Searcharxiv⌕ Search

arXiv subjects

A. A. Golovatenko

Publications and source records attributed to A. A. Golovatenko.

8 recordsLinked to original sources

Band offsets in InP/ZnSe nanocrystals evaluated using two-photon transitions analysis

We present a semi-analytical theoretical kp-study of the energy structure and optical transitions in spherical core-shell InP/ZnSe nanocrystals. We use the eight-band Kane model and the six-band Luttinger Hamiltonian in the spherical approximation to calculate the electron and hole energy spectra, respectively. The influence of the Coulomb interaction is considered perturbatively. The one- and two-photon absorption spectra are calculated as functions of the band offsets between the InP core and ZnSe shell. Exciton states responsible for the main features in the two-photon absorption spectra of InP/ZnSe nanocrystals are identified and the spectral dependence of the linear-circular dichroism signal is predicted. We show that in the presence of inhomogeneous broadening, the transition to the ground two-photon-active exciton state can be hidden behind intense transitions to higher-lying states. A comparison of the calculated one- and two-photon absorption spectra with the available experimental data shows that, depending on the lattice strain in the InP core, the range of possible valence band offsets is 0.85-1 eV. The determined range exceeds the natural valence band offset of 0.57 eV and indicates the presence of electric dipoles formed by the preferential Zn-P bonds at the InP/ZnSe heterointerface.

cond-mat.mes-hall↗

Cascade spin dynamics of excitons localized in indirect-band-gap (In,Al)As/AlAs quantum dots with type-I band alignment

We investigate the spin dynamics of excitons localized in type I (In,Al)As/AlAs quantum dots with an indirect in momentum space band structure. Polarized selective photoluminescence spectroscopy, i.e. fluorescence line narrowing, under magnetic fields up to 5 T applied in the Faraday geometry is employed. The experiment reveals a cascade spin evolution process of excitons in the indirect band-gap quantum dots: an initial short term spin dynamics associated with excited direct exciton states possessing a large oscillator strength is followed by electron relaxation into the X valley of the Brillouin zone and subsequent long term spin dynamics of indirect excitons. The two step mechanism manifests itself in the distinct features of the magnetic field dependences of photoluminescence: two component recovery of optical orientation, two component linear to circular polarization conversion and the presence of the linear polarization plane rotation. At the same time, suppression of the optical alignment shows one-component behavior governed by the spin dynamics of the indirect exciton states. Within the pseudospin formalism, we derive analytical expressions that quantitatively describe the observed dependences and yield estimates for the anisotropic exchange splitting: 210 μeV for direct excitons and 1.3 μeV for indirect excitons. Further analysis using the density matrix formalism agrees well with the pseudospin model calculations and shows that the finite optical orientation at zero magnetic field is due to comparable magnitudes of the anisotropic splitting of the indirect exciton states and the splitting of the X-valley electron states caused by the hyperfine interaction with nuclei.

cond-mat.mes-hall↗

Cubic anisotropy of hole Zeeman splitting in semiconductor nanocrystals

We study theoretically cubic anisotropy of Zeeman splitting of a hole localized in semiconductor nanocrystal. This anisotropy originates from three contributions: crystallographic cubically-symmetric spin and kinetic energy terms in the bulk Luttinger Hamiltonian and the spatial wave function distribution in a cube-shaped nanocrystal. From symmetry considerations, an effective Zeeman Hamiltonian for the hole lowest even state is introduced, containing a spherically symmetric and a cubically symmetric term. The values of these terms are calculated numerically for spherical and cube-shaped nanocrystals as functions of the Luttinger Hamiltonian parameters. We demonstrate that the cubic shape of the nanocrystal and the cubic anisotropy of hole kinetic energy (so called valence band warping) significantly affect effective $g$ factors of hole states. In both cases, the effect comes from the cubic symmetry of the hole wave functions in zero magnetic field. Estimations for the effective $g$ factor values in several semiconductors with zinc-blende crystal lattices are made. Possible experimental manifestations and potential methods of measurement of the cubic anisotropy of the hole Zeeman splitting are suggested.

cond-mat.mes-hall↗

Electron, hole and exciton effective g-factors in semiconductor nanocrystals

We review the existing and present the new results of $\bf kp$ calculations of the electron, hole, and exciton effective $g$-factors in semiconductor nanocrystals of different shape and symmetry. We propose a simple yet accurate method for calculation of electron $g$-factor size dependence in bare nanocrystals within the eight-band Kane model. Using the spherical approximation for Luttinger Hamiltonian we find the dependence of hole $g$-factor on light to heavy hole effective mass ratio in semiconductor nanostructures with spherical, axial, and cubically symmetric shape. We show that the non-equidistant Zeeman splitting of the four-fold degenerate hole state may take place in cube and spheroidal nanocrystals. We present a comparison of the calculated hole $g$-factors in nanostructures based on II-VI and III-V semiconductors for different sets of the Luttinger parameters and analyze the main effects contributing to the $g$-factor renormalization with the respect to the bulk value. We discuss different approaches to the definition of the hole and exciton $g$-factors which should be taken into account during the analysis of the experimental data and compare our results of $g$-factor calculations with the experimental data for semiconductor spherical nanocrystals and thin nanoplatelets available in the literature.

