Colloidal lead sulfide quantum dot (PbS QD) solar cells have recently shown attractive improvements in efficiency [1]. PbS QDs have been investigated in various device architectures—including Schottky junction, depleted planar heterojunction, and ordered bulk heterojunction photovoltaic (PV) architectures—with the aim of maximizing light absorption while maintaining efficient charge transport ^[1] . However, the thickness of the PbS QD layer in the aforementioned architectures remains limited by the relatively short exciton diffusion length characteristic of all QD films.  We developed a novel architecture in which PbS QDs and zinc oxide (ZnO) nanoparticles are co-deposited from solution to form a bulk heterojunction (BHJ). Much like a typical polymer BHJ solar cell, these PbS QD PV devices can decouple the light absorption, which is proportional to device thickness, from the exciton diffusion length ^[2] . We fabricated these BHJ PbS QD:ZnO solar cells in solution by layer-by-layer deposition in which each step is followed by ligand exchange as shown in Figure 1a. By conducting preliminary optimization of the processing condition, we obtained the current density as a function of the applied voltage graph shown in Figure 1b. Further studies aim at improving device performance while studying the morphological conformation of PbS and ZnO domains.

Figure 1: a) Schematic of the solution process for fabrication of bulk heterojunction lead sulfide quantum dots (PbS QD) and zinc oxide (ZnO) solar cells. The devices are fabricated by layer-by-layer deposition in which each step is followed by ligand exchange. b) JV characteristics under dark (squares) and AM 1.5 illumination (circles) for planar (control – red) and bulk heterojunction (blue) PbS QD:ZnO devices.

1. J. Tang and E. H. Sargent, “Infrared colloidal quantum dots for photovoltaics: Fundamentals and recent progress,” Advanced Materials, vol. 23, no. 1, pp. 12–29, Jan. 2011.
2. C. J. Brabec, S. Gowrisanker, J. J. M. Halls, D. Laird, S. J. Jia, and S. P. Williams, “Polymer-fullerene bulk-heterojunction solar cells,” Advanced Materials, vol. 22, pp. 3839–3856, Aug. 2010.

Nanostructured solar cells are attracting increasing attention as a promising photovoltaic (PV) technology ^[1] . Generation of free charge carriers in nanostructured PV devices occurs at the electron donor-acceptor interface, analogous to the pn-junction interface in traditional crystalline silicon solar cells. However, recombination at this interface constitutes one of the major charge carrier loss pathways. Thus characterizing and controlling recombination dynamics is critical for informing the design of novel device architectures. Recombination parameters also enable comparisons between different device architectures.

In this work, we employ the transient photovoltage (TPV) technique ^[2] to probe recombination mechanisms under standard operating conditions in three different solar cells, as shown in Figure 1: a poly(3-hexylthiophene) and phenyl-C₆₁-butyric acid methyl ester (P3HT:PCBM) bulk heterojunction; a chloroaluminium phthalocyanine and fullerene (ClAlPc:C₆₀) planar mixed heterojunction; and a lead sulfide quantum dot and zinc oxide (QD PbS:ZnO) pn-heterojunction. The normalized TPV data acquired at 0.5-sun illumination intensity are shown in Figure 2a, which compares the recombination lifetimes of charge carriers in these devices. The observed differences in carrier lifetimes may arise from variations in the respective interface morphologies: for example, the slower recombination transients observed in the ClAlPc:C₆₀ device may be attributed to the intrinsic planarity of this particular architecture.  We can also measure the charge carrier lifetime as a function of the light intensity, as shown in Figure 2b; this result confirms that recombination dynamics are faster in P3HT:PCBM and QD PbS:ZnO than in ClAlPc:C₆₀ PV devices.

1. Anonymous, “A sunny outlook,” Nature Photonics, vol. 6, no. 3, p. 129, Mar. 2012.
2. C. G. Shuttle, B. O’Regan, A. M. Ballantyne, J. Nelson, D. D. C. Bradley, J. de Mello, and J. R. Durrant, “Experimental determination of the rate law for charge carrier decay in a polythiophene: Fullerene solar cell,” Applied Physics Letters, vol. 92, p. 3, 2008.