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Negative thermal expansion in ZrW2O8 was investigated using a flexibilityanalysis of ab-initio phonons. It was shown that no previously proposedmechanism adequately describes the atomic-scale origin of negative thermalexpansion in this material. Instead it was found that NTE in ZrW2O8 is driven,not by a single mechanism, but by wide bands of phonons that resemblevibrations of near-rigid WO4 units and Zr-O bonds at low frequency, withdeformation of O-W-O and O-Zr-O bond angles steadily increasing with increasingNTE phonon frequency. It is asserted that this phenomenon is likely to providea more accurate explanation for NTE in many complex systems not yet studied.

The negative thermal expansion mechanism of zirconium tungstate, ZrW2O8