Marco Marceddu

Exciton-Exciton Interaction and Optical Gain in Colloidal CdSe/CdS Dot/Rod Nanocrystals.

Exciton-exciton interaction in dot/rod CdSe/CdS nanocrystals has proved to be very sensitive to the shape of nanocrystals, due to the unique band alignment between CdSe and CdS. Repulsive exciton-exciton interaction is demonstrated, which makes CdSe/CdS dot/rods promising gain media for solution-processable lasers, with projected pump threshold densities below 1 kW cm(-2) for continuous wave lasing.

Light-Induced Charged and Trap States in Colloidal Nanocrystals Detected by Variable Pulse Rate Photoluminescence Spectroscopy

Intensity instabilities are a common trademark of the photoluminescence of nanoemitters. This general behavior is commonly attributed to random fluctuations of free charges and activation of charge traps reducing the emission yield intermittently. However, the actual physical origin of this phenomenon is actively debated. Here we devise an experiment, variable pulse rate photoluminescence, to control the accumulation of charges and the activation of charge traps. The dynamics of these states is studied, with pulse repetition frequencies from the single-pulse to the megahertz regime, by monitoring photoluminescence spectrograms with picosecond temporal resolution. We find that both photocharging and charge trapping contribute to photoluminescence quenching, and both processes can be reversibly induced by light. Our spectroscopic technique demonstrates that charge accumulation and trap formation are strongly sensitive to the environment, showing different dynamics when nanocrystals are dispersed in solution or deposited as a film.

Charged excitons, Auger recombination and optical gain in CdSe/CdS nanocrystals.

CdSe/CdS colloidal nanocrystals are members of a novel class of light-emitting nanoparticles with remarkable optical properties such as suppressed fluorescence blinking and enhanced emission from multiexciton states. These properties have been linked to the suppression of non-radiative Auger recombination. In this work we employ ultrafast spectroscopy techniques to identify optical signatures of neutral and charged excitonic and multiexcitonic states. We show that Auger recombination of biexcitons is not suppressed, while we observe optical gain and amplified spontaneous emission from multiexciton states and from long-lived charged-exciton states.

On the formation of aggregates in silica – rhodamine 6G type II hybrids

The spectroscopic features of dye aggregates in organic–inorganic Rhodamine 6G–silica hybrids are investigated in sol–gel prepared type II bulk and thick film samples in the 10−4–10−3 mol l−1 concentration range. No aggregates are observed in film samples irrespective of the dye concentration and the spectroscopic features are ascribed to fluorescent monomers. On the contrary, by means of excitation and emission fluorescence measurements and the analysis of fluorescence decay kinetics the formation of fluorescent aggregates is reported in bulk samples and the geometry of the formed aggregates at the silica surface is discussed on the single exciton theory framework. Beside the distribution of a single emitting specie observed in bulk samples and individuated as oblique J dimers, the analysis of the excitation spectra indicate also the presence of “dark” monomer units. An energy transfer mechanism is hypothesized to explain the interaction of the monomer–dimer pair.

The temperature dependence of Cr3+:YAG zero-phonon lines

This paper deals with the photoluminescence temperature dependence of the zero-phonon lines of Cr(3+) ions in an yttrium aluminium garnet (YAG) matrix. Experimental data were analysed in the framework of electron-phonon coupling in the quadratic approximation and it was found that Cr(3+) ions in the YAG matrix are strongly coupled with lattice vibrations, with a Debye temperature of about 550 K and a value of the quadratic coupling constant of 0.65. The analysis of both homogeneous and inhomogeneous contributions to the photoluminescence linewidth is performed and the results obtained are compared with previously reported data for Fe(3+):YAG and discussed with respect to the different dependences of the two transition metal ions on the crystal field.

The temperature dependence of Cr 3+:YAG zero-phonon lines

This paper deals with the photoluminescence temperature dependence of the zero-phonon lines of Cr(3+) ions in an yttrium aluminium garnet (YAG) matrix. Experimental data were analysed in the framework of electron-phonon coupling in the quadratic approximation and it was found that Cr(3+) ions in the YAG matrix are strongly coupled with lattice vibrations, with a Debye temperature of about 550 K and a value of the quadratic coupling constant of 0.65. The analysis of both homogeneous and inhomogeneous contributions to the photoluminescence linewidth is performed and the results obtained are compared with previously reported data for Fe(3+):YAG and discussed with respect to the different dependences of the two transition metal ions on the crystal field.

The temperature dependence of Cr3

This paper deals with the photoluminescence temperature dependence of the zero-phonon lines of Cr(3+) ions in an yttrium aluminium garnet (YAG) matrix. Experimental data were analysed in the framework of electron-phonon coupling in the quadratic approximation and it was found that Cr(3+) ions in the YAG matrix are strongly coupled with lattice vibrations, with a Debye temperature of about 550 K and a value of the quadratic coupling constant of 0.65. The analysis of both homogeneous and inhomogeneous contributions to the photoluminescence linewidth is performed and the results obtained are compared with previously reported data for Fe(3+):YAG and discussed with respect to the different dependences of the two transition metal ions on the crystal field.

Exciton Nonlinearities and Optical Gain in Colloidal CdSe/CdS Dot/rod Nanocrystals

We characterized the optical nonlinearities of CdSe nanocrystals surrounded by rod-like CdS shells with ultrafast measurements of time-resolved photoluminescence. We measured the exciton-exciton interaction to be, depending on structure details, attractive or repulsive, by as much as 29 meV, due to the unique band alignment in the CdSe/CdS. This feature makes CdSe/CdS dot/rods promising gain media for solution-processable lasers, as it appears combined with 80% photoluminescence quantum yield, narrow size and shape distributions and the antenna effect of the CdS rod shell enhancing optical absorption by more than a factor 50 with respect to bare dots.

An organic laser in the monomolecular regime

We demonstrated laser action in the regime of linear recombination of singlet excitons in para-sexiphenyl crystalline films in the form of nanofibers under optical excitation with femto- and nanosecond pulses.