No Arabic abstract
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.
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.
Lead-halide perovskite nanocrystals (PNCs) exhibit unique optoelectronic properties, many of which originate from a purported bright-triplet exciton fine-structure. A major impediment to measuring this fine-structure is inhomogeneous spectral broadening, which has limited most experimental studies to single-nanocrystal spectroscopies. It is shown here that the linearly-polarized single-particle selection rules in PNCs are preserved in nonlinear spectroscopies of randomly-oriented ensembles. Simulations incorporating rotational-averaging demonstrate that techniques such as transient absorption and two-dimensional coherent spectroscopy are capable of resolving exciton fine-structure in PNCs, even in the presence of inhomogeneous broadening and orientation disorder.
We study the dependence of the quantum yield of photoluminescence of a dense, periodic array of semiconductor nanocrystals (NCs) on the level of doping and NC size. Electrons introduced to NCs via doping quench photoluminescence by the Auger process, so that practically only NCs without electrons contribute to the photoluminescence. Computer simulation and analytical theory are used to find a fraction of such empty NCs as a function of the average number of donors per NC and NC size. For an array of small spherical NCs, the quantization gap between 1S and 1P levels leads to transfer of electrons from NCs with large number of donors to those without donors. As a result, empty NCs become extinct, and photoluminescence is quenched abruptly at an average number of donors per NC close to 1.8. The relative intensity of photoluminescence is shown to correlate with the type of hopping conductivity of an array of NCs.
We investigate the photoconductance of single-walled carbon nanotube-nanocrystalhybrids. The nanocrystals are bound to the nanotubes via molecular recognition. We find that the photoconductance of the hybrids can be adjusted by the absorption characteristics of the nanocrystals. In addition, the photoconductance of the hybrids surprisingly exhibits a slow time constant of about 1 ms after excitation of the nanocrystals. The data are consistent with a bolometrically induced current increase in the nanotubes caused by photon absorption in the nanocrystals.
We study the neutral exciton energy spectrum fine structure and its spin dephasing in transition metal dichalcogenides such as MoS$_2$. The interaction of the mechanical exciton with its macroscopic longitudinal electric field is taken into account. The splitting between the longitudinal and transverse excitons is calculated by means of the both electrodynamical approach and $mathbf k cdot mathbf p$ perturbation theory. This long-range exciton exchange interaction can induce valley polarization decay. The estimated exciton spin dephasing time is in the picosecond range, in agreement with available experimental data.