Carbon materials are excellent candidates for photovoltaic solar cells: they are Earth-abundant, possess high optical absorption, and maintain superior thermal and photostability. Here we report on solar cells with active layers made solely of carbon nanomaterials that present the same advantages of conjugated polymer-based solar cells, namely, solution processable, potentially flexible, and chemically tunable, but with increased photostability and the possibility to revert photodegradation. The device active layer composition is optimized using ab initio density functional theory calculations to predict type-II band alignment and Schottky barrier formation. The best device fabricated is composed of PC(70)BM fullerene, semiconducting single-walled carbon nanotubes, and reduced graphene oxide. This active-layer composition achieves a power conversion efficiency of 1.3%-a record for solar cells based on carbon as the active material-and we calculate efficiency limits of up to 13% for the devices fabricated in this work, comparable to those predicted for polymer solar cells employing PCBM as the acceptor. There is great promise for improving carbon-based solar cells considering the novelty of this type of device, the high photostability, and the availability of a large number of carbon materials with yet untapped potential for photovoltaics. Our results indicate a new strategy for efficient carbon-based, solution-processable, thin film, photostable solar cells.

Despite the potentials and the efforts put in the development of uncooled carbon nanotube infrared detectors during the past two decades, their figure-of-merit detectivity remains orders of magnitude lower than that of conventional semiconductor counterparts due to the lack of efficient exciton dissociation schemes. In this paper, we report an extraordinary photocurrent harvesting configuration at a semiconducting single-walled carbon nanotube (s-SWCNT)/polymer type-II heterojunction interface, which provides highly efficient exciton dissociation through the intrinsic energy offset by designing the s-SWCNT/polymer interface band alignment. This results in significantly enhanced near-infrared detectivity of 2.3 × 10(8) cm·Hz(1/2)/W, comparable to that of the many conventional uncooled infrared detectors. With further optimization, the s-SWCNT/polymer nanohybrid uncooled infrared detectors could be highly competitive for practical applications.

Iron pyrite (fool's gold, FeS2) is a promising earth abundant and environmentally benign semiconductor material that shows promise as a strong and broad absorber for photovoltaics and high energy density cathode material for batteries. However, controlling FeS2 nanocrystal formation (composition, size, shape, stoichiometry, etc.) and defect mitigation still remains a challenge. These problems represent significant limitations in the ability to control electrical, optical and electrochemical properties to exploit pyrite's full potential for sustainable energy applications. Here, we report a symmetry-defying oriented attachment FeS2 nanocrystal growth by examining the nanostructure evolution and recrystallization to uncover how the shape, size and defects of FeS2 nanocrystals changes during growth. It is demonstrated that a well-controlled reaction temperature and annealing time results in polycrystal-to-monocrystal formation and defect annihilation, which correlates with the performance of photoresponse devices. This knowledge opens up a new tactic to address pyrite's known defect problems.

Porous materials such as cellular cytosol, hydrogels, and block copolymers have nanoscale features that determine macroscale properties. Characterizing the structure of nanopores is difficult with current techniques due to imaging, sample preparation, and computational challenges. We produce a super-resolution optical image that simultaneously characterizes the nanometer dimensions of and diffusion dynamics within porous structures by correlating stochastic fluctuations from diffusing fluorescent probes in the pores of the sample, dubbed here as "fluorescence correlation spectroscopy super-resolution optical fluctuation imaging" or "fcsSOFI". Simulations demonstrate that structural features and diffusion properties can be accurately obtained at sub-diffraction-limited resolution. We apply our technique to image agarose hydrogels and aqueous lyotropic liquid crystal gels. The heterogeneous pore resolution is improved by up to a factor of 2, and diffusion coefficients are accurately obtained through our method compared to diffraction-limited fluorescence imaging and single-particle tracking. Moreover, fcsSOFI allows for rapid and high-throughput characterization of porous materials. fcsSOFI could be applied to soft porous environments such hydrogels, polymers, and membranes in addition to hard materials such as zeolites and mesoporous silica.

Single molecule tracking (SMT) and fluorescence correlation spectroscopy (FCS) are used to investigate probe molecule diffusion within the mesophase structures of Pluronic F127 gels. Mixtures are prepared in the hexagonal, lamellar, and cubic regions of the ternary F127/water/butanol phase diagram and are doped with nanomolar concentrations of a perylene diimide dye (DTPDI). Flow aligned F127 gels comprised of hexagonally arranged cylindrical micelles exhibit distinct one-dimensional (1D) DTPDI motion in wide-field videos, with diffusion occurring parallel to the flow alignment direction. The slow 1D dye motion observed is attributed to single molecule diffusion within the viscous, hydrophobic micelle cores. FCS data acquired from the same samples reveal a bimodal distribution of diffusion coefficients with the slower component assigned to 1D motion in the micelle core and the faster component to 3D diffusion in the interconnected micelle coronas. The rate of diffusion for both components increases with decreasing F127 concentration, reflecting a decrease in gel microviscosity. SMT data from the lamellar and cubic mesophases depict isotropic 2D and 3D diffusion, respectively, and provide supporting evidence for the role of the micelle core and corona in governing diffusion. Trajectory angle distributions from 1D diffusing species in the hexagonal mesophase provide quantitative information on the alignment of the cylindrical micelles. These results, and the rare observation of misaligned trajectories, indicate the hexagonal phase is highly ordered.