The exciton and biexciton binding energy have been studied for a ZnSe/ZnS core/shell quantum dot using WKB (Wentzel-Kramers-Brillouin) approximation. The exciton binding energy increases for small shell thickness and for large thickness, the binding energy again starts decreasing. A similar result is obtained for biexcitons where for thicker shells, the biexciton attains antibonding.
Using the transfer matrix method and the effective-mass approximation, the effect of resonant states on spin transport is studied in ZnSe/ZnMnSe/ZnSe/ZnMnSe/ZnSe structures under the influence of both electric and magnetic fields. The numerical results show that the ZnMnSe layers, which act as spin filters, polarize the electric currents. Variation of thickness of the central ZnSe layer shifts the resonant levels and exhibits an oscillatory behavior in spin current densities. It is also shown that the spin polarization of the tunneling current in geometrical asymmetry of the heterostructure wh…
We present a detailed investigation of excitonic absorption in $Zn_{0.69}Cd_{0.31}Se/ZnSe$ quantum wells under the application of a perpendicular magnetic field. The large energy separation between heavy- and light-hole excitons allows us to clearly resolve and identify magneto-excitonic absorption resonant with the continuum edge of the 1S heavy-hole exciton. Experimental values of the exciton binding energy are compared with results of a theoretical model that includes the exciton-phonon interaction. The remarkable agreemeent found unambiguously indicates the predominant polaronic character …
In this work we present how the optical properties of ZnSe nanowires are modified by the presence of Ag nanoparticles on the sidewalls of the ZnSe nanowires. In particular we show that the low-temperature luminescence of the ZnSe nanowires changes its shape, enhancing the phonon-replicas of impurity related recombination and affecting rise and decay times of the transient absorption bleaching at room temperatures, with an increase of the former and a decrease of the latter. In contrast, the deposition of Au NPs on the ZnSe nanowires does not change the optical properties of the sample. We sugg…
We have studied the effects of Mn concentration on the ballistic spin-polarized transport through diluted magnetic semiconductor heterostructures with a single paramagnetic layer. Using a fitted function for zero-field conduction band offset based on the experimental data, we found that the spin current densities strongly depend on the Mn concentration. The magnitude as well as the sign of the electron-spin polarization and the tunnel magnetoresistance can be tuned by varying the Mn concentration, the width of the paramagnetic layer, and the external magnetic field. By an appropriate choice of…
Optical emission from type-II ZnTe/ZnSe quantum dots demonstrates large and persistent oscillations in both the peak energy and intensity indicating the formation of coherently rotating states. Furthermore, the Aharanov-Bohm (AB) effect is shown to be remarkably robust and persists until 180K. This is at least one order of magnitude greater than the typical temperatures in lithographically defined rings. To our knowledge this is the highest temperature at which the AB effect has been observed in semiconductor structures.
We calculate the tunneling magnetoresistance (TMR) of Fe$\mid$ZnSe$\mid$Fe$\mid$ZnSe$\mid$Fe (001) double magnetic tunnel junctions as a function of the in-between Fe layer's thickness, and compare these results with those of Fe$\mid$ZnSe$\mid$Fe simple junctions. The electronic band structures are modeled by a parametrized tight-binding Hamiltonian fitted to {\it ab initio} calculations, and the conductance is calculated within the Landauer formalism expressed in terms of Green's functions. We find that the conductances for each spin channel and the TMR strongly depend on the in-between Fe la…
Radiative cascades emit correlated photon pairs, providing a pathway for the generation of entangled photons. The realization of a radiative cascade with impurity atoms in semiconductors, a leading platform for the generation of quantum light, would therefore provide a new avenue for the development of entangled photon pair sources. Here we demonstrate a radiative cascade from the decay of a biexciton at an impurity-atom complex in a ZnSe quantum well. The emitted photons show clear temporal correlations revealing the time--ordering of the cascade. Our result establishes impurity atoms in ZnSe…
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…
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 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…
Quantum dots consisting of an axial Zn0.97Mg0.03Te insertion inside a large bandgap Zn0.9Mg0.1Te nanowire cores are fabricated in a molecular beam epitaxy system by employing the vapor-liquid-solid growth mechanism. Additionally, this structure is coated with a thin ZnSe radial shell which forms type II interface with the dot semiconductor. The resulting radial electron-hole separation is evidenced by several distinct effects which occur in the presence of ZnSe shell, including: the optical emission redshift of about 250 meV, a significant decrease of the emission intensity, the increase of th…
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…
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 study optical harmonic generation on the 1S exciton-polariton in the semiconductor ZnSe. Intense and spectrally narrow exciton resonances are found in optical second (SHG), third (THG), and fourth (FHG) harmonic generation spectra. The resonances are shifted to higher energy by 3.2 meV from the exciton energy in the linear reflectivity spectrum. Additional resonances are observed in the THG and FHG spectra and assigned to combinations of incident and backscattered photons in the crystal. Rotational anisotropy diagrams are measured and further information on the origin of the optical harmoni…
