CdSe/ZnSe quantum dot with a single Mn$^{2+}$ ion - a new system for a single spin manipulation
Tomasz Smoleński
备注：
7 pages, 4 figures, submitted to Journal of Applied Physics as proceedings of the 32nd International Conference on the Physics of Semiconductors (ICPS 2014)
We present a magneto-optical study of individual self-assembled CdSe/ZnSe quantum dots doped with single Mn$^{2+}$ ions. Properties of the studied dots are analyzed analogously to more explored system of Mn-doped CdTe/ZnTe dots. Characteristic sixfold splitting of the neutral exciton emission line as well as its evolution in the magnetic field are described using a spin Hamiltonian model. Dynamics of both exciton recombination and Mn$^{2+}$ spin relaxation are extracted from a series of time-resolved experiments. Presence of a single dopant is shown not to affect the average excitonic lifetime measured for a number of nonmagnetic and Mn-doped dots. On the other hand, non-resonant pumping is demonstrated to depolarize the Mn$^{2+}$ spin in a quantum dot placed in external magnetic field. This effect is utilized to determine the ion spin relaxation time in the dark.
Circularly polarized optical excitation is used to demonstrate the efficient injection of spin-polarized excitons to individual self-assembled CdSe quantum dots in ZnSe barrier. The exciton spin-transfer is studied by means of polarization-resolved single dot spectroscopy performed in magnetic field applied in Faraday configuration. Detailed analysis of the neutral exciton photoluminescence spectra reveals the presence of exciton spin relaxation during its lifetime in a quantum dot. This process is seen for both nonmagnetic dots and those containing single Mn$^{2+}$ ions. Taking this into acco…
We present a polarization-resolved photoluminescence study of the exchange interaction effects in a prototype system consisting of an individual Fe2+ ion and a single neutral exciton confined in a CdSe/ZnSe quantum dot. Maximal possible number of eight fully linearly-polarized lines in the bright exciton emission spectrum is observed, evidencing complete degeneracy lifting in the investigated system. We discuss conditions required for such a scenario to take place: anisotropy of the electron-hole interaction and the zero-field splitting of the Fe2+ ion spin states. Neglecting of either of thes…
ZnSe nanowire heterostructures were grown by molecular beam epitaxy in the vapour-liquid-solid growth mode assisted by gold catalysts. Size, shape and crystal structure are found to strongly depend on the growth conditions. Both, zinc-blende and wurtzite crystal structures are observed using transmission electron microscopy. At low growth temperature, cone-shaped nano-needles are formed. For higher growth temperature, the nanowires are uniform and have a high aspect ratio with sizes of 1-2 $μ$m in length and 20-50 nm in width as observed by scanning electron microscopy. Growing a nanowire on t…
We present a detailed spectroscopic study of the photoluminescence quenching in an epitaxial structures containing CdSe/ZnSe quantum dots doped with low concentration of Mn$^{2+}$ ions. Our time-resolved and time-integrated experiments reveal the origin of the quenching observed in macro-photoluminescence studies of ensembles of such dots. We show that incorporation of even a few ions to an individual dot does not quench its luminescence effectively, although some fingerprints of expected spin-dependent quenching are visible. At the same time, the presence of Mn$^{2+}$ ions in the sample signi…
Exciton luminescence of a CdSe quantum dot (QD) inserted in a ZnSe nanowire is strongly influenced by the dark exciton states. Because of the small size of these QDs (2-5nm), exchange interaction between hole and electron is highly enhanced and we measured large energy splitting between bright and dark exciton states ($ΔE\in [4, 9.2 ]$ meV) and large spin flip rates between these states. Statistics on many QDs showed that this splitting depends on the QD size. Moreover, we measured an increase of the spin flip rate to the dark states with increasing energy splitting. We explain this observatio…
Magnetic doping of semiconductor nanostructures is actively pursued for applications in magnetic memory and spin-based electronics. Central to these efforts is a drive to control the interaction strength between carriers (electrons and holes) and the embedded magnetic atoms. In this respect, colloidal nanocrystal heterostructures provide great flexibility via growth-controlled `engineering' of electron and hole wavefunctions within individual nanocrystals. Here we demonstrate a widely tunable magnetic sp-d exchange interaction between electron-hole excitations (excitons) and paramagnetic manga…
Ultrafast transmission changes around the fundamental trion resonance are studied after exciting a p-shell exciton in a negatively charged II-VI quantum dot. The biexcitonic induced absorption reveals quantum beats between hot trion states at 133 GHz. While interband dephasing is dominated by relaxation of the P-shell hole within 390 fs, trionic coherence remains stored in the spin system for 85 ps due to Pauli blocking of the triplet electron. The complex spectro-temporal evolution of transmission is explained analytically by solving the Maxwell-Liouville equations. Pump and probe polarizatio…
We present a comparative study of two self-assembled quantum dot (QD) systems based on II-VI compounds: CdTe/ZnTe and CdSe/ZnSe. Using magneto-optical techniques we investigated a large population of individual QDs. The systematic photoluminescence studies of emission lines related to the recombination of neutral exciton X, biexciton XX, and singly charged excitons (X$^+$, X$^-$) allowed us to determine average parameters describing CdTe QDs (CdSe QDs): X-XX transition energy difference 12 meV (24 meV); fine-structure splitting $δ_{1}=$0.14 meV ($δ_{1}=$0.47 meV); $g$-factor $g=$2.12 ($g=$1.71…
Colloidal core/shell InP/ZnSe quantum dots (QDs), recently produced using an improved synthesis method, have a great potential in life-science applications as well as in integrated quantum photonics and quantum information processing as single-photon emitters. Single-particle spectroscopy of 10-nm QDs with 3.2-nm cores reveals strong photon antibunching attributed to fast (70-ps) Auger recombination of multiple excitons. The QDs exhibit very good photostability under strong optical excitation. We demonstrate that the antibunching is preserved when the QDs are excited above the saturation inten…
Cd(Se,Te) Quantum Dots (QD) in ZnSe barrier typically exhibit a very high spectral density, which precludes investigation of single dot photoluminescence. We design, grow and study individual Cd(Se,Te)/ZnSe QDs of low spectral density of emission lines achieved by implementation of a Mn-assisted epitaxial growth. We find an unusually large variation of exciton-biexciton energy difference (3 meV $\leq$ $Δ\mathrm{E_{X-XX}}$ $\leq$ 26 meV) and of exciton radiative recombination rate in the statistics of QDs. We observe a strong correlation between the exciton-biexciton energy difference, exciton …
The lattice mismatch strain field of core/multishell structures with spherical symmetry is modeled by a linear continuum elasticity approach. The effect of the strain on the energy structure and linear optical absorption in large core/shell/shell spherical semiconductor quantum dots is analyzed. Localization of the photoexcited carriers induced by coating is found to play an important role in explaining the optical stability of large CdSe/CdS/ZnS and ZnTe/ZnSe/ZnS quantum dots.
