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International audienceWe investigate initial cumulative irradiation effects leading to variable surface topographies and nanoscale  roughness,  and  triggering  eventually  the  formation  of  laser-induced  periodic  surface  structures (LIPSS) on Zr-based  bulk  metallic  glasses  (Zr41.2Ti13.8Cu12.5Ni10Be25.5 (at%)).  We  discuss  interconnected  aspects  related  to  electronic  excitation  and  optical  transients,  potential  variations  in  the cartography of thermally-driven chemical modifications and topographical features assisting the surface  coupling  of  the  electromagnetic  field.  The  transient  optical  properties  of  Zr-based  BMG  surfaces  upon  ultrafast  irradiation,  measured  by  a  two-angle  time-resolved  single-pump  double-probe  ellipsometry  method,  show  a  remarkable  constancy  up  to  the  point  of  optical  damage and rapid  gas-phase  transition  beyond.  In  intermediate  and  low  exposure  conditions,  in  the  vicinity  of  the  damage  domain,  mult i-pulse incubation effects  determine  the  appearance  of  nanoscale  surface  structures.  The  aspects  discussed  here  involve  primarily  the  progression  of  nanoscale  structuring  with an increasing  number  of  fs  laser  pulses  starting  from  a  rough  surface  and  evolving  towards  ordered  corrugation.  We  emphasize  the  role  of  initial  roughness  in  determining  light  coupling  and  the  generation  of  regular  stationary  patterns  of  scattered  light,  localized  energy  absorption  and spatially-variant ablation or modulated temperature-driven factors for surface relief. From a material perspective,   energy   dispersive   X-ray   spectrometry   (EDX)   analysis   shows   potential   selective vaporization  of  light  elements,  leading  to  gradual  compositional  changes  and  proving  a  spatially-modulated temperature pattern. A formation scenario is proposed involving interference between the incident  laser  and  scattered  light  potentially  mediated  by  localized  surface  plasmons.  Finite-difference  time-domain  (FDTD)  simulations  are  applied  to  validate  the  mechanism,  showing  that  LIPSS appear intrinsically related to the surface superposition of electromagnetic waves

Initial Cumulative Effects in Femtosecond Pulsed Laser-induced Periodic Surface Structures on Bulk Metallic Glasses