4.8 Article

A Hot Electron-Hole Pair Breaks the Symmetry of a Semiconductor Quantum Dot

期刊

NANO LETTERS
卷 13, 期 12, 页码 6091-6097

出版社

AMER CHEMICAL SOC
DOI: 10.1021/nl403368y

关键词

quantum dots; hot carriers; selection rules; symmetry breaking; transient absorption; Stark effect

资金

  1. Department of Energy [ER46673 DE-SC0001928]
  2. U.S. Department of Energy, Office of Basic Energy Sciences [DE-AC02-98CH10886]

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The best-understood property of semiconductor quantum dots (QDs) is the size-dependent optical transition energies due to the quantization of charge carriers near the band edges. In contrast, much less is known about the nature of hot electron-hole pairs resulting from optical excitation significantly above the bandgap. Here, we show a transient Stark effect imposed by a hot electron-hole pair on optical transitions in PbSe QDs. The hot electron-hole pair does not behave as an exciton, but more bulk-like as independent carriers, resulting in a transient and varying dipole moment which breaks the symmetry of the QD. As a result, we observe redistribution of optical transition strength to dipole forbidden transitions and the broadening of dipole-allowed transitions during the picosecond lifetime of the hot carriers. The magnitude of symmetry breaking scales with the amount of excess energy of the hot carriers, diminishes as the hot carriers cool down and disappears as the hot electron-hole pair becomes an exciton. Such a transient Stark effect should be of general significance to the understanding of QD photophysics above the bandgap.

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