纳秒脉冲激光诱导的水中双空泡振荡研究 下载: 973次
Focused laser-induced cavitation in liquid is crucial in numerous applications, e.g., targeted cell lysis, microfluidic operations (such as switching, pumping, and mixing), and perforation of cell membranes. Depending on the focusing conditions and laser pulse energy, single or multiple bubble formations may occur, which may be accompanied by bubble coalescence, high-speed jet formation, ring vortex generation, and multiple shock wave emission. Owing to its promising application prospect on microsurgery, micropumping, and tissue cutting, laser-induced multiple bubbles and their interactions have been studied extensively. It has been confirmed that the dynamics of multiple bubbles are strongly related to the relative bubble positions as well as the time and size difference between bubbles. For example, by adjusting these parameters, the strength and direction of the emerging liquid jets can be controlled. Shock wave and rebound bubbles generated after cavitation bubble collapse are susceptible to their asymmetrical collapse. Without a doubt, the mutual interaction of bubbles causes the asymmetrical oscillation process of bubbles. However, to the best of our knowledge, the influence of multiple bubble interactions on shock wave emission and rebound bubble process has not been studied yet. Therefore, in this study, two bubbles with similar sizes were generated using a single nanosecond laser pulse to investigate the influence of relative interval on multiple bubble dynamics, especially on collapse shock wave emission and rebound bubble generation.
A frequency-doubled Q-switched Nd∶YAG laser was introduced to generate optical breakdown in water. The laser pulse was split into two parts using a variable beam splitter. Then, the split laser pulses were focused on water from different directions to generate bubble pairs. Three methods were introduced to measure the bubble pair dynamics: high-speed shadowgraph, optical scattering technique, and acoustic detection technique. It was easy to generate bubble pairs with variable relative interval by adjusting the incidence direction of laser pulses, focusing objective position, and pulse energy. First, the bubble pair dynamics with different relative intervals were discussed experimentally and compared with the Rayleigh-Plesset model. Second, the influences of the relative interval between bubble pairs on the collapse shock wave strength and rebound bubble oscillation period were investigated. In this part, a high-speed camera was replaced by an EMCCD to picture the plasmas generated during an optical breakdown, and the bubble size was calculated by its first oscillation period.
For a single bubble in free liquid, the maximum radius of the bubble linearly increases with the cube root of the pulse energy and its first oscillation period, respectively, (Fig. 3), which means that the bubble size can be calculated from the pulse energy or its first oscillation period. The oscillation process of bubble pairs is significantly influenced by its relative interval (γ) (Fig. 4). For γ=1.36, the bubble pairs oscillates spherically, without contacting each other before their first collapse, but both of their first oscillation periods significantly increases [Figs. 4(a) and (b)]. For γ≈0.49, the two bubbles begin to coalesce during the early stage of expansion, and their shapes deform. The evolution of the equivalent radius of the coalesced bubble fits well with the Rayleigh-Plesset simulation [Figs. 4(c) and (d)]. For γ≈0.18, the coalesced bubble oscillates spherically again during its first period [Figs. 4(e) and (f)], which is similar to the single bubble case. Then, we experimentally examine the influence of relative interval of bubble pairs on the collapse shock wave emission and rebound bubble generation. The results revealed that the first oscillation period was uninfluenced by the relative interval (γ<0.75) (Table 1). However, with the increase in relative interval, the collapse shock wave strength first reduced, then increased, and then reduced again; however, an opposite trend was observed in the rebound bubble oscillation period (Fig. 6), which meant that the relative interval affected the energy distribution between shock wave and rebound bubble. Owing to the multiple shock wave formation induced by the asymmetric collapse of the coalesced bubble, the evolution of shock wave strength and rebound bubble oscillation over relative interval were not synchronous.
In this study, we investigate the dynamics of laser-induced bubble pairs with variable relative interval. The bubble pair oscillation process significantly varies with relative interval. For a noncoalesced bubble pair, the oscillation is nearly spherically during the first period, but both of their oscillation processes are prolonged. For a coalesced bubble pair, the smaller the relative interval, the more spherical the bubble shape during its first period. The first oscillation period is longer than that of every single bubble and unaffected by the relative interval when it is less than 0.75. Besides, the evolution of coalesced bubble could still be described by Rayleigh-Plesset model. However, the relative interval of bubble pairs significantly influences the collapse shock wave emission and rebound bubble generation after the collapse of the coalesced bubble. The findings of this study are expected to facilitate the applications of laser-induced bubbles in microfluidic operations, such as rapid mixing and cell sorting.
