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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Spectral hole burning of strongly confined CdSe quantum dots

Christine Spiegelberg, F. Henneberger, Joachim Puls

Published Feb 1, 1991• 0 citations
Publisher

Abstract

The paper presents ns-hole-burning experiments of the quantum-confined transitions in CdSe quantum dots. By means of respective model calculations the contribution of inhomogeneous and homogeneous broadening of the spectra are deduced at 77 K and room temperature. Tuning the excitation wavelength over a broad spectral range demonstrates a common blocking of three electronic states about 160 meV apart.

DOI
10.1117/12.24498

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The paper presents ns-hole-burning experiments of the quantum-confined transitions in CdSe quantum dots. By means of respective model calculations the contribution of inhomogeneous and homogeneous broadening of the spectra are deduced at 77 K and room temperature. Tuning the excitation wavelength over a broad spectral range demonstrates a common blocking of three electronic states about 160 meV apart.
The persistent spectral hole-burning (PSHB) phenomenon was observed in semiconductor quantum dots, CdSe , CuCl , and CuBr , embedded in glass and crystal. In inhomogeneously broadened exciton absorption spectra of these dots, the narrow bleaching hole and its associated structure are made by the narrowband laser excitation and are conserved for more than several hours at 2 K after the laser irradiation. The observation of the PSHB phenomenon in these four kinds of samples shows the generality of the phenomenon in semiconductor quantum dots and requires the existence of more than one ground-state configurations of the total system consisting of quantum dots and surrounding matrix. It means that not only the size distribution but also these ground-state configurations give inhomoge-neous broadening to semiconductor quantum dots. Thermally annealing and light-induced hole-filling phenomena were observed. Hole-burning and hole-filling mechanisms are discussed. Quantum dots consisting of 103–104 atoms behave like molecules or ions in matrix to give the PSHB phenomenon.
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.
We investigate the dephasing times in highly excited CdSe and CdS0.3Se0.7 nanocrystals by spectral hole burning throughout the gain region. The energy dependence of the dephasing time T2 is compared between quantum dots in the strong-confinement regime and bulklike microcrystals. T2 in strongly confined quantum dots remains rather constant, whereas the bulklike sample shows a continuous increase of T2 toward the transparency point. This observation is attributed to the different gain mechanisms in the strong and the weak quantum-confinement regimes.
Persistent spectral-hole-burning (PSHB) phenomena have been observed in many kinds of semiconductor quantum dots (QDs). Luminescence hole burning and charged excitons have been observed in CuCl QDs in NaCl crystals. The observed PSHB phenomena are explained by the ionization of QDs. The energy of photoionized QDs is changed from the original energy and their new energies depend on the spatial arrangement of trapped carriers. Quantum confinement of carriers and the resulting strong Coulomb interaction between confined carriers and trapped carriers cause the energy change. PSHB has been widely applied to site-selective spectroscopy of QDs. Size-dependent excited exciton quantum states in CuCl quantum cubes, size-dependent excited electron-hole quantum states in CdTe QDs and renormalization of longitudinal optical phonons confined in CuCl QDs have been revealed by studying sideband holes. This also allowed the measurement of accumulated photon echo, which clarified the very sharp homogeneous spectral linewidth of QDs under weak excitation conditions.
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.
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.