@article{2a8067f1c04e4d86a426fd4ca73f894a,
title = "Strong Valence Band Convergence to Enhance Thermoelectric Performance in PbSe with Two Chemically Independent Controls",
abstract = "We present an effective approach to favorably modify the electronic structure of PbSe using Ag doping coupled with SrSe or BaSe alloying. The Ag 4d states make a contribution to in the top of the heavy hole valence band and raise its energy. The Sr and Ba atoms diminish the contribution of Pb 6s2 states and decrease the energy of the light hole valence band. This electronic structure modification increases the density-of-states effective mass, and strongly enhances the thermoelectric performance. Moreover, the Ag-rich nanoscale precipitates, discordant Ag atoms, and Pb/Sr, Pb/Ba point defects in the PbSe matrix work together to reduce the lattice thermal conductivity, resulting a record high average ZTavg of around 0.86 over 400–923 K.",
keywords = "band convergence, lead chalcogenides, nanostructuring, silver doping, thermoelectricity",
author = "Luo, {Zhong Zhen} and Songting Cai and Shiqiang Hao and Bailey, {Trevor P.} and Ioannis Spanopoulos and Yubo Luo and Jianwei Xu and Ctirad Uher and Christopher Wolverton and Dravid, {Vinayak P.} and Qingyu Yan and Kanatzidis, {Mercouri G.}",
note = "Funding Information: This work was supported mainly by the Department of Energy, Office of Science Basic Energy Sciences under grant DE‐SC0014520, DOE Office of Science (sample preparation, synthesis, XRD, TE measurements, TEM measurements, DFT calculations). ZZL and QY gratefully acknowledge the National Natural Science Foundation of China (61728401). This work also made use of the EPIC facility of Northwestern University's NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS‐1542205); the MRSEC program (NSF DMR‐1720139) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; the State of Illinois, through the IIN; the Office of Science of the U.S. Department of Energy under Contract No. DE‐AC02‐06CH11357 and DE‐AC02‐05CH11231. Access to facilities of high performance computational resources at the Northwestern University is acknowledged. The authors also acknowledge Singapore MOE AcRF Tier 2 under Grant Nos. 2018‐T2‐1‐010, Singapore A*STAR Pharos Program SERC 1527200021 and 1527200022, Singapore A*STAR project A19D9a0096, the support from FACTs of Nanyang Technological University for sample analysis. Funding Information: This work was supported mainly by the Department of Energy, Office of Science Basic Energy Sciences under grant DE-SC0014520, DOE Office of Science (sample preparation, synthesis, XRD, TE measurements, TEM measurements, DFT calculations). ZZL and QY gratefully acknowledge the National Natural Science Foundation of China (61728401). This work also made use of the EPIC facility of Northwestern University's NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205); the MRSEC program (NSF DMR-1720139) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; the State of Illinois, through the IIN; the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-06CH11357 and DE-AC02-05CH11231. Access to facilities of high performance computational resources at the Northwestern University is acknowledged. The authors also acknowledge Singapore MOE AcRF Tier 2 under Grant Nos. 2018-T2-1-010, Singapore A*STAR Pharos Program SERC 1527200021 and 1527200022, Singapore A*STAR project A19D9a0096, the support from FACTs of Nanyang Technological University for sample analysis.",
year = "2021",
month = jan,
day = "4",
doi = "10.1002/anie.202011765",
language = "English (US)",
volume = "60",
pages = "268--273",
journal = "Angewandte Chemie - International Edition",
issn = "1433-7851",
publisher = "John Wiley and Sons Ltd",
number = "1",
}