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Title: Polymer morphology and interfacial charge transfer dominate over energy-dependent scattering in organic-inorganic thermoelectrics

Abstract

Hybrid (organic-inorganic) materials have emerged as a promising class of thermoelectric materials, achieving power factors (S 2σ) exceeding those of either constituent. The mechanism of this enhancement is still under debate, and pinpointing the underlying physics has proven difficult. In this work, we combine transport measurements with theoretical simulations and first principles calculations on a prototypical PEDOT:PSS-Te(Cu x) nanowire hybrid material system to understand the effect of templating and charge redistribution on the thermoelectric performance. Further, we apply the recently developed Kang-Snyder charge transport model to show that scattering of holes in the hybrid system, defined by the energy-dependent scattering parameter, remains the same as in the host polymer matrix; performance is instead dictated by polymer morphology manifested in an energy-independent transport coefficient. We build upon this language to explain thermoelectric behavior in a variety of PEDOT and P3HT based hybrids acting as a guide for future work in multiphase materials.

Authors:
 [1];  [2];  [3];  [1];  [3];  [4];  [1]
  1. Institute of Materials Research and Engineering (Singapore)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  3. Institute of High Performance Computing (Singapore)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1493278
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Kumar, Pawan, Zaia, Edmond W., Yildirim, Erol, Repaka, D. V. Maheswar, Yang, Shuo-Wang, Urban, Jeffrey J., and Hippalgaonkar, Kedar. Polymer morphology and interfacial charge transfer dominate over energy-dependent scattering in organic-inorganic thermoelectrics. United States: N. p., 2018. Web. doi:10.1038/s41467-018-07435-z.
Kumar, Pawan, Zaia, Edmond W., Yildirim, Erol, Repaka, D. V. Maheswar, Yang, Shuo-Wang, Urban, Jeffrey J., & Hippalgaonkar, Kedar. Polymer morphology and interfacial charge transfer dominate over energy-dependent scattering in organic-inorganic thermoelectrics. United States. doi:10.1038/s41467-018-07435-z.
Kumar, Pawan, Zaia, Edmond W., Yildirim, Erol, Repaka, D. V. Maheswar, Yang, Shuo-Wang, Urban, Jeffrey J., and Hippalgaonkar, Kedar. Mon . "Polymer morphology and interfacial charge transfer dominate over energy-dependent scattering in organic-inorganic thermoelectrics". United States. doi:10.1038/s41467-018-07435-z. https://www.osti.gov/servlets/purl/1493278.
@article{osti_1493278,
title = {Polymer morphology and interfacial charge transfer dominate over energy-dependent scattering in organic-inorganic thermoelectrics},
author = {Kumar, Pawan and Zaia, Edmond W. and Yildirim, Erol and Repaka, D. V. Maheswar and Yang, Shuo-Wang and Urban, Jeffrey J. and Hippalgaonkar, Kedar},
abstractNote = {Hybrid (organic-inorganic) materials have emerged as a promising class of thermoelectric materials, achieving power factors (S2σ) exceeding those of either constituent. The mechanism of this enhancement is still under debate, and pinpointing the underlying physics has proven difficult. In this work, we combine transport measurements with theoretical simulations and first principles calculations on a prototypical PEDOT:PSS-Te(Cux) nanowire hybrid material system to understand the effect of templating and charge redistribution on the thermoelectric performance. Further, we apply the recently developed Kang-Snyder charge transport model to show that scattering of holes in the hybrid system, defined by the energy-dependent scattering parameter, remains the same as in the host polymer matrix; performance is instead dictated by polymer morphology manifested in an energy-independent transport coefficient. We build upon this language to explain thermoelectric behavior in a variety of PEDOT and P3HT based hybrids acting as a guide for future work in multiphase materials.},
doi = {10.1038/s41467-018-07435-z},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {12}
}

Journal Article:
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Cited by: 6 works
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Figures / Tables:

Fig. 1 Fig. 1: Morphology of hybrids and alignment of PEDOT:PSS at the inorganic interface (a, b) False-color scanning electron microscope (SEM) images of (a) PEDOT:PSS-Te and (b) PEDOT:PSS-Cu1.75Te films illustrate the overall morphology of the hybrid films – inorganic nanowires in a PEDOT:PSS matrix. The green color shows the surface nanowiresmore » and blue illustrates the 3D plane underneath, where the PEDOT:PSS polymer matrix is transparent (and hence invisible) in the SEM. (c, d) Representative high-resolution transmission electron microscopy (HR-TEM) images of (c) straight Te domains and (d) kinked Cu1.75Te alloy domains confirm the identity and crystallinity of these two phases. The insets show selected area electron diffraction (SAED) patterns consistent with the identified crystal structures. (e, f) MD simulations elucidate the polymer morphology and alignment at the organic-inorganic interface. Here, the final polymer structures are depicted after simulated annealing of five chains of EDOT18 and SS36 on (e) Te and (f) Cu1.75Te surfaces, both accompanied by respective atomic concentration profiles. The polymer concentration profiles are tracked using the atomic concentration of S in either PEDOT or PSS. There is a high concentration of S atoms in PEDOT observed at 3–5 Å from the nanowire surfaces, suggestive of highly ordered and aligned PEDOT chains at the organic-inorganic interface. Similar structures and concentration profiles were observed for both Te nanowires (NW) and Cu1.75Te heteronanowires (Supplementary Figures 1-2, Supplementary Movies 1–5), however, though alignment occurs, self-assembly of chains is reduced on the kinked Cu1.75Te surface, unlike on the Te surface (Supplementary Figure 3, Supplementary Movies 6-7)« less

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