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Victor F. Sapega

Publications and source records attributed to Victor F. Sapega.

5 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 Landé $g$-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↗

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↗

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↗