Optical harmonic generation on excitons is found in ZnSe/BeTe quantum wells with type-II band alignment. Two experimental approaches with spectrally-broad femtosecond laser pulses and spectrally-narrow picosecond pulses are used for spectroscopic studies by means of second and third harmonic generation (SHG and THG). The SHG signal is symmetry-forbidden for light propagation along the structure's growth axis, which is the [001] crystal axis, but can be induced by an external magnetic field. The THG signal is detected at zero magnetic field and its intensity is field independent. A group theory…
Temperature dependence and recombination behavior of trapped charge carriers in ZnCdSe/ZnSe multiple quantum wells are investigated employing surface acoustic waves. These weakly perturb the carrier system, but remain highly sensitive even at small conductivities. Using this non-invasive probe we are able to detect persistent photoconductivity minutes after optical excitation. Measurement of exciting photon energies, the temperature dependence and ability to quench the conductivity with energies lower than the bandgap, support the notion of spatial separation of electrons and holes in the well…
The in-plane transport of excitons in ZnSe quantum wells is investigated directly by microphotoluminescence in combination with a solid immersion lens. Due to the strong Froehlich coupling, the initial kinetic energy of the excitons is well controlled by choosing the excess energy of the excitation laser. When increasing the laser excess energy, we find a general trend of increasing transport length and more importantly a pronounced periodic quenching of the transport length when the excess energy corresponds to multiples of the LO-phonon energy. Such features show the dominant role of the kin…
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…
Electronic structure and transport characteristics of coupled CdS and ZnSe quantum dots are studied using density functional theory and non equilibrium Greens function method respectively. Our investigations show that in these novel coupled dots, the frontier occupied and unoccupied molecular orbitals are spatially located in two different parts of the coupled dot, thereby indicating the possibility of asymmetry in electronic transport. We have calculated electronic transport through the coupled quantum dot by varying the coupling strength between the individual quantum dots in the limits of w…
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…
The spin dynamics of the strongly localized, donor-bound electrons in fluorine-doped ZnSe epilayers is studied by pump-probe Kerr rotation techniques. A method exploiting the spin inertia is developed and used to measure the longitudinal spin relaxation time, $T_1$, in a wide range of magnetic fields, temperatures, and pump densities. The $T_1$ time of the donor-bound electron spin of about 1.6 $μ$s remains nearly constant for external magnetic fields varied from zero up to 2.5 T (Faraday geometry) and in a temperature range $1.8-45$ K. The inhomogeneous spin dephasing time, $T_2^*=8-33$ ns, i…
We have studied the electronic structure of CdS/ZnSe coupled quantum dot, a novel heterostructure at the nano-scale. Our calculations reveal CdS/ZnSe coupled quantum dots to be of type-II in nature where the anion-p states play an important role in deciding the band offset for the highest occupied molecular orbitals (HOMO). We show that the offsets of HOMO as well as the lowest unoccupied molecular orbitals (LUMO) can be tuned by changing the sizes of the components of the coupled quantum dot, thereby providing an additional control parameter to tune the band gap and the optical properties. Ou…
Defects in wide-bandgap semiconductors are promising qubit candidates for quantum communication and computation. Epitaxially grown II-VI semiconductors are particularly promising host materials due to their direct bandgap and potential for isotopic purification to a spin-zero nuclear background. Here, we show a new type of single photon emitter with potential electron spin qubit based on Cl impurities in ZnSe. We utilize a quantum well to increase the binding energies of donor emission and confirm single photon emission with short radiative lifetimes of 192 ps. Furthermore, we verify that the …
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…
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…
Photoluminescence (PL) of the 50 nm $Zn_{0.9}Be_{0.05}Mn_{0.05}Se$/ $d$ nm $Zn_{0.943}Be_{0.057}Se$/ 2.5 nm $ZnSe$/ 30 nm $Zn_{0.943}Be_{0.057}Se$ structures is investigated as a function of magnetic field ($B$) and thickness ($d$) of intermediate $Zn_{0.943}Be_{0.057}Se$ nonmagnetic barrier between the $Zn_{0.9}Be_{0.05}Mn_{0.05}Se$ semimagnetic barrier and $ZnSe$ quantum well at the temperature 1.2 K. The rate of the shift of different PL bands of the structures under study is estimated in low and high magnetic fields. The causes of the shift rate increase under pass from low to high magneti…
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…
Using a single-band model, the lowest transition energy was analysed between the lowest unoccupied molecular orbital (LUMO) of the conduction band and the highest occupied molecular orbital (HOMO) of the valence band. We focus on categorising the confinement strength in type-II core-shell quantum dots (CSQDs) based on the step-potential and show how it will affect their transition energy. Our model is applied to CSQDs of the heterostructures PbS/CdS and ZnTe/ZnSe through narrow and wide band gaps, respectively. It found that PbS/CdS CSQDs demonstrates a strong confinement in which their transi…
We used continuous wave photoluminescence (cw-PL) and time resolved photoluminescence (TR-PL) spectroscopy to compare the properties of magnetic polarons (MP) in two related spatially indirect II-VI epitaxially grown quantum dot systems. In the ZnTe/(Zn,Mn)Se system the holes are confined in the non-magnetic ZnTe quantum dots (QDs), and the electrons reside in the magnetic (Zn,Mn)Se matrix. On the other hand, in the (Zn,Mn)Te/ZnSe system, the holes are confined in the magnetic (Zn,Mn)Te QDs, while the electrons remain in the surrounding non-magnetic ZnSe matrix. The magnetic polaron formation …
