Si-based inorganic electronics have long dominated the semiconductor industry. However, in recent years conjugated polymers have attracted increasing attention because such systems are flexible and offer the potential for low-cost, large-area production via roll-to-roll processing. The state-of-the-art organic conjugated molecular crystals can exhibit charge carrier mobilities (μ) that nearly match or even exceed that of amorphous silicon (1-10 cm(2) V(-1) s(-1)). The mean free path of the charge carriers estimated from these mobilities corresponds to the typical intersite (intermolecular) hopping distances in conjugated organic materials, which strongly suggests that the conduction model for the electronic band structure only applies to μ > 1 cm(2) V(-1) s(-1) for the translational motion of the charge carriers. However, to analyze the transport mechanism in organic electronics, researchers conventionally use a disorder formalism, where μ is usually less than 1 cm(2) V(-1) s(-1) and dominated by impurities, disorders, or defects that disturb the long-range translational motion. In this Account, we discuss the relationship between the alternating-current and direct-current mobilities of charge carriers, using time-resolved microwave conductivity (TRMC) and other techniques including field-effect transistor, time-of-flight, and space-charge limited current. TRMC measures the nanometer-scale mobility of charge carriers under an oscillating microwave electric field with no contact between the semiconductors and the metals. This separation allows us to evaluate the intrinsic charge carrier mobility with minimal trapping effects. We review a wide variety of organic electronics in terms of their charge carrier mobilities, and we describe recent studies of macromolecules, molecular crystals, and supramolecular architecture. For example, a rigid poly(phenylene-co-ethynylene) included in permethylated cyclodextrin shows a high intramolecular hole mobility of 0.5 cm(2) V(-1) s(-1), based on a combination of flash-photolysis TRMC and transient absorption spectroscopy (TAS) measurements. Single-crystal rubrene showed an ambipolarity with anisotropic charge carrier transport along each crystal axis on the nanometer scale. Finally, we describe the charge carrier mobility of a self-assembled nanotube consisting of a large π-plane of hexabenzocoronene (HBC) partially appended with an electron acceptor. The local (intratubular) charge carrier mobility reached 3 cm(2) V(-1) s(-1) for the nanotubes that possessed well-ordered π-stacking, but it dropped to 0.7 cm(2) V(-1) s(-1) in regions that contained greater amounts of the electron acceptor because those molecules reduced the structural integrity of π-stacked HBC arrays. Interestingly, the long-range (intertubular) charge carrier mobility was on the order of 10(-4) cm(2) V(-1) s(-1) and monotonically decreased when the acceptor content was increased. These results suggest the importance of investigating charge carrier mobilities by frequency-dependent charge carrier motion for...
State-of-the-art low band gap conjugated polymers have been investigated for application in organic photovoltaic cells (OPVs) to achieve efficient conversion of the wide spectrum of sunlight into electricity. A remarkable improvement in power conversion efficiency (PCE) has been achieved through the use of innovative materials and device structures. However, a reliable technique for the rapid screening of the materials and processes is a prerequisite toward faster development in this area. Here we report the realization of such a versatile evaluation technique for bulk heterojunction OPVs by the combination of time-resolved microwave conductivity (TRMC) and submicrosecond white light pulse from a Xe-flash lamp. Xe-flash TRMC allows examination of the OPV active layer without requiring fabrication of the actual device. The transient photoconductivity maxima, involving information on generation efficiency, mobility, and lifetime of charge carriers in four well-known low band gap polymers blended with phenyl-C(61)-butyric acid methyl ester (PCBM), were confirmed to universally correlate with the PCE divided by the open circuit voltage (PCE/V(oc)), offering a facile way to predict photovoltaic performance without device fabrication.
We synthesized a series of new low-band gap donor-acceptor copolymers containing 4,4 0 -bis(alkyl)-[6,6 0 -bithieno[3,2-b]pyrrolylidene]-5,5 0 (4H,4 0 H)-dione. This acceptor unit, so-called dithienoketopyrrole (DTKP), is an analogue of isoindigo, the phenyl rings of which are replaced by thiophenes. Donor moieties such as benzodithiophene, cyclopentadithiophene, fluorene, and dithienothiophene are polymerized with DTKP in an alternating fashion by Stille or Suzuki-Miyaura coupling methods. Exceedingly low-band gaps (E g ¼ 1.0-1.6 eV) were achieved in these copolymers through internal charge transfer interactions between the donor and acceptor moieties. The structural, photophysical, and electrochemical properties of the resultant copolymers were characterized, and field-effect transistor (FET) mobilities were measured. The copolymers showed electronic absorption spectra extending to the near infrared region (600-1400 nm) with absorption maxima at 745-971 nm, along with a low-lying LUMO of À3.8 eV. Density functional theory (DFT) calculation indicated high planarity for the copolymer backbone when compared to that of its phenyl-isoindigo counterparts. FET hole mobilities on the order of 10 À4 to 10 À3 cm 2 V À1 s À1 were obtained, demonstrating a feasibility to use them in organic photovoltaic cells.
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