A path to practical Solar Pumped Lasers via Radiative Energy Transfer.

The optical conversion of incoherent solar radiation into a bright, coherent laser beam enables the application of nonlinear optics to solar energy conversion and storage. Here, we present an architecture for solar pumped lasers that uses a luminescent solar concentrator to decouple the conventional trade-off between solar absorption efficiency and the mode volume of the optical gain material. We report a 750-µm-thick Nd(3+)-doped YAG planar waveguide sensitized by a luminescent CdSe/CdZnS (core/shell) colloidal nanocrystal, yielding a peak cascade energy transfer of 14%, a broad spectral response in the visible portion of the solar spectrum, and an equivalent quasi-CW solar lasing threshold of 23 W-cm(-2), or approximately 230 suns. The efficient coupling of incoherent, spectrally broad sunlight in small gain volumes should allow the generation of coherent laser light from intensities of less than 100 suns.

Energy harvesting of non-emissive triplet excitons in tetracene by emissive PbS nanocrystals.

Triplet excitons are ubiquitous in organic optoelectronics, but they are often an undesirable energy sink because they are spin-forbidden from emitting light and their high binding energy hinders the generation of free electron-hole pairs. Harvesting their energy is consequently an important technological challenge. Here, we demonstrate direct excitonic energy transfer from 'dark' triplets in the organic semiconductor tetracene to colloidal PbS nanocrystals, thereby successfully harnessing molecular triplet excitons in the near infrared. Steady-state excitation spectra, supported by transient photoluminescence studies, demonstrate that the transfer efficiency is at least (90 ± 13)%. The mechanism is a Dexter hopping process consisting of the simultaneous exchange of two electrons. Triplet exciton transfer to nanocrystals is expected to be broadly applicable in solar and near-infrared light-emitting applications, where effective molecular phosphors are lacking at present. In particular, this route to 'brighten' low-energy molecular triplet excitons may permit singlet exciton fission sensitization of conventional silicon solar cells.

Efficient luminescent down-shifting detectors based on colloidal quantum dots for dual-band detection applications.

A colloidal quantum dot (QD) luminescent down-shifting (LDS) layer is used to sensitize an InGaAs short wavelength infrared photodetector to the near UV spectral band. An average improvement in the external quantum efficiency (EQE) from 1.8% to 21% across the near UV is realized using an LDS layer consisting of PbS/CdS core/shell QDs embedded in PMMA. A simple model is used to fit the experimental EQE data. A UV sensitive InGaAs imaging array is demonstrated and the effect of the LDS layer on the optical resolution is calculated. The bandwidth of the LDS detector under UV illumination is characterized and shown to be determined by the photoluminescence lifetime of the QDs.