cond-mat.mes-hall↗

Magneto-optics of excitons interacting with magnetic ions in CdSe/CdMnS colloidal nanoplatelets

Excitons in diluted magnetic semiconductors represent excellent probes for studying the magnetic properties of these materials. Various magneto-optical effects, which depend sensitively on the exchange interaction of the excitons with the localized spins of the magnetic ions can be used for probing. Here, we study core/shell CdSe/(Cd,Mn)S colloidal nanoplatelets hosting diluted magnetic semiconductor layers. The inclusion of the magnetic Mn$^{2+}$ ions is evidenced by three magneto-optical techniques using high magnetic fields up to 15 T: polarized photoluminescence, optically detected magnetic resonance, and spin-flip Raman scattering. In particular, information on the Mn$^{2+}$ concentration in the CdS shell layers can be obtained from the spin-lattice relaxation dynamics of the Mn$^{2+}$ spin system.

cond-mat.mes-hall↗

Ground state of the holes localized in II-VI quantum dots with Gaussian potential profiles

We report on the theoretical study of the hole states in II-IV quantum dots of a spherical and ellipsoidal shape, described by a smooth potential confinement profiles, that can be modelled by a Gaussian functions in all three dimensions. The universal dependencies of the hole energy, $g$-factor and localization length on a quantum dot barrier height, as well as the ratio of effective masses of the light and heavy holes are presented for the spherical quantum dots. The splitting of the four-fold degenerate ground state into two doublets is derived for anisotropic (oblate or prolate) quantum dots. Variational calculations are combined with numerical ones in the framework of the Luttinger Hamiltonian. Constructed trial functions are optimized by comparison with the numerical results. The effective hole $g$-factor is found to be independent on the quantum dot size and barrier height and is approximated by simple universal expression depending only on the effective mass parameters. The results can be used for interpreting and analyzing experimental spectra measured in various structures with the quantum dots of different semiconductor materials.

cond-mat.mes-hall↗

Förster energy transfer of dark excitons enhanced by a magnetic field in an ensemble of CdTe colloidal nanocrystals

We present a systematic experimental study along with theoretical modeling of the energy transfer in an ensemble of closely-packed CdTe colloidal nanocrystals identified as the Förster resonant energy transfer (FRET). We prove that at low temperature of 4.2 K, mainly the ground dark exciton states in the initially excited small-size (donor) nanocrystals participate in the dipole-dipole FRET leading to additional excitation of the large-size (acceptor) nanocrystals. The FRET becomes possible due to the weak admixture of the bright exciton states to the dark states. The admixture takes place even in zero magnetic field and allows the radiative recombination of the dark excitons. An external magnetic field considerably enhances this admixture, thus increasing the energy transfer rate by a factor of 2-3 in a field of 15T, as well as the radiative rates of the dark excitons in the donor and acceptor nanocrystals. The theoretical modeling allows us to determine the spectral dependence of the probability for the NC to serve as a donor for larger nanocrystals, to evaluate the energy transfer rates as well as to predict their dependencies on the magnetic field, to describe the spectral shift of the photoluminescence maximum due to the energy transfer and to reproduce the experimentally observed spectral dependencies of the photoluminescence recombination dynamics in the magnetic field.

cond-mat.mes-hall↗

Exciton spin dynamics of colloidal CdTe nanocrystals in magnetic field

The recombination and spin dynamics of excitons in colloidal CdTe nanocrystals (NCs) are studied by time-resolved photoluminescence in high magnetic fields up to 15 T and at cryogenic temperatures. The recombination decay shows a nonexponential temporal behavior, with the longest component corresponding to the dark excitons having 260 ns decay time at zero magnetic field and 4.2 K temperature. This long component shortens to 150 ns at 15 T due to the magnetic-field-induced mixing of the bright and dark exciton states. The spin dynamics, assessed through the evolution of the magnetic-field-induced circular polarization degree of the photoluminescence, has a fast component shorter than 1 ns related to the bright excitons and a slow component of 5-10 ns associated with the dark excitons. The latter shortens with increasing magnetic field, which is characteristic for a phonon-assisted spin relaxation mechanism. The relatively low saturation level of the associated magnetic-field-induced circular polarization degree of -30 % is explained by a model that suggests the CdTe NCs to constitute an ensemble of prolate and oblate NCs, both having a structural quantization axis. The exciton g-factor of 2.4-2.9 evaluated from fitting the experimental data in the frame of the suggested approach is in good agreement with the expected value for the dark excitons in CdTe NCs.

cond-mat.mes-hall↗