Search

The state-to-state intraband relaxation dynamics of charge carriers photogenerated within CdTe quantum wires (QWs) are characterized via transient absorption spectroscopy. Overlapping signals from the energetic-shifting of the quantum-confinement features and the occupancy of carriers in the states associated with these features are separated using the quantum-state renormalization model. Holes generated with an excitation energy of 2.75 eV reach the band edge within the instrument response of the measurement, ∼200 fs. This extremely short relaxation time is consistent with the low photoluminescence quantum yield of the QWs, ∼0.2%, and the presence of alternative relaxation pathways for the holes. The electrons relax through the different energetically available quantum-confinement states, likely via phonon coupling, with an overall rate of ∼0.6 eV ps -1 .

The excitation energy dependence (EED) of the photoluminescence quantum yield (Φ PL ) of semiconductor nanoparticles with varying dimensionalities is reported. Specifically, the EEDs of CdSe quantum dots, CdSe quantum platelets, CdSe quantum belts, and CdTe quantum wires were determined via measurements of individual Φ PL values and photoluminescence efficiency (PL Eff ( E )) spectra. There is a general trend of overall decreasing efficiency for radiative recombination with increasing excitation energy. In addition, there are often local minima in the PL Eff ( E ) spectra that are most often at energies between quantum-confinement transitions. The average PL lifetimes of the samples do not depend on the excitation energy, suggesting that the EED of Φ PL arises from charge carrier trapping that competes efficiently with intraband carrier relaxation to the band edge. The local minima in the PL Eff ( E ) spectra are attributed to excitation into optically coupled states that results in the loss of carriers in the semiconductor. The EED data suggest that the PL Eff ( E ) spectra depend on the sample synthesis, preparation, surface passivation, and environment.

The photoluminescence (PL) intensity of semiconductor quantum dots (QDs) is routinely monitored to track the chemical and physical properties within a sample or device incorporating the QDs. A dependence of the PL quantum yields (QYs) on the excitation energy could lead to erroneous conclusions but is commonly not considered. We summarize previous evidence and present results from two methodologies that confirm the possibility of a dependence of the PL QYs on the excitation energy. The data presented indicate that PL QYs of CdSe and CdSe/ZnS QDs suspended in toluene are highest for excitation just above the band gap, Eg, of each. The PL QYs decrease with increasing excitation energies up to 1 eV above Eg. The PL intensity decay profiles recorded for these samples at varying emission and excitation energies indicate that the changes in the PL QYs result from the nonradiative relaxation pathways sampled as the charge carriers relax down to the band edge.

Photogenerated electron-hole pairs are observed to be bound as 1D excitons in CdSe quantum wires (QWs) at room temperature. Microscopy experiments performed on dilute samples of CdSe QWs prepared on coverslips with patterned electrodes reveal that there is no change in either the overall photoluminescence (PL) intensity or the distribution of the PL intensity with the application of an external electric field. Changes in the PL intensity, and thus evidence for separate charge carriers within the QWs, are observed only for concentrated samples. In these concentrated samples, a thin film of other compounds, including trioctylphosphine oxide and a bismuth salt formed in the synthesis, is observed to encompass the QWs. The separate charge carriers that influence the PL intensity are attributed to the other compounds in the sample.