Femtosecond Transfer and Manipulation of Persistent Hot-Trion Coherence in a Single CdSe/ZnSe Quantum Dot
Philipp Henzler, Christian Traum, Matthias Holtkemper, David Nabben, Marcel Erbe, Doris E. Reiter, Tilmann Kuhn, Suddhassatta Mahapatra, Karl Brunner, Denis V. … 展开作者
Philipp Henzler, Christian Traum, Matthias Holtkemper, David Nabben, Marcel Erbe, Doris E. Reiter, Tilmann Kuhn, Suddhassatta Mahapatra, Karl Brunner, Denis V. Seletskiy, Alfred Leitenstorfer
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 polarizations provide full control over amplitude and phase of the quantum beats.
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…
We present a theoretical description of excitons and positively and negatively charged trions in "giant" CdSe/CdS core-shell nanocrystals (NCs). The developed theory provides the parameters describing the fine structure of excitons in CdSe/CdS core/thick shell NCs as a function of the CdSe/CdS conduction band offset and the CdSe core radius. We have also developed a general theory describing the fine structure of positively charged trions created in semiconductor NCs with a degenerate valence band. The calculations take into account the complex structure of the CdSe valence band and inter-part…
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…
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…
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…
The optoelectronic properties of metal chalcogenide colloidal nanoplatelets are often interpreted in terms of excitonic states. However, recent spectroscopic experiments evidence the presence of trion states, enabled by the slow Auger recombination in these structures. We analyze how the presence of an additional charge in trions modifies the emission energy and oscillator strength as compared to neutral excitons. These properties are very sensitive to dielectric confinement and electronic correlations, which we describe accurately using image-charge and variational Quantum Monte Carlo methods…
A theory of the trion and biexciton in a nanowire (NW) in the framework of the effective-mass model using the Born-Oppenheimer approximation is presented. We consider the formation of trions and biexcitons under the action of both the lateral confinement and the localization potential. The analytical expressions for the binding energy and eigenfunctions of the trion and biexciton are obtained and expressed by means of matrix elements of the effective one-dimensional cusp-type Coulomb potentials whose parameters are determined self-consistently by employing the same eigenfunctions of the confin…
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…
The photon statistics of CdSe/CdS dot-in-rods nanocrystals is studied with a method involving post-selection of the photon detection events based on the photoluminescence count rate. We show that flickering between two states needs to be taken into account to interpret the single-photon emission properties. With post-selection we are able to identify two emitting states: the exciton and the charged exciton (trion), characterized by different lifetimes and different second order correlation functions. Measurements of the second order autocorrelation function at zero delay with post- selection s…
Recent experiments suggest that the photoluminescence line width of CdSe and CdSe/CdS nanoplatelets (NPLs) may be broadened by the presence of shakeup (SU) lines from negatively charged trions. We carry out a theoretical analysis, based on effective mass and configuration interaction (CI) simulations, to identify the physical conditions that enable such processes. We confirm that trions in colloidal NPLs are susceptible of presenting SU lines up to one order of magnitude stronger than in epitaxial quantum wells, stimulated by dielectric confinement. For these processes to take place trions mus…
We discuss photo-luminescence characteristics of CdSe core/shell quantum dots at cryogenic temperatures using a hybrid system of a single quantum dot and an optical nanofiber. The key point is to control the emission species of quantum dot to charged excitons, known as trions, which have superior characteristics to neutral excitons. We investigate the photocharging behavior for the quantum dots by varying the wavelength and intensity of irradiating laser light, and establish a method to create a permanently charged situation which lasts as long as the cryogenic temperature is maintained. The p…
We have analyzed the energetics of decay of the X^- trion (exciton + electron) on the assumption that the exciton and trion are independent excitations of a single two-dimensional semiconducting quantum well. For the first time, it has been shown that in filling a well with electrons from a selective donor-doped matrix, the binding energy of the trion (of the electron with the exciton) increases linearly with a shift of the Fermi level into the depth of the c band. This agrees with the well-known experimental data on the low-temperature radiative decay (photoluminescence) of trions in the hete…
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…
A computational model is presented to calculate the ground state energy of neutral and charged excitons confined in semiconductor quantum dots. The model is based on the variational Quantum Monte Carlo method and effective mass Hamiltonians. Through an iterative Newton-Rhapson process, minimizing the local energy, and (optional) parallelization of random walkers, fast and accurate estimates of both confinement and Coulomb binding energies can be obtained in standard desktop computers. To illustrate the reach of the model, we provide Fortran programs and illustrative calculations for colloidal …
We report on the experimental and theoretical studies of optical alignment and optical orientation effects in an ensemble of core/shell CdSe/CdS colloidal nanoplatelets. The dependences of three Stokes parameters on the magnetic field applied in the Faraday geometry are measured under continuous wave resonant excitation of the exciton photoluminescence. Theoretical model is developed to take into account both bright and dark exciton states in the case of strong electron and hole exchange interaction and random in-plane orientation of the nanoplatelets in ensemble. The data analysis allows us t…
We address spin properties and spin dynamics of carriers and charged excitons in CdSe/CdS colloidal nanoplatelets with thick shells. Magneto-optical studies are performed by time-resolved and polarization-resolved photoluminescence, spin-flip Raman scattering and picosecond pump-probe Faraday rotation in magnetic fields up to 30 T. We show that at low temperatures the nanoplatelets are negatively charged so that their photoluminescence is dominated by radiative recombination of negatively charged excitons (trions). Electron g-factor of 1.68 is measured and heavy-hole g-factor varying with incr…
The multiplication rates of hot carriers in CdSe quantum dots are quantified using an atomistic pseudopotential approach and first order perturbation theory. Both excited holes and electrons are considered, and electron-hole Coulomb interactions are accounted for. We find that holes have much higher multiplication rates than electrons with the same excess energy due to the larger density of final states (positive trions). When electron-hole pairs are generated by photon absorption, however, the net carrier multiplication rate is dominated by photogenerated electrons, because they have on avera…
We demonstrate the optical initialization of a hole-spin qubit bound to an isoelectronic center (IC) formed by a pair of Te impurities in ZnSe, an impurity/host system providing high optical homogeneity, large electric dipole moments, and long coherence times. The initialization scheme is based on the spin-preserving tunneling of a resonantly excited donor-bound exciton to a positively charged Te IC, thus forming a positive trion. The radiative decay of the trion within less than 50 ps leaves a heavy hole in a well-defined polarization-controlled spin state. The initialization fidelity exceeds…
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.
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 …
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…
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…
Photoluminescence (PL) intermittency is a ubiquitous phenomenon detrimentally reducing the temporal emission intensity stability of single colloidal quantum dots (CQDs) and the emission quantum yield of their ensembles. Despite efforts for blinking reduction via chemical engineering of the QD architecture and its environment, blinking still poses barriers to the application of QDs, particularly in single-particle tracking in biology or in single-photon sources. Here, we demonstrate the first deterministic all-optical suppression of quantum dot blinking using a compound technique of visible and…
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…
