The importance of phase equilibrium for doping efficiency: iodine doped PbTe

Male, James; Agne, Matthias T.; Goyal, Anuj; Anand, Shashwat; Witting, Ian T.; Stevanovic, Vladan; Snyder, G. Jeffrey

doi:10.1039/C9MH00294D

Title: The importance of phase equilibrium for doping efficiency: iodine doped PbTe

Journal Article · Wed Apr 03 00:00:00 EDT 2019 · Materials Horizons

DOI:https://doi.org/10.1039/C9MH00294D· OSTI ID:1559781

Male, James ^[1]; Agne, Matthias T. ^[1];

^[2]; Anand, Shashwat ^[1]; Witting, Ian T. ^[1]; Stevanovic, Vladan ^[3]; Snyder, G. Jeffrey ^[1]

Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
National Renewable Energy Laboratory (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States)
National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Semiconductor engineering relies heavily on doping efficiency and dopability. Low doping efficiency may cause low mobility and failure to reach target carrier concentrations or even the desired carrier type. Semiconducting thermoelectric materials perform best with degenerate carrier concentrations, meaning high performance in new materials might not be realized experimentally without a route to optimal doping. Doping in the classic PbTe thermoelectric system has been largely successful but reported doping efficiencies can vary, raising concerns about reproducibility. Here, we stress the importance of phase equilibria considerations during synthesis to avoid undesired intrinsic defects leading to sub-optimal doping. By saturation annealing at 973 K, we decidedly fix the composition in single crystal iodine-doped PbTe samples to be Pb-rich or Te-rich without introducing impurity phases. We show that, regardless of iodine concentration, degenerate n-type carrier concentrations with ideal doping efficiency require Pb-rich compositions. Electrons in Te-rich samples are heavily compensated by charged intrinsic Pb vacancy defects. From Hall effect measurements and a simple defect model supported by modern defect calculations, we map out the 973 K ternary Pb–Te–I phase diagram to explicitly link carrier concentration and composition. Furthermore, we discuss unintentional composition changes due to loss of volatile Te during synthesis and measurements. The methods and concepts applied here may guide doping studies on other lead chalcogenide systems as well as any doped, complex semiconductor.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1559781

Report Number(s):: NREL/JA-5K00-74711; MHAOAL

Journal Information:: Materials Horizons, Vol. 6, Issue 7; ISSN 2051-6347

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 36 works

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Title: The importance of phase equilibrium for doping efficiency: iodine doped PbTe

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