Kagome metals, characterized by their two-dimensional lattices of corner-sharing triangles, have recently been predicted to host compact molecular orbitals, or standing-wave patterns of electrons that could potentially facilitate unconventional superconductivity and novel magnetic orders that can be made active by electron correlation effects. In most materials, these flat bands remain too far from active energy levels to have any significant impact; however, in CsCr3Sb5, they are actively involved and directly influence the material's properties.
Pengcheng Dai, Ming Yi and Qimiao Si of Rice's Department of Physics and Astronomy and Smalley-Curl Institute, along with Di-Jing Huang of Taiwan's National Synchrotron Radiation Research Center, led the study.
"Our results confirm a surprising theoretical prediction and establish a pathway for engineering exotic superconductivity through chemical and structural control," said Dai, the Sam and Helen Worden Professor of Physics and Astronomy.
The finding provides experimental proof for ideas that had only existed in theoretical models. It also shows how the intricate geometry of kagome lattices can be used as a design tool for controlling the behavior of electrons in solids.
"By identifying active flat bands, we've demonstrated a direct connection between lattice geometry and emergent quantum states," said Yi, an associate professor of physics and astronomy.
The research team employed two advanced synchrotron techniques alongside theoretical modeling to investigate the presence of active standing-wave electron modes. They used angle-resolved photoemission spectroscopy (ARPES) to map electrons emitted under synchrotron light, revealing distinct signatures associated with compact molecular orbitals. Resonant inelastic X-ray scattering (RIXS) measured magnetic excitations linked to these electronic modes.
"The ARPES and RIXS results of our collaborative team give a consistent picture that flat bands here are not passive spectators but active participants in shaping the magnetic and electronic landscape," said Si, the Harry C. and Olga K. Wiess Professor of Physics and Astronomy, "This is amazing to see given that, until now, we were only able to see such features in abstract theoretical models."
Theoretical support was provided by analyzing the effect of strong correlations starting from a custom-built electronic lattice model, which replicated the observed features and guided the interpretation of results. Fang Xie, a Rice Academy Junior Fellow and co-first author, led that portion of the study.
Obtaining such precise data required unusually large and pure crystals of CsCr3Sb5, synthesized using a refined method that produced samples 100 times larger than previous efforts, said Zehao Wang, a Rice graduate student and co-first author.
The work underscores the potential of interdisciplinary research across fields of study, said Yucheng Guo, a Rice graduate student and co-first author who led the ARPES work.
"This work was possible due to the collaboration that consisted of materials design, synthesis, electron and magnetic spectroscopy characterization and theory," Guo said.
Research Report:Spin excitations and flat electronic bands in aCr-based kagome superconductor
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