2011
DOI: 10.1021/nl1040385
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Excitation Isotropy of Single CdSe/ZnS Nanocrystals

Abstract: We study the dimensionality of the excitation transition dipole moment for single CdSe/ZnS core-shell nanocrystals using azimuthally and radially polarized laser modes. The comparison of measured and simulated single nanocrystal excitation patterns shows that single CdSe/ZnS quantum dots possess a spherically degenerated excitation transition dipole. We show that the dimensionality of the excitation transition dipole moment distribution is the same for all individual CdSe/ZnS nanocrystals, disregarding the dif… Show more

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Cited by 49 publications
(56 citation statements)
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“…The particles were excited with an azimuthally polarized laser beam of 485 nm wavelength, focused into a diffraction-limited spot using a 1.49 numerical aperture objective lens. The azimuthal polarization of the excitation light allowed us to verify that every measured SiO 2 NP behaves indeed as a single dipole emitter (figure 1(c)) 26 . Further details of the SiO 2 NPs synthesis and PL measurements can be found in the Supplementary Information.…”
Section: Resultsmentioning
confidence: 90%
“…The particles were excited with an azimuthally polarized laser beam of 485 nm wavelength, focused into a diffraction-limited spot using a 1.49 numerical aperture objective lens. The azimuthal polarization of the excitation light allowed us to verify that every measured SiO 2 NP behaves indeed as a single dipole emitter (figure 1(c)) 26 . Further details of the SiO 2 NPs synthesis and PL measurements can be found in the Supplementary Information.…”
Section: Resultsmentioning
confidence: 90%
“…For this reason, for a 1D dipole, one can write Iðα exc Þ ∝ jd:Ẽ exc j 2 ∝ I 0 jũ d :ũ α j 2 ¼ I 0 cos 2 ðΦ − α exc Þsin 2 Θ: (37) In this case, as pointed out in earlier work on singlemolecule orientation [1,10], the in-plane angle Φ can be obtained as the angle α exc that maximizes Iðα exc Þ, but the out-of-plane angle Θ cannot be obtained because the value I 0 is not known. It is clear, by comparison of expressions (25) and (37), that the polarization analyses in excitation and emission are two very different situations.…”
Section: Theoretical Resultsmentioning
confidence: 99%
“…It is not clear if this effect may operate in three-dimensional carbon nanostructures. Also, the nanoscale systems with loosely bound excitons confined in all three directions display optically isotropic fluorescence response [212] and because of such isotropic three-dimensional behavior, the QDs are considered as "dots". However, in some rare cases the excitation transition dipole moment was observed (e.g., in single silicon nanocrystals) and it is attributed to local defect centers [212].…”
Section: On the Involvement Of Wannier-mott Loosely Bound Excitonsmentioning
confidence: 99%
“…Also, the nanoscale systems with loosely bound excitons confined in all three directions display optically isotropic fluorescence response [212] and because of such isotropic three-dimensional behavior, the QDs are considered as "dots". However, in some rare cases the excitation transition dipole moment was observed (e.g., in single silicon nanocrystals) and it is attributed to local defect centers [212]. Still, the analogy of carbon nanostructures with such systems is unclear and the numerous experimental data on C-dots show high level of their optical anisotropy on excitation by polarized light (see Section 5.2).…”
Section: On the Involvement Of Wannier-mott Loosely Bound Excitonsmentioning
confidence: 99%