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Chemical Physics Letters

Dephasing time in solids and homogeneous optical linewidth: are the mechanisms of the electron-phonon coupling the same?

Игорь Сергеевич Осадько, N.N. Zaitsev

Published Nov 1, 1985• 9 citations
Publisher
DOI
10.1016/0009-2614(85)85512-3

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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.

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Recently there has been growing interest in optical dephasing (homogeneous linewidth) mechanisms in solids, both for scientific and technological1 reasons. The role of spin flip-flops (SFF) in producing dephasing has long been recognized in nuclear and electron magnetic resonance, and these studies are now being extended to optical transitions. In particular direct proof of host nuclear SFF optical dephasing of unlike dopant nuclei has been achieved by the observation of magic- angle homogeneous line narrowing.2 This work reports on a new technique for homogeneous line narrowing that demonstrates the existence of electronic SFF optical dephasing by like spins in ruby. The technique relies on selective depopulation of ground- state levels by R2 optical pumping as well as on novel spin thermodynamics in the ground state produced by the strong dipolar coupling between electron spins.

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A picosecond photon echo study of a chromophore in an organic glass: Temperature dependence and comparison to nonphotochemical hole burning

Cecilia A. Walsh, Mark A. Berg, L. R. Narasimhan +1 more

The first two-pulse photon echo experiments on a chromophore in an organic glass are reported. The homogeneous electronic dephasing of resorufin in ethanol glass is measured from 1.5–11.4 K. The temperature dependence of the dephasing time does not fit the power law frequently predicted by theory for the dephasing characteristic of glasses. However, the temperature dependence can be accounted for by including dephasing from librations or acoustic phonons, mechanisms known to be important in crystals. The dephasing decay is found to be a single exponential for over six factors of e. The dephasing is also shown to be uncorrelated with the extent of nonphotochemical hole burning (NPHB). However, the homogeneous linewidth deduced from the photon echo is four times narrower than the linewidth obtained from NPHB, demonstrating that the hole is broadened by additional processes.

The Journal of Chemical Physics•Jan 1, 1987•92 citations
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.
Recently there has been growing interest in optical dephasing (homogeneous linewidth) mechanisms in solids, both for scientific and technological1 reasons. The role of spin flip-flops (SFF) in producing dephasing has long been recognized in nuclear and electron magnetic resonance, and these studies are now being extended to optical transitions. In particular direct proof of host nuclear SFF optical dephasing of unlike dopant nuclei has been achieved by the observation of magic- angle homogeneous line narrowing.2 This work reports on a new technique for homogeneous line narrowing that demonstrates the existence of electronic SFF optical dephasing by like spins in ruby. The technique relies on selective depopulation of ground- state levels by R2 optical pumping as well as on novel spin thermodynamics in the ground state produced by the strong dipolar coupling between electron spins.
The first two-pulse photon echo experiments on a chromophore in an organic glass are reported. The homogeneous electronic dephasing of resorufin in ethanol glass is measured from 1.5–11.4 K. The temperature dependence of the dephasing time does not fit the power law frequently predicted by theory for the dephasing characteristic of glasses. However, the temperature dependence can be accounted for by including dephasing from librations or acoustic phonons, mechanisms known to be important in crystals. The dephasing decay is found to be a single exponential for over six factors of e. The dephasing is also shown to be uncorrelated with the extent of nonphotochemical hole burning (NPHB). However, the homogeneous linewidth deduced from the photon echo is four times narrower than the linewidth obtained from NPHB, demonstrating that the hole is broadened by additional processes.