Strategies for increasing the efficiency of heterojunction organic solar cells: material selection and device architecture.

Thin-film blends or bilayers of donor- and acceptor-type organic semiconductors form the core of heterojunction organic photovoltaic cells. Researchers measure the quality of photovoltaic cells based on their power conversion efficiency, the ratio of the electrical power that can be generated versus the power of incident solar radiation. The efficiency of organic solar cells has increased steadily in the last decade, currently reaching up to 6%. Understanding and combating the various loss mechanisms that occur in processes from optical excitation to charge collection should lead to efficiencies on the order of 10% in the near future. In organic heterojunction solar cells, the generation of photocurrent is a cascade of four steps: generation of excitons (electrically neutral bound electron-hole pairs) by photon absorption, diffusion of excitons to the heterojunction, dissociation of the excitons into free charge carriers, and transport of these carriers to the contacts. In this Account, we review our recent contributions to the understanding of the mechanisms that govern these steps. Starting from archetype donor-acceptor systems of planar small-molecule heterojunctions and solution-processed bulk heterojunctions, we outline our search for alternative materials and device architectures. We show that non-planar phthalocynanines have appealing absorption characteristics but also have reduced charge carrier transport. As a result, the donor layer needs to be ultrathin, and all layers of the device have to be tuned to account for optical interference effects. Using these optimization techniques, we illustrate cells with 3.1% efficiency for the non-planar chloroboron subphthalocyanine donor. Molecules offering a better compromise between absorption and carrier mobility should allow for further improvements. We also propose a method for increasing the exciton diffusion length by converting singlet excitons into long-lived triplets. By doping a polymer with a phosphorescent molecule, we demonstrate an increase in the exciton diffusion length of a polymer from 4 to 9 nm. If researchers can identify suitable phosphorescent dopants, this method could be employed with other materials. The carrier transport from the junction to the contacts is markedly different for a bulk heterojunction cell than for planar junction cells. Unlike for bulk heterojunction cells, the open-circuit voltage of planar-junction cells is independent of the contact work functions, as a consequence of the balance of drift and diffusion currents in these systems. This understanding helps to guide the development of new materials (particularly donor materials) that can further boost the efficiency of single-junction cells to 10%. With multijunction architectures, we expect that efficiencies of 12-16% could be attained, at which point organic photovoltaic cells could become an important renewable energy source.

[1]  Shijun Jia,et al.  Polymer–Fullerene Bulk‐Heterojunction Solar Cells , 2009, Advanced materials.

[2]  Barry P Rand,et al.  Organic solar cells with sensitized phosphorescent absorbing layers , 2009 .

[3]  Barry P Rand,et al.  The characterization of chloroboron (III) subnaphthalocyanine thin films and their application as a donor material for organic solar cells , 2009 .

[4]  Nelson E. Coates,et al.  Bulk heterojunction solar cells with internal quantum efficiency approaching 100 , 2009 .

[5]  P. Heremans,et al.  Nanoimprinted semiconducting polymer films with 50 nm features and their application to organic heterojunction solar cells , 2008, Nanotechnology.

[6]  K. Leo,et al.  Small-molecule solar cells—status and perspectives , 2008, Nanotechnology.

[7]  Charlotte K. Williams,et al.  Charge recombination in organic photovoltaic devices with high open-circuit voltages. , 2008, Journal of the American Chemical Society.

[8]  Jean Manca,et al.  The Relation Between Open‐Circuit Voltage and the Onset of Photocurrent Generation by Charge‐Transfer Absorption in Polymer : Fullerene Bulk Heterojunction Solar Cells , 2008 .

[9]  Barry P Rand,et al.  The angular response of ultrathin film organic solar cells , 2008 .

[10]  Jan Genoe,et al.  Analytical model for the open-circuit voltage and its associated resistance in organic planar heterojunction solar cells , 2008 .

[11]  Jean M. J. Fréchet,et al.  Polymer—Fullerene Composite Solar Cells. , 2008 .

[12]  Weimin Zhang,et al.  Charge carrier formation in polythiophene/fullerene blend films studied by transient absorption spectroscopy. , 2008, Journal of the American Chemical Society.

