Recent developments in photovoltaic materials have led to continual improvements in their efficiency. We review the electrical characteristics of 16 widely studied geometries of photovoltaic materials with efficiencies of 10 to 29%. Comparison of these characteristics to the fundamental limits based on the Shockley-Queisser detailed-balance model provides a basis for identifying the key limiting factors, related to efficient light management and charge carrier collection, for these materials. Prospects for practical application and large-area fabrication are discussed for each material.

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Photovoltaic materials: Present efficiencies and future challenges

All nanomaterials share a common feature of large surface-to-volume ratio, making their surfaces the dominant player in many physical and chemical processes. Surface ligands - molecules that bind to the surface - are an essential component of nanomaterial synthesis, processing and application. Understanding the structure and properties of nanoscale interfaces requires an intricate mix of concepts and techniques borrowed from surface science and coordination chemistry. Our Review elaborates these connections and discusses the bonding, electronic structure and chemical transformations at nanomaterial surfaces. We specifically focus on the role of surface ligands in tuning and rationally designing properties of functional nanomaterials. Given their importance for biomedical (imaging, diagnostics and therapeutics) and optoelectronic (light-emitting devices, transistors, solar cells) applications, we end with an assessment of application-targeted surface engineering.

The surface science of nanocrystals.

Graham H. Carey,† Ahmed L. Abdelhady,‡ Zhijun Ning, Susanna M. Thon, Osman M. Bakr,‡ and Edward H. Sargent*,† †Department of Electrical and Computer Engineering, University of Toronto, 10 King’s College Road, Toronto, Ontario M5S 3G4, Canada ‡Division of Physical Sciences and Engineering, Solar & Photovoltaics Engineering Center, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi Arabia School of Physical Science and Technology, ShanghaiTech University, 100 Haike Road, Shanghai 201210, China Department of Electrical and Computer Engineering, Johns Hopkins University, 3400 North Charles Street, Baltimore, Maryland 21218, United States

Colloidal Quantum Dot Solar Cells.

Colloidal nanocrystals (NCs, i.e., crystalline nanoparticles) have become an important class of materials with great potential for applications ranging from medicine to electronic and optoelectronic devices. Today’s strong research focus on NCs has been prompted by the tremendous progress in their synthesis. Impressively narrow size distributions of just a few percent, rational shape-engineering, compositional modulation, electronic doping, and tailored surface chemistries are now feasible for a broad range of inorganic compounds. The performance of inorganic NC-based photovoltaic and light-emitting devices has become competitive to other state-of-the-art materials. Semiconductor NCs hold unique promise for near- and mid-infrared technologies, where very few semiconductor materials are available. On a purely fundamental side, new insights into NC growth, chemical transformations, and self-organization can be gained from rapidly progressing in situ characterization and direct imaging techniques. New phenom...

Prospects of Nanoscience with Nanocrystals

The electronic properties of colloidal quantum dots (QDs) are critically dependent on both QD size and surface chemistry. Modification of quantum confinement provides control of the QD bandgap, while ligand-induced surface dipoles present a hitherto underutilized means of control over the absolute energy levels of QDs within electronic devices. Here, we show that the energy levels of lead sulfide QDs, measured by ultraviolet photoelectron spectroscopy, shift by up to 0.9 eV between different chemical ligand treatments. The directions of these energy shifts match the results of atomistic density functional theory simulations and scale with the ligand dipole moment. Trends in the performance of photovoltaic devices employing ligand-modified QD films are consistent with the measured energy level shifts. These results identify surface-chemistry-mediated energy level shifts as a means of predictably controlling the electronic properties of colloidal QD films and as a versatile adjustable parameter in the perfo...

Energy level modification in lead sulfide quantum dot thin films through ligand exchange.

Fabricating low-temperature solution-processed solar cells with good power-conversion efficiency and stability in ambient conditions has proved challenging. The use of ligands that protect colloidal quantum dots from degradation in air and tune their energy levels is now shown to be a viable approach for the realization of spin-coated solar cells with very high efficiency. Solution processing is a promising route for the realization of low-cost, large-area, flexible and lightweight photovoltaic devices with short energy payback time and high specific power. However, solar cells based on solution-processed organic, inorganic and hybrid materials reported thus far generally suffer from poor air stability, require an inert-atmosphere processing environment or necessitate high-temperature processing1, all of which increase manufacturing complexities and costs. Simultaneously fulfilling the goals of high efficiency, low-temperature fabrication conditions and good atmospheric stability remains a major technical challenge, which may be addressed, as we demonstrate here, with the development of room-temperature solution-processed ZnO/PbS quantum dot solar cells. By engineering the band alignment of the quantum dot layers through the use of different ligand treatments, a certified efficiency of 8.55% has been reached. Furthermore, the performance of unencapsulated devices remains unchanged for over 150 days of storage in air. This material system introduces a new approach towards the goal of high-performance air-stable solar cells compatible with simple solution processes and deposition on flexible substrates.

Improved performance and stability in quantum dot solar cells through band alignment engineering

Quantum dot photovoltaics (QDPV) offer the potential for low-cost solar cells. To develop strategies for continued improvement in QDPVs, a better understanding of the factors that limit their performance is essential. Here, we study carrier recombination processes that limit the power conversion efficiency of PbS QDPVs. We demonstrate the presence of radiative sub-bandgap states and sub-bandgap state filling in operating devices by using photoluminescence (PL) and electroluminescence (EL) spectroscopy. These sub-bandgap states are most likely the origin of the high open-circuit-voltage (VOC) deficit and relatively limited carrier collection that have thus far been observed in QDPVs. Combining these results with our perspectives on recent progress in QDPV, we conclude that eliminating sub-bandgap states in PbS QD films has the potential to show a greater gain than may be attainable by optimization of interfaces between QDs and other materials. We suggest possible future directions that could guide the design of high-performance QDPVs.

Open-Circuit Voltage Deficit, Radiative Sub-Bandgap States, and Prospects in Quantum Dot Solar Cells

Chemical oxidation of under-charged Pb atoms reduces the density of trap states by a factor of 40 in films of colloidal PbS quantum dots for devices. These emissive sub-bandgap states are a byproduct of several standard ligand-exchange procedures. X-ray photoelectron spectro-scopy measurements and density function theory simulations demonstrate that they are associated with under-charged Pb.

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Chia-Hao Marcus Chuang

Papers

Improved performance and stability in quantum dot solar cells through band alignment engineering

Improved performance and stability in quantum dot solar cells through band alignment engineering

Open-Circuit Voltage Deficit, Radiative Sub-Bandgap States, and Prospects in Quantum Dot Solar Cells

Identifying and Eliminating Emissive Sub-bandgap States in Thin Films of PbS Nanocrystals.

Enhanced Photocurrent in PbS Quantum Dot Photovoltaics via ZnO Nanowires and Band Alignment Engineering