The elementary CuO2 plane sustaining cuprate high temperature superconductivity occurs typically at the base of a periodic array of edge-sharing CuO5 pyramids. Virtual transitions of electrons between adjacent planar Cu and O atoms, occurring at a rate t/ℏ and across the charge-transfer energy gap E, generate ‘superexchange’ spin-spin interactions of energy J≈4t4/E3 in an antiferromagnetic correlated-insulator state. However, hole doping this CuO2 plane converts this into a very high temperature superconducting state whose electron-pairing is exceptional. A leading proposal for the mechanism of this intense electron-pairing is that, while hole doping destroys magnetic order it preserves pair-forming superexchange interactions governed by the charge-transfer energy scale E.
To explore this hypothesis directly at atomic-scale, we developed high-voltage single-electron and electron-pair (Josephson) scanning tunneling microscopy, to visualize the interplay of E and the electron-pair density nP in Bi2Sr2CaCu2O8+x. Changing the distance δ between each pyramid’s apical O atom and the CuO2 plane below, should alter the energy levels of the planar Cu and O orbitals and thus vary E. Hence, the responses of both E and nP to alterations in δ that occur naturally in Bi2Sr2CaCu2O8+x were visualized. These data revealed, directly at atomic scale, the crux of strongly correlated superconductivity in CuO2: the response of the electron-pair condensate to varying the charge transfer energy. Strong concurrence between these observations and recent three-band Hubbard model DMFT predictions for superconductivity in hole-doped Bi2Sr2CaCu2O8+x (PNAS 118, e2106476118 (2021)) indicate that charge-transfer superexchange is the electron-pairing mechanism (PNAS 119, 2207449119 (2022)).
Self-organized complex structures in nature, from hierarchical biopolymers to viral capsids and organisms, offer efficiency, adaptability, robustness, and multifunctionality. How are these structures assembled? Can we understand the fundamental principles behind their formation, and assemble similar structures in the lab using simple inorganic building blocks? What’s the purpose of these complex structures in nature, and can we utilize similar mechanisms to program new functions in metamaterials? In this talk, we will start from the perspective of geometric frustration, to explore answers to these questions. I will discuss our recent work on developing analytic theories based on crystal structures in non-Euclidean space for the self-assembly of nanoparticles into complex structures, mechanical properties of materials in which geometric frustration causes prestress, as well as our ongoing effort in designing topological mechanical metamaterials with and without geometric frustration.
