Driven by functionality and purity demand for applications of inorganic nanoparticle colloids in optics, biology, and energy, their surface chemistry has become a topic of intensive research interest. Consequently, ligand-free colloids are ideal reference materials for evaluating the effects of surface adsorbates from the initial state for application-oriented nanointegration purposes. After two decades of development, laser synthesis and processing of colloids (LSPC) has emerged as a convenient and scalable technique for the synthesis of ligand-free nanomaterials in sealed environments. In addition to the high-purity surface of LSPC-generated nanoparticles, other strengths of LSPC include its high throughput, convenience for preparing alloys or series of doped nanomaterials, and its continuous operation mode, suitable for downstream processing. Unscreened surface charge of LSPC-synthesized colloids is the key to achieving colloidal stability and high affinity to biomolecules as well as support materials,...

Laser Synthesis and Processing of Colloids: Fundamentals and Applications

During femtosecond laser fabrication, photons are mainly absorbed by electrons, and the subsequent energy transfer from electrons to ions is of picosecond order. Hence, lattice motion is negligible within the femtosecond pulse duration, whereas femtosecond photon-electron interactions dominate the entire fabrication process. Therefore, femtosecond laser fabrication must be improved by controlling localized transient electron dynamics, which poses a challenge for measuring and controlling at the electron level during fabrication processes. Pump-probe spectroscopy presents a viable solution, which can be used to observe electron dynamics during a chemical reaction. In fact, femtosecond pulse durations are shorter than many physical/chemical characteristic times, which permits manipulating, adjusting, or interfering with electron dynamics. Hence, we proposed to control localized transient electron dynamics by temporally or spatially shaping femtosecond pulses, and further to modify localized transient materials properties, and then to adjust material phase change, and eventually to implement a novel fabrication method. This review covers our progresses over the past decade regarding electrons dynamics control (EDC) by shaping femtosecond laser pulses in micro/nanomanufacturing: (1) Theoretical models were developed to prove EDC feasibility and reveal its mechanisms; (2) on the basis of the theoretical predictions, many experiments are conducted to validate our EDC-based femtosecond laser fabrication method. Seven examples are reported, which proves that the proposed method can significantly improve fabrication precision, quality, throughput and repeatability and effectively control micro/nanoscale structures; (3) a multiscale measurement system was proposed and developed to study the fundamentals of EDC from the femtosecond scale to the nanosecond scale and to the millisecond scale; and (4) As an example of practical applications, our method was employed to fabricate some key structures in one of the 16 Chinese National S&T Major Projects, for which electron dynamics were measured using our multiscale measurement system.

/pdf/electrons-dynamics-control-by-shaping-femtosecond-laser-535kqykqpo.pdf

Electrons dynamics control by shaping femtosecond laser pulses in micro/nanofabrication: modeling, method, measurement and application

Self-assembly of fundamental elements through weak, long-range interactions plays a central role in both supramolecular DNA assembly and bottom-up synthesis of nanostructures. Optical solitons, analogous in many ways to particles, arise from the balance between nonlinearity and dispersion and have been studied in numerous optical systems. Although both short- and long-range interactions between optical solitons have attracted extensive interest for decades, stable soliton supramolecules, with multiple aspects of complexity and flexibility, have thus far escaped experimental observation due to the absence of techniques for enhancing and controlling the long-range inter-soliton forces. Here we report that long-range soliton interactions originating from optoacoustic effects and dispersive-wave radiations can be precisely tailored in a fibre laser cavity, enabling self-assembly of large numbers of optical solitons into highly-ordered supramolecular structures. We demonstrate several features of such optical structures, highlighting their potential applications in optical information storage and ultrafast laser-field manipulation. Optical solitons have been studied in a variety of systems for their unique properties. Here, the authors report on optically observed solitonic supramolecules, made up of large-scale structures of many solitons interacting within a fiber cavity, and study their fundamental characteristics.

/pdf/formation-of-optical-supramolecular-structures-in-a-fibre-3fcmlvqw39.pdf

Formation of optical supramolecular structures in a fibre laser by tailoring long-range soliton interactions

Plasmonic resonances in metallic nanoparticles have been used since antiquity to colour glasses. The use of metal nanostructures for surface colourization has attracted considerable interest following recent developments in plasmonics. However, current top-down colourization methods are not ideally suited to large-scale industrial applications. Here we use a bottom-up approach where picosecond laser pulses can produce a full palette of non-iridescent colours on silver, gold, copper and aluminium. We demonstrate the process on silver coins weighing up to 5 kg and bearing large topographic variations (∼1.5 cm). We find that colours are related to a single parameter, the total accumulated fluence, making the process suitable for high-throughput industrial applications. Statistical image analyses of laser-irradiated surfaces reveal various nanoparticle size distributions. Large-scale finite-difference time-domain computations based on these nanoparticle distributions reproduce trends seen in reflectance measurements, and demonstrate the key role of plasmonic resonances in colour formation. The use of metal nanostructures for surface colourization has attracted considerable interest following recent developments in plasmonics. Here, Guayet al. use a bottom-up approach where picosecond laser pulses can produce a full palette of non-iridescent colours on silver, gold, copper, and aluminium.

