Is it feasible to alter the ground-state properties of a material by engineering its electromagnetic environment? Inspired by theoretical predictions1–12, experimental realizations of such cavity-controlled properties without optical excitation are beginning to emerge13–19. 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 confinement20–24. We interfaced hexagonal boron nitride (hBN) with the molecular superconductor κ-(BEDT-TTF)2CuN(CN)2Br (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. A new platform making use of hexagonal boron nitride interfaced with the molecular superconductor κ-(BEDT-TTF)2CuN(CN)2Br is demonstrated for realizing cavity-altered materials, confirmed by magnetic force microscopy and nano-optical measurements.
Keren et al. (Wed,) studied this question.