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.

To achieve high energy and power density simultaneously in miniaturized electronic devices, a zinc-ion micro-supercapacitor (ZmSC) is constructed for the first time by integrating a battery-type zinc micro-anode and a capacitor-type carbon nanotube micro-cathode. In the meantime, an electroplating method is developed to in situ replenish the zinc anode when needed without destroying the configuration of the ZmSC, in which the micro-cathode, micro-anode and electrolyte of the ZmSC function as the working electrode, counter electrode and plating solution in the plating process, respectively. This strategy effectively avoids the irreversible consumption of the zinc anode and the fading of the capacitance and cycle life. As a result, the prepared ZmSC exhibits an excellent electrochemical performance, including a high area capacitance of 83.2 mF cm⁻² at 1 mA cm⁻², a high energy density of 29.6 μW h cm⁻² and a high power density of 8 mW cm⁻². After 6000 cycles, the ZmSC shows about 87.4% retention (60.9 mF cm⁻²) of its initial area capacitance at 5 mA cm⁻². Furthermore, a higher capacitance (76 mF cm⁻²) and a longer cycling life are obtained after re-plating the zinc anode. This method features a simple configuration and easy operation, and holds great promise for use in other long cycle life zinc-based microdevices.

Zero-dimensional MoS₂ quantum dots (QDs) possess distinct physical and chemical properties, which have garnered them considerable attention and facilitates their use in a broad range of applications. In this study, we prepared monolayer MoS₂ QDs using temporally shaped femtosecond laser ablation of bulk MoS₂ targets in water. The morphology, crystal structures, chemical, and optical properties of the MoS₂ QDs were characterized by transmission electron microscopy, X-ray diffraction, Raman spectroscopy, X-ray photoelectron spectroscopy, UV–vis absorption spectra, and photoluminescence spectra. The analysis results show that highly pure, uniform, and monolayer MoS₂ QDs can be successfully prepared. Moreover, by temporally shaping a conventional single pulse into a two-subpulse train, the production rate of MoS₂ nanomaterials (including nanosheets, nanoparticles, and QDs) and the ratio of small size MoS₂ QDs can be substantially improved. The underlying mechanism is a combination of multilevel photoexfoliation of monolayer MoS₂ and water photoionization–enhanced light absorption. The as-prepared MoS₂ QDs exhibit excellent electrocatalytic activity for hydrogen evolution reactions because of the abundant active edge sites, high specific surface area, and excellent electrical conductivity. Thus, this study provides a simple and green alternative strategy for the preparation of monolayer QDs of transition metal dichalcogenides or other layered materials.

Microdevice integrating energy storage with wireless charging could create opportunities for electronics design, such as moveable charging. Herein, we report seamlessly integrated wireless charging micro-supercapacitors by taking advantage of a designed highly consistent material system that both wireless coils and electrodes are of the graphite paper. The transferring power efficiency of the wireless charging is 52.8%. Benefitting from unique circuit structure, the intact device displays low resistance and excellent voltage tolerability with a capacitance of 454.1 mF cm⁻², superior to state-of-the-art conventional planar micro-supercapacitors. Besides, a record high energy density of 463.1 μWh cm⁻² exceeds the existing metal ion hybrid micro-supercapacitors and even commercial thin film battery (350 μWh cm⁻²). After charging for 6 min, the integrated device reaches up to a power output of 45.9 mW, which can drive an electrical toy car immediately. This work brings an insight for contactless micro-electronics and flexible micro-robotics.

A high-temperature sensor based on a Mach–Zehnder interferometer (MZI) in a conventional single-mode optical fiber is proposed and fabricated by concatenating two microcavities separated by a middle section. A femtosecond laser is used to fabricate a microhole on the center of a fiber end. Then a micro-air-cavity is formed by splicing the microholed fiber end with a normal fiber end. The interferometer is applied for high-temperature sensing, in the range of $500–1200°\mathrm{C}$, with a sensitivity of $109\mathrm{pm}/°\mathrm{C}$ that, to the best of our knowledge, is highest in silica fiber temperature sensors. Also, the interferometer is insensitive to external refractive index (RI), which is desirable for temperature sensors.