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).     

Geometrical effects on the optical properties of quantum dots doped with a single magnetic atom

The emission spectra of individual self-assembled 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-manganese 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).     

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.     

ODMR Study of Zn1−x Mn x Se/Zn1−y Be y Se and (Cd1−x ,Mn)Te/Cd1−y Mg y Te Diluted Magnetic Semiconductor Quantum Wells

The effects of microwave pumping with a frequency of 60 GHz on the magneto-optical properties of diluted magnetic semiconductors (DMSs) are studied in (Zn,Mn)Se/(Zn,Be)Se and (Cd,Mn)Te/(Cd,Mg)Te quantum wells. Resonant heating of the Mn²⁺ ions in the electron spin resonance conditions leads to an increase in the Mn-spin temperature, which exceeds the bath temperature by up to 5.2 K, as detected by the shift of exciton emission line and decrease of its integral intensity. Nonresonant heating mediated by free carriers is also observed through variation of the polarization degree of emission. Direct measurements of spin–lattice relaxation times for both materials using time-resolved optically detected magnetic resonance (ODMR) technique have been performed. The mechanisms of ODMR in nanostructures of DMSs are discussed.     

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.     

Energy Structure of an Individual Mn Acceptor in GaAs : Mn

The energy structure of the Mn acceptor, which is a complex of Mn²⁺ ion plus valence band hole, is investigated in the external magnetic field and under presence of an uniaxial stress has been studied. The spin-flip Raman spectra are studied under resonant excitation of exciton bound to the Mn acceptor. The gfactors of the ground F = 1 and the first excited F = 2 states are determined and selection rules for the optical transitions between the acceptor states are described. The value of the random field (stress or electric field) acting on manganese acceptor and the deformation potential for the exchange interaction constant of the Mn²⁺ + hole complex are obtained. A theoretical model is developed that takes into account the influence of random internal and uniaxial external stress and magnetic field. The proposed model describes well the lines of spin-flip Raman scattering of Mn acceptor.     

Spin relaxation of Mn ions in (CdMn)Te/(CdMg)Te quantum wells under picosecond optical pumping

Spin relaxation of Mn ions in a Cd_0.97Mn_0.03Te/Cd_0.75Mg_0.25Te quantum well with photogenerated quasi-two-dimensional electron-hole plasma at liquid helium temperatures in an external magnetic field has been investigated. Heating of Mn ions by photogenerated carriers due to spin and energy exchange between the hot electron-hole plasma and Mn ions through direct sd-interaction between electron and Mn spins has been detected. This process has a short characteristic time of about 4 ns, which leads to appreciable heating of the Mn spin subsystem in about 0.5 ns. Even under uniform excitation of a dense electron-hole plasma, the Mn heating is spatially nonuniform, and leads to formation of spin domains in the quantum well magnetic subsystem. The relaxation time of spin domains after pulsed excitation is measured to be about 70 ns. Energy relaxation of excitons in the random exchange potential due to spin domains results from exciton diffusion in magnetic field B=14 T with a characteristic time of 1 to 4 ns. The relaxation time decreases with decreasing optical pump power, which indicates smaller dimensions of spin domains. In weak magnetic fields (_B=2 T) a slow down in the exciton diffusion to 15 ns has been detected. This slow down is due to exciton binding to neutral donors (formation of bound excitons) and smaller spin domain amplitudes in low magnetic fields. The optically determined spin-lattice relaxation time of Mn ions in a magnetic field of 14 T is 270±10 and 16±7 ns for Mn concentrations of 3% and 12%, respectively. Zh. éksp. Teor. Fiz. 112, 1440–1463 (October 1997)     

Ferroelectricity of polycrystalline GdMnO3 and multifold magnetoelectric responses

The multiferroic behaviors of polycrystalline GdMnO₃ are investigated by focusing on the ferroelectric response to the spin ordering sequence and external magnetic field. The polarization current shows sensitive response to both the Mn cycloidal spin order and Gd antiferromagnetic (AFM) order. The complicated magnetoelectric behaviors suggest that the Mn cycloidal spin order can be modulated by the Gd AFM order at low temperature via the Gd–Mn spin interaction. Due to the possible disorder and defects in polycrystalline nature, polycrystalline GdMnO₃ may accommodate the cycloidal spin order in addition to the A-type AFM order at Mn sites, as illustrated by simulation based on the two-orbit double exchange model and measured hysteresis loops of polarization against magnetic field, indicating the switching of the ferroelectric domains coupled with the magnetic domains in response to magnetic field.     

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.     

