Learning Complexity to Guide Light-Induced Self-Organized Nanopatterns.

Ultrafast laser irradiation can induce spontaneous self-organization of surfaces into dissipative structures with nanoscale reliefs. These surface patterns emerge from symmetry-breaking dynamical processes that occur in Rayleigh-Bénard-like instabilities. In this study, we demonstrate that the coexistence and competition between surface patterns of different symmetries in two dimensions can be numerically unraveled using the stochastic generalized Swift-Hohenberg model. We originally propose a deep convolutional network to identify and learn the dominant modes that stabilize for a given bifurcation and quadratic model coefficients. The model is scale-invariant and has been calibrated on microscopy measurements using a physics-guided machine learning strategy. Our approach enables the identification of experimental irradiation conditions for a desired self-organization pattern. It can be generally applied to predict structure formation in situations where the underlying physics can be approximately described by a self-organization process and data is sparse and nontime series. Our Letter paves the way for supervised local manipulation of matter using timely controlled optical fields in laser manufacturing.

Boosted Spontaneous Formation of High-Aspect Ratio Nanopeaks on Ultrafast Laser-Irradiated Ni Surface.

The capacity to synthesize and design highly intricated nanoscale objects of different sizes, surfaces, and shapes dramatically conditions the development of multifunctional nanomaterials. Ultrafast laser technology holds great promise as a contactless process able to rationally and rapidly manufacture complex nanostructures bringing innovative surface functions. The most critical challenge in controlling the growth of laser-induced structures below the light diffraction limit is the absence of external order associated to the inherent local interaction due to the self-organizing nature of the phenomenon. Here high aspect-ratio nanopatterns driven by near-field surface coupling and architectured by timely-controlled polarization pulse shaping are reported. Electromagnetic coupled with hydrodynamic simulations reveal why this unique optical manipulation allows peaks generation by inhomogeneous local absorption sustained by nanoscale convection. The obtained high aspect-ratio surface nanotopography is expected to prevent bacterial proliferation, and have great potential for catalysis, vacuum to deep UV photonics and sensing.

Self-Organization Regimes Induced by Ultrafast Laser on Surfaces in the Tens of Nanometer Scales.

A laser-irradiated surface is the paradigm of a self-organizing system, as coherent, aligned, chaotic, and complex patterns emerge at the microscale and even the nanoscale. A spectacular manifestation of dissipative structures consists of different types of randomly and periodically distributed nanostructures that arise from a homogeneous metal surface. The noninstantaneous response of the material reorganizes local surface topography down to tens of nanometers scale modifying long-range surface morphology on the impact scale. Under ultrafast laser irradiation with a regulated energy dose, the formation of nanopeaks, nanobumps, nanohumps and nanocavities patterns with 20-80 nm transverse size unit and up to 100 nm height are reported. We show that the use of crossed-polarized double laser pulse adds an extra dimension to the nanostructuring process as laser energy dose and multi-pulse feedback tune the energy gradient distribution, crossing critical values for surface self-organization regimes. The tiny dimensions of complex patterns are defined by the competition between the evolution of transient liquid structures generated in a cavitation process and the rapid resolidification of the surface region. Strongly influencing the light coupling, we reveal that initial surface roughness and type of roughness both play a crucial role in controlling the transient emergence of nanostructures during laser irradiation.

Sub-100 nm 2D nanopatterning on a large scale by ultrafast laser energy regulation.

Coupling ultrafast light irradiation 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 scaling up of one-step manufacturing processes. 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.

Growth Twinning and Generation of High-Frequency Surface Nanostructures in Ultrafast Laser-Induced Transient Melting and Resolidification.

The structural changes generated in surface regions of single crystal Ni targets by femtosecond laser irradiation are investigated experimentally and computationally for laser fluences that, in the multipulse irradiation regime, produce sub-100 nm high spatial frequency surface structures. Detailed experimental characterization of the irradiated targets combining electron back scattered diffraction analysis with high-resolution transmission electron microscopy reveals the presence of multiple nanoscale twinned domains in the irradiated surface regions of single crystal targets with (111) surface orientation. Atomistic- and continuum-level simulations performed for experimental irradiation conditions reproduce the generation of twinned domains and establish the conditions leading to the formation of growth twin boundaries in the course of the fast transient melting and epitaxial regrowth of the surface regions of the irradiated targets. The observation of growth twins in the irradiated Ni(111) targets provides strong evidence of the role of surface melting and resolidification in the formation of high spatial frequency surface structures. This also suggests that the formation of twinned domains can be used as a sensitive measure of the levels of liquid undercooling achieved in short pulse laser processing of metals.