SearcharxivSearch

arXiv subjects

Anna V. Rodina

Publications and source records attributed to Anna V. Rodina.

10 recordsLinked to original sources

Spin-dependent Raman and Brillouin light scattering on excitons in CsPbBr$_3$ perovskite crystals

The spin properties of excitons and charge carriers in CsPbBr$_3$ lead halide perovskite crystals are investigated by spin-dependent light scattering in magnetic fields up to 10 T. Spin-flip Raman scattering spectra measured under resonant excitation of exciton-polaritons show a rich variety of features provided by the Zeeman splittings of excitons and of electrons and holes interacting with the excitons. The magnitudes and anisotropies of their Land\'e $g$-factors are measured. A detailed consideration of the responsible mechanisms is presented and discussed in relation to the experimental data, in particular on the polarization properties of the Raman spectra. We consider several mechanisms for the combined spin-flip Raman scattering processes involving resident carriers and photoexcited excitons and suggest new ones, involving trions in the intermediate scattering state. A double electron spin-flip caused by the exciton interaction with two localized or donor-bound electrons is revealed. The spectral lines of Brillouin light scattering on exciton-polaritons shift in energy and become polarization-sensitive in magnetic field, evidencing the splitting of the exciton-polariton dispersion.

cond-mat.mtrl-sci

Coherent spin dynamics in ensembles of randomly oriented singly charged colloidal nanoplatelets and nanocrystals

We present a theoretical study of the pump-probe Faraday rotation and ellipticity signals in ensembles of uniaxially anisotropic CdSe nanoplatelets and nanocrystals. We use the Faraday rotation mechanism based on the excitation of negative heavy hole trions for a magnetic field applied in the Voigt geometry. Three types of ensembles with typical spatial distributions of the orientation of the anisotropy axis with respect to the direction of light propagation are considered. Faraday rotation and ellipticity signals are modeled for excitation by single and repeated pump pulses, taking into account the anisotropy of the electron g-factor. We show that spin dephasing caused by the electron g-factor anisotropy and the arbitrary orientation of nanoplatelets or nanocrystals result only in partial damping of oscillation amplitude in contrast to the dephasing caused by the dispersion of the electron g-factor in the ensemble. We demonstrate that regardless of the g-factor anisotropy degree the oscillation frequency of the Faraday rotation and ellipticity signals for a randomly oriented ensemble is determined by the transverse electron g-factor component.

cond-mat.mes-hall

Landé g-factors and spin dynamics of charge carriers in CuCl nanocrystals in a glass matrix

The spin properties of charge carriers confined in CuCl semiconductor nanocrystals (NCs) of different sizes (radius from 1.8 nm up to 28 nm) crystallized in a glass matrix are studied experimentally and theoretically. By means of photoluminescence, spin-flip Raman scattering, time-resolved Faraday ellipticity, and time-resolved differential transmission performed at temperatures in the range of $1.6 - 120$ K at magnetic fields up to 8 T, comprehensive information on the Landé $g$-factors as well as the population and spin dynamics is received. The spin signals are contributed by confined electrons with a $g$-factor close to 2, which shows a weak increase with decreasing NC size, i.e. increasing electron confinement energy. We revisit the theory of exciton confinement as a whole in spherical NCs within the six-band valence band model in order to describe the size dependence of the $Z_3$ and $Z_{1,2}$ exciton energies in CuCl NCs. We demonstrate theoretically that the stronger increase of the $Z_{1,2}$ energy transitions with decreasing radius can be explained by the strong absorption from the excited exciton state caused by strong heavy hole-light hole mixing in the exciton. The parameters of the six-band Hamiltonian describing both the exciton and hole kinetic energies are estimated from the comparison of the calculated and experimental size dependences of the exciton transitions. A theoretical model of the size-dependent Landé $g$-factors for electron and hole confined in spherical NCs of semiconductors with negative spin-orbit splitting of the valence band is developed.

cond-mat.mes-hall

Polarized emission of CdSe nanocrystals in magnetic field: the role of phonon-assisted recombination of the dark exciton

The recombination dynamics and spin polarization of excitons in CdSe nanocrystals synthesized in a glass matrix are investigated using polarized photoluminescence in high magnetic fields up to 30 Tesla. The dynamics are accelerated by increasing temperature and magnetic field, confirming the dark exciton nature of the low-temperature photoluminescence (PL). The circularly polarized PL in magnetic fields reveals several unusual appearances: (i) a spectral dependence of the polarization degree, (ii) its low saturation value, and (iii) a stronger intensity of the Zeeman component which is higher in energy. The latter feature is the most surprising being in contradiction with the thermal population of the exciton spin sublevels. The same contradiction was previously observed in the ensemble of wet-chemically synthesized CdSe nanocrystals, but was not understood. We present a theory which explains all the observed features and shows that the inverted ordering of the circular polarized PL maxima from the ensemble of nanocrystals is a result of competition between the zero phonon (ZPL) and one optical phonon (1PL) assisted emission of the dark excitons. The essential aspects of the theoretical model are different polarization properties of the dark exciton emission via ZPL and 1PL recombination channels and the inhomogeneous broadening of the PL spectrum from the ensemble of nanocrystals exceeding the optical phonon energy.