Laser-induced plasmonic colours on metals.

Structural coloring is production of color by surfaces that have microstructure fine enough to interfere with visible light; this phenomenon provides a novel paradigm for color printing. Plasmonic color is an emergent property of the interaction between light and metallic surfaces. This phenomenon can surpass the diffraction limit and achieve near unlimited lifetime. We categorize plasmonic color filters according to their designs (hole, rod, metal–insulator–metal, grating), and also describe structures supported by Mie resonance. We discuss the principles, and the merits and demerits of each color filter. We also discuss a new concept of color filters with tunability and reconfigurability, which enable printing of structural color to yield dynamic coloring at will. Approaches for dynamic coloring are classified as liquid crystal, chemical transition and mechanical deformation. At the end of review, we highlight a scale-up of fabrication methods, including nanoimprinting, self-assembly and laser-induced process that may enable real-world application of structural coloring.

/pdf/plasmonic-and-dielectric-based-structural-coloring-from-3p0w43rw8n.pdf

Plasmonic- and dielectric-based structural coloring: from fundamentals to practical applications.

The use of femtosecond laser pulses allows precise and thermal-damage-free removal of material (ablation) with wide-ranging scientific, medical and industrial applications. However, its potential is limited by the low speeds at which material can be removed and the complexity of the associated laser technology. The complexity of the laser design arises from the need to overcome the high pulse energy threshold for efficient ablation. However, the use of more powerful lasers to increase the ablation rate results in unwanted effects such as shielding, saturation and collateral damage from heat accumulation at higher laser powers. Here we circumvent this limitation by exploiting ablation cooling, in analogy to a technique routinely used in aerospace engineering. We apply ultrafast successions (bursts) of laser pulses to ablate the target material before the residual heat deposited by previous pulses diffuses away from the processing region. Proof-of-principle experiments on various substrates demonstrate that extremely high repetition rates, which make ablation cooling possible, reduce the laser pulse energies needed for ablation and increase the efficiency of the removal process by an order of magnitude over previously used laser parameters. We also demonstrate the removal of brain tissue at two cubic millimetres per minute and dentine at three cubic millimetres per minute without any thermal damage to the bulk.

/pdf/ablation-cooled-material-removal-with-ultrafast-bursts-of-wexy1sgkib.pdf

Ablation-cooled material removal with ultrafast bursts of pulses

3.5-GHz intra-burst repetition rate ultrafast Yb-doped fiber laser

We report a novel ultrafast burst mode fiber laser system and results on ablation of rat brain tissue at rates approaching an order of magnitude improvement over previous reports, with no discernible thermal damage.

/pdf/high-speed-thermal-damage-free-ablation-of-brain-tissue-with-34ar8brcfj.pdf

High-speed, thermal damage-free ablation of brain tissue with femtosecond pulse bursts

There are a number of applications that would avail a pulse pattern in the form of closely grouped and uniformly spaced pulses, i.e., bursts. Closely grouped pulses with pulse to pulse separation in the order of a few nanoseconds have a potential for increasing material removal rates and thereby reducing the thermal effects. Besides, keeping the burst repetition period in the order of thermal relaxation time has the advantage of keeping the overall average power at lower levels in order to prevent the cumulative heating of the material.

/pdf/non-thermal-material-and-tissue-processing-with-100-mhz-and-54dlnw46l2.pdf

Non-thermal material and tissue processing with 100 MHz and 500 MHz repetition rate bursts

Femtosecond pulses hold great promise for high-precision tissue removal. However, ablation rates are severely limited by the need to keep average laser power low to avoid collateral damage due to heat accumulation. Furthermore, previously reported pulse energies preclude delivery in flexible fibers, hindering in vivo operation. Both of these problems can be addressed through use of groups of high-repetition-rate pulses, or bursts. Here, we report a novel fiber laser and demonstrate ultrafast burst-mode ablation of brain tissue at rates approaching 1 mm$^3$/min, an order of magnitude improvement over previous reports. Burst mode operation is shown to be superior in terms of energy required and avoidance of thermal effects, compared to uniform repetition rates. These results can pave the way to in vivo operation at medically relevant speeds, delivered via flexible fibers to surgically hard-to-reach targets, or with simultaneous magnetic resonance imaging.

Can Kerse

Papers

Ablation-cooled material removal with ultrafast bursts of pulses

3.5-GHz intra-burst repetition rate ultrafast Yb-doped fiber laser

High-speed, thermal damage-free ablation of brain tissue with femtosecond pulse bursts

Non-thermal material and tissue processing with 100 MHz and 500 MHz repetition rate bursts

Efficient, high-speed ablation of soft tissue with few-microjoule, femtosecond pulse bursts