Harald Ade

Aggregation and morphology control enables multiple cases of high-efficiency polymer solar cells

Although the field of polymer solar cell has seen much progress in device performance in the past few years, several limitations are holding back its further development. For instance, current high-efficiency (>9.0%) cells are restricted to material combinations that are based on limited donor polymers and only one specific fullerene acceptor. Here we report the achievement of high-performance (efficiencies up to 10.8%, fill factors up to 77%) thick-film polymer solar cells for multiple polymer:fullerene combinations via the formation of a near-ideal polymer:fullerene morphology that contains highly crystalline yet reasonably small polymer domains. This morphology is controlled by the temperature-dependent aggregation behaviour of the donor polymers and is insensitive to the choice of fullerenes. The uncovered aggregation and design rules yield three high-efficiency (>10%) donor polymers and will allow further synthetic advances and matching of both the polymer and fullerene materials, potentially leading to significantly improved performance and increased design flexibility.

Energy‐Level Modulation of Small‐Molecule Electron Acceptors to Achieve over 12% Efficiency in Polymer Solar Cells

Fine energy-level modulations of small-molecule acceptors (SMAs) are realized via subtle chemical modifications on strong electron-withdrawing end-groups. The two new SMAs (IT-M and IT-DM) end-capped by methyl-modified dicycanovinylindan-1-one exhibit upshifted lowest unoccupied molecular orbital (LUMO) levels, and hence higher open-circuit voltages can be observed in the corresponding devices. Finally, a top power conversion efficiency of 12.05% is achieved.

Interferometer-controlled scanning transmission X-ray microscopes at the Advanced Light Source

Two new soft X-ray scanning transmission microscopes located at the Advanced Light Source (ALS) have been designed, built and commissioned. Interferometer control implemented in both microscopes allows the precise measurement of the transverse position of the zone plate relative to the sample. Long-term positional stability and compensation for transverse displacement during translations of the zone plate have been achieved. The interferometer also provides low-distortion orthogonal x, y imaging. Two different control systems have been developed: a digital control system using standard VXI components at beamline 7.0, and a custom feedback system based on PC AT boards at beamline 5.3.2. Both microscopes are diffraction limited with the resolution set by the quality of the zone plates. Periodic features with 30 nm half period can be resolved with a zone plate that has a 40 nm outermost zone width. One microscope is operating at an undulator beamline (7.0), while the other is operating at a novel dedicated bending-magnet beamline (5.3.2), which is designed specifically to illuminate the microscope. The undulator beamline provides count rates of the order of tens of MHz at high-energy resolution with photon energies of up to about 1000 eV. Although the brightness of a bending-magnet source is about four orders of magnitude smaller than that of an undulator source, photon statistics limited operation with intensities in excess of 3 MHz has been achieved at high energy resolution and high spatial resolution. The design and performance of these microscopes are described.

High Performance All-Polymer Solar Cell via Polymer Side-Chain Engineering

Acknowledge support from the Office of Naval Research (N00014-14-1-0142), KAUST Center for Advanced Molecular Photovoltaics at Stanford and the Stanford Global Climate and Energy Program, NSF DMR-1303742 and the National Natural Science Foundation of China (Projects 21174004 and 21222403). Soft X-ray characterization and analysis by NCSU supported by the U.S. Department of Energy, Office of Science, Basic Energy Science, Division of Materials Science and Engineering under Contract DE-FG02-98ER45737. Soft X-ray data was acquired at beamlines 11.0.1.2 at the Advanced Light Source, which is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U. S. Department of Energy under Contract No. DE-AC02-05CH11231. We thank Professor Michael D. McGehee, Dr. George F. Burkhard and Dr. Eric T. Hoke for their help in discussion of the recombination mechanism.

