Entropically stabilized local dipole formation in lead chalcogenides

Emil S. Božin, Christos D. Malliakas, Petros Souvatzis, Thomas Proffen, Nicola A. Spaldin, Mercouri G Kanatzidis, Simon J L Billinge

Research output: Contribution to journalArticle

182 Citations (Scopus)

Abstract

We report the observation of local structural dipoles that emerge from an undistorted ground state on warming, in contrast to conventional structural phase transitions in which distortions emerge on cooling. Using experimental and theoretical probes of the local structure, we demonstrate this behavior in binary lead chalcogenides, which were believed to adopt the ideal, undistorted rock-salt structure at all temperatures. The behavior is consistent with a simple thermodynamic model in which the emerging dipoles are stabilized in the disordered state at high temperature due to the extra configurational entropy despite the fact that the undistorted structure has lower internal energy. Our findings shed light on the anomalous electronic and thermoelectric properties of the lead chalcogenides. Similar searches may show that the phenomenon is more widespread.

Original languageEnglish
Pages (from-to)1660-1663
Number of pages4
JournalScience
Volume330
Issue number6011
DOIs
Publication statusPublished - Dec 17 2010

Fingerprint

Temperature
Phase Transition
Entropy
Thermodynamics
Salts
Observation
Lead

ASJC Scopus subject areas

  • General

Cite this

Božin, E. S., Malliakas, C. D., Souvatzis, P., Proffen, T., Spaldin, N. A., Kanatzidis, M. G., & Billinge, S. J. L. (2010). Entropically stabilized local dipole formation in lead chalcogenides. Science, 330(6011), 1660-1663. https://doi.org/10.1126/science.1192759

Entropically stabilized local dipole formation in lead chalcogenides. / Božin, Emil S.; Malliakas, Christos D.; Souvatzis, Petros; Proffen, Thomas; Spaldin, Nicola A.; Kanatzidis, Mercouri G; Billinge, Simon J L.

In: Science, Vol. 330, No. 6011, 17.12.2010, p. 1660-1663.

Research output: Contribution to journalArticle

Božin, ES, Malliakas, CD, Souvatzis, P, Proffen, T, Spaldin, NA, Kanatzidis, MG & Billinge, SJL 2010, 'Entropically stabilized local dipole formation in lead chalcogenides', Science, vol. 330, no. 6011, pp. 1660-1663. https://doi.org/10.1126/science.1192759
Božin ES, Malliakas CD, Souvatzis P, Proffen T, Spaldin NA, Kanatzidis MG et al. Entropically stabilized local dipole formation in lead chalcogenides. Science. 2010 Dec 17;330(6011):1660-1663. https://doi.org/10.1126/science.1192759
Božin, Emil S. ; Malliakas, Christos D. ; Souvatzis, Petros ; Proffen, Thomas ; Spaldin, Nicola A. ; Kanatzidis, Mercouri G ; Billinge, Simon J L. / Entropically stabilized local dipole formation in lead chalcogenides. In: Science. 2010 ; Vol. 330, No. 6011. pp. 1660-1663.
@article{258012ad3db04479a68c4a924ed7db43,
title = "Entropically stabilized local dipole formation in lead chalcogenides",
abstract = "We report the observation of local structural dipoles that emerge from an undistorted ground state on warming, in contrast to conventional structural phase transitions in which distortions emerge on cooling. Using experimental and theoretical probes of the local structure, we demonstrate this behavior in binary lead chalcogenides, which were believed to adopt the ideal, undistorted rock-salt structure at all temperatures. The behavior is consistent with a simple thermodynamic model in which the emerging dipoles are stabilized in the disordered state at high temperature due to the extra configurational entropy despite the fact that the undistorted structure has lower internal energy. Our findings shed light on the anomalous electronic and thermoelectric properties of the lead chalcogenides. Similar searches may show that the phenomenon is more widespread.",
author = "Božin, {Emil S.} and Malliakas, {Christos D.} and Petros Souvatzis and Thomas Proffen and Spaldin, {Nicola A.} and Kanatzidis, {Mercouri G} and Billinge, {Simon J L}",
year = "2010",
month = "12",
day = "17",
doi = "10.1126/science.1192759",
language = "English",
volume = "330",
pages = "1660--1663",
journal = "Science",
issn = "0036-8075",
publisher = "American Association for the Advancement of Science",
number = "6011",

}

TY - JOUR

T1 - Entropically stabilized local dipole formation in lead chalcogenides

AU - Božin, Emil S.

AU - Malliakas, Christos D.

AU - Souvatzis, Petros

AU - Proffen, Thomas

AU - Spaldin, Nicola A.

AU - Kanatzidis, Mercouri G

AU - Billinge, Simon J L

PY - 2010/12/17

Y1 - 2010/12/17

N2 - We report the observation of local structural dipoles that emerge from an undistorted ground state on warming, in contrast to conventional structural phase transitions in which distortions emerge on cooling. Using experimental and theoretical probes of the local structure, we demonstrate this behavior in binary lead chalcogenides, which were believed to adopt the ideal, undistorted rock-salt structure at all temperatures. The behavior is consistent with a simple thermodynamic model in which the emerging dipoles are stabilized in the disordered state at high temperature due to the extra configurational entropy despite the fact that the undistorted structure has lower internal energy. Our findings shed light on the anomalous electronic and thermoelectric properties of the lead chalcogenides. Similar searches may show that the phenomenon is more widespread.

AB - We report the observation of local structural dipoles that emerge from an undistorted ground state on warming, in contrast to conventional structural phase transitions in which distortions emerge on cooling. Using experimental and theoretical probes of the local structure, we demonstrate this behavior in binary lead chalcogenides, which were believed to adopt the ideal, undistorted rock-salt structure at all temperatures. The behavior is consistent with a simple thermodynamic model in which the emerging dipoles are stabilized in the disordered state at high temperature due to the extra configurational entropy despite the fact that the undistorted structure has lower internal energy. Our findings shed light on the anomalous electronic and thermoelectric properties of the lead chalcogenides. Similar searches may show that the phenomenon is more widespread.

UR - http://www.scopus.com/inward/record.url?scp=78650351443&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=78650351443&partnerID=8YFLogxK

U2 - 10.1126/science.1192759

DO - 10.1126/science.1192759

M3 - Article

C2 - 21164012

AN - SCOPUS:78650351443

VL - 330

SP - 1660

EP - 1663

JO - Science

JF - Science

SN - 0036-8075

IS - 6011

ER -