[13]  N. Armstrong,et al.  Titanyl phthalocyanine/C60 heterojunctions: Band-edge offsets and photovoltaic device performance , 2008 .

[14]  Jan Genoe,et al.  Solar cells utilizing small molecular weight organic semiconductors , 2007 .

[15]  P. Heremans,et al.  Electro‐Optical Study of Subphthalocyanine in a Bilayer Organic Solar Cell , 2007 .

[16]  N. E. Coates,et al.  Efficient Tandem Polymer Solar Cells Fabricated by All-Solution Processing , 2007, Science.

[17]  Barry P Rand,et al.  Near-infrared sensitive small molecule organic photovoltaic cells based on chloroaluminum phthalocyanine , 2007 .

[18]  K. Leo,et al.  Improved efficiency of zinc phthalocyanine/C60 based photovoltaic cells via nanoscale interface modification , 2007 .

[19]  Stephen R. Forrest,et al.  Offset energies at organic semiconductor heterojunctions and their influence on the open-circuit voltage of thin-film solar cells , 2007 .

[20]  S. Forrest,et al.  Efficient Solar Cells Using All‐Organic Nanocrystalline Networks , 2007 .

[21]  Barry P Rand,et al.  Enhanced open-circuit voltage in subphthalocyanine/C60 organic photovoltaic cells. , 2006, Journal of the American Chemical Society.

[22]  Valentin D. Mihailetchi,et al.  Ultimate efficiency of polymer/fullerene bulk heterojunction solar cells , 2006 .

[23]  Stephen R. Forrest,et al.  Mixed donor-acceptor molecular heterojunctions for photovoltaic applications. I. Material properties , 2005 .

[24]  S. Forrest,et al.  Organic solar cells with sensitivity extending into the near infrared , 2005 .

[25]  Yang Yang,et al.  High-efficiency solution processable polymer photovoltaic cells by self-organization of polymer blends , 2005 .

[26]  Valentin D. Mihailetchi,et al.  Device model for the operation of polymer/fullerene bulk heterojunction solar cells , 2005 .

[27]  Stephen R. Forrest,et al.  A Hybrid Planar–Mixed Molecular Heterojunction Photovoltaic Cell , 2005 .

[28]  V. Mihailetchi,et al.  Cathode dependence of the open-circuit voltage of polymer:fullerene bulk heterojunction solar cells , 2003 .

[29]  Stephen R. Forrest,et al.  Efficient bulk heterojunction photovoltaic cells using small-molecular-weight organic thin films , 2003, Nature.

[30]  H. Ogata,et al.  Electronic absorption spectra of substituted phthalocyanines in solution and as films , 2003 .

[31]  H. Bässler,et al.  Sensitized intrinsic phosphorescence from a poly(phenylene-vinylene) derivative , 2003 .

[32]  Stephen R. Forrest,et al.  Small molecular weight organic thin-film photodetectors and solar cells , 2003 .

[33]  Brian A. Gregg,et al.  Comparing organic to inorganic photovoltaic cells: Theory, experiment, and simulation , 2003 .

[34]  Neil C. Greenham,et al.  Modeling the current-voltage characteristics of bilayer polymer photovoltaic devices , 2003 .

[35]  Tomás Torres,et al.  Subphthalocyanines: singular nonplanar aromatic compounds-synthesis, reactivity, and physical properties. , 2002, Chemical reviews.

[36]  A. Tortschanoff,et al.  Site Torsional Motion and Dispersive Excitation Hopping Transfer in π-Conjugated Polymers† , 2000 .

[37]  L. S. Roman,et al.  Modeling photocurrent action spectra of photovoltaic devices based on organic thin films , 1999 .

[38]  James S. Shirk,et al.  The Alpha Substitution Effect on Phthalocyanine Aggregation , 1998 .

[39]  Y. Saito,et al.  Photothermal investigation of the triplet state of carbon molecule (C60) , 1991 .

[40]  C. Tang Two‐layer organic photovoltaic cell , 1986 .