Optical Transparency Enabled by Anomalous Stokes Shift in Visible Light-Emitting CuAlS₂-Based Quantum Dots

Abstract

We observe and study the anomalous Stokes shift of CuAlS2/CdS quantum dots. While all known I–III–VI2 semiconductor core/shell quantum dots show Stokes shifts in excess of 100 meV, the shift associated with CuAlS2/CdS quantum dots is uniquely large, even exceeding 1.4 eV in some cases. CuAlS2/CdS quantum dots are thus associated with cross sections less than 10–17 cm2 under the emission maximum. We investigate this anomaly using spectroscopic techniques and ascribe it to the existence of a strong type-II offset between CuAlS2 and CdS layers. Besides their strong Stokes shift, CuAlS2/CdS quantum dots also exhibit high quantum yields (63%) as well as long emission lifetimes (∼1500 ns). Because of the combined existence of these properties, CuAlS2/CdS quantum dots can act as tunable, transparent emitters over the entire visible spectrum. As a demonstration of their potential, we describe the construction of a wide area transparent lighting device with waveguided optical excitation and a clear aperture of 7.5 cm2.