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<p>High-temperature superconductivity in cuprates can be realized by doping holes into an antiferromagnetic insulator. To understand the mechanism by which this happens, one must elucidate the electronic state of a single doped hole and the coupling between them that gradually leads to pairing. Experimental progress has been hindered by the technical challenges in probing the electronic properties of a small number of holes dispersed into an insulating oxide. Here we show that in Ca<sub>2</sub>CuO<sub>2</sub>Cl<sub>2</sub> with dilute hole doping, an isolated dopant exhibits an in-gap electronic state with a spatial pattern consistent with a localized Zhang–Rice singlet. The dopant forms a bound state with a hole in a copper orbital. With increasing hole density, the overlap of Zhang–Rice singlets generates rod-shaped patterns. These electronic molecules spontaneously segregate into plaquettes with a lateral size of approximately four lattice constants. Our spectroscopic-imaging scanning tunnelling microscopy shows that the first indication of pairing is a U-shaped energy gap that emerges in the electronic molecules. It evolves smoothly into a sharp V-shaped gap characteristic of d-wave superconductivity in extended islands of electronic molecules. These results provide insights into the emergence of Cooper pairing in cuprates.</p>

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Visualization of the Zhang–Rice singlet, electronic molecules and Cooper pair formation in a cuprate superconductor

  • 期刊论文

  • 发表日期：

    2026年7月7日

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  • Shusen Ye,
  • Jianfa Zhao,
  • Zhiheng Yao,
  • Sixuan Chen,
  • Runze Yu,
  • Zehao Dong,
  • Zhenqi Hao,
  • Xintong Li,
  • Luchuan Shi,
  • Qingqing Liu,
  • Changqing Jin,
  • Yayu Wang

摘要

High-temperature superconductivity in cuprates can be realized by doping holes into an antiferromagnetic insulator. To understand the mechanism by which this happens, one must elucidate the electronic state of a single doped hole and the coupling between them that gradually leads to pairing. Experimental progress has been hindered by the technical challenges in probing the electronic properties of a small number of holes dispersed into an insulating oxide. Here we show that in Ca2CuO2Cl2 with dilute hole doping, an isolated dopant exhibits an in-gap electronic state with a spatial pattern consistent with a localized Zhang–Rice singlet. The dopant forms a bound state with a hole in a copper orbital. With increasing hole density, the overlap of Zhang–Rice singlets generates rod-shaped patterns. These electronic molecules spontaneously segregate into plaquettes with a lateral size of approximately four lattice constants. Our spectroscopic-imaging scanning tunnelling microscopy shows that the first indication of pairing is a U-shaped energy gap that emerges in the electronic molecules. It evolves smoothly into a sharp V-shaped gap characteristic of d-wave superconductivity in extended islands of electronic molecules. These results provide insights into the emergence of Cooper pairing in cuprates.