Origin of Low Sensitizing Efficiency of Quantum Dots in Organic Solar Cells

Organic semiconductors are of great interest for application in cheap and flexible solar cells. They have a typical absorption onset in the visible. Infrared light can be harvested by use of lead-chalcogenide quantum dot sensitizers. However, bulk-heterojunction solar cells with quantum-dot sensitizers are inefficient. Here we use ultrafast transient absorption and time-domain terahertz spectroscopy to show that charge localization on the quantum dot leads to enhanced coulomb attraction of its counter charge in the organic semiconductor. This localization-enhanced coulomb attraction is the fundamental cause of the poor efficiency of these photovoltaic architectures. It is of prime importance for improving solar cell efficiency to directly photogenerate spatially separated charges. This can be achieved when both charges are delocalized. Our findings provide a rationalization in the development of photovoltaic architectures that exploit quantum dots to harvest the near-infrared part of the solar spectrum more efficiently

Activating Carrier Multiplication in PbSe Quantum Dot Solids by Infilling with Atomic Layer Deposition

Carrier multiplicationthe generation of multiple electron–hole pairs by a single photonis currently of great interest for the development of highly efficient photovoltaics. We study the effects of infilling PbSe quantum-dot solids with metal oxides by atomic layer deposition on carrier multiplication. Using time-resolved microwave conductivity measurements, we find, for the first time, that carrier multiplication occurs in 1,2-ethanedithiol-linked PbSe quantum-dot solids infilled with Al₂O₃ or Al₂O₃/ZnO, while it is negligible or absent in noninfilled films. The carrier-multiplication efficiency of the infilled quantum-dot solids is close to that of solution-dispersed PbSe quantum dots, and not significantly limited by Auger recombination

Broadband and Picosecond Intraband Absorption in Lead-Based Colloidal Quantum Dots

Using femtosecond transient absorption spectroscopy, we demonstrate that lead chalcogenide nanocrystals show considerable photoinduced absorption (PA) in a broad wavelength range just below the band gap. The time-dependent decay of the PA signal correlates with the recovery of the band gap absorption, indicating that the same carriers are involved. On this basis, we assign this PA signal to intraband absorption, that is, the excitation of photogenerated carriers from the bottom of the conduction band or the top of the valence band to higher energy levels in the conduction and valence band continuum. We confirm our experiments with tight-binding calculations. This broadband response in the commercially interesting near- to mid-infrared range is very relevant for ultra-high-speed all-optical signal processing. We benchmark the performance with bulk Si and Si nanocrystals