Photothermoelectric (PTE) materials are promising candidates for solar energy harvesting and photodetection applications, especially for near-infrared (NIR) wavelengths. Although the processability and tunability of organic materials are highly advantageous, examples of organic PTE materials are comparatively rare and their PTE performance is typically limited by poor photothermal (PT) conversion. Here, we report the use of redox-active Sn complexes of tetrathiafulvalene-tetrathiolate (TTFtt) as transmetalating agents for the synthesis of presynthetically redox tuned NiTTFtt materials. Unlike the neutral material NiTTFtt, which exhibits n-type glassy-metallic conductivity, the reduced materials Li1.2Ni0.4[NiTTFtt] and [Li(THF)1.5]1.2Ni0.4[NiTTFtt] (THF = tetrahydrofuran) display physical characteristics more consistent with p-type semiconductors. The broad spectral absorption and electrically conducting nature of these TTFtt-based materials enable highly efficient NIR-thermal conversion and good PTE performance. Furthermore, in contrast to conventional PTE composites, these NiTTFtt coordination polymers are notable as single-component PTE materials. As a result, the presynthetically tuned metal-to-insulator transition in these NiTTFtt systems directly modulates their PT and PTE properties.
Xie, Jiaze, et al. "Presynthetic Redox Gated Metal-to-Insulator Transition and Photothermoelectric Properties in Nickel Tetrathiafulvalene-Tetrathiolate Coordination Polymers." Journal of the American Chemical Society, vol. 144, no. 41, Oct. 2022. https://doi.org/10.1021/jacs.2c07864
Xie, Jiaze, Pan, Jia-Ahn, Cheng, Baorui, Ma, Tengzhou, Filatov, Alexander S., Patel, Shrayesh N., Park, Jiwoong, Talapin, Dmitri V., & Anderson, John S. (2022). Presynthetic Redox Gated Metal-to-Insulator Transition and Photothermoelectric Properties in Nickel Tetrathiafulvalene-Tetrathiolate Coordination Polymers. Journal of the American Chemical Society, 144(41). https://doi.org/10.1021/jacs.2c07864
Xie, Jiaze, Pan, Jia-Ahn, Cheng, Baorui, et al., "Presynthetic Redox Gated Metal-to-Insulator Transition and Photothermoelectric Properties in Nickel Tetrathiafulvalene-Tetrathiolate Coordination Polymers," Journal of the American Chemical Society 144, no. 41 (2022), https://doi.org/10.1021/jacs.2c07864
@article{osti_1976083,
author = {Xie, Jiaze and Pan, Jia-Ahn and Cheng, Baorui and Ma, Tengzhou and Filatov, Alexander S. and Patel, Shrayesh N. and Park, Jiwoong and Talapin, Dmitri V. and Anderson, John S.},
title = {Presynthetic Redox Gated Metal-to-Insulator Transition and Photothermoelectric Properties in Nickel Tetrathiafulvalene-Tetrathiolate Coordination Polymers},
annote = {Photothermoelectric (PTE) materials are promising candidates for solar energy harvesting and photodetection applications, especially for near-infrared (NIR) wavelengths. Although the processability and tunability of organic materials are highly advantageous, examples of organic PTE materials are comparatively rare and their PTE performance is typically limited by poor photothermal (PT) conversion. Here, we report the use of redox-active Sn complexes of tetrathiafulvalene-tetrathiolate (TTFtt) as transmetalating agents for the synthesis of presynthetically redox tuned NiTTFtt materials. Unlike the neutral material NiTTFtt, which exhibits n-type glassy-metallic conductivity, the reduced materials Li1.2Ni0.4[NiTTFtt] and [Li(THF)1.5]1.2Ni0.4[NiTTFtt] (THF = tetrahydrofuran) display physical characteristics more consistent with p-type semiconductors. The broad spectral absorption and electrically conducting nature of these TTFtt-based materials enable highly efficient NIR-thermal conversion and good PTE performance. Furthermore, in contrast to conventional PTE composites, these NiTTFtt coordination polymers are notable as single-component PTE materials. As a result, the presynthetically tuned metal-to-insulator transition in these NiTTFtt systems directly modulates their PT and PTE properties.},
doi = {10.1021/jacs.2c07864},
url = {https://www.osti.gov/biblio/1976083},
journal = {Journal of the American Chemical Society},
issn = {ISSN 0002-7863},
number = {41},
volume = {144},
place = {United States},
publisher = {American Chemical Society (ACS)},
year = {2022},
month = {10}}
Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 372, Issue 2013https://doi.org/10.1098/rsta.2013.0008