and with electron and anisotropy of the quantum dot, is compared with photoluminescence spectroscopy of CdTe dots with single magnetic ions. We show how the design of the electronic levels of a quantum dot enables the design of an exciton, control of the quantum interference, and hence engineering of light-Mn interaction.     

磁场对非对称量子点中极化子性质的影响

采用线性组合算符和幺正变换方法研究磁场对非对称量子点中弱耦合磁极化子性质的影响.导出了非对称量子点中弱耦合磁极化子的振动频率、基态能量和基态结合能随量子点的横向和纵向有效受限长度、磁场和电子-声子耦合强度的变化关系.数值计算结果表明:非对称量子点中弱耦合磁极化子的基态能量和基态结合能随量子点的横向和纵向有效受限长度的增加而迅速增大.随回旋频率的增加而增大,随电子-声子耦合强度的增加而减小.     

Optical manipulation of a single Mn spin in a CdTe quantum dot

In this paper we demonstrate optical writing of information on the spin state of a single Mn ion embedded in a CdTe/ZnTe quantum dot. As a tool for Mn spin orientation we use a spin-conserving transfer of excitation between two coupled quantum dots, one of them containing the Mn ion. Excitons created by circularly polarized light act on the Mn ion via the sp–d exchange interaction and orient its spin. The magnetic field of 1 T strongly enhances the orientation efficiency due to suppression of fast Mn spin relaxation mechanisms. Dynamics of the Mn spin under polarized excitation was measured in a time-resolved experiment, in which the intensity and polarization of excitation were modulated. Observed dynamics of the Mn spin can be described with a simple rate equation model.     

Charged magneto-exciton states in semiconductor quantum dots

By embedding a layer of self-assembled quantum dots into a field-effect structure, we are able to control the exciton charge in a single dot. We present the results of photoluminescence experiments as a function of both charge and magnetic field. The results demonstrate a hierarchy of energy scales determined by quantization, the direct Coulomb interaction, the electron–electron exchange interaction, and the electron–hole exchange interaction. For excitons up to the triply charged exciton, the behavior can be understood from a model assuming discrete levels within the quantum dot. For the triply charged exciton, this is no longer the case. In a magnetic field, we discover a coherent interaction with the continuum states, the Landau levels associated with the wetting layer.     

Effect of a magnetic impurity on the optical properties of a spherical ZnSe quantum dot

We consider the electron and hole states in a semiconductor ZnSe spherical quantum dot, in the center of which a magnetic impurity atom of manganese is located. In calculations the quantum dot is approximated by a spherical rectangular well with a finite depth. Within the framework of perturbation theory, the effect of exchange spin interaction of an electron and a hole with a magnetic impurity on the band structure of the system is considered. The optical spectrum of the system for different polarizations of the incident light is studied also.     

Magnetic exchange interactions in quantum dots containing electrons and magnetic ions

We present a theory of magnetic exchange interactions in quantum dots containing electrons and magnetic ions. We find the interaction between the electron and Mn ion to depend strongly on the number of electrons. It can be switched off for closed shell configurations and maximized for partially filled shells. However, unlike the total electron spin S which is maximized for half-filled shells, we predict the exchange interaction to be independent of the filling of the electronic shell. We show how this unusual effect manifests itself in quantum dot addition and excitation spectrum.     

Signature of symmetry of laterally coupled quantum dots in far-infrared spectrum

We study the effect of structure asymmetry on the energy spectrum and the far-infrared spectrum (FIR) of a lateral coupled quantum dot. The calculated spectrum shows that the parity break of coupled quantum dot results in more coherent superpositions in the low-lying states and exhibits unique anti-crossing in the two-electron FIR spectrum modulated by a magnetic field. We also find that the Coulomb correlation effect can make the FIR spectrum of coupled quantum dot without strict parity deviate greatly from Kohn theorem, which is just contrary to the symmetric case. Our results therefore suggest that FIR spectrum may be used to determine the symmetry of coupled quantum dot and to evaluate the degree of Coulomb interaction.     

Magnetooptics and dynamics of a magnetic polaron in semimagnetic CdSe/ZnMnSe quantum dots

The magnetooptics and picosecond dynamics of the radiative recombination of excitons in self-assembled semimagnetic CdSe/ZnMnSe quantum dots is studied at low temperatures. The behavior of individual quantum dots in a magnetic field and with an increase in temperature is indicative of a strong exchange interaction of excitons and magnetic Mn ions giving rise to a quasi-zero-dimensional exciton magnetic polaron. When the exciton energy exceeds the intracenter transition energy in Mn, the energy is rapidly transferred from excitons to Mn ions (faster than 20 ps). In the opposite case, a substantial red shift (～15 meV) of the emission line maximum is observed during the exciton lifetime ～500 ps, presenting the dynamics of the formation of a magnetic polaron with a characteristic time of ～110 ps.     

