Researchers at the U.S. Department of Energy's Brookhaven National Laboratory have combined atoms with multiple orbitals and precisely pinned down their electron distributions. Using advanced electron diffraction techniques, the scientists discovered that orbital fluctuations in iron-based compounds induce strongly coupled polarizations that can enhance electron pairing—the essential mechanism behind superconductivity. The study, set to publish soon in the journal Physical Review Letters, provides a breakthrough method for exploring and improving superconductivity in a wide range of new materials.

"For the first time, we obtained direct experimental evidence of the subtle changes in electron orbitals by comparing an unaltered, non-superconducting material with its doped, superconducting twin," said Brookhaven Lab physicist and project leader Yimei Zhu.

"Now superconductor theory can incorporate proof of strong coupling between iron and arsenic in these dense electron cloud interactions," said Brookhaven Lab physicist and study coauthor Weiguo Yin. "This unexpected discovery brings together both orbital fluctuation theory and the 50-year-old 'excitonic' theory for high-temperature superconductivity, opening a new frontier for condensed matter physics."

"For the first time, we obtained direct experimental evidence of the subtle changes in electron orbitals..."Yimei Zhu, Brookhaven National Laboratory.

"Consider measuring waves crashing across the ocean's surface," Zhu said. "We needed to pinpoint those complex fluctuations without having the data obscured by the deep water underneath. The waves represent the all-important electrons in the outer orbital shells, which are barely distinguishable from the layers of inner electrons. For example, each barium atom alone has 56 electrons, but we're only concerned with the two in the outermost layer."

The Brookhaven researchers used a technique called quantitative convergent beam electron diffraction (CBED) to reveal the orbital clouds with subatomic precision. After an electron beam strikes the sample, it bounces off the charged particles to reveal the configuration of the atomic lattice, or the exact arrays of nuclei orbited by electrons. The scientists took thousands of these measurements, subtracted the inner electrons, and converted the data into probabilities—balloon-shaped areas where the valence electrons were most likely to be found.

The researchers first examined the electron clouds of non-superconducting samples of barium iron arsenic. The CBED data revealed that the arsenic atoms exhibited little shift or polarization of valence electrons. However, when the scientists transformed the compound into a superconductor by doping it with cobalt, the electron distribution radically changed.
"Cobalt doping pushed the orbital electrons in the arsenic outward, concentrating the negative charge on the outside of the 'sandwich' and creating a positively charged pocket closer to the central layer of iron," Zhu said. "We created very precise electronic and atomic displacement that might actually drive the critical temperature of these superconductors higher."

Yin added: "What's really exciting is that this electron polarization exhibits strong coupling. The quadrupole polarization of the iron, which indicates the orbital fluctuation, couples intimately with the arsenic dipole polarization—this mechanism may be key to the emergence of high-temperature superconductivity in these iron-based compounds. And our results may guide the design of new materials."

This story is reprinted from material from Brookhaven National Laboratory, with editorial changes made by Materials Today. The views expressed in this article do not necessarily represent those of Elsevier. Link to original source.