From Binary to Ternary Solvent: Morphology Fine‐tuning of D/A Blends in PDPP3T‐based Polymer Solar Cells

For the PDPP3T/PCBM system investigated here, atomic force microscopy, resonant soft X-ray scattering, and grazing incidence wide angle X-ray scattering are used as an initial set of tools to determine the surface texture, the bulk compositional morphology, and the crystallization behavior, respectively. We find systematic variations and relate them to device performance. A solvent mixture of DCB/CF/DIO = 76:19:5 (v/v/v) yields a PCE of 6.71%.

Soft x-ray scattering facility at the Advanced Light Source with real-time data processing and analysis

We present the development and characterization of a dedicated resonant soft x-ray scattering facility. Capable of operation over a wide energy range, the beamline and endstation are primarily used for scattering from soft matter systems around the carbon K-edge (∼285 eV). We describe the specialized design of the instrument and characteristics of the beamline. Operational characteristics of immediate interest to users such as polarization control, degree of higher harmonic spectral contamination, and detector noise are delineated. Of special interest is the development of a higher harmonic rejection system that improves the spectral purity of the x-ray beam. Special software and a user-friendly interface have been implemented to allow real-time data processing and preliminary data analysis simultaneous with data acquisition.

Enhanced Photovoltaic Performance by Modulating Surface Composition in Bulk Heterojunction Polymer Solar Cells Based on PBDTTT-C-T/PC71BM

For the blend film of PBDTTT-C-T:PC71 BM, the use of 1,8-diiodooctane as the solvent additive enriches the polymer at the top surface, so that a power conversion efficiency of 9.13% is recorded in the inverted polymer solar cell based on the blend, which is much higher than that of the device with conventional structure.

High‐Efficiency All‐Polymer Solar Cells Based on a Pair of Crystalline Low‐Bandgap Polymers

All-polymer solar cells based on a pair of crystalline low-bandgap polymers (NT and N2200) are demonstrated to achieve a high short-circuit current density of 11.5 mA cm-2 and a power conversion efficiency of up to 5.0% under the standard AM1.5G spectrum with one sun intensity. The high performance of these NT:N2200-based cells can be attributed to the low optical bandgaps of the polymers and the reasonably high and balanced electron and hole mobilities of the NT:N2200 blends due to the crystalline nature of the two polymers.

Polarized X-ray scattering reveals non-crystalline orientational ordering in organic films

Molecular orientation critically influences the mechanical, chemical, optical and electronic properties of organic materials. So far, molecular-scale ordering in soft matter could be characterized with X-ray or electron microscopy techniques only if the sample exhibited sufficient crystallinity. Here, we show that the resonant scattering of polarized soft X-rays (P-SoXS) by molecular orbitals is not limited by crystallinity and that it can be used to probe molecular orientation down to size scales of 10 nm. We first apply the technique on highly crystalline small-molecule thin films and subsequently use its high sensitivity to probe the impact of liquid-crystalline ordering on charge mobility in polymeric transistors. P-SoXS also reveals scattering anisotropy in amorphous domains of all-polymer organic solar cells where interfacial interactions pattern orientational alignment in the matrix phase, which probably plays an important role in the photophysics. The energy and q-dependence of the scattering anisotropy allows the identification of the composition and the degree of orientational order in the domains.

Mobility-Controlled Performance of Thick Solar Cells Based on Fluorinated Copolymers

Developing novel materials and device architectures to further enhance the efficiency of polymer solar cells requires a fundamental understanding of the impact of chemical structures on photovoltaic properties. Given that device characteristics depend on many parameters, deriving structure-property relationships has been very challenging. Here we report that a single parameter, hole mobility, determines the fill factor of several hundred nanometer thick bulk heterojunction photovoltaic devices based on a series of copolymers with varying amount of fluorine substitution. We attribute the steady increase of hole mobility with fluorine content to changes in polymer molecular ordering. Importantly, all other parameters, including the efficiency of free charge generation and the coefficient of nongeminate recombination, are nearly identical. Our work emphasizes the need to achieve high mobility in combination with strongly suppressed charge recombination for the thick devices required by mass production technologies.