Transport through a single discrete level for non-collinear magnetic polarizations of the electron reservoirs

Spin-polarized transport through a non-interacting single-level quantum dot coupled to two ferromagnetic leads with non-collinear magnetizations is analyzed theoretically by the non-equilibrium Green function technique. It is shown that spin of an electron that has tunnelled on the dot precesses around an effective exchange field before it leaves the dot. The exchange field originates from interaction between the electron and external electrodes. Electric current, tunnel magnetoresistance, and average value of spin accumulated on the dot are calculated for an arbitrary angle between magnetic moments of the electrodes.     

Spin-polarized Mn2+ emission from Mn-doped colloidal nanocrystals

We report magnetophotoluminescence studies of strongly quantum-confined 0D diluted magnetic semiconductors (DMS), realized in Mn(2+)-doped ZnSe/CdSe core-shell colloidal nanocrystals. In marked contrast to their 3D (bulk), 2D (quantum well), 1D (quantum wire), and 0D (self-assembled quantum dot) DMS counterparts, the ubiquitous yellow emission band from internal d-d ((4)T(1)→(6)A(1)) transitions of the Mn(2+) ions in these nanocrystals is not suppressed in applied magnetic fields and does become circularly polarized. This polarization tracks the Mn(2+) magnetization, and is accompanied by a sizable energy splitting between right- and left-circular emission components that scales with the exciton-Mn sp-d coupling strength (which, in turn, is tunable with nanocrystal size). These data highlight the influence of strong quantum confinement on both the excitation and the emission mechanisms of magnetic ions in DMS nanomaterials.     

Multi-exciton spectroscopy on a self-assembled InGaAs/GaAs quantum dot

We report about spatially resolved magneto-optical experiments on a self-assembled InGaAs quantum dot. Using electron beam lithograpy for patterning a metal shadow mask we can isolate a single dot. This allows us to study the optical response of a single dot as a function of excitation power and magnetic field. We investigate the influence of many body interaction in the emission spectra for different exciton occupation numbers of the dot. The diamagnetic/orbital shift as well as Zeeman splitting in a magnetic field can be fully resolved and are used to identify the observed emission lines. Further we report on absorption properties of the quantum dot as a function of magnetic field. We analyse in detail the phonon-assisted absorption process connected with the GaAs LO-phonon 36 meV above the single-exciton ground state.     

Cancellation of fine-structure splitting in quantum dots by a magnetic field

We demonstrate control of the fine-structure splitting of the exciton emission lines in single InAs quantum dots by the application of an in-plane magnetic field. The composition of the barrier material and the size and symmetry of the quantum dot are found to determine decrease or increase in the linear polarization splitting of the dominant exciton emission lines with increasing magnetic field. This enables the selection of dots for which the splitting can to be tuned to zero, within the resolution of our experiments. General differences in the g-factors and exchange splittings are found for different types of dot.     

Spin–spin interaction in magnetic semiconductor quantum dots

Self-assembled Cd(Mn)Se/Zn(Mn)Se quantum dots have been investigated by means of spatially and time-resolved magneto-optical spectroscopy. In such quasi zero-dimensional diluted magnetic semiconductors, the exchange interaction couples the spins of optically generated charge carriers with localized magnetic ion spins. We demonstrate that this can be used on the one hand to monitor nanoscale magnetization with a resolution of <100 μ_B by a purely optical technique and on the other hand to optically manipulate the magnetization in a semiconductor quantum dot.     

磁场对非对称量子点中束缚磁极化子性质的影响

采用线性组合算符和幺正变换方法研究磁场对非对称量子点中弱耦合束缚磁极化子性质的影响。导出量子点中弱耦合束缚磁极化子振动频率和基态能量随量子点的横向和纵向有效受限长度、库仑束缚势、磁场的回旋共振频率和电子-声子耦合强度的变化关系。数值计算结果表明:非对称量子点中弱耦合束缚磁极化子的振动频率和基态能量随量子点的横向和纵向有效受限长度的减小而迅速增大。振动频率随库仑束缚势和磁场的回旋共振频率的增加而增大。基态能量随库仑束缚势和电子-声子耦合强度的增加而减小。     

Theory of electron mediated Mn-Mn interactions in quantum dots

We present a theory of interaction of magnetic Mn ions depending strongly on the number (Ne) of electrons in a quantum dot. For closed electronic shells, we derive the RKKY interaction and its dependence on magnetic ion positions, quantum dot energy quantization omega0, and the number of filled shells Ns. For partially filled shells, the many-electron magnetopolaron effect leads to effective carrier mediated ferromagnetic Mn-Mn interactions. The dependence of the magnetopolaron energy on magnetic ion positions, quantum dot energy quantization omega0, and the number of electrons Ne is predicted.