Xuesong Shi

Subwavelength ripples adjustment based on electron dynamics control by using shaped ultrafast laser pulse trains

This study reveals that the periods, ablation areas and orientations of periodic surface structures (ripples) in fused silica can be adjusted by using designed femtosecond (fs) laser pulse trains to control transient localized electron dynamics and corresponding material properties. By increasing the pulse delays from 0 to 100 fs, the ripple periods are changed from ~550 nm to ~255 nm and the orientation is rotated by 90°. The nearwavelength/subwavelength ripple periods are close to the fundamental/second-harmonic wavelengths in fused silica respectively. The subsequent subpulse of the train significantly impacts free electron distributions generated by the previous subpulse(s), which might influence the formation mechanism of ripples and the surface morphology.

Femtosecond laser rapid fabrication of large-area rose-like micropatterns on freestanding flexible graphene films

We developed a simple, scalable and high-throughput method for fabrication of large-area three-dimensional rose-like microflowers with controlled size, shape and density on graphene films by femtosecond laser micromachining. The novel biomimetic microflower that composed of numerous turnup graphene nanoflakes can be fabricated by only a single femtosecond laser pulse, which is efficient enough for large-area patterning. The graphene films were composed of layer-by-layer graphene nanosheets separated by nanogaps (~10–50 nm), and graphene monolayers with an interlayer spacing of ~0.37 nm constituted each of the graphene nanosheets. This unique hierarchical layering structure of graphene films provides great possibilities for generation of tensile stress during femtosecond laser ablation to roll up the nanoflakes, which contributes to the formation of microflowers. By a simple scanning technique, patterned surfaces with controllable densities of flower patterns were obtained, which can exhibit adhesive superhydrophobicity. More importantly, this technique enables fabrication of the large-area patterned surfaces at centimeter scales in a simple and efficient way. This study not only presents new insights of ultrafast laser processing of novel graphene-based materials but also shows great promise of designing new materials combined with ultrafast laser surface patterning for future applications in functional coatings, sensors, actuators and microfluidics.

Femtosecond laser pulse-train induced breakdown in fused silica: the role of seed electrons

Femtosecond laser pulse-train induced breakdown in fused silica is investigated theoretically, with a focus on the role of ultrafast seed electrons during the pulse-train excitation. Material breakdown threshold is investigated by a model, which consists of both the excitation model and an improved optical model by including the optical absorption of self-trapped excitons (STEs). It is found that the evolution of a single train induced breakdown threshold is governed by the interplay of three competing sources of seed electrons initiating an electronic avalanche: residual conduction-band electrons left by the previous pulse, photoionization of atoms in dense media and photoionization of STEs by subsequent pulses. The third source provides a key to the understanding of some potential and existing problems involved, and leads to many pulse-separation independent phenomena (e.g. surface damage/ablation size) for pulse-train processing when it becomes dominant, and can contribute to the repeatable processing. For a single train of two or several femtosecond pulses, the third source can become dominant and sustained at large pulse-separations only when the first-pulse energy is over a critical value, ~65?75% of the single-pulse breakdown threshold. Our calculations are in agreement with the experimental data.

Femtosecond double-pulse fabrication of hierarchical nanostructures based on electron dynamics control for high surface-enhanced Raman scattering

This Letter presents a simple, efficient approach for high surface-enhanced Raman scattering by one-step controllable fabrication of hierarchical structures (nanoparticles+subwavelength ripples) on silicon substrates in silver nitrate solutions using femtosecond double pulses based on nanoscale electron dynamics control. As the delays of the double pulses increase from 0 fs to 1 ps, the hierarchical structures can be controlled with (1) nanoparticles--the number of nanoparticles in the range of 40-100 nm reaches the maximum at 800 fs and (2) ripples--the subwavelength ripples become intermittent with decreased ablation depths. The redistributed nanoparticles and the modified ripple structures contribute to the maximum enhancement factor of 2.2×10(8) (measured by 10(-6)  M rhodamine 6G solution) at the pulse delay of 800 fs.

Nanopillar arrays with nanoparticles fabricated by a femtosecond laser pulse train for highly sensitive SERRS

This work presents a novel method for fabricating repeatable, uniform, large-area, highly sensitive, surface-enhanced resonance Raman scattering (SERRS) substrates combined with silicon nanopillar arrays and silver nanoparticles. The proposed method consists of two steps: (1) induce periodic ripples in deionized water using a linearly polarized femtosecond laser; and (2) generate dense 80-nm-diameter nanopillar arrays with silver nanoparticles in silver nitrate solution with a 90° rotated polarization, femtosecond double-pulse train. As the pulse delay increases from 0 to 1000 fs, the mean size of the silver nanoparticles reduces, and the average number of nanoparticles increases, which, in turn, increases the enhancement factor of SERRS signals up to 1.1×10(9). Furthermore, melamine (down to 125 ppb) was detected by the fabricated SERRS substrates.

Temporal femtosecond pulse shaping dependence of laser-induced periodic surface structures in fused silica

The dependence of periodic structures and ablated areas on temporal pulse shaping is studied upon irradiation of fused silica by femtosecond laser triple-pulse trains. Three types of periodic structures can be obtained by using pulse trains with designed pulse delays, in which the three-dimensional nanopillar arrays with ∼100–150 nm diameters and ∼200 nm heights are first fabricated in one step. These nanopillars arise from the break of the ridges of ripples in the upper portion, which is caused by the split of orthogonal ripples in the bottom part. The localized transient electron dynamics and corresponding material properties are considered for the morphological observations.

Shape-Controllable Gold Nanoparticle–MoS2 Hybrids Prepared by Tuning Edge-Active Sites and Surface Structures of MoS2 via Temporally Shaped Femtosecond Pulses

Edge-active site control of MoS2 is crucial for applications such as chemical catalysis, synthesis of functional composites, and biochemical sensing. This work presents a novel nonthermal method to simultaneously tune surface chemical (edge-active sites) and physical (surface periodic micro/nano structures) properties of MoS2 using temporally shaped femtosecond pulses, through which shape-controlled gold nanoparticles are in situ and self-assembly grown on MoS2 surfaces to form Au-MoS2 hybrids. The edge-active sites with unbound sulfurs of laser-treated MoS2 drive the reduction of gold nanoparticles, while the surface periodic structures of laser-treated MoS2 assist the shape-controllable growth of gold nanoparticles. The proposed novel method highlights the broad application potential of MoS2; for example, these Au-MoS2 hybrids exhibit tunable and highly sensitive SERS activity with an enhancement factor up to 1.2 × 107, indicating the marked potential of MoS2 in future chemical and biological sensing applications.

Production rate enhancement of size-tunable silicon nanoparticles by temporally shaping femtosecond laser pulses in ethanol

This paper proposes an efficient approach for production-rate enhancement and size reduction of silicon nanoparticles produced by femtosecond (fs) double-pulse ablation of silicon in ethanol. Compared with a single pulse, the production rate is ~2.6 times higher and the mean size of the NPs is reduced by ~1/5 with a delay of 2 ps. The abnormal enhancement in the production rate is obtained at pulse delays Δt > 200 fs. The production-rate enhancement is mainly attributed to high photon absorption efficiency. It is caused by an increase in localized transient electron density, which results from the first sub-pulse ionization of ethanol molecules before the second sub-pulse arrives. The phase-change mechanism at a critical point might reduce nanoparticle size.