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Register a new userAddressing the exciton fine structure in colloidal nanocrystals: the case of CdSe nanoplatelets
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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.
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The photoluminescence spectra of spherical CdTe nanocrystals with zincblende structure are studied by size-selective spectroscopic techniques. We observe a resonant Stokes shift of 15 meV when the excitation laser energy is tuned to the red side of the absorption band at 2.236 eV. The experimental data are analyzed within a symmetry-based tight-binding theory of the exciton spectrum, which is first shown to account for the size dependence of the fundamental gap reported previously in the literature. The theoretical Stokes shift presented as a function of the gap shows a good agreement with the experimental data, indicating that the measured Stokes shift indeed arises from the electron-hole exchange interaction.
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.
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.
We present the phase diagram of free charges (electrons and holes), excitons, and biexcitons in highly excited CdSe nanoplatelets that predicts a crossover to a biexciton-dominated region at easily attainable low temperatures or high photoexcitation densities. Our findings extend previous work describing only free charges and excitons by introducing biexcitons into the equation of state, while keeping the exciton and biexciton binding energies constant in view of the relatively low density of free charges in this material. Our predictions are experimentally testable in the near future and offer the prospect of creating a quantum degenerate, and possibly even superfluid, biexciton gas. Furthermore, we also provide simple expressions giving analytical insight into the regimes of photoexcitation densities and temperatures in which excitons and biexcitons dominate the response of the nanoplatelets.
We measured the intrinsic ground-state exciton dephasing and population dynamics in colloidal quasi two-dimensional (2D) CdSe nanoplatelets at low temperature (5-50K) using transient resonant four-wave mixing in heterodyne detection. Our results indicate that below 20K the exciton dephasing is lifetime limited, with the exciton population lifetime being as fast as 1ps. This is consistent with an exciton lifetime given by a fast radiative decay due to the large in-plane coherence area of the exciton center-of-mass motion in these quasi 2D systems compared to spherical nanocrystals.
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