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摘要:
消费电子市场正推动柔性电子器件向集成化、小型化及可穿戴的方向发展，同时也对柔性电子器件的制备提出了新的要求。光刻工艺加工精度高，但其成本昂贵、加工流程复杂且效率低。相比而言，飞秒激光加工兼有加工精度高和工艺流程简单的特点，已展现在制备柔性电子器件方面的独特优势和应用前景。为了更好地了解这一新兴领域的进展，本文概述了与柔性电子器件制备相关的五种飞秒激光加工工艺机理，包括激光液相纳米材料合成、激光纳米材料还原、激光诱导纳米连接、激光电极图案化及激光表面织构化，并介绍了制备的典型柔性电子器件性能，对存在的问题和未来发展趋势进行了分析和展望。
Abstract:Consumer electronical markets are now promoting a rapid advance in flexible electronics with high integration, miniaturization, and wearable properties, which in turn puts forward new requirements for the fabrication of flexible electronics. Photolithography techniques are advantageous for their high accuracy, but it is disadvantageous due to high cost, complexity, and low efficiency. In comparison, femtosecond (fs) laser micro-nano fabrication, as a high-efficiency and simple technique, has shown its capacity and potential for the fabrication of flexible electronics. This review summarizes five fs-laser based techniques for the fabrication of flexible electronics, including laser synthesis of nanomaterials in liquids, laser-induced nanomaterial chemical-reduction, laser-induced nano joining, laser electrode patterning, and laser surface texturing. The corresponding mechanisms are briefly introduced, followed by a demonstration of typical flexible electronics and their properties. Finally, the challenges in this field are analyzed, and our perspective is provided.
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Key words:
- femtosecond laser /
- micro-nano fabrication /
- flexible electronics /
- nanojoining /
- nanomaterial synthesis
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Overview: With the rapid development of information technology and the rise of consumer electronics, flexible electronic devices with high integration, miniaturization and lightweight have attracted wide research attentions. Such flexible electronic devices are typically composed of functional parts, conductive structures, and flexible substrates. The functional parts can respond to external stimuli and convert them into electrical signals. The conductive structures are used for electrical signal transmission and the flexible substrates are used to support functional and conductive structures. The preparation of flexible electronic devices requires nanomaterial synthesis, sintering, processing, and patterning, which is an intrinsically interdisciplinary subject that integrates material science, electronics science, and engineering science.
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图 2 (a) 飞秒激光烧蚀合成氧化锌量子点制备光电探测器示意图; (b) 深紫外光下光电探测器的瞬时光电流产生; (c) 光电探测器的响应值随器件弯曲角度、次数变化关系，插图为光电探测器弯曲角度的照片[72]
Figure 2. (a) Schematic illustration of femtosecond laser ablation synthesis with ZnO QDs to fabricate photodetectors; (b) Transient photocurrent generation under deep-ultraviolet illumination for photodetector; (c) Responsivity measurement of photodetector as a function of the number of bending cycles. The inset photos show the photodetector bending degree[72]
图 3 (a) 飞秒激光还原离子态铜盐前驱体制备铜微电极流程图；(b), (c) 不同激光功率下制备铜微电极的SEM图和XRD图；(d) 铜微电极方阻随激光功率变化曲线，插图：铜微电极所制备LED电路照片[39]
Figure 3. (a) Manufacturing process of femtosecond laser reduction based on Cu ionic precursor; (b), (c) SEM images and XRD pattern of Cu microelectrode prepared with different laser powers; (d) Copper microelectrode sheet resistance change curve with laser power, inset: photograph of the LED circuit prepared from Cu microelectrode[39]
图 4 (a) 飞秒激光制备还原氧化石墨烯/PDMS复合材料声学传感器制造工艺流程[85]；(b) 水分子与GO纳米片之间相互作用示意图[86]；(c) 模拟人类皮肤的非接触式湿度传感的电子皮肤原型演示[86]
