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Register a new userHigh thermoelectric power factor of poly(3-hexylthiophene) through in-plane alignment and doping with a molybdenum dithiolene complex
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Dorothea Scheunemann
Publication date
2021
fields
Physics
and research's language is
English
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Here we report a record thermoelectric power factor of up to 160 $mu$ W m-1 K-2 for the conjugated polymer poly(3-hexylthiophene) (P3HT). This result is achieved through the combination of high-temperature rubbing of thin films together with the use of a large molybdenum dithiolene p-dopant with a high electron affinity. Comparison of the UV-vis-NIR spectra of the chemically doped samples to electrochemically oxidized material reveals an oxidation level of 10%, i.e. one polaron for every 10 repeat units. The high power factor arises due to an increase in the charge-carrier mobility and hence electrical conductivity along the rubbing direction. We conclude that P3HT, with its facile synthesis and outstanding processability, should not be ruled out as a potential thermoelectric material.
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The spectral breadth of conjugated polymers gives these materials a clear advantage over other molecular compounds for organic photovoltaic applications and is a key factor in recent efficiencies topping 10%. But why do excitonic transitions, which are inherently narrow, lead to absorption over such a broad range of wavelengths in the first place? Using single-molecule spectroscopy, we address this fundamental question in a model material, poly(3-hexylthiophene). Narrow zero-phonon lines from single chromophores are found to scatter over 200nm, an unprecedented inhomogeneous broadening which maps the ensemble. The giant red-shift between solution and bulk films arises from energy transfer to the lowest-energy chromophores in collapsed polymer chains which adopt a highly-ordered morphology. We propose that the extreme energetic disorder of chromophores is structural in origin. This structural disorder on the single-chromophore level may actually enable the high degree of polymer chain ordering found in bulk films: both structural order and disorder are crucial to materials physics in devices.
Control of chain length and morphology in combination with single-molecule spectroscopy techniques provide a comprehensive photophysical picture of excited-state losses in the prototypical conjugated polymer poly(3-hexylthiophene) (P3HT). A universal self-quenching mechanism is revealed, based on singlet-triplet exciton annihilation, which accounts for the dramatic loss in fluorescence quantum yield of a single P3HT chain between its solution (unfolded) and bulk-like (folded) state. Triplet excitons fundamentally limit the fluorescence of organic photovoltaic materials, which impacts on the conversion of singlet excitons to separated charge carriers, decreasing the efficiency of energy harvesting at high excitation densities. Interexcitonic interactions are so effective that a single P3HT chain of >100 kDa weight behaves like a two-level system, exhibiting perfect photon-antibunching.
We show that synthesis-induced Metal -Insulator transition (MIT) for electronic transport along the orthorombic c axis of FeSb$_{2}$ single crystals has greatly enhanced electrical conductivity while keeping the thermopower at a relatively high level. By this means, the thermoelectric power factor is enhanced to a new record high S$^{2}$$sigma$ $sim$ 8000 $mu$WK$^{-2}$cm$^{-1}$ at 28 K. We find that the large thermopower in FeSb$_{2}$ can be rationalized within the correlated electron model with two bands having large quasiparaticle disparity, whereas MIT is induced by subtle structural differences. The results in this work testify that correlated electrons can produce extreme power factor values.
Thermoelectrics are promising by directly generating electricity from waste heat. However, (sub-)room-temperature thermoelectrics have been a long-standing challenge due to vanishing electronic entropy at low temperatures. Topological materials offer a new avenue for energy harvesting applications. Recent theories predicted that topological semimetals at the quantum limit can lead to a large, non-saturating thermopower and a quantized thermoelectric Hall conductivity approaching a universal value. Here, we experimentally demonstrate the non-saturating thermopower and quantized thermoelectric Hall effect in the topological Weyl semimetal (WSM) tantalum phosphide (TaP). An ultrahigh longitudinal thermopower Sxx= 1.1x10^3 muV/K and giant power factor ~525 muW/cm/K^2 are observed at ~40K, which is largely attributed to the quantized thermoelectric Hall effect. Our work highlights the unique quantized thermoelectric Hall effect realized in a WSM toward low-temperature energy harvesting applications.
Blinking of the photoluminescence (PL) emitted from individual conjugated polymer chains is one of the central observations made by single-molecule spectroscopy (SMS). Important information, e.g., regarding excitation energy transfer, can be extracted by evaluating dynamic quenching. However, the nature of trap states, which are responsible for PL quenching, often remains obscured. We present a detailed investigation of the photon statistics of single poly(3-hexylthiophene) (P3HT) chains obtained by SMS. The photon statistics provide a measure of the number and brightness of independently emitting areas on a single chain. These observables can be followed during blinking. A decrease in PL intensity is shown to be correlated with either (i) a decrease in the average brightness of the emitting sites; or (ii) a decrease in the number of emitting regions. We attribute these phenomena to the formation of (i) shallow charge traps, which can weakly affect all emitting areas of a single chain at once; and (ii) deep traps, which have a strong effect on small regions within the single chains.
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