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Negative-pressure polymorphs made by heterostructural alloying.

ABSTRACT: The ability of a material to adopt multiple structures, known as polymorphism, is a fascinating natural phenomenon. Various polymorphs with unusual properties are routinely synthesized by compression under positive pressure. However, changing a material's structure by applying tension under negative pressure is much more difficult. We show how negative-pressure polymorphs can be synthesized by mixing materials with different crystal structures-a general approach that should be applicable to many materials. Theoretical calculations suggest that it costs less energy to mix low-density structures than high-density structures, due to less competition for space between the atoms. Proof-of-concept experiments confirm that mixing two different high-density forms of MnSe and MnTe stabilizes a Mn(Se,Te) alloy with a low-density wurtzite structure. This Mn(Se,Te) negative-pressure polymorph has 2× to 4× lower electron effective mass compared to MnSe and MnTe parent compounds and has a piezoelectric response that none of the parent compounds have. This example shows how heterostructural alloying can lead to negative-pressure polymorphs with useful properties-materials that are otherwise nearly impossible to make.

SUBMITTER: Siol S

PROVIDER: S-EPMC5930396 | biostudies-literature | 2018 Apr

REPOSITORIES: biostudies-literature

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Negative-pressure polymorphs made by heterostructural alloying.

Siol Sebastian S Holder Aaron A Steffes James J Schelhas Laura T LT Stone Kevin H KH Garten Lauren L Perkins John D JD Parilla Philip A PA Toney Michael F MF Huey Bryan D BD Tumas William W Lany Stephan S Zakutayev Andriy A

Science advances 20180420 4

The ability of a material to adopt multiple structures, known as polymorphism, is a fascinating natural phenomenon. Various polymorphs with unusual properties are routinely synthesized by compression under positive pressure. However, changing a material's structure by applying tension under negative pressure is much more difficult. We show how negative-pressure polymorphs can be synthesized by mixing materials with different crystal structures-a general approach that should be applicable to many ...[more]

PMID: 29725620

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Project description:Pressure sensitive adhesives made with blends of thermoplastic polyurethanes (TPUs PSAs) with satisfactory tack, cohesion, and adhesion have been developed. A simple procedure consisting of the physical blending of methyl ethyl ketone (MEK) solutions of two thermoplastic polyurethanes (TPUs) with very different properties-TPU1 and TPU2-was used, and two different blending procedures have been employed. The TPUs were characterized by infra-red spectroscopy in attenuated total reflectance mode (ATR-IR spectroscopy), differential scanning calorimetry, thermal gravimetric analysis, and plate-plate rheology (temperature and frequency sweeps). The TPUs PSAs were characterized by tack measurement, creep test, and the 180° peel test at 25 °C. The procedure for preparing the blends of the TPUs determined differently their viscoelastic properties, and the properties of the TPUs PSAs as well, the blending of separate MEK solutions of the two TPUs imparted higher tack and 180° peel strength than the blending of the two TPUs in MEK. TPU1 + TPU2 blends showed somewhat similar contributions of the free and hydrogen-bonded urethane groups and they had an almost similar degree of phase separation, irrespective of the composition of the blend. Two main thermal decompositions at 308-317 °C due to the urethane hard domains and another at 363-373 °C due to the soft domains could be distinguished in the TPU1 + TPU2 blends, the weight loss of the hard domains increased and the one of the soft domains decreased by increasing the amount of TPU2 in the blends. The storage moduli of the TPU1 + TPU2 blends were similar for temperatures lower than 20 °C and the moduli at the cross over of the moduli were lower than in the parent TPUs. The improved properties of the TPU1 + TPU2 blends derived from the creation of a higher number of hydrogen bonds upon removal of the MEK solvent, which lead to a lower degree of phase separation between the soft and the hard domains than in the parent TPUs. As a consequence, the properties of the TPU1 + TPU2 PSAs were improved because good tack, high 180° peel strength, and sufficient cohesion were obtained, particularly in 70 wt% TPU1 + 30 wt% TPU2 PSA.

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Negative-pressure polymorphs made by heterostructural alloying.

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Negative-pressure polymorphs made by heterostructural alloying.

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