<p>Is it feasible to alter the ground-state properties of a material by engineering its electromagnetic environment? Inspired by theoretical predictions<sup><CitationRef AdditionalCitationIDS="CR2 CR3 CR4 CR5 CR6 CR7 CR8 CR9 CR10 CR11" CitationID="CR1">1</CitationRef>–<CitationRef CitationID="CR12">12</CitationRef></sup>, experimental realizations of such cavity-controlled properties without optical excitation are beginning to emerge<sup><CitationRef AdditionalCitationIDS="CR14 CR15 CR16 CR17 CR18" CitationID="CR13">13</CitationRef>–<CitationRef CitationID="CR19">19</CitationRef></sup>. Here we devised and implemented a new platform to realize cavity-altered materials. Single crystals of hyperbolic van der Waals (vdW) compounds provide a resonant electromagnetic environment with enhanced density of photonic states and prominent mode confinement<sup><CitationRef AdditionalCitationIDS="CR21 CR22 CR23" CitationID="CR20">20</CitationRef>–<CitationRef CitationID="CR24">24</CitationRef></sup>. We interfaced hexagonal boron nitride (hBN) with the molecular superconductor κ-(BEDT-TTF)<sub>2</sub>Cu[N(CN)<sub>2</sub>]Br (κ-ET). The frequencies of infrared hyperbolic modes (HMs) of hBN (refs. <sup><CitationRef CitationID="CR25">25</CitationRef>,<CitationRef CitationID="CR26">26</CitationRef></sup>) match the infrared-active carbon–carbon (C=C) stretching molecular resonance of κ-ET implicated in superconductivity<sup><CitationRef CitationID="CR27">27</CitationRef></sup>. Nano-optical data supported by first-principles molecular Langevin dynamics simulations confirm the presence of resonant coupling between the hBN hyperbolic cavity modes and the C=C stretching mode in κ-ET. Meissner-effect measurements using magnetic force microscopy (MFM) demonstrate a strong suppression of superfluid density near the hBN/κ-ET interface. Non-resonant control heterostructures, including RuCl<sub>3</sub>/κ-ET and hBN/Bi<sub>2</sub>Sr<sub>2</sub>CaCu<sub>2</sub>O<sub>8+<i>x</i></sub> (BSCCO), do not show the pronounced superfluid suppression. These observations suggest that hBN/κ-ET realizes a cavity-altered superconducting ground state. Our work highlights the potential of dark cavities devoid of external photons for engineering electronic ground-state properties of complex quantum materials.</p>

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Cavity-altered superconductivity

  • Itai Keren,
  • Tatiana A. Webb,
  • Shuai Zhang,
  • Jikai Xu,
  • Dihao Sun,
  • Brian S. Y. Kim,
  • Dongbin Shin,
  • Songtian S. Zhang,
  • Junhe Zhang,
  • Giancarlo Pereira,
  • Juntao Yao,
  • Takuya Okugawa,
  • Marios H. Michael,
  • Emil Viñas Boström,
  • James H. Edgar,
  • Stuart Wolf,
  • Matthew Julian,
  • Rohit P. Prasankumar,
  • Kazuya Miyagawa,
  • Kazushi Kanoda,
  • Genda Gu,
  • Matthew Cothrine,
  • David Mandrus,
  • Michele Buzzi,
  • Andrea Cavalleri,
  • Cory R. Dean,
  • Dante M. Kennes,
  • Andrew J. Millis,
  • Qiang Li,
  • Michael A. Sentef,
  • Angel Rubio,
  • Abhay N. Pasupathy,
  • D. N. Basov

摘要

Is it feasible to alter the ground-state properties of a material by engineering its electromagnetic environment? Inspired by theoretical predictions112, experimental realizations of such cavity-controlled properties without optical excitation are beginning to emerge1319. Here we devised and implemented a new platform to realize cavity-altered materials. Single crystals of hyperbolic van der Waals (vdW) compounds provide a resonant electromagnetic environment with enhanced density of photonic states and prominent mode confinement2024. We interfaced hexagonal boron nitride (hBN) with the molecular superconductor κ-(BEDT-TTF)2Cu[N(CN)2]Br (κ-ET). The frequencies of infrared hyperbolic modes (HMs) of hBN (refs. 25,26) match the infrared-active carbon–carbon (C=C) stretching molecular resonance of κ-ET implicated in superconductivity27. Nano-optical data supported by first-principles molecular Langevin dynamics simulations confirm the presence of resonant coupling between the hBN hyperbolic cavity modes and the C=C stretching mode in κ-ET. Meissner-effect measurements using magnetic force microscopy (MFM) demonstrate a strong suppression of superfluid density near the hBN/κ-ET interface. Non-resonant control heterostructures, including RuCl3/κ-ET and hBN/Bi2Sr2CaCu2O8+x (BSCCO), do not show the pronounced superfluid suppression. These observations suggest that hBN/κ-ET realizes a cavity-altered superconducting ground state. Our work highlights the potential of dark cavities devoid of external photons for engineering electronic ground-state properties of complex quantum materials.