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We present a method to separately tune the multiphoton absorption (MPA) and multiphoton excited photoluminescence using semiconductor core/enlarged-shell quantum dots (QDs), where the enlarged shell greatly enhances the MPA cross-sections while varying the core size facilitates emission wavelength selectivity. Following two-photon absorption (2PA) primarily in the shell and ultrafast charge-carrier localization to the core, luminescence occurs. We exemplify the validity of this method with CdSe/CdS nanorod heterostructures and find that the 2PA cross-section is enlarged to ∼1.4×106 GM for 180 nm nanorods (with 800 nm, 150 fs laser pulse excitation) which is two to four orders larger than that of CdSe QDs.

Enhanced tunability of the multiphoton absorption cross-section in seeded CdSe/CdS nanorod heterostructures