2007
DOI: 10.1021/nl072487g
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Uncovering Forbidden Optical Transitions in PbSe Nanocrystals

Abstract: The 1S(h,e)-1P(e,h) exciton transition energy of PbSe nanocrystals was determined via two-photon photoluminescence excitation spectroscopy and was found to be in good agreement with predictions from a tight-binding calculation. The two-photon excitation peak occurs at energies very close to a strong feature in the one-photon absorption spectrum and suggests that it should be assigned as a formally forbidden S-P transition. Leading explanations for the unusual strength of the forbidden transition are discussed.

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Cited by 52 publications
(70 citation statements)
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References 26 publications
(67 reference statements)
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“…[13] have contributed this peak to the photon assisted S-P transition. In similar studies as reported in [14], experimentally observed absorption peaks were at 0.91 eV, 1.175 eV and 1.42 eV, out of which the first peak and the third peak were devoted to the single photon absorption process of l S h → l S e and l P h → l P e , respectively. Interestingly, they observed the second absorption peak for both single photon absorption as well as the two photon absorption processes.…”
Section: Discussionsupporting
confidence: 81%
“…[13] have contributed this peak to the photon assisted S-P transition. In similar studies as reported in [14], experimentally observed absorption peaks were at 0.91 eV, 1.175 eV and 1.42 eV, out of which the first peak and the third peak were devoted to the single photon absorption process of l S h → l S e and l P h → l P e , respectively. Interestingly, they observed the second absorption peak for both single photon absorption as well as the two photon absorption processes.…”
Section: Discussionsupporting
confidence: 81%
“…For maximum size focusing and minimal Ostwald ripening, the optimum time for terminating the reaction was 5-6 min after CdCl 2 injection (Figure 1 a). This protocol produced NCs with well-defi ned 1st, 2nd, and 3rd excitonic transitions [63][64][65] (Figure S1, Supporting Information). To eliminate the effects of size distribution when comparing passivated and unpassivated samples, we ensured that both NC samples have the same HWHMs (Table S1, Supporting Information).…”
Section: Synthesis Characterization and Stability Of Pbse Ncsmentioning
confidence: 99%
“…3b,c we display a typical absorption spectrum of PbSe NCs and its second derivative. We assign the optical transitions according to the selection rules between symmetric wavefunctions determined by Kang and Wise [14,32]; the first transition is the 1S e -1S h transition, and the second transition has been a source of controversy [33,34] because within the k · p description this transition is assigned to a symmetry forbidden 1S e -1P h /1S h -1P e transition. Each pair of states has a high level of degeneracy that increases …”
Section: Introduction To Semiconductor Ncsmentioning
confidence: 99%