As a result of quantum-confinement effects, the emission colour of semiconductor nanocrystals can be modified dramatically by simply changing their size. Such spectral tunability, together with large photoluminescence quantum yields and high photostability, make nanocrystals attractive for use in a variety of light-emitting technologies--for example, displays, fluorescence tagging, solid-state lighting and lasers. An important limitation for such applications, however, is the difficulty of achieving electrical pumping, largely due to the presence of an insulating organic capping layer on the nanocrystals. Here, we describe an approach for indirect injection of electron-hole pairs (the electron-hole radiative recombination gives rise to light emission) into nanocrystals by non-contact, non-radiative energy transfer from a proximal quantum well that can in principle be pumped either electrically or optically. Our theoretical and experimental results indicate that this transfer is fast enough to compete with electron-hole recombination in the quantum well, and results in greater than 50 per cent energy-transfer efficiencies in the tested structures. Furthermore, the measured energy-transfer rates are sufficiently large to provide pumping in the stimulated emission regime, indicating the feasibility of nanocrystal-based optical amplifiers and lasers based on this approach.

We observe ultrafast 1P-to-1S intraband relaxation in PbSe and CdSe nanocrystals (NCs) that have distinct energy spectra. While ultrafast dynamics in CdSe NCs has typically been interpreted in terms of electron-hole energy transfer, this mechanism is not active in PbSe NCs because of sparse densities of states in the conduction and valence bands. Our observations of temperature activation and confinement-enhanced relaxation in PbSe NCs can be explained by efficient multiphonon emission triggered by nonadiabatic electron-phonon interactions and are indicative of large, size-dependent, intraband Huang-Rhys parameters.

Recently, we demonstrated that PbSe nanocrystal quantum dots can efficiently produce multiple electron-hole pairs (excitons) in response to a single absorbed photon. To address the generality of this carrier-multiplication phenomenon to other materials, we perform a comparative study of multiexciton generation in PbSe and CdSe nanocrystals that have distinctly different electronic structures. We find that both materials exhibit high-efficiency carrier multiplication and the activation threshold is lower in CdSe nanocrystals than in PbSe nanocrystals (∼2.5 vs ∼2.9 energy gaps). Furthermore, the efficiencies of multiexciton generation are nearly identical for both materials despite a vast difference in both energy structures and carrier relaxation behaviors, strongly suggesting that this phenomenon is general to quantum-confined semiconductor nanocrystals.

We study spectrally resolved dynamics of Förster energy transfer in single monolayers and bilayers of semiconductor nanocrystal quantum dots assembled using Langmuir-Blodgett (LB) techniques. For a single monolayer, we observe a distribution of transfer times from ~50 ps to ~10 ns, which can be quantitatively modeled assuming that the energy transfer is dominated by interactions of a donor nanocrystal with acceptor nanocrystals from the first three "shells" surrounding the donor. We also detect an effective enhancement of the absorption cross section (up to a factor of 4) for larger nanocrystals on the "red" side of the size distribution, which results from strong, inter-dot electrostatic coupling in the LB film (the light-harvesting antenna effect). By assembling bilayers of nanocrystals of two different sizes, we are able to improve the donor-acceptor spectral overlap for engineered transfer in a specific ("vertical") direction. These bilayers show a fast, unidirectional energy flow with a time constant of ~120 ps.