Ye Fan, Ayub Ahsan, Karimi Reza, Wettig Shawn, Sanderson Joseph, Musselman Kevin P
Department of Mechanical and Mechatronics Engineering, University of Waterloo, 200 University Ave. West, Waterloo, ON, N2L 3G1, Canada.
Waterloo Institute for Nanotechnology, University of Waterloo, 200 University Ave. West, Waterloo, ON, N2L 3G1, Canada.
Adv Mater. 2023 Jul;35(30):e2301129. doi: 10.1002/adma.202301129. Epub 2023 Jun 7.
MoSe 2H/1T hybrid nanoparticles are prepared by femtosecond laser ablation of MoSe powder in isopropyl alcohol with different laser powers and ablation times, and their formation mechanisms and photothermal conversion efficiencies (PTCEs) are studied. Two types of spherical nanoparticles are observed. The first type is onion-structured nanoparticles that are formed by nucleation on the surfaces of melted droplets followed by inward growth of {002} planes of MoSe . The second type is polycrystalline nanoparticles, formed by coalescence of crystalline nanoclusters fragmented from the powder during the laser ablation. The nanoparticle size in all samples shows a bimodal distribution, corresponding to different fragmentation mechanisms. The 2H-to-1T phase transition in the nanoparticles is likely caused by electron doping from the laser-induced plasma. The PTCEs of the nanoparticles increase with laser power and ablation time; the highest PTCE is around 38%. After examining the bandgaps and the Urbach energies of the nanoparticles, it is found that the high PTCEs are primarily attributed to defects and structural disorder in the laser-synthesized nanoparticles, which allow absorption of photons with energies smaller than the bandgap energy and facilitate non-radiative recombination of photoexcited carriers.
通过飞秒激光在异丙醇中以不同激光功率和烧蚀时间烧蚀MoSe粉末制备了MoSe 2H/1T混合纳米颗粒,并研究了它们的形成机制和光热转换效率(PTCE)。观察到两种类型的球形纳米颗粒。第一种是洋葱结构的纳米颗粒,它是由在熔滴表面成核,随后MoSe的{002}面内生长而形成的。第二种是多晶纳米颗粒,它是由激光烧蚀过程中从粉末破碎的结晶纳米团簇聚结形成的。所有样品中的纳米颗粒尺寸呈现双峰分布,对应于不同的破碎机制。纳米颗粒中的2H到1T相变可能是由激光诱导等离子体的电子掺杂引起的。纳米颗粒的PTCE随着激光功率和烧蚀时间的增加而增加;最高PTCE约为38%。在研究了纳米颗粒的带隙和乌尔巴赫能量后,发现高PTCE主要归因于激光合成纳米颗粒中的缺陷和结构无序,这使得能够吸收能量小于带隙能量的光子,并促进光激发载流子的非辐射复合。