High‐Performance n‐Type Organic Thermoelectrics Enabled by Control Over Microstructure, Orientation and Contact Plane in Naphthalenediimide‐Bithiazole‐Copolymer Films
Abstract
Conjugated polymers are promising thermoelectric materials offering solution processability, flexibility, and versatile synthesis. However, n-type polymers lag behind their p-type counterparts. Herein, we demonstrate that the combination of precise doping with control over crystalline contact plane, orientation, and microstructure helps design efficient n-type films of a naphthalenediimide-bithiazole-based copolymer (PNDIOE7-Tz2). Favorable fibrillar morphology and enhanced planarity lead to tight packing in films doped with N-DMBI, resulting in a high electrical conductivity σ ≈ 10 S cm−1. GIWAXS indicates a predominantly face-on orientation in pristine films with a short π–π stacking distance of 3.47 Å. Incremental concentration doping enhances the σ to 45 S cm−1 with a power factor (PF≈17.5 µW m−1 K−2). Rubbing alignment causes a detrimental shift from face-on to edge-on, reducing σ below 5 S cm−1 and PF below 4 µW m−1 K−2. Subsequent solvent vapor annealing converts aligned crystallites to mixed face-on/edge-on, promoting a strong enhancement of TE performance with a high PF up to 41µW m−1 K−2, among the highest reported for n-type polymers. This work underscores that controlling the contact plane effectively decouples σ and S for high-performance n-type polymer thermoelectrics.
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BibTeX
@article{wang2026highperformance,
title = {{High‐Performance n‐Type Organic Thermoelectrics Enabled by Control Over Microstructure, Orientation and Contact Plane in Naphthalenediimide‐Bithiazole‐Copolymer Films}},
author = {Suhao Wang and Saïd Oummouch and Huan Wei and Karl Thorley and Adam Marks and Arianna Magni and Xiuming Sun and Alessandra Pistillo and Bruno Schmaltz and Olivier Bardagot and Sabine Ludwigs and Alberto Salleo and Yuanyuan Hu and Martin Brinkmann},
journal = {Advanced Functional Materials},
year = {2026},
month = jul,
doi = {10.1002/adfm.77341},
url = {https://hal.science/hal-05727926v2},
note = {CC BY 4.0},
}
RIS
TY - JOUR
TI - High‐Performance n‐Type Organic Thermoelectrics Enabled by Control Over Microstructure, Orientation and Contact Plane in Naphthalenediimide‐Bithiazole‐Copolymer Films
AU - Suhao Wang
AU - Saïd Oummouch
AU - Huan Wei
AU - Karl Thorley
AU - Adam Marks
AU - Arianna Magni
AU - Xiuming Sun
AU - Alessandra Pistillo
AU - Bruno Schmaltz
AU - Olivier Bardagot
AU - Sabine Ludwigs
AU - Alberto Salleo
AU - Yuanyuan Hu
AU - Martin Brinkmann
PY - 2026
DA - 2026/07/29
JO - Advanced Functional Materials
DO - 10.1002/adfm.77341
UR - https://hal.science/hal-05727926v2
AB - Conjugated polymers are promising thermoelectric materials offering solution processability, flexibility, and versatile synthesis. However, n-type polymers lag behind their p-type counterparts. Herein, we demonstrate that the combination of precise doping with control over crystalline contact plane, orientation, and microstructure helps design efficient n-type films of a naphthalenediimide-bithiazole-based copolymer (PNDIOE7-Tz2). Favorable fibrillar morphology and enhanced planarity lead to tight packing in films doped with N-DMBI, resulting in a high electrical conductivity σ ≈ 10 S cm−1. GIWAXS indicates a predominantly face-on orientation in pristine films with a short π–π stacking distance of 3.47 Å. Incremental concentration doping enhances the σ to 45 S cm−1 with a power factor (PF≈17.5 µW m−1 K−2). Rubbing alignment causes a detrimental shift from face-on to edge-on, reducing σ below 5 S cm−1 and PF below 4 µW m−1 K−2. Subsequent solvent vapor annealing converts aligned crystallites to mixed face-on/edge-on, promoting a strong enhancement of TE performance with a high PF up to 41µW m−1 K−2, among the highest reported for n-type polymers. This work underscores that controlling the contact plane effectively decouples σ and S for high-performance n-type polymer thermoelectrics.
SN - 1616-301X
SN - 1616-3028
ER -