<p>Recently, the Ruddlesden–Popper bilayer nickelate La<sub>3</sub>Ni<sub>2</sub>O<sub>7</sub> has emerged as a superconductor with a transition temperature (<i>T</i><sub>c</sub>) of approximately 80 K above 14 GPa (refs. <sup><CitationRef AdditionalCitationIDS="CR2" CitationID="CR1">1</CitationRef>–<CitationRef CitationID="CR3">3</CitationRef></sup>). Achieving a higher <i>T</i><sub>c</sub> in nickelate superconductors, along with the synthesis of reproducible high-quality single crystals without relying on high-oxygen-pressure growth conditions, remains a significant challenge<sup><CitationRef AdditionalCitationIDS="CR5 CR6" CitationID="CR4">4</CitationRef>–<CitationRef CitationID="CR7">7</CitationRef></sup>. Here we report superconductivity up to 96 K under high pressure in bilayer nickelate single crystals synthesized at ambient pressure. Energy-dispersive spectroscopy, single-crystal X-ray diffraction, nuclear quadrupole resonance and scanning transmission electron microscopy evidenced high crystal quality of the flux-grown La<sub>2</sub>SmNi<sub>2</sub>O<sub>7−<i>δ</i></sub> single crystals. La<sub>2</sub>SmNi<sub>2</sub>O<sub>7</sub> exhibits clear bulk superconductivity, including zero resistivity (<InlineEquation ID="IEq1"> <EquationSource Format="TEX">\({T}_{{\rm{c}},\max }^{{\rm{onset}}}\)</EquationSource> <EquationSource Format="MATHML"><math> <msubsup> <mrow> <mi>T</mi> </mrow> <mrow> <mi mathvariant="normal">c</mi> <mo>,</mo> <mi>max</mi> </mrow> <mrow> <mi mathvariant="normal">onset</mi> </mrow> </msubsup> </math></EquationSource> </InlineEquation> = 92 K and <InlineEquation ID="IEq2"> <EquationSource Format="TEX">\({T}_{{\rm{c}},\max }^{{\rm{zero}}}\)</EquationSource> <EquationSource Format="MATHML"><math> <msubsup> <mrow> <mi>T</mi> </mrow> <mrow> <mi mathvariant="normal">c</mi> <mo>,</mo> <mi>max</mi> </mrow> <mrow> <mi mathvariant="normal">zero</mi> </mrow> </msubsup> </math></EquationSource> </InlineEquation> = 73 K at 21.6 GPa) and the Meissner effect (<i>T</i><sub>c</sub> = 60 K at 20.6 GPa). A low-temperature high-pressure structural study indicates that both monoclinic and tetragonal structures can support superconductivity in this bilayer nickelate. Furthermore, we established a correlation between higher <i>T</i><sub>c</sub> under high pressures and larger in-plane lattice distortion under ambient conditions, corroborated by observing even higher <InlineEquation ID="IEq3"> <EquationSource Format="TEX">\({T}_{{\rm{c}}}^{{\rm{onset}}}\)</EquationSource> <EquationSource Format="MATHML"><math> <msubsup> <mrow> <mi>T</mi> </mrow> <mrow> <mi mathvariant="normal">c</mi> </mrow> <mrow> <mi mathvariant="normal">onset</mi> </mrow> </msubsup> </math></EquationSource> </InlineEquation> of 96 K in La<sub>1.57</sub>Sm<sub>1.43</sub>Ni<sub>2</sub>O<sub>7−<i>δ</i></sub>. This study overcomes key limitations in growing nickelate superconductor crystals, resolves the crystal structure in the superconducting state and demonstrates an effective pathway towards achieving higher <i>T</i><sub>c</sub>.</p>

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Bulk superconductivity up to 96 K in pressurized nickelate single crystals

  • Feiyu Li,
  • Zhenfang Xing,
  • Di Peng,
  • Jie Dou,
  • Ning Guo,
  • Liang Ma,
  • Yulin Zhang,
  • Lingzhen Wang,
  • Jun Luo,
  • Jie Yang,
  • Jian Zhang,
  • Tieyan Chang,
  • Yu-Sheng Chen,
  • Weizhao Cai,
  • Jinguang Cheng,
  • Yuzhu Wang,
  • Yuxin Liu,
  • Tao Luo,
  • Naohisa Hirao,
  • Takahiro Matsuoka,
  • Hirokazu Kadobayashi,
  • Zhidan Zeng,
  • Qiang Zheng,
  • Rui Zhou,
  • Qiaoshi Zeng,
  • Xutang Tao,
  • Junjie Zhang

摘要

Recently, the Ruddlesden–Popper bilayer nickelate La3Ni2O7 has emerged as a superconductor with a transition temperature (Tc) of approximately 80 K above 14 GPa (refs. 13). Achieving a higher Tc in nickelate superconductors, along with the synthesis of reproducible high-quality single crystals without relying on high-oxygen-pressure growth conditions, remains a significant challenge47. Here we report superconductivity up to 96 K under high pressure in bilayer nickelate single crystals synthesized at ambient pressure. Energy-dispersive spectroscopy, single-crystal X-ray diffraction, nuclear quadrupole resonance and scanning transmission electron microscopy evidenced high crystal quality of the flux-grown La2SmNi2O7−δ single crystals. La2SmNi2O7 exhibits clear bulk superconductivity, including zero resistivity ( \({T}_{{\rm{c}},\max }^{{\rm{onset}}}\) T c , max onset  = 92 K and \({T}_{{\rm{c}},\max }^{{\rm{zero}}}\) T c , max zero  = 73 K at 21.6 GPa) and the Meissner effect (Tc = 60 K at 20.6 GPa). A low-temperature high-pressure structural study indicates that both monoclinic and tetragonal structures can support superconductivity in this bilayer nickelate. Furthermore, we established a correlation between higher Tc under high pressures and larger in-plane lattice distortion under ambient conditions, corroborated by observing even higher \({T}_{{\rm{c}}}^{{\rm{onset}}}\) T c onset of 96 K in La1.57Sm1.43Ni2O7−δ. This study overcomes key limitations in growing nickelate superconductor crystals, resolves the crystal structure in the superconducting state and demonstrates an effective pathway towards achieving higher Tc.