We have studied spectral diffusion of the photoluminescence of a single CdSe quantum dot inserted in a ZnSe nanowire. We have measured the characteristic diffusion time as a function of pumping power and temperature using a recently developed technique [G. Sallen et al, Nature Photon. \textbf{4}, 696 (2010)] that offers subnanosecond resolution. These data are consistent with a model where only a \emph{single} carrier wanders around in traps located in the vicinity of the quantum dot.
The radiative recombination rates of interacting electron-hole pairs in a quantum dot are strongly affected by quantum correlations among electrons and holes in the dot. Recent measurements of the biexciton recombination rate in single self-assembled quantum dots have found values spanning from two times the single exciton recombination rate to values well below the exciton decay rate. In this paper, a Feynman path-integral formulation is developed to calculate recombination rates including thermal and many-body effects. Using real-space Monte Carlo integration, the path-integral expressions f…
We investigate spin properties of a Fe2+ dopant, known for having single nondegenerate ground state in bulk host semiconductor. Due to zero magnetic moment such a ground state is of little use for spintronics and solotronics. We show that this well-established picture of Fe2+ spin configuration can be contradicted by subjecting the Fe2+ ion to sufficiently high strain, e.g., resulting from lattice mismatched epitaxial heterostructures. Our analysis reveals that high strain induces qualitative change in the ion energy spectrum and results in doubly degenerate ground state with spin projection S…
We report magneto-photoluminescence studies of strongly quantum-confined "0-D" diluted magnetic semiconductors (DMS), realized in Mn$^{2+}$-doped ZnSe/CdSe core/shell colloidal nanocrystals. In marked contrast to their 3-D (bulk), 2-D (quantum well), 1-D (quantum wire), and 0-D (self-assembled quantum dot) DMS counterparts, the ubiquitous yellow emission band from internal \emph{d-d} ($^4T_1 \rightarrow ^6A_1$) transitions of the Mn$^{2+}$ ions in these nanocrystals is \emph{not} suppressed in applied magnetic fields and \emph{does} become circularly polarized. This polarization tracks the Mn$…
Owing to exchange interaction between the exciton and magnetic ion, a quantum dot embedding a single magnetic ion is a great platform for optical control of individual spin. In particular, a quantum dot provides strong and sharp optical transitions, which give experimental access to spin states of an individual magnetic ion. We show, however, that physics of quantum dot excitons also complicate spin readout and optical spin manipulation in such a system. This is due to electron-hole exchange interaction in anisotropic quantum dots, which affects the polarization of the emission lines. One of t…
Nanoscale devices are being extensively studied for their tunable electronic and optical properties, but the influence of impurities and defects is amplified at these length scales and can lead to poorly understood variations in characteristics of semiconducting materials. By performing a large ensemble of photoconductivity measurements in nanogaps bridged by core-shell CdSe/ZnS semiconductor nanocrystals, we discover optoelectronic methods for affecting solid-state charge trap populations. We introduce a model that unifies previous work and transforms the problem of irreproducibility in nanoc…
Semiconductor nanowires offer the possibility to grow high-quality quantum-dot heterostructures, and, in particular, CdSe quantum dots inserted in ZnSe nanowires have demonstrated the ability to emit single photons up to room temperature. In this paper, we demonstrate a bottom-up approach to fabricate a photonic fiberlike structure around such nanowire quantum dots by depositing an oxide shell using atomic-layer deposition. Simulations suggest that the intensity collected in our NA = 0.6 microscope objective can be increased by a factor 7 with respect to the bare nanowire case. Combining micro…
Electron transfer to an individual quantum dot promotes the formation of charged excitons with enhanced recombination pathways and reduced lifetimes. Excitons with only one or two extra charges have been observed and exploited for very efficient lasing or single quantum dot LEDs. Here, by room-temperature time-resolved experiments on individual giant-shell CdSe/CdS quantum dots, we show the electrochemical formation of highly charged excitons containing more than twelve electrons and one hole. We report the control over intensity blinking, along with a deterministic manipulation of quantum dot…
