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Combining Solid-state and Solution-based Techniques: Synthesis and Reactivity of Chalcogenidoplumbates(II or IV)
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Entropically stabilized local dipole formation in lead chalcogenides.

Emil S Božin1, Christos D Malliakas, Petros Souvatzis

  • 1Condensed Matter Physics and Materials Science Department, Brookhaven National Laboratory, Upton, NY 11973, USA.

Science (New York, N.Y.)
|December 18, 2010
PubMed
Summary
This summary is machine-generated.

Local structural dipoles emerge upon warming in lead chalcogenides, defying conventional phase transitions. This discovery, driven by configurational entropy, explains their unusual electronic and thermoelectric properties.

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Area of Science:

  • Materials Science
  • Solid-State Physics
  • Crystallography

Background:

  • Conventional structural phase transitions involve distortions emerging upon cooling.
  • Binary lead chalcogenides were presumed to possess an undistorted rock-salt structure across all temperatures.
  • Understanding local structure is crucial for materials with anomalous properties.

Purpose of the Study:

  • To report the novel observation of local structural dipoles emerging upon warming in binary lead chalcogenides.
  • To investigate the thermodynamic driving forces behind this unusual phase behavior.
  • To elucidate the connection between local structure and the anomalous electronic/thermoelectric properties of these materials.

Main Methods:

  • Experimental probes of local structure.
  • Theoretical modeling and simulations.
  • Analysis of thermodynamic models incorporating configurational entropy.

Main Results:

  • Observation of local structural dipoles appearing from an undistorted ground state on warming.
  • Demonstration of this phenomenon in binary lead chalcogenides.
  • Validation of a thermodynamic model where configurational entropy stabilizes dipoles at high temperatures.

Conclusions:

  • The emergence of local structural dipoles on warming is a novel phenomenon, distinct from conventional phase transitions.
  • Configurational entropy plays a key role in stabilizing these dipoles at higher temperatures.
  • These findings provide insight into the anomalous electronic and thermoelectric behavior of lead chalcogenides and suggest the phenomenon may be widespread.