Characterization of the Dynamics of Photoluminescence Degradation in Aqueous CdTe/CdS Core-Shell Quantum Dots.

We investigate the effects of the excitation power on the photoluminescence spectra of aqueous CdTe/CdS core-shell quantum dots. We have focused our efforts on nanoparticles that are drop-cast on a silicon nitride substrate and dried out. Under such conditions, the emission intensity of these nanocrystals decreases exponentially and the emission center wavelength shifts with the time under laser excitation, displaying a behavior that depends on the excitation power. In the low-power regime a blueshift occurs, which we attribute to photo-oxidation of the quantum dot core. The blueshift can be suppressed by performing the measurements in a nitrogen atmosphere. Under high-power excitation the nanoparticles thermally expand and aggregate, and a transition to a redshift regime is then observed in the photoluminescence spectra. No spectral changes are observed for nanocrystals dispersed in the solvent. Our results show a procedure that can be used to determine the optimal conditions for the use of a given set of colloidal quantum dots as light emitters for photonic crystal optical cavities.

Modeling of Fano resonances in the reflectivity of photonic crystal cavities with finite spot size excitation.

We study the reflectivity spectra of photonic crystal slab cavities using an extension of the scattering matrix method that allows treating finite sizes of the spot of the excitation beam. The details of the implementation of the method are presented and then we show that Fano resonances arise as a consequence of the electromagnetic interference between the discrete contribution of the fundamental cavity mode and the continuum contribution of the light scattered by the photonic crystal pattern. We control the asymmetry lineshape of the Fano resonance through the polarization of the incident field, which determines the relative phase between the two electromagnetic contributions to the interference. We analyse the electric field profile inside and outside of the crystal to help in the understanding of the dependence on polarization of the reflectivity lineshape. We also study with our implementation the dependence of the Fano resonances on the size of the incident radiation spot.

Identification of the optically active vibrational modes in the photoluminescence of MEH-PPV films.

The temperature dependence of the photoluminescence properties of a thin film of poly[2-methoxy-5-(2(')-ethylhexyloxy)-p-phenylene-vinylene], MEH-PPV, fabricated by spin coating, is analyzed. The evolution with temperature of the peak energy of the purely electronic transition, of the first vibronic band, of the effective conjugation length, and of the Huang-Rhys factors are discussed. The asymmetric character of the pure electronic transition peak and the contribution of the individual vibrational modes to the first vibronic band line shape are considered by a model developed by Cury et al. [J. Chem. Phys. 121, 3836 (2004)]. The temperature dependence of the Huang-Rhys factors of the main vibrational modes pertaining to the first vibronic band allows us to identify two competing vibrational modes. These results show that the electron coupling to different vibrational modes depends on temperature via reduction of thermal disorder.

Quantum dot dipole orientation and excitation efficiency of micropillar modes.

The relative intensity of photonic modes in microcavity pillars with embedded self-assembled quantum dots is shown to be a sensitive function of quantum dot dipole orientation and position. This is deduced from a comparison of experiment and calculated intensities of light emission for many nominally identical pillars. We are able to obtain the overall degree of in-plane polarization of the quantum dot ensemble and also to obtain information on the degree of polarization along the growth axis.

Photon emission as a source of coherent behavior of polaritons.

We show that the combined effect of photon emission and Coulomb interactions may drive an exciton-polariton system towards a dynamical coherent state, even without phonon thermalization or any other relaxation mechanism. Exact diagonalization results for a finite system (a multilevel quantum dot interacting with the lowest-energy photon mode of a microcavity) are presented in support of this statement.

Asymmetric line shape in the emission spectra of conjugated polymer thin films: an experimental signature of one-dimensional electronic states.

The photoluminescence (PL) properties of thin films of the conjugated polymer [poly(2,5-bis(2(')-ethyl-hexyl)-1,4-phenylenevinylene] have been investigated. At low temperatures the PL spectra show a narrow peak for the electronic transition and a series of well defined vibronic sidebands, which clearly reveal the electron coupling with two different vibronic modes. The purely electronic transition peak is observed to be very asymmetric so that it cannot be adjusted by a single Lorentzian or Gaussian function. In order to understand and explain this asymmetry we have considered a model where the purely electronic transition line shape is partially generated by a broadened square-root singularity representing one-dimensional electron states, and partially by localized (zero-dimensional) states. The localized states are assumed to be those very close to the band edges and are represented in our model by a single Gaussian function. Numerical Franck-Condon analysis was performed, resulting in a very good agreement between the theoretical and the experimental emission spectra. This procedure has confirmed the one-dimensional character of the electron states as the basis for the understanding of the purely electronic line shape asymmetry in the PL spectra of conjugated polymers at low temperatures.