Cavity-Altered Superconductivity

Abstract: Is it feasible to alter the ground state properties of a material by engineering its electromagnetic environment? Inspired by theoretical predictions, experimental realizations of such cavity-controlled properties without optical excitation are beginning to emerge. Here, we devised and implemented a novel 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 superior quality factor. We interfaced hexagonal boron nitride (hBN) with the molecular superconductor $\kappa$-(BEDT-TTF)$2$Cu[N(CN)$_2$]Br ($\kappa$-ET). The frequencies of infrared (IR) hyperbolic modes of hBN match the IR-active carbon-carbon stretching molecular resonance of ($\kappa$-ET) implicated in superconductivity. 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 carbon-carbon stretching mode in ($\kappa$-ET). Meissner effect measurements via magnetic force microscopy demonstrate a strong suppression of superfluid density near the hBN/($\kappa$-ET) interface. Non-resonant control heterostructures, including RuCl$_3$/($\kappa$-ET) and hBN/$\text{Bi}_2\text{Sr}_2\text{CaCu}_2\text{O}{8+x}$, do not display the superfluid suppression. These observations suggest that hBN/($\kappa$-ET) realizes a cavity-altered superconducting ground state. This work highlights the potential of dark cavities devoid of external photons for engineering electronic ground state properties of materials using IR-active phonons.