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Quantum Electronics and Laser Science Conference

Homogeneous linewidth in CdSe/ZnS core/shell nanocrystals

Phedon Palinginis, Hailin Wang

Published Nov 13, 2002• 2 citations
Publisher

Abstract

Summary form only given. Understanding dephasing in quantum dots, especially dephasing due to electron-phonon interactions, is essential for the use of quantum dots as artificial atoms in applications such as quantum information processing. In this paper, we report experimental studies on dephasing in CdSe/ZnS core/shell nanocrystals using high resolution spectral hole burning. These studies not only allow us to determine the homogeneous linewidth, but also reveal directly discrete acoustic phonon sidebands. The extremely small homogeneous linewidth (32 /spl mu/eV) obtained at low temperature along with the nonlinear temperature dependence of the homogeneous linewidth indicates that the quantization of acoustic phonon modes leads to strong suppression of dephasing associated with electron-phonon interactions in nanocrystals. The dependence of the spectral hole width on the modulation frequency also reveals exciton spectral migration occurring on a time scale of order of 100 /spl mu/s.

DOI
10.1109/qels.2001.961771

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Summary form only given. Understanding dephasing in quantum dots, especially dephasing due to electron-phonon interactions, is essential for the use of quantum dots as artificial atoms in applications such as quantum information processing. In this paper, we report experimental studies on dephasing in CdSe/ZnS core/shell nanocrystals using high resolution spectral hole burning. These studies not only allow us to determine the homogeneous linewidth, but also reveal directly discrete acoustic phonon sidebands. The extremely small homogeneous linewidth (32 /spl mu/eV) obtained at low temperature along with the nonlinear temperature dependence of the homogeneous linewidth indicates that the quantization of acoustic phonon modes leads to strong suppression of dephasing associated with electron-phonon interactions in nanocrystals. The dependence of the spectral hole width on the modulation frequency also reveals exciton spectral migration occurring on a time scale of order of 100 /spl mu/s.
We report the first direct measurements of femtosecond electronic dephasing in CdSe nanocrystals using three-pulse photon echoes and a novel mode-suppression technique. We are able to separate the dynamics of the coherently excited LO phonons from the underlying electron-hole dephasing by suppressing the quantum beats. The homogeneous linewidth of these materials at 15 K results from electronic dephasing in \ensuremath{\sim}85 fs, approximately half of which is due to acoustic phonon modes. Contributions from acoustic phonons dominate the homogeneous linewidth at room temperature.
The temperature-dependent homogeneous width of confined excitons in CuCl, CuBr and CdSe quantum dots was investigated at very low temperatures down to 0.6 K by means of accumulated photon echo. The observed nonlinear temperature dependence of the homogeneous width at low temperatures is explained by the interaction with confined acoustic phonons for CdSe quantum dots or very small excitation in the two-level system for CuCl and CuBr quantum dots. At the lowest temperature, the homogeneous width of confined excitons in CuCl, CuBr and CdSe quantum dots becomes 1–2 μeV, 23–59 μeV and 0.16–0.25 meV, respectively. It depends on the surrounding matrix for CuCl quantum dots and the radius of dots for CuBr and CdSe quantum dots. These results suggest surroundings of quantum dots dominate the low temperature dephasing mechanism, i.e. homogeneous width of the optical spectra, of real quantum dots.
We study CuBr nanocrystals embedded in a borosilicate matrix. The excitonic absorption line is strongly inhomogeneously broadened by the size dispersion of the quantum dots. We explore two ways in order to study the dephasing processes of the transition. The homogeneous absorption linewidth is first determined by spectral hole-burning (SHB) measurements, using a nanosecond dye laser excitation. We then perform degenerate four-wave-mixing experiments (FWM), using 100 fs pulses from a frequency-doubled Ti:sapphire laser. Due to the inhomogeneous broadening, we observe a so-called photon-echo signal and we measure its dynamics. From SHB experiments, we obtain homogeneous linewidths larger than 0.3 meV. From the FWM experiment, we obtain values smaller than 0.2 meV. These discrepancies between SHB and FWM measurements can be explained if we take into account the high excitation intensity necessary to induce absorption saturation in SHB experiments. Moreover, during the 20 ns pulses used, spectral diffusion may occur due to interactions between the nanocrystals and their matrix. Spectrally resolved four-wave-mixing experiments (SR-FWM) are also performed. The oscillations with a 250 fs period we observe at short time delays could be interpreted in terms of quantum beats between two-exciton and one-exciton states.
Temperature dependence of the homogeneous linewidth of CuBr quantum dots in glass and NaBr matrices and CdSe quantum dots in glass matrix has been investigated using heterodyne-detected accumulated photon echo. We can reproduce the observed nonlinear temperature dependence considering two characteristic mechanisms: the small energy excitation in two-level system and the two-phonon Raman process of confined acoustic phonons. The interaction with the two-level system is dominant below 15 K and 10 K for CuBr and CdSe quantum dots, respectively. Above these temperatures the interaction with confined phonons is dominant. These results are similar to those of a previous study of CuCl quantum dots in glass, showing the universal influence of confined phonons and surrounding matrices on the low-temperature dephasing process of very small semiconductor quantum dots.
We report the use of continuous wave spectral hole burning to perform high-resolution spectroscopy of the homogeneous linewidth of self-assembled InGaAs-GaAs quantum dots at low temperature. We use this technique to examine the power broadening behavior of the homogeneous InGaAs-GaAs quantum dot line. We find that at a temperature of 9.8 K and over the majority of the pump powers considered, the spectral hole signal is well fit by a single Lorentizian line shape. Analysis of the power broadening yields a full width at half maximum of 0.74μeV for the homogeneous linewidth and a corresponding coherence time T2 of 1.76 ns.
Summary form only given. Excitons confined in nanocrystals or quantum dots attract much attention because they have a very long phase relaxation time that opens the way to the artificial coherent control of the excitons. CuCl quantum dot is a typical material in which the translational motion of the exciton is confined. In this paper, we report on the high resolution measurement of the resonant luminescence of CuCl quantum dots embedded in glass and NaCl matrices under weak excitation condition, and show that the zero-phonon line of the resonant luminescence has a narrow homogeneous linewidth reflecting the long phase relaxation time.