Three-photon excited band edge and trap emission of CdS semiconductor nanocrystals

We report on three-photon excited band edge and trap emission of CdS semiconductor nanocrystals. While the band edge emission intensity clearly shows a cubic dependence on excitation intensity, demonstrating three-photon absorption process, the trap emission does not exhibit such a cubic dependence. A simple theoretical model based on the assumption that there exist a limited number of trap states in nanocrystals shows good agreement with the experiment, suggesting that the number of trap states play an important role in their emission intensity dependence of multiphoton excitation. The three-photon absorption cross section of CdS nanocrystals is measured to be ∼10−79 cm6 s2 photon−2, which is three to four orders of magnitude higher than those of the previously reported common UV fluorescent dyes.