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Register a new userTheory of single and double electron spin-flip Raman scattering in semiconductor nanoplatelets
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A theory of electron spin-flip Raman scattering (SFRS) is presented that describes the Raman spectral signals shifted by both single and twice the electron Zeeman energy under nearly resonant excitation of the heavy hole excitons in semiconductor nanoplatelets. We analyze the spin structure of photoexcited intermediate states, derive compound matrix elements of the spin-flip scattering and obtain polarization properties of the one- and two-electron SFRS common for all the intermediate states. We show that, in the resonant scattering process under consideration, the complexes exciton plus localized resident electrons play the role of main intermediate states rather than tightly bound trion states. It is demonstrated that, in addition to the direct photoexcitation (and similar photorecombination) channel, there is another indirect channel contributing to the SFRS process. In the indirect channel, the photohole forms the exciton state with the resident electron removed from the localization site while the photoelectron becomes localized on this site. The theoretical results are compared with recent experimental findings for ensembles of CdSe nanoplatelets.
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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.
We use temporally resolved intensity cross-correlation measurements to identify the biexciton-exciton radiative cascades in a negatively charged QD. The polarization sensitive correlation measurements show unambiguously that the excited two electron triplet states relax non-radiatively to their singlet ground state via a spin non conserving flip-flop with the ground state heavy hole. We explain this mechanism in terms of resonant coupling between the confined electron states and an LO phonon. This resonant interaction together with the electron-hole exchange interaction provides an efficient mechanism for this, otherwise spin-blockaded, electronic relaxation.
We present experimental data and associated theory for correlations in a series of experiments involving repeated Landau-Zener sweeps through the crossing point of a singlet state and a spin aligned triplet state in a GaAs double quantum dot containing two conduction electrons, which are loaded in the singlet state before each sweep, and the final spin is recorded after each sweep. The experiments reported here measure correlations on time scales from 4 $mu$s to 2 ms. When the magnetic field is aligned in a direction such that spin-orbit coupling cannot cause spin flips, the correlation spectrum has prominent peaks centered at zero frequency and at the differences of the Larmor frequencies of the nuclei, on top of a frequency-independent background. When the spin-orbit field is relevant, there are additional peaks, centered at the frequencies of the individual species. A theoretical model which neglects the effects of high-frequency charge noise correctly predicts the positions of the observed peaks, and gives a reasonably accurate prediction of the size of the frequency-independent background, but gives peak areas that are larger than the observed areas by a factor of two or more. The observed peak widths are roughly consistent with predictions based on nuclear dephasing times of the order of 60 $mu$s. However, there is extra weight at the lowest observed frequencies, which suggests the existence of residual correlations on the scale of 2 ms. We speculate on the source of these discrepancies.
The discovery of 2-dimensional (2D) materials, such as CrI3, that retain magnetic ordering at monolayer thickness has resulted in a surge of research in 2D magnetism from both pure and applied perspectives. Here, we report a magneto-Raman spectroscopy study on multilayered CrI3, focusing on two new features in the spectra which appear at temperatures below the magnetic ordering temperature and were previously assigned to high frequency magnons. We observe a striking evolution of the Raman spectra with increasing magnetic field in which clear, sudden changes in intensities of the modes are attributed to the interlayer ordering changing from antiferromagnetic to ferromagnetic at a critical magnetic field. Our work highlights the sensitivity of the Raman modes to weak interlayer spin ordering in CrI3. In addition, we theoretically examine potential origins for the new modes, which we deduce are unlikely single magnons.
Spin-flip Raman scattering of electrons and heavy-holes is studied for resonant excitation of neutral and charged excitons in a CdTe/Cd$_{0.63}$Mg$_{0.37}$Te quantum well. The spin-flip scattering is characterized by its dependence on the incident and scattered light polarization as well as on the magnetic field strength and orientation. Model schemes of electric-dipole allowed spin-flip Raman processes in the exciton complexes are compared to the experimental observations, from which we find that lowering of the exciton symmetry, time of carrier spin relaxation, and mixing between electron states and, respectively, light- and heavy-hole states play an essential role in the scattering. At the exciton resonance, anisotropic exchange interaction induces heavy-hole spin-flip scattering, while acoustic phonon interaction is mainly responsible for the electron spin-flip. In resonance with the positively and negatively charged excitons, anisotropic electron-hole exchange as well as mixed electron states allow spin-flip scattering. Variations in the resonant excitation energy and lattice temperature demonstrate that localization of resident electrons and holes controls the Raman process probability and is also responsible for symmetry reduction. We show that the intensity of the electron spin-flip scattering is strongly affected by the lifetime of the exciton complex and in tilted magnetic fields by the angular dependence of the anisotropic electron-hole exchange interaction.
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