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Quantum confinement of the perpendicular motion of electrons insingle-crystalline metallic superconducting nanofilms splits the conductionband into a series of single-electron subbands. A distinctive feature of such ananoscale multi-band superconductor is that the energetic position of eachsubband can vary significantly with changing nanofilm thickness, substratematerial, protection cover and other details of the fabrication process. It canoccur that the bottom of one of the available subbands is situated in thevicinity of the Fermi level. We demonstrate that the character of thesuperconducting pairing in such a subband changes dramatically and exhibits aclear molecule-like trend, which is very similar to the well-known crossoverfrom the Bardeen-Cooper-Schrieffer regime to Bose-Einstein condensation(BCS-BEC) observed in trapped ultracold fermions. For Pb nanofilms withthickness of 4 and 5 monolayers (ML) this will lead to a spectacular scenario:up to half of all the Cooper pairs nearly collapse, shrinking in the lateralsize (parallel to the nanofilm) down to a few nanometers. As a result, thesuperconducting condensate will be a coherent mixture of almost molecule-likefermionic pairs with ordinary, extended Cooper pairs.

Superconducting nanofilms: molecule-like pairing induced by quantum confinement