1 引言
当液体介质的局部区域中由能量沉积引起的温度或者压强改变超过一定阈值时,会产生空化现象(cavitation)。空化气泡(以下简称“空泡”)是其中最显著的一个物理过程,其振荡会引起周围液体的流动、压强的改变,以及坍塌时伴随着冲击波的激发等。空泡的振荡过程很容易受到周围环境因素的影响,温度[1]和压强[2]的改变,外源性声场[3-5]、壁[6-7]的存在,以及多空泡相互作用[8-9]等都会引起空泡的非对称振荡并伴随着新的物理现象的产生。特别是多空泡同时形成时,其振荡过程会相互影响并导致空泡形状和振荡周期发生改变,并出现高速射流和涡环现象,以及空泡发生相互融合、靠近、偏离甚至分裂。这虽然增加了空泡演变过程的复杂性,但同时也拓展了光致空化的应用范围,例如,高速射流具有更小的尺寸且具有更强的穿刺性,在细胞膜微手术、显微切割等方面有良好的应用前景;空泡的非对称振荡所引起的周围液体介质的流动不再是径向流,可用于提高微流控芯片中的快速融合效率等。因此,多空泡之间的相互作用及其振荡过程受到广泛关注。
诱导空泡的形成通常是利用脉冲激光[8,10-15]、电火花[9,16]、压力脉冲[17-18]、水下爆炸[19]等来实现,其中利用脉冲激光诱导空泡形成具有非接触、精准度高及可控性强等优点,已在纳米材料制备[20]、细胞穿孔[21]等方面得到广泛应用。人们从20世纪70年代就开始关注双空泡的相互作用及其振荡过程。Mitchell等[22]利用高速相机拍摄了两个电火花空泡的相互作用及其动态过程。Lauterborn等[23-24]利用脉冲激光诱导反相的两个空泡来研究射流和涡环等现象和形成机制。在此基础上,Tomita等[12]利用脉冲激光研究空泡相对大小和相对位置的改变对空泡振荡行为的影响。Chew等[25]利用电火花的方式来产生两个不同大小的空泡,研究空泡大小、相位对射流的影响。Fong等[16]则对两个相似尺寸空泡在不同相对位置情况下的振荡过程包括不同方向射流、空泡弹弓效应、空泡融合过程展开研究。南京理工大学的韩冰[26]对双空泡相互作用以及非对称溃灭的力学特性进行了系统研究。当空泡附近存在壁或者空气面时,双空泡的振荡行为更加复杂[27-30]。此外,人们也对更多空泡相互作用下的振荡行为进行了研究,例如当具有相同能量的多个同时形成的空泡排成一列时,靠外的空泡会先坍塌,且在坍塌时形成指向中间空泡的射流[31]。Bremond等[17]利用超声的负向压在水中产生多个空泡,发现在边缘位置的空泡尽管尺寸最大,但是整个空泡群呈现由外向内逐渐坍塌的方式。Lim等[13]利用空间光调制技术来形成多点击穿,利用多空泡的相互融合来形成具有不同形状的融合空泡。Fu等[11]利用单脉冲激光来诱导间隔很小的多点击穿,并探究多点击穿对融合空泡重建过程以及坍塌冲击波的影响。随着计算机技术的发展,更多的数值计算方法被用于仿真多空泡振荡所引起的空泡内部变化、周围液体流场分布,以及压强变化[8,30,32-34]。Li等[35-36]研究了双空泡的融合过程,并对融合过程进行了理论推导和拟合。
上述研究表明,多空泡相互作用下的振荡过程与空泡数量、相对位置、空泡大小以及空泡间的相位差都有密切关系,例如,对于两个大小相同且同时形成的空泡,在距离比较远时,会在坍塌时形成指向对方的射流[22,32]。随着相对位置的靠近,即使在未接触的情况下,两个空泡会在膨胀过程中相互挤压;进一步减小空泡间隔时会出现融合现象[9,35]。而对于两个尺寸不相同的空泡,在距离较远时,小的空泡坍塌时会形成一束指向大空泡的高速射流[30]。随着间隔的减小,小空泡坍塌形成的射流可以刺穿大空泡并明显改变大空泡的振荡过程,如坍塌时形成反向射流[28]。当两个空泡的尺寸差异进一步增大时,小的空泡在坍塌时会被撕裂,形成两束指向相反的射流[21]。两个相同尺寸的空泡的形成时刻不同所造成的相位差异也会诱导射流的形成,当相差π/2个相位时,所形成的空泡在膨胀过程会形成指向另一个空泡的射流,而自身坍塌时也会形成反向射流,且射流特性与相位差密切相关。因此,通过控制空泡的相对大小、位置和相位,可以形成强弱、方向及尺寸可控的射流[8]。这种利用空泡相互作用形成的射流已经被成功地用于改变细胞膜的通透性,实现外源性物质的导入[37]。目前,多空泡相互作用下振荡行为的主要影响因素以及射流的控制方面已经受到广泛关注,但鲜有关于多空泡相互作用下融合空泡的演变过程以及其坍塌时冲击波的激发等方面的研究,而这些对于多空泡振荡在生物医学领域的应用是至关重要的。
