@article{ZaldenQuirinSchumacheretal.2019, author = {Zalden, Peter and Quirin, Florian and Schumacher, Mathias and Siegel, Jan and Wei, Shuai and Koc, Azize and Nicoul, Matthieu and Trigo, Mariano and Andreasson, Pererik and Enquist, Henrik and Shu, Michael J. and Pardini, Tommaso and Chollet, Matthieu and Zhu, Diling and Lemke, Henrik and Ronneberger, Ider and Larsson, J{\"o}rgen and Lindenberg, Aaron M. and Fischer, Henry E. and Hau-Riege, Stefan and Reis, David A. and Mazzarello, Riccardo and Wuttig, Matthias and Sokolowski-Tinten, Klaus}, title = {Femtosecond x-ray diffraction reveals a liquid-liquid phase transition in phase-change materials}, series = {Science}, volume = {364}, journal = {Science}, number = {6445}, publisher = {American Assoc. for the Advancement of Science}, address = {Washington, DC}, issn = {0036-8075}, doi = {10.1126/science.aaw1773}, pages = {1062 -- 1067}, year = {2019}, abstract = {In phase-change memory devices, a material is cycled between glassy and crystalline states. The highly temperature-dependent kinetics of its crystallization process enables application in memory technology, but the transition has not been resolved on an atomic scale. Using femtosecond x-ray diffraction and ab initio computer simulations, we determined the time-dependent pair-correlation function of phase-change materials throughout the melt-quenching and crystallization process. We found a liquid-liquid phase transition in the phase-change materials Ag4In3Sb67Te26 and Ge15Sb85 at 660 and 610 kelvin, respectively. The transition is predominantly caused by the onset of Peierls distortions, the amplitude of which correlates with an increase of the apparent activation energy of diffusivity. This reveals a relationship between atomic structure and kinetics, enabling a systematic optimization of the memory-switching kinetics.}, language = {en} } @misc{SpiekermannHarderGilmoreetal.2019, author = {Spiekermann, Georg and Harder, M. and Gilmore, Keith and Zalden, Peter and Sahle, Christoph J. and Petitgirard, Sylvain and Wilke, Max and Biedermann, Nicole and Weis, Thomas and Morgenroth, Wolfgang and Tse, John S. and Kulik, E. and Nishiyama, Norimasa and Yava{\c{s}}, Hasan and Sternemann, Christian}, title = {Persistent Octahedral Coordination in Amorphous GeO₂ Up to 100 GPa by Kβ'' X-Ray Emission Spectroscopy}, series = {Postprints der Universit{\"a}t Potsdam Mathematisch-Naturwissenschaftliche Reihe}, journal = {Postprints der Universit{\"a}t Potsdam Mathematisch-Naturwissenschaftliche Reihe}, number = {699}, issn = {1866-8372}, doi = {10.25932/publishup-42775}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-427755}, year = {2019}, abstract = {We measure valence-to-core x-ray emission spectra of compressed crystalline GeO₂ up to 56 GPa and of amorphous GeO₂ up to 100 GPa. In a novel approach, we extract the Ge coordination number and mean Ge-O distances from the emission energy and the intensity of the Kβ'' emission line. The spectra of high-pressure polymorphs are calculated using the Bethe-Salpeter equation. Trends observed in the experimental and calculated spectra are found to match only when utilizing an octahedral model. The results reveal persistent octahedral Ge coordination with increasing distortion, similar to the compaction mechanism in the sequence of octahedrally coordinated crystalline GeO₂ high-pressure polymorphs.}, language = {en} } @article{SpiekermannHarderGilmoreetal.2019, author = {Spiekermann, Georg and Harder, M. and Gilmore, Keith and Zalden, Peter and Sahle, Christoph J. and Petitgirard, Sylvain and Wilke, Max and Biedermann, Nicole and Weis, Thomas and Morgenroth, Wolfgang and Tse, John S. and Kulik, E. and Nishiyama, Norimasa and Yava{\c{s}}, Hasan and Sternemann, Christian}, title = {Persistent Octahedral Coordination in Amorphous GeO₂ Up to 100 GPa by Kβ'' X-Ray Emission Spectroscopy}, series = {Physical Review X}, volume = {9}, journal = {Physical Review X}, number = {1}, publisher = {American Physical Society by the American Institute of Physics}, address = {Melville, NY}, issn = {2469-9926}, doi = {10.1103/PhysRevX.9.011025}, pages = {10}, year = {2019}, abstract = {We measure valence-to-core x-ray emission spectra of compressed crystalline GeO₂ up to 56 GPa and of amorphous GeO₂ up to 100 GPa. In a novel approach, we extract the Ge coordination number and mean Ge-O distances from the emission energy and the intensity of the Kβ'' emission line. The spectra of high-pressure polymorphs are calculated using the Bethe-Salpeter equation. Trends observed in the experimental and calculated spectra are found to match only when utilizing an octahedral model. The results reveal persistent octahedral Ge coordination with increasing distortion, similar to the compaction mechanism in the sequence of octahedrally coordinated crystalline GeO₂ high-pressure polymorphs.}, language = {en} }