cond-mat.mes-hall

Single and double electron spin-flip Raman scattering in CdSe colloidal nanoplatelets

CdSe colloidal nanoplatelets are studied by spin-flip Raman scattering in magnetic fields up to 5 T. We find pronounced Raman lines shifted from the excitation laser energy by an electron Zeeman splitting. Their polarization selection rules correspond to those expected for scattering mediated by excitons interacting with resident electrons. Surprisingly, Raman signals shifted by twice the electron Zeeman splitting are also observed. The theoretical analysis and experimental dependencies show that the mechanism responsible for the double flip involves two resident electrons interacting with a photoexcited exciton. Effects related to various orientations of the nanoplatelets in the ensemble and different orientations of the magnetic field are analyzed.

cond-mat.mes-hall

Surface spin magnetism controls the polarized exciton emission from CdSe nanoplatelets

The surface of nominally diamagnetic colloidal CdSe nanoplatelets can demonstrate paramagnetism owing to the uncompensated spins of dangling bonds (DBSs). We reveal that by optical spectroscopy in high magnetic fields up to 15 Tesla using the exciton spin as probe of the surface magnetism. The strongly nonlinear magnetic field dependence of the circular polarization of the exciton emission is determined by the DBS and exciton spin polarization as well as by the spin-dependent recombination of dark excitons. The sign of the exciton-DBS exchange interaction can be adjusted by the nanoplatelet growth conditions.

cond-mat.mes-hall

Electron and hole g-factors and spin dynamics of negatively charged excitons in CdSe/CdS colloidal nanoplatelets with thick shells

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 increasing magnetic field from -0.4 to -0.7 is evaluated. Hole g-factors for two-dimensional structures are calculated for various hole confining potentials for cubic- and wurtzite lattice in CdSe core. These calculations are extended for various quantum dots and nanoplatelets based on II-VI semiconductors. We developed a magneto-optical technique for the quantitative evaluation of the nanoplatelets orientation in ensemble.

cond-mat.mes-hall

Addressing the exciton fine structure in colloidal nanocrystals: the case of CdSe nanoplatelets

We study the band-edge exciton fine structure and in particular its bright-dark splitting in colloidal semiconductor nanocrystals by four different optical methods based on fluorescence line narrowing and time-resolved measurements at various temperatures down to 2 K. We demonstrate that all these methods provide consistent splitting values and discuss their advances and limitations. Colloidal CdSe nanoplatelets with thicknesses of 3, 4 and 5 monolayers are chosen for experimental demonstrations. The bright-dark splitting of excitons varies from 3.2 to 6.0 meV and is inversely proportional to the nanoplatelet thickness. Good agreement between experimental and theoretically calculated size dependence of the bright-dark exciton slitting is achieved. The recombination rates of the bright and dark excitons and the bright to dark relaxation rate are measured by time-resolved techniques.

cond-mat.mes-hall

Nonradiative and radiative Förster energy transfer between quantum dots

We study theoretically nonradiative and radiative energy transfer between two localized quantum emitters, donor one (i.e. initially excited) and acceptor one (i.e. receiving the excitation). The rates of nonradiative and radiative processes are calculated depending on the spatial and spectral separation between donor and acceptor states and for different donor and acceptor lifetimes for typical parameters of semiconductor quantum dots. We find that the donor lifetime can be significantly modified only due to the nonradiative Förster energy transfer process at donor-acceptor separations $\sim 10~$nm (depending on the acceptor radiative lifetime) and for the energy detuning not larger than 1$÷$2 meV. The efficiency of the nonradiative Förster energy transfer process under these conditions is close to unity and decreases rapidly with the increase of donor-acceptor distance or energy detuning. At large donor-acceptor separations $>40~$nm the radiative corrections to the donor lifetime are comparable with nonradiative ones but are relatively weak.

cond-mat.mes-hall

Effects of strain on the valence band structure and exciton-polariton energies in ZnO

The uniaxial stress dependence of the band structure and the exciton-polariton transitions in wurtzite ZnO is thoroughly studied using modern first-principles calculations based on the HSE+G0W0 approach, k p modeling using the deformation potential framework, and polarized photoluminescence measurements. The ordering of the valence bands [A(G7), B(G9), C(G7)] is found to be robust even for high uniaxial and biaxial strains. Theoretical results for the uniaxial pressure coefficients and splitting rates of the A, B, and C valence bands and their optical transitions are obtained including the effects of the spin-orbit interaction. The excitonic deformation potentials are derived and the stress rates for hydrostatic pressure are determined based on the results for uniaxial and biaxial stress. In addition, the theory for the stress dependence of the exchange interaction and longitudinal-transversal splitting of the exciton-polaritons is developed using the basic exciton functions of the quasi-cubic approximation and taking the interaction between all exciton states into account. It is shown that the consideration of these effects is crucial for an accurate description of the stress dependence of the optical spectra in ZnO. The theoretical results are compared to polarized photoluminescence measurements of different ZnO substrates as function of uniaxial pressure and experimental values reported in the literature demonstrating an excellent agreement with the computed pressure coefficients.

cond-mat.mtrl-sci