The development of optical gain in chemically synthesized semiconductor nanoparticles (nanocrystal quantum dots) has been intensely studied as the first step toward nanocrystal quantum dot lasers. We examined the competing dynamical processes involved in optical amplification and lasing in nanocrystal quantum dots and found that, despite a highly efficient intrinsic nonradiative Auger recombination, large optical gain can be developed at the wavelength of the emitting transition for close-packed solids of these dots. Narrowband stimulated emission with a pronounced gain threshold at wavelengths tunable with the size of the nanocrystal was observed, as expected from quantum confinement effects. These results unambiguously demonstrate the feasibility of nanocrystal quantum dot lasers.

We have resolved single-exponential relaxation dynamics of the 2-, 3-, and 4-electron-hole pair states in nearly monodisperse cadmium selenide quantum dots with radii ranging from 1 to 4 nanometers. Comparison of the discrete relaxation constants measured for different multiple-pair states indicates that the carrier decay rate is cubic in carrier concentration, which is characteristic of an Auger process. We observe that in the quantum-confined regime, the Auger constant is strongly size-dependent and decreases with decreasing the quantum dot size as the radius cubed.

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The linear absorption cross section is a crucial parameter to the design of nanocrystal quantum dot devices and to the interpretation of spectroscopic data. We measure and report the size-dependent absorption cross section of CdSe nanocrystal quantum dots. We compare the results for absorption far above the band edge, where the quantum dot density of states may be approximated as a continuum, to simple theoretical models of light scattering from light-absorbing small particles. Excellent agreement with theory is found for dilute dispersions in hexane. We find that for absorption at 350 nm the per particle absorption cross section C abs (in cm 2 ) for CdSe is C abs ) (5.501 × 10 5 )a 3 cm -1 , where a is the particle radius in cm. The absorption cross section is observed to be largely insensitive to the solvent refractive index. Detailed modeling of the effect of the ligand shell may be necessary to understand the lack of sensitivity of the absorption properties of nanocrystal quantum dots to the refractive index of the medium.