Optical pumping and a nondestructive readout of a single magnetic impurity spin in an InAs/GaAs quantum dot

We report on the resonant optical pumping of the | ± 1? spin states of a single Mn dopant in an InAs/GaAs quantum dot which is embedded in a charge tunable device. The experiment relies on a W scheme of transitions reached when a suitable longitudinal magnetic field is applied. The optical pumping is achieved via the resonant excitation of the central Λ system at the neutral exciton X(0) energy. For a specific gate voltage, the redshifted photoluminescence of the charged exciton X- is observed, which allows a nondestructive readout of the spin polarization. An arbitrary spin preparation in the | + 1? or |-1? state characterized by a polarization near or above 50% is evidenced.     

Nuclear and ion spins in semiconductor nanostructures

Spin interactions are studied between conduction band electrons in GaAs heterostructures and local moments, specifically the spins of constituent lattice nuclei and of partially filled electronic shells of impurity atoms. Nuclear spin polarizations are addressed through the contact hyperfine interaction resulting in the development of a method for high-field optically detected nuclear magnetic resonance sensitive to 10⁸ nuclei. This interaction is then used to generate nuclear spin polarization profiles within a single parabolic quantum well; the position of these nanometer-scale sheets of polarized nuclei can be shifted along the growth direction using an externally applied electric field. In order to directly investigate ion spin dynamics, doped GaMnAs quantum wells are fabricated in the regime of very low Mn concentrations. Measurements of coherent electron spin dynamics show an antiferromagnetic exchange between s-like conduction band electrons and electrons localized in the d-shell of the Mn impurities, which varies as a function of well width.     

Tuning of exciton states in a magnetic quantum ring

The exciton states in a CdTe quantum ring subjected to an external magnetic field containing a single magnetic impurity are investigated. We have used the multiband approximation which includes the heavy hole–light hole coupling effects. The electron–hole spin interactions and the s, p–d interactions between the electron, the hole and the magnetic impurity are also included. The exciton energy levels and optical transitions are evaluated using the exact diagonalization scheme. We show that due to the spin interactions it is possible to change the bright exciton state into the dark state and vice versa with the help of a magnetic field. We propose a new route to experimentally estimate the s, p–d spin interaction constants.     

Influence of the Fe2+ ion triple clusters on the magnetic susceptibility of Fe-based diluted magnetic semiconductors

Low lying energy levels of Fe²⁺ ion triples in the cubic-structure iron-based diluted magnetic semiconductors are calculated on the basis of a model which includes crystal field, spin–orbit interaction, Zeeman interaction and Heisenberg-type exchange interaction. Using this energy level diagram the magnetic susceptibility of a crystal is calculated in the nearest-neighbour (NN) and in the extended NN pair approximation. We find that the Fe²⁺ ion triples contribute to the temperature dependent susceptibility up to the lowest temperatures investigated, T⩾1 K. It appears that the triple Fe²⁺ ion clusters may explain at least a part of the low-temperature increase of the magnetic susceptibility which is observed in these magnetic materials.     

Magnetic pair making and breaking effect of Ru in La0.7Sr0.3Mn0.9Ru0.1O3 and La0.5Sr0.5Co0.9Ru0.1O3

The substitutional effect of Ru on the magnetic and transport properties of double exchange ferromagnets, La_0.7Sr_0.3MnO₃ and La_0.5Sr_0.5CoO₃ has been investigated. It is found that substitution of 10% Ru at the Mn site of La_0.7Sr_0.3MnO₃ decreases the Curie temperature by 20 K than that of the parent compound. However, a large decrease in the Curie temperature, ΔT_c80 K and the system undergoes a transition from metallic state to insulating state is observed when 10% Ru is doped in La_0.5Sr_0.5CoO₃. The marginal effect of Ru in the Mn–O–Mn sublattice in comparison to the Co–O–Co sublattice could be due to the magnetic exchange interaction between Mn and Ru by virtue of the fact that Ru exhibits variable valence states, Ru⁺⁴/Ru⁺⁵. The e_g and t_2g parentage of Ru⁺⁵ is similar to Mn⁺⁴ and therefore, Ru⁺⁵ ion appears to participate in the double exchange mediated ferromagnetic (FM) interaction. On the other hand, Ruthenium (IV) ion disrupts an intermediate spin state of cobalt (Co⁺³: t_2g⁵e_g¹), forcing a double exchange FM state to anti-FM state.     