本文搭建了光致击穿实验平台,利用单激光脉冲分束聚焦在水中形成具有相似尺寸的双空泡,并针对不同间隔下的空泡融合过程进行研究。结果表明,发生融合的双空泡振荡过程依旧可用Rayleigh-Plesset模型[38-39]来描述,空泡间相对距离的变化不会对融合空泡的振荡周期产生明显影响,但会影响重建空泡的振荡周期和坍塌冲击波的强度。
2 实验装置和检测方法
击穿空泡的检测分为三个模块:散射光检测模块、成像模块和声学检测模块。散射光检测模块是通过检测空泡振荡所引起的探测光强度变化来间接检测空泡振荡过程,能得到精确的空泡脉冲振荡周期。散射光检测模块使用一个波长为632 nm、功率为2 mW的He-Ne激光器(Thorlabs,HNL020LB)作为散射光探测光源。输出的激光经过一个二向色镜(Thorlabs,DMLP567R)与脉冲光合束后,聚焦到样品池内。利用一个高速的光电探测器(FEMTO, 带宽为25 kHz~200 MHz)来检测探测光的强度变化。为避免脉冲激光的影响,在探测器前端增加一个限波片(Thorlabs,NF533-17)和一个滤波片(Thorlabs,FB630-10)。成像模块由样品池侧面的一个超高速摄像机(Photron, Fastcam SA-Z)以及在相机前端的4倍成像物镜组成,用于直接对空化气泡成像。将输出波长为660 nm的半导体激光器(Coherent,OBIS660)作为成像光源。在样品池上方放置一个声学探头(Olympus, V324-N-SU)组成声学监测模块,用于探测光致击穿过程产生的冲击波信号。此外,采用多通道的示波器(Rohde & Schwarz, PTE1204)记录声学探头和光电探测器的信号。通过一台脉冲延时/发生器(Stanford Research Systems Inc., DG645)来实现脉冲激光器、高速成像仪及示波器之间的时序控制。
通过声学信号探测可精确地获得空泡第一振荡周期,但重建空泡的尺寸小且振荡呈非对称性,导致空泡坍塌时形成的冲击波很弱,这限制了通过声学信号测量重建空泡及后续空泡脉动振荡周期的能力。此外,壁对冲击波的反射也会进一步增加利用声学方法监测空泡重建过程的难度。散射光检测方法具有更高的灵敏度,可检测百纳米量级的空泡振荡过程,能避免声学检测方法所受的干扰,且能对空泡附近液体温度的变化进行检测。因此,散射光检测方法和声学检测方法的结合,能相互补充和配合,更全面地检测光致空化过程。
3 空泡振荡理论模型
早在20世纪初,人们就对水中的空泡振荡过程进行研究,当时为了解决船只推进器被空泡腐蚀的问题,Rayleigh通过Navier-Stokes方程首先提出了用于描述空泡演变过程的动力学模型,即Rayleigh模型[38]。该模型将空泡振荡置于无限、均匀及不可压缩的流体环境中,且不考虑表面张力以及黏滞力对振荡过程的影响。Plesset在考虑表面张力和液体黏性的基础上,对该模型进行了修正,得到了Rayleigh-Plesset模型[39-40],即R-P模型。其具体描述为
值得注意的是,空泡振荡过程中表面张力
4 结果分析与讨论
4.1 单空泡的振荡
首先,利用脉冲激光在水中诱导形成单点击穿。将两束激光固定在同一光轴上,调整可调分束器上半波片的偏振方向,使得分束的两束激光能量相近,以使产生的空泡具有相似的尺寸。调整完成后,分束器保持不动,阻挡其中一路激光,只保留光强较强的一路光,以形成单点击穿。受到聚焦条件和光束质量的影响,聚焦脉冲激光诱导光致击穿所形成的等离子体并不是严格的球形,而是呈现细长的椭球形或者倒三角锥形,这在之前的研究[11,42-44]中被多次提及,但源自高温等离子体的空泡在膨胀过程中会迅速变成球形空泡。
图 2. 单空泡的检测结果(EL=468 μJ, Rmax=321.2 μm, Tosc1=61.2 μs)。(a)高速摄像机所拍摄的空泡动态演变图,帧间隔为3.33 μs;(b)空泡半径随时间的演变及与R-P模型的比较;(c)散射光信号图;(d)远场声学信号图
