摘要： Coupling ultrafast light to surface nanoreliefs leads to periodic patterns achieving record processing scales down to tens of nanometers. Driven by near-field interactions, the promising potential of the spontaneous pattern formation relies on the scale-up manufacturing one-step process. Here, we report the self-assembly of unconventional arrays of nanocavities of 20 nm diameter with a periodicity down to 60 nm upon ultrafast laser irradiation of a nickel surface. In stark contrast to laser-induced surface ripples, which are stochastic and suffer from a lack of regularity, the 2D patterns present an unprecedented uniformity on extreme scales. The onset of nanocavity arrays ordered in a honeycomb lattice is achieved by overcoming the anisotropic polarization response of the surface by a delayed action of cross-polarized laser pulses. The origin of this self-arrangement is identified as a manifestation of Marangoni convection instability in a nanoscale melt layer, destabilized by the laser-induced rarefaction wave.