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Design and Validation of a Droplet-based Microfluidic System To Study Non-Photochemical Laser-Induced Nucleation of Potassium Chloride Solutions
Crystal Growth & Design ( IF 3.2 ) Pub Date : 2023-07-19 , DOI: 10.1021/acs.cgd.3c00591 Vikram Korede 1 , Frederico Marques Penha 2 , Vincent de Munck 1 , Lotte Stam 1 , Thomas Dubbelman 1 , Nagaraj Nagalingam 1 , Maheswari Gutta 1 , PingPing Cui 3 , Daniel Irimia 1 , Antoine E D M van der Heijden 1 , Herman J M Kramer 1 , Hüseyin Burak Eral 1
Crystal Growth & Design ( IF 3.2 ) Pub Date : 2023-07-19 , DOI: 10.1021/acs.cgd.3c00591 Vikram Korede 1 , Frederico Marques Penha 2 , Vincent de Munck 1 , Lotte Stam 1 , Thomas Dubbelman 1 , Nagaraj Nagalingam 1 , Maheswari Gutta 1 , PingPing Cui 3 , Daniel Irimia 1 , Antoine E D M van der Heijden 1 , Herman J M Kramer 1 , Hüseyin Burak Eral 1
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Non-photochemical laser-induced nucleation (NPLIN) has emerged as a promising primary nucleation control technique offering spatiotemporal control over crystallization with potential for polymorph control. So far, NPLIN was mostly investigated in milliliter vials, through laborious manual counting of the crystallized vials by visual inspection. Microfluidics represents an alternative to acquiring automated and statistically reliable data. Thus we designed a droplet-based microfluidic platform capable of identifying the droplets with crystals emerging upon Nd:YAG laser irradiation using the deep learning method. In our experiments, we used supersaturated solutions of KCl in water, and the effect of laser intensity, wavelength (1064, 532, and 355 nm), solution supersaturation (S), solution filtration, and intentional doping with nanoparticles on the nucleation probability is quantified and compared to control cooling crystallization experiments. Ability of dielectric polarization and the nanoparticle heating mechanisms proposed for NPLIN to explain the acquired results is tested. Solutions with lower supersaturation (S = 1.05) exhibit significantly higher NPLIN probabilities than those in the control experiments for all laser wavelengths above a threshold intensity (50 MW/cm2). At higher supersaturation studied (S = 1.10), irradiation was already effective at lower laser intensities (10 MW/cm2). No significant wavelength effect was observed besides irradiation with 355 nm light at higher laser intensities (≥50 MW/cm2). Solution filtration and intentional doping experiments showed that nanoimpurities might play a significant role in explaining NPLIN phenomena.
中文翻译：
基于液滴的微流体系统的设计和验证，用于研究氯化钾溶液的非光化学激光诱导成核
非光化学激光诱导成核（NPLIN）已成为一种有前景的初级成核控制技术，可提供对结晶的时空控制，并具有多晶型控制的潜力。到目前为止，NPLIN 主要在毫升小瓶中进行研究，通过目视检查对结晶小瓶进行费力的手动计数。微流体技术代表了获取自动化且统计上可靠的数据的另一种选择。因此，我们设计了一个基于液滴的微流控平台，能够使用深度学习方法识别在 Nd:YAG 激光照射下出现的晶体液滴。在我们的实验中，我们使用过饱和的 KCl 水溶液，激光强度、波长（1064、532 和 355 nm）、溶液过饱和度 ( S )、溶液过滤和有意掺杂纳米粒子对成核概率的影响为量化并与控制冷却结晶实验进行比较。测试了为 NPLIN 提出的介电极化和纳米粒子加热机制解释所获得结果的能力。对于高于阈值强度 (50 MW/cm 2 ) 的所有激光波长，具有较低过饱和度 ( S = 1.05) 的解决方案表现出比对照实验中的解决方案更高的 NPLIN 概率。在研究的较高过饱和度（ S = 1.10）下，照射在较低激光强度（10 MW/cm 2 ）下已经有效。除了以较高激光强度（≥50 MW/cm 2 ）照射355 nm 光外，未观察到明显的波长效应。溶液过滤和有意掺杂实验表明纳米杂质可能在解释 NPLIN 现象中发挥重要作用。
更新日期：2023-07-19
中文翻译：
基于液滴的微流体系统的设计和验证，用于研究氯化钾溶液的非光化学激光诱导成核
非光化学激光诱导成核（NPLIN）已成为一种有前景的初级成核控制技术，可提供对结晶的时空控制，并具有多晶型控制的潜力。到目前为止，NPLIN 主要在毫升小瓶中进行研究，通过目视检查对结晶小瓶进行费力的手动计数。微流体技术代表了获取自动化且统计上可靠的数据的另一种选择。因此，我们设计了一个基于液滴的微流控平台，能够使用深度学习方法识别在 Nd:YAG 激光照射下出现的晶体液滴。在我们的实验中，我们使用过饱和的 KCl 水溶液，激光强度、波长（1064、532 和 355 nm）、溶液过饱和度 ( S )、溶液过滤和有意掺杂纳米粒子对成核概率的影响为量化并与控制冷却结晶实验进行比较。测试了为 NPLIN 提出的介电极化和纳米粒子加热机制解释所获得结果的能力。对于高于阈值强度 (50 MW/cm 2 ) 的所有激光波长，具有较低过饱和度 ( S = 1.05) 的解决方案表现出比对照实验中的解决方案更高的 NPLIN 概率。在研究的较高过饱和度（ S = 1.10）下，照射在较低激光强度（10 MW/cm 2 ）下已经有效。除了以较高激光强度（≥50 MW/cm 2 ）照射355 nm 光外，未观察到明显的波长效应。溶液过滤和有意掺杂实验表明纳米杂质可能在解释 NPLIN 现象中发挥重要作用。
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