We developed an ab initio quantum chemistry framework for faithful simulations of high-temperature superconductors (cuprates). The method allows for spin SU(2) and particle-number U(1) symmetry-breaking states such that the superconducting orders spontaneously emerge during the self-consistency. We directly computed the superconducting pairing order of several doped cuprate materials and structures. We found that we could correctly capture two well-known trends: the pressure effect, where the pairing order increases with intra-layer pressure, and the layer effect, where the pairing order varies with the number of copper-oxygen layers. From these calculations, we observed that the strength of superexchange and the covalency at optimal doping are the best descriptors of the maximal pairing order. Our microscopic analysis further identified short-range copper spin fluctuations, together with multi-orbital charge fluctuations, as central to the pairing trends. Our work demonstrates the possibility of a quantitative computational understanding of high-temperature superconducting materials.

Dr. ZhiHao Cui received his bachelor’s degree from Peking University in 2017 (under the supervision of Prof. Hong Jiang). After that, he obtained his Ph.D. in Theoretical Chemistry from Caltech in 2023 (under the supervision of Prof. Garnet Chan). He is currently a postdoctoral scholar at Columbia University (working with Prof. David Reichman). His Ph.D. research has been focused on establishing a theoretical framework for simulations of high-temperature superconductors and other strongly correlated quantum materials. In particular, he is the leading author of several high-impact research works, including in the area of ab initio quantum embedding theories (density matrix embedding theory and dynamical mean-field theory), and the fully ab initio simulation of the magnetic and superconducting properties of high-temperature superconductors.  He is now working on electron-boson coupled systems, such as polariton and polaron chemistry. Dr. Cui has received many awards and distinctions, including the Herbert Newby McCoy Award from Caltech, the Chemical Computing Group Excellence Award for Graduate Students from ACS, the Eddleman Graduate Research Fellowship, the Caltech C Fellowship, etc.