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 report on a comprehensive experimental and theoretical study of optical third harmonic generation (THG) on the exciton-polariton resonances in the zinc-blende semiconductors GaAs, CdTe, and ZnSe subject to an external magnetic field, representing a topic that had remained unexplored so far. In these crystals, crystallographic THG is allowed in the electric-dipole approximation, so that no strong magnetic-field-induced changes of the THG are expected. Therefore, it comes as a total surprise that we observe a drastic enhancement of the THG intensity by a factor of fifty for the $1s$-exciton-p…
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…
Having already achieved near-unity quantum yields, with promising properties for light-emitting diode, lasing, and charge separation applications, colloidal core/shell quantum dots have great technological potential. The shell thickness and band alignment of the shell and core materials are known to influence the efficiency of these devices. In many such applications, a key to improving the efficiency requires a deep understanding of multiexcitonic states. Herein, we elucidate the shell thickness and band alignment dependencies of the biexciton Auger recombination lifetime for quasi-type-II Cd…
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 optimized the performance of quantum confined Stark effect QCSE based voltage nanosensors. A high throughput approach for single particle QCSE characterization was developed and utilized to screen a library of such nanosensors. Type II ZnSe CdS seeded nanorods were found to have the best performance among the different nanosensors evaluated in this work. The degree of correlation between intensity changes and spectral changes of the excitons emission under applied field was characterized. An upper limit for the temporal response of individual ZnSe CdS nanorods to voltage modulation was char…
A one-band model within the effective mass approximation is adopted to characterize the energy structure and oscillator strength of type-II semiconductor spherical core-shell quantum dots. The heteroepitaxial strain of the core-shell heterostructure is modeled by the elastic continuum approach. The model is applied to ZnTe/ZnSe core-shell, a wide band gap type-II heterostructure. The simulated absorption spectra are in fair agreement with available experimental results.
New schemes for the nuclear spin quantum memory are proposed based on a system composed of two electrons or one electron coupled to a single nuclear spin in isotopically purified group IV elemental and II-VI compound semiconductors. The qubit consists of the singlet state and one of the triplet states of two electrons or simply of an electron spin. These systems are free from the decoherence due to the nuclear dipole-dipole interaction and are advantageous for the long memory time. In the case of two electrons, the protocol for the quantum state transfer between the electron spin qubit and the…
Current imaging scanning tunneling microscopy is used to observe the electronic wavefunctions in InAs/ZnSe core/shell nanocrystals. Images taken at a bias corresponding to the s conduction band state show that it is localized in the central core region, while images at higher bias probing the p state reveal that it extends to the shell. This is supported by optical and tunneling spectroscopy data demonstrating that the s-p gap closes upon shell growth. Shapes of the current images resemble atom-like envelope wavefunctions of the quantum dot calculated within a particle in a box model.
Excitons in vertically stacked type-II quantum dots experience the topological magnetic phase and demonstrate the Aharonov-Bohm oscillations in the emission intensity. Photoluminescence of vertically stacked ZnTe/ZnSe quantum dots is measured in magnetic fields up to 31 T. The Aharonov-Bohm oscillations are found in the magnetic-field dependence of emission intensity. The positions of the peaks of the emission intensity are in a good agreement with numerical simulations of excitons in stacked quantum dots.
We report on the first experimental determination of the coherence length of excitons in semiconductors using the combination of spatially resolved photoluminescence with phonon sideband spectroscopy. The coherence length of excitons in ZnSe quantum wells is determined to be 300 ~ 400 nm, about 25 ~ 30 times the exciton de Broglie wavelength. With increasing exciton kinetic energy, the coherence length decreases slowly. The discrepancy between the coherence lengths measured and calculated by only considering the acoustic phonon scattering suggests an important influence of static disorder.
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.
We theoretically investigate the nonlinear optical response of a heterodimer comprising a semiconductor quantum dot strongly coupled to a metal nanoparticle. The quantum dot is considered as a three-level ladder system with ground, one-exciton, and bi-exction states. As compared to the case of a two-level quantum dot model, adding the third (bi-exciton) state produces fascinating effects in the optical response of the hybrid system. Specifically, we demonstrate that the system may exhibit picosecond and sub-picosecond self-oscillations and quasi-chaotic behaviour under {\it single}-frequency c…
We investigate the energy relaxation of excitons during the real-space transport in ZnSe quantum wells by using microphotoluminescence with spatial resolution enhanced by a solid immersion lens. The spatial evolution of the LO-phonon sideband, originating from the LO-phonon assisted recombination of hot excitons, is measured directly. By calculating the LO-phonon assisted recombination probability, we obtain the nonthermal energy distribution of excitons and observe directly the energy relaxation of hot excitons during their transport. We find the excitons remain hot during their transport on …
