Enhanced Energy Absorption and Electron Excitation in Crystalline Silicon Induced by Two-Color Intense Femtosecond Laser Pulses

M. Tani, Kakeru Sasaki, Yasushi Shinohara, Kenichi L. Ishikawa
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Abstract

Over the past decades, the interaction between femtosecond intense lasers and semiconductors or dielectrics has been attracting significant attention as for high harmonic generation [1], high-quality laser micromachining without the thermal damage [2]. Several experimental and theoretical studies have reported that the use of two-color laser pulses enables highly efficient laser ablation of transparent materials compared to a single-color pump pulse [3], [4]. In the present work, to elucidate how two-color femtosecond laser pulses deposit energy to electrons in semiconductors and dielectrics, we utilize the time-dependent density functional theory (TDDFT) and examine the energy absorption of crystalline silicon under overlapped two-color [ultraviolet (UV) and infrared (IR)] intense femtosecond laser pulses as a function of relative intensity with the total fluence conserved. The deposited energy is dramatically enhanced by two-color laser field and maximized when they are equally mixed [see Fig. 1(a)]. The interplay between intraband electron motion in the valence band (before excitation) driven by the IR component and resonant valence-to-conduction interband excitation (carrier injection) induced by the UV component is identified as the underlying mechanism. Interestingly, the former plays an influential role, increases the excited electrons [see Fig. 1(b)]. The effect of multiple multiphoton absorption paths, relative phase of carrier waves, or intraband motion of the created carriers in the conduction band play a minor role.
双色强飞秒激光脉冲诱导晶体硅增强能量吸收和电子激发
在过去的几十年里,飞秒强激光与半导体或电介质之间的相互作用已经引起了人们的极大关注,如高谐波产生[1],无热损伤的高质量激光微加工[2]。一些实验和理论研究报道,与单色泵浦脉冲相比,使用双色激光脉冲可以高效地对透明材料进行激光烧蚀[3],[4]。在本工作中,为了阐明双色飞秒激光脉冲如何将能量沉积到半导体和电介质中的电子中,我们利用时间依赖密度泛函理论(TDDFT),并研究了在重叠的双色[紫外(UV)和红外(IR)]强飞秒激光脉冲下晶体硅的能量吸收作为相对强度的函数,并且总通量守恒。双色激光场显著增强了沉积能量,当两者均匀混合时,沉积能量达到最大[见图1(a)]。红外成分驱动的价带(激发前)带内电子运动与紫外成分诱导的价导共振带间激发(载流子注入)之间的相互作用被确定为潜在的机制。有趣的是,前者起着重要的作用,增加了激发电子[见图1(b)]。多个多光子吸收路径、载波的相对相位或在导带中产生的载流子的带内运动的影响较小。
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