Fig. 2. Multimodality measurement of laser-induced single bubble in free liquid under EL=468 μJ, Rmax=321.2 μm, and Tosc1 =61.2 μs. (a) Photographs of bubble dynamics with an inter-frame interval of 3.33 μs obtained by high-speed camera; (b) time evolution of bubble radius and comparation with R-P simulations; (c) light scattering signal of cavitation bubble collected by photodetector; (d) far-field acoustic signal measured by a piezoelectric transducer
对于脉冲激光诱导的水中光致击穿,空泡的能量与脉冲激光能量之间通常呈线性相关[43],这意味着空泡的最大半径与脉冲能量的三分之一次方线性相关。此外,对于微米级以上尺寸的空泡,其受到表面张力和黏滞力的影响较小,空泡最大半径与第一振荡周期也呈线性相关。本实验结果也进一步证实了这一点,如
图 3. 自由场中空泡最大半径与脉冲能量、第一振荡周期之间的关系。(a)最大半径与脉冲能量的三分之一次方的关系;(b)最大半径与第一振荡周期的关系
Fig. 3. Bubble maximum radius related to pulse energy and the first oscillation period in free field. (a) Maximum radius as a function of the cube root of pulse energy; (b) maximum radius as a function of the first oscillation period
4.2 不同间隔下的双空泡振荡行为
本节引入一个无量纲的参数——相对间隔γ来描述空泡间的相对间隔,其定义为两个击穿点的间隔与两个空泡最大半径之和的比值,即
随着相对间隔的减小,空泡间的相互作用增强,并开始出现空泡融合现象。
当相对间隔进一步减小时,空泡的融合时间点进一步提前,整个融合空泡的振荡过程的不对称性减弱,与单空泡的振荡过程不再有明显的差异。
4.3 相对间隔对坍塌冲击波和重建空泡的影响
空泡的每次坍塌通常都伴随着坍塌冲击波的形成,且空泡的绝大部分能量是通过坍塌冲击波的形式耗散出去,剩下的一部分能量被重建空泡继承进行后续的脉动过程。在自由场中,空泡坍塌形成的冲击波强度会比光致击穿形成的冲击波强度略高,且都与空泡最大半径呈线性关系[45-46]。但是,受到壁、外源性声场及多点击穿等的影响,空泡振荡呈现非对称性,并在坍塌时会形成多个冲击波,从而降低冲击波的峰值强度[7,11,47-48]。而空泡间的相互作用会显著增强空泡的非对称振荡特性,因此坍塌冲击波的强度会受到影响。本节主要分析空泡相对间隔对坍塌冲击波强度和重建空泡的影响。
在接下来的实验中,对原来的系统进行了部分改变,即利用一台EMCCD来替代高速成像仪,用于对两点击穿的等离子体进行成像。由于等离子体自身的发光强度较大,因此不需要额外的成像光源。同时,为了避免同轴时两个聚焦点距离减小所导致的光场相互作用加强对击穿空泡的影响,调整其中一束光的位置,使其聚焦点在另一个焦点的下方。进一步调整可调分束器,实现两束光能量均分。随后在具有不同的击穿间隔情况下,记录两点击穿时的空泡振荡周期,重建空泡振荡周期以及坍塌冲击波远场强度的变化,并根据
图 5. 不同击穿间隔下的两点击穿等离子体图像
Fig. 5. Plasma image of two-point breakdown with variable intervals
4.3.5 相对间隔对融合空泡第一振荡周期的影响
