Disordered
ridge-splitting on laser-induced periodic surface structures
(LIPSSs) often reduces structure quality and degrades application
performance but introduces a potential route for laser structuring
accuracy with access to the deep-subwavelength scale. Here, nanolithography
based on the homogeneous ridge-splitting mechanism is implemented
on a molybdenum surface using two-color (400 and 800 nm) temporally
delayed femtosecond laser pulses with identical linear polarizations.
The achieved splitting LIPSS, with a periodicity down to 140 nm and
a feature size down to 70 nm, was uniformly distributed in the long
range without any wavy or interruption defects, presenting improvements
on the structure’s accuracy and quality relative to the observation
of single-beam femtosecond 400 nm laser irradiation. The generation
and suppression of the homogeneous ridge-splitting phenomenon can
be manipulated via altering the time delay or the fluences of the
two-color laser pulses, which results in transitions between the regular
near-subwavelength and deep-subwavelength LIPSSs. The underlying physical
origins are attributed to the excitation of various electromagnetic
field enhancement modes during the transiently correlated dynamic
process of two-color laser–material interactions. Our investigations
facilitate the laser nanostructuring of metals with an accessible
100 nm feature size, and the nanostructured Mo surface enables specific
applications in the field of concentrated solar energy devices.