Conversion of waste heat to voltage has the potential to significantly reduce the carbon footprint of a number of critical energy sectors, such as the transportation and electricity-generation sectors, and manufacturing processes. Thermal energy is also an abundant low-flux source that can be harnessed to power portable/wearable electronic devices and critical components in remote off-grid locations. As such, a number of different inorganic and organic materials are being explored for their potential in thermoelectric-energy-harvesting devices. Carbon-based thermoelectric materials are particularly attractive due to their use of nontoxic, abundant source-materials, their amenability to high-throughput solution-phase fabrication routes, and the high specific energy (i.e., W g ) enabled by their low mass. Single-walled carbon nanotubes (SWCNTs) represent a unique 1D carbon allotrope with structural, electrical, and thermal properties that enable efficient thermoelectric-energy conversion. Here, the progress made toward understanding the fundamental thermoelectric properties of SWCNTs, nanotube-based composites, and thermoelectric devices prepared from these materials is reviewed in detail. This progress illuminates the tremendous potential that carbon-nanotube-based materials and composites have for producing high-performance next-generation devices for thermoelectric-energy harvesting.

Transparent conducting (TC) films of single-walled carbon nanotubes (SWNTs) have the potential to replace conventional TC oxides in a wide variety of optoelectronic devices. [1][2][3][4][5] TC-SWNT films are particularly attractive for photovoltaics (PV) due to their high transparency over much of the solar spectrum, excellent electrical conductivity, and the potential for inexpensive roll-to-roll processing. SWNT films have been used, by us and others, in cadmium telluride, [6] copper indium gallium diselenide, [7] and organic PV (OPV) devices. [8][9][10] In several reports, SWNTelectrodes for OPV have been prepared by filtering a sodium dodecyl sulfate (SDS)-stabilized dispersion of SWNTs to form a thin film. [9,10] The film can be released by dissolution of the filter, and then transferred to a transparent substrate.[11] This so-called ''transfer method'' produces highly transparent films with excellent conductivity, but the films possess irregular morphologies and significant roughness, which can lead to short-circuits and overall poor reproducibility during device fabrication.[12] Moreover, the process is not scalable. TC-SWNT films have also been produced for optical and electrical studies by air-brush spraying using surfactant-stabilized SWNT inks. Such films are inhomogeneous because SWNTs sprayed from surfactant solutions agglomerate on heated substrates. To move TC-SWNT electrodes beyond the proof-of-concept stage for PV and other optoelectronic applications, methods are required for producing large-area, transparent, conducting SWNT films that are smooth and homogeneous over large areas.Here, we report methods to prepare SWNT films with high transparency, electrical conductivity, and uniformity, with exceptionally low surface roughness, on arbitrarily large (6 inch  6 inch) substrates by ultrasonic spraying. A side-by-side comparison of OPV devices fabricated on SWNT and indiumdoped tin oxide (ITO) electrodes showed very good performance with energy-conversion efficiencies of $3.1 and 3.6%, respectively, under AM 1.5 illumination. Several factors are critical to the success of the approach. First, we prepared aqueous SWNT dispersions using a high-molecular-weight (MW $90 000) polymeric derivative of cellulose (sodium carboxymethyl cellulose (CMC)). CMC has been previously reported as an excellent agent for dispersing SWNTs in water, [13] and transparent films have been drop-cast, [14] but this is the first report of CMC-based dispersions for spraying SWNT films. A second advance is the use of ultrasonic spraying, which, when combined with the CMC-based dispersions, permits precise amounts of SWNTs to be reproducibly and uniformly dispensed over arbitrarily large areas. In fact, by measuring the weight and optical properties of films as a function of the number of deposited layers, the SWNT absorption coefficient could be accurately determined. Finally, we used SWNTs produced by laser vaporization (LV), which have lower defect densities [15,16] than tubes produced by chemical vapor deposition (CVD). Th...

During the past decade, time-resolved microwave conductivity (TRMC) has evolved to an established, powerful technique to study photoactive layers. With this feature paper, we aim to fulfill two goals: (1) give a full description of the photoinduced TRMC technique, including experimental details and data analysis, and discuss to what extent the TRMC technique differs from more conventional DC techniques and (2) illustrate the potential of this technique for probing charge carrier dynamics in photoactive materials. For these reasons recent studies on conjugated polymer:fullerene blends will be presented and discussed. The findings from these studies have advanced the insight into the mechanism of charge carrier generation and decay in polymer:fullerene blends, which allows us to improve the efficiency of organic photovoltaic cells based on this active layer architecture. In short, it is shown how the TRMC technique can be used as a versatile method to screen the potential of new photovoltaic materials.

Using flash photolysis, time-resolved microwave conductivity we report the sub-200 ns photoconductivity transients for neat poly(3-hexylthiophene), P3HT, and four associated blends containing 1%, 5%, 20%, and 50%, by weight, of the soluble fullerene, [6,6]-phenyl-c 61 -butyric acid methyl ester, PCBM. We propose a detailed kinetic scheme that when solved numerically is consistent with all the data recorded as a function of excitation density and that describes the fate of mobile and trapped carriers in the system. In the neat polymer, mobile holes are the only contributor to the photoconductance transients, which decay according to first-order kinetics at all light intensities due to the presence of a large concentration of dark carriers present in the polymer. The signal decays with a characteristic rate constant (∼1 Â 10 7 s À1 ) that describes the re-equilibration of trapped and mobile holes. In all four blends, the microwave absorption contains a significant contribution due to electrons in the PCBM clusters, even at the lowest blend ratio of 1%. The magnitude of the second-order rate coefficient, γ b , for carrier recombination in all four blends (3.25 Â 10 À12 cm 3 s À1 < γ b < 10 Â 10 À12 cm 3 s À1 ), and also that identified for the neat polymer, corresponds to a slow process that is not limited by diffusion but is activation controlled.

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The generation of excitons and their interaction with holes in films of neat regioregular poly(3-hexylthiophene) and the polymer blended with 1 wt% of the electron-acceptor [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) have been studied using flash-photolysis time-resolved microwave conductivity. The sublinear relationship between the photogenerated hole density and the incident light intensity, in both the neat polymer and the donor−acceptor blend, can be attributed to the quenching of excitons by holes, at a rate characterized by a second-order rate constant (γ2) of 3 × 10−8 cm3/s. This value is larger than that found for other, luminescent conjugated polymers; the difference may be attributed to a greater collision probability, due to the higher mobility of the interacting species, or to an enhancement of the quenching rate once they are in close proximity. The phenomenon has consequences for the ultimate efficiency of organic photovoltaic solar cells that are based on the simple polymer:PCBM bulk heterojunction, especially under conditions of solar concentration.

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Polymer-free semiconducting carbon nanotube networks demonstrate unprecedented equivalent n- and p-type thermoelectric performance.