由4.2节可知,空泡的相互作用会导致空泡振荡周期延长。随着相对间隔的增大,在相同能量下形成的空泡融合时间点会滞后。这种由相对间隔改变引起的滞后是否会导致融合空泡的振荡周期发生改变?目前还不清楚。因此,本小节研究了击穿间隔的增加对融合空泡振荡周期的影响。在保持脉冲能量不变的情况下,在不同间隔处,首先挡住右边脉冲,测量左边脉冲单独产生光致击穿时的空泡振荡周期;然后挡住左边脉冲,测量右边脉冲单独产生光致击穿时的空泡振荡周期;最后测量两个脉冲同时产生光致击穿时融合空泡的第一振荡周期。考虑到纳秒脉冲激光的不稳定性,在每个间隔点测量200个脉冲,只记录脉冲能量在95%到105%能量节点间的数据作为有效数据。
表 1. 脉冲能量为450 μJ时,空泡相对间隔对融合空泡振荡周期的影响
Table 1. Influenced of relative interval on the first oscillation period of coalesced bubble with pulse energy of 450 μJ
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4.3.6 相对间隔对坍塌冲击波和重建空泡振荡的影响
接下来分析相对间隔对坍塌冲击波和重建空泡振荡周期Tosc2的影响,并统计了这两者随击穿间隔的变化,结果如
图 6. 相对间隔对坍塌冲击波峰值强度和重建空泡振荡周期的影响。(a)坍塌冲击波峰值强度随相对间隔的变化;(b)重建空泡振荡周期随相对间隔的变化
Fig. 6. Influence of relative interval on relative magnitude of collapse shock wave and rebound bubble period of coalesced bubble. (a) Relative magnitude of collapse shock wave as a function of relative interval; (b) rebound bubble oscillation period as a function of relative interval
由于双空泡的相互作用会引起空泡的非对称振荡,特别是对于发生融合现象的空泡,其非对称振荡的现象更加明显。这种空泡的非对称振荡会形成多个坍塌冲击波,进而降低其峰值强度。之前的研究[11]表明多点击穿的产生会导致更多的空泡能量转移到重建空泡中,从而进一步降低坍塌冲击波的强度。本实验则进一步证实了空泡间相互作用对坍塌冲击波和重建空泡的影响,且这种影响与相对间隔密切相关。在空泡坍塌时大部分能量以冲击波的形式耗散,另一部分能量则被转移到重建空泡中。空泡相对间隔的改变会影响空泡相互作用的程度,进而改变空泡能量在坍塌时的转移比例。当转移到坍塌冲击波的空泡能量减小时,意味着转移到重建空泡中的能量增加,这也解释了为何重建空泡的振荡周期变化趋势与坍塌冲击波强度的变化趋势相反。从
5 结论
利用单脉冲激光诱导形成位置、大小可控的两点击穿,引入高速摄像机、散射光检测和声学检测等方式来研究具有相似大小的双空泡振荡行为。实验结果表明,具有相似尺寸的融合双空泡的振荡行为与相对间隔密切相关。相对间隔的增加能显著增强融合空泡振荡的非对称性,但融合空泡的第一振荡周期不受相对间隔的影响,且整体振荡行为依旧可用R-P模型来描述。相对间隔的改变对于坍塌冲击波的形成和重建空泡的振荡影响非常大,随着相对间隔的增大,坍塌冲击波强度呈现先减小、再增大、又减小的趋势,而重建空泡振荡周期的变化趋势则相反。
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Article Outline
付磊, 王萍, 王斯佳, 辛静, 张璐薇, 张镇西, 王晶, 姚翠萍. 纳秒脉冲激光诱导的水中双空泡振荡研究[J]. 中国激光, 2022, 49(4): 0407001. Lei Fu, Ping Wang, Sijia Wang, Jing Xin, Luwei Zhang, Zhenxi Zhang, Jing Wang, Cuiping Yao. Dynamics of Bubble Pairs in Water Induced by Focused Nanosecond Laser Pulse[J]. Chinese Journal of Lasers, 2022, 49(4): 0407001.