TY - JOUR
T1 - Inverse Design of Ultralow Lattice Thermal Conductivity Materials via Materials Database Screening of Lone Pair Cation Coordination Environment
AU - Isaacs, Eric B.
AU - Lu, Grace M.
AU - Wolverton, Christopher
N1 - Funding Information:
We acknowledge support from the U.S. Department of Energy under Contract DE-SC0014520 (lattice dynamical calculations) and Toyota Research Institute through the Accelerated Materials Design and Discovery program (materials design). Computational resources were provided by the National Energy Research Scientific Computing Center (U.S. Department of Energy Contract DE-AC02-05CH11231), the Extreme Science and Engineering Discovery Environment (National Science Foundation Contract ACI-1548562), and the Quest high performance computing facility at Northwestern University.
Publisher Copyright:
© 2020 American Chemical Society.
PY - 2020/7/16
Y1 - 2020/7/16
N2 - The presence of lone pair (LP) electrons is strongly associated with the disruption of lattice heat transport, which is a critical component of strategies to achieve efficient thermoelectric energy conversion. By exploiting an empirical relationship between lattice thermal conductivity, κL, and the bond angles of pnictogen group LP cation coordination environments, we develop an inverse design strategy based on a materials database screening to identify chalcogenide materials with ultralow κL for thermoelectrics. Screening the ∼635000 real and hypothetical inorganic crystals of the Open Quantum Materials Database based on the constituent elements, nominal electron counting, LP cation coordination environment, and synthesizability, we identify 189 compounds expected to exhibit ultralow κL. As a validation, we explicitly compute the lattice dynamical properties of two of the compounds (Cu2AgBiPbS4 and MnTl2As2S5) using first-principles calculations and successfully find both achieve ultralow κL values at room temperature of ∼0.3-0.4 W/(m·K) corresponding to the amorphous limit. Our data-driven approach provides promising candidates for thermoelectric materials and opens new avenues for the design of phononic properties of materials.
AB - The presence of lone pair (LP) electrons is strongly associated with the disruption of lattice heat transport, which is a critical component of strategies to achieve efficient thermoelectric energy conversion. By exploiting an empirical relationship between lattice thermal conductivity, κL, and the bond angles of pnictogen group LP cation coordination environments, we develop an inverse design strategy based on a materials database screening to identify chalcogenide materials with ultralow κL for thermoelectrics. Screening the ∼635000 real and hypothetical inorganic crystals of the Open Quantum Materials Database based on the constituent elements, nominal electron counting, LP cation coordination environment, and synthesizability, we identify 189 compounds expected to exhibit ultralow κL. As a validation, we explicitly compute the lattice dynamical properties of two of the compounds (Cu2AgBiPbS4 and MnTl2As2S5) using first-principles calculations and successfully find both achieve ultralow κL values at room temperature of ∼0.3-0.4 W/(m·K) corresponding to the amorphous limit. Our data-driven approach provides promising candidates for thermoelectric materials and opens new avenues for the design of phononic properties of materials.
UR - http://www.scopus.com/inward/record.url?scp=85088255937&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85088255937&partnerID=8YFLogxK
U2 - 10.1021/acs.jpclett.0c01077
DO - 10.1021/acs.jpclett.0c01077
M3 - Article
C2 - 32574059
AN - SCOPUS:85088255937
VL - 11
SP - 5577
EP - 5583
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
SN - 1948-7185
IS - 14
ER -