Figure 4. (a) Manufacturing process of femtosecond laser writing rGO/PDMS composite acoustic sensor[85]; (b) Schematic illustration of the interaction between water molecules and GO nanosheets[86]; (c) Prototype demonstration of e-skin used for simulation of noncontact sensing properties of human skin[86]
图 5 (a) 利用空间形状的飞秒激光制备LIG/MnO2超级电容器的示意图; (b) 飞秒激光诱导形成LIG/MnO2复合材料机理图; (c) 不同形状超级电容器在不同电流密度下的面积比电容; (d) 叉指超级电容器在不同测试扫描速率下的面积比电容及体积比电容[87]
Figure 5. (a) Schematics of spatially shaped femtosecond laser strategy to fabricate the graphene/MnO2 micro-supercapacitors; (b) Schematic diagram of the formation of LIG/MnO2 composites induced by femtosecond laser; (c) The area-specific capacitance of different geometries under different current density; (d) The areal capacitance and volumetric capacitance of interdigital micro-supercapacitors under different scan rates[87]
图 6 (a) 飞秒激光直写石墨烯柔性热敏电阻制备方法[89]；(b) 飞秒激光碳化制备微型超级电容器流程图及照片，不同弯曲程度的微超级电容器的循环伏安(CV)曲线(扫描速度为1 V/s)[90]；(c) 飞秒激光微加工法制备传感器阵列原理图[91]；(d) 传感器阵列同时检测不同物体的温度及压力[91]；(e) 受温度变化影响的温度传感器的电信号输出[91]；(f) 受负载压力变化影响的压力传感器的电信号输出[91]
Figure 6. (a) Schematic diagram of femtosecond laser direct writing graphene flexible thermistor[89]; (b) Schematic diagram of fabrication of micro-supercapacitors by femtosecond laser carbonization and photographic image of micro-supercapacitor, cyclic voltammetry (CV) curves of micro-supercapacitors with different bending degrees ( the scanning speed is 1 V/s)[90]; (c) Schematic diagram of sensor array fabricated by femtosecond laser micromachining method[91]; (d) Sensor array simultaneously detects the temperature and pressure of different objects[91]; (e) Electrical signal output of the temperature sensor affected by temperature changes[91]; (f) Electrical signal output of the pressure sensor affected by load pressure changes[91]
图 7 (a) 960 mW飞秒激光辐照下Cu纳米颗粒二聚体的相对电场增强(|E/E0|)分布[39]; (b) 960 mW飞秒激光辐照下 Cu纳米颗粒二聚体在5 ps后的温度场分布[39]; (c) 不同功率单脉冲激光下，前5 ps内Cu颗粒电子及晶格温度随时间变化关系[39]; (d), (e) 飞秒激光辐照前后Ag NWs薄膜的方阻变化及透射光谱变化[98]; (f) 飞秒激光辐照Ag NW连接接头及不同部位的SAED图案[98]
Figure 7. (a) Relative electric field enhancement |E/E0| distribution of the Cu nanoparticle dimer under 960 mW laser irradiation[39]; (b) Temperature field distribution of a Cu nanoparticle dimer under 960 mW single pulse laser irradiation after 5 ps[39]; (c) Relationship between electron and lattice temperature of Cu nanoparticles in the first 5 ps under different laser powers of single pulse laser irradiation[39]; (d), (e) Sheet resistances and transmittance spectra of Ag NWs films before and after femtosecond laser irradiation[98]; (f) SAED patterns of Ag NW joints and different parts irradiated by femtosecond laser[98]
图 9 (a) 飞秒激光一步刻蚀制备双面微型超级电容器工艺流程图；(b) 12螺旋形单元间不同连接方式组成的“花瓣”图案超级电容器的照片[105]
Figure 9. (a) Schematic of fabrication of double sided micro-supercapacitors by one-step femtosecond laser etching; (b) Photographs of double-side micro-supercapacitors and different connections of twelve spiral units in ‘flower petal’ pattern[105]
图 10 飞秒激光烧蚀的Cu微/纳锥结构及PDMS微碗状结构制备的TENG的制造工艺流程图[108]；(b) 飞秒激光辐照制备PDMS摩擦层的示意图，29 mW和132 mW激光功率下制备的PDMS的SEM图像[27]；0～132 mW激光功率范围下制备的TENGs的(c) 开路电压及(d) 短路电流[27]
Figure 10. Schematic of the fabrication process of TENG prepared by femtosecond laser ablation of Cu micro/nano-cones and PDMS micro-bowl[108]; (b) Schematic illustration of the fabrication of the PDMS by femtosecond laser irradiation and SEM images of the PDMS at laser power of 29 mW and 132 mW[27]; (c) open-circuit voltage (d) short-circuit current of the fabricated TENGs with laser power ranging from 0 to 132 mW[27]
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