Relation of magneto-optical properties of free excitons to spin alignment of Mn2+ ions in Cd1−xMnxTe

A direct comparison of the splitting of free exciton states with the magnetic moment of the Mn²⁺ ion system shows excellent agreement with simple exchange interaction model throughout the composition range studied (0.005 < x < 0.3) at liquid helium temperature in magnetic field up to 5.6 T. Measurements of magnetic moments up to 15.5 T at 1.5 K show paramagnetic behaviour of samples with low manganese contents. With increasing amount of manganese mile fraction, strong influence of interaction of antiferromagnetic type between Mn²⁺ ions is observed. Comparison of optical and magnetic data yields refined values of exchange integrals of Mn²⁺ ions with conduction and valence electrons: 0.22 and ?0.88 eV, respectively.     

量子点操控的光子探测和圆偏振光子发射

半导体量子点是研究光子与电子态相互作用的优选固态体系,并在光子探测和发射两个方向上展现出独特的技术机遇.其中基于量子点的共振隧穿结构被认为在单光子探测方面综合性能最佳,但受到光子数识别、工作温度两个关键性能的制约.利用腔模激子态外场耦合效应,有望获得圆偏振态可控的高频单光子发射.本文介绍作者提出的量子点耦合共振隧穿（QD-cRTD）的光子探测机理,利用量子点量子阱复合电子态的隧穿放大,将QD-cRTD光子探测的工作温度由液氦提高至液氮条件,光电响应的增益达到10⁷以上,并具备双光子识别能力;同时,由量子点能级的直接吸收,原型器件获得了近红外的光子响应.在量子点光子发射机理的研究方面,作者实现了量子点激子跃迁和微腔腔模共振耦合的磁场调控,在Purcell效应的作用下增强激子自旋态的自发辐射速率,从而增强量子点中左旋或右旋圆偏振光的发射强度,圆偏度达到90%以上,形成一种光子自旋可控发射的新途径.     

Studies on Electronic Structure and Magnetic Properties of an Organic Magnet with Metallic Mn^2＋ and Cu^2＋ Ions

The electronic structure and the magnetic properties of the non-pure organic ferromagnetic compound MnCu(pbaOH)(H2O)3 with pbaOH=2-hydroxy-1, 3-propylenebis (oxamato) are studied by using the density-functional theory with local-spin-density approximation. The density of states, total energy, and the spin magnetic moment are calculated. The calculations reveal that the compound MnCu(pbaOH)(H2O)3 has a stable metal-ferromagnetic ground state, and the spin magnetic moment per molecule is 2.208 μa, and the spin magnetic moment is mainly from Mn ionand Cu ion. An antiferromagnetic order is expected and the antiferromagnetic exchange interaction of d-electrons of Cu and Mn passes through the antiferromagnetic interaction between the adjacent O, 0, and N atoms along the path linking the atoms Cu and Mn.     

金属有机化学气相沉积生长Zn1-xMnxSe薄膜的发光和磁光性质

利用金属有机化学气相沉积(MOCVD)方法在GaAs衬底上生长了不同组分的Zn_1-xMn_xSe薄膜。X射线衍射和X射线摇摆曲线证明样品具有较好的结晶质量。在低温、强磁场下对样品的发光进行了研究,在带边附近观察到两个发光峰的相对强度随着磁场增强发生了变化。通过变温光谱探讨了这两个发光峰的来源,并被分别归因于自由激子跃迁和与Mn有关的束缚态激子跃迁。同时随着磁场的增强,ZnMnSe带隙发光红移是由于类S带和类P带电子与Mn离子的3d⁵电子的自旋交换作用。     

Effects of a longitudinal magnetic field on spin injection and detection in InAs/GaAs quantum dot structures

Effects of a longitudinal magnetic field on optical spin injection and detection in InAs/GaAs quantum dot (QD) structures are investigated by optical orientation spectroscopy. An increase in the optical and spin polarization of the QDs is observed with increasing magnetic field in the range 0-2?T, and is attributed to suppression of exciton spin depolarization within the QDs that is promoted by the hyperfine interaction and anisotropic electron-hole exchange interaction. This leads to a corresponding enhancement in spin detection efficiency of the QDs by a factor of up to 2.5. At higher magnetic fields, when these spin depolarization processes are quenched, the electron spin polarization in anisotropic QD structures (such as double QDs that are preferably aligned along a specific crystallographic axis) still exhibits a rather strong field dependence under non-resonant excitation. In contrast, such a field dependence is practically absent in more 'isotropic' QD structures (e.g.?single QDs). We attribute the observed effect to stronger electron spin relaxation in the spin injectors (i.e.?wetting layer and GaAs barriers) of the lower-symmetry QD structures, which also explains the lower spin injection efficiency observed in these structures.