Naturally formed CdTe/CdS core/shell quantum dot (QD) structures in the presence of surface stabilizing agents have been synthesized by a hydrothermal method. Size and temperature dependent photoluminescence (PL) spectra have been investigated to understand the exciton-phonon interaction, and radiative and nonradiative relaxation of carriers in these QDs. The PL of these aqueous CdTe QDs (3.0-4.8 nm) has been studied in the temperature range 15-300 K. The strength of the exciton-LO-phonon coupling, as reflected in the Huang-Rhys parameter 'S' is found to increase from 1.13 to 1.51 with the QD size varying from 4.8 to 3.0 nm. The PL linewidth (FWHM) increases with increase in temperature and is found to have a maximum in the case of QDs of 3.0 nm in size, where the exciton-acoustic phonon coupling coefficient is enhanced to 51 μeV K(-1), compared to the bulk value of 0.72 μeV K(-1). To understand the nonradiative processes, which affect the relaxation of carriers, the integrated PL intensity is observed as a function of temperature. The integrated PL intensity remains constant until 50 K for relatively large QDs (3.9-4.8 nm) beyond which a thermally activated process takes over. Below 150 K, a small activation energy, 45-19 meV, is found to be responsible for the quenching of the PL. Above 150 K, the thermal escape from the dot assisted by scattering with multiple longitudinal optical (LO) phonons is the main mechanism for the fast quenching of the PL. Besides this high temperature quenching, interestingly for relatively smaller size QDs (3.4-3.0 nm), the PL intensity enhances as the temperature increases up to 90-130 K, which is attributed to the emission of carriers from interface/trap states having an activation energy in the range of 6-13 meV.
We report the nonlinear optical absorption studies in two differently sized water-soluble cadmium telluride quantum dot (QD) samples, exhibiting first excitonic absorption peaks at 493 nm and 551 nm, respectively. An optical limiting behavior is observed for near-resonant excitation at 532 nm using nanosecond laser pulses, originating from the effective two-photon absorption (TPA) mechanism. The effective TPA coefficient (βeff) is measured to be in the range of 10−12 m/W. This is one order of magnitude higher than the TPA coefficient (β) reported for off-resonant excitation. At this excitation wavelength, the smaller QD shows a relatively weaker photoluminescence and stronger nonlinear absorption.
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