金纳米粒子飞秒激发产生的纳米级热梯度中 DNA 变性的机理理解,ACS Applied Materials & Interfaces

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金纳米粒子飞秒激发产生的纳米级热梯度中 DNA 变性的机理理解
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2022-01-04 , DOI: 10.1021/acsami.1c19411
David A Hastman _{1,

2} , Parth Chaturvedi ₃ , Eunkeu Oh ₄ , Joseph S Melinger ₅ , Igor L Medintz ₁ , Lela Vuković ₃ , Sebastián A Díaz ₁

Affiliation

人们对开发能够通过局部温度调制精确控制生物分子的结构和功能的光热系统产生了浓厚的兴趣。一种具体应用是通过金纳米粒子 (AuNP) 的飞秒 (fs) 激光脉冲光学加热使双链 (ds) DNA 变性；然而，这些系统中 DNA 熔解的机制尚不完全清楚。在这里，我们使用具有表面束缚 dsDNA 的 55 nm AuNPs，使用 fs 激光脉冲局部加热以诱导 DNA 熔化。通过改变 dsDNA 与 AuNP 表面的距离和激光脉冲能量注量，该系统用于研究纳秒持续时间的温度增加和 AuNP 周围的陡峭温度梯度如何影响 dsDNA 去杂交。通过将 dsDNA 和 AuNP 表面之间的距离修改 3。²，去杂交率范围为每脉冲 0.002 至 0.05 个 DNA，并且仅在 100 秒的照射时间内，释放到溶液中的 DNA 总量控制在 26-93% 的范围内。通过将 dsDNA 位置移动小至 ∼1.1 nm，平均 dsDNA 去杂交率可改变高达 30 ± 2%，从而对 DNA 熔解和释放提供高水平的控制。通过将 dsDNA 周围的理论温度与实验得出的温度进行比较，我们发现当 dsDNA 更接近 AuNP 表面以及使用较低的激光脉冲能量密度时，最大或峰值温度对去杂化率的影响更大。此外，模拟金纳米粒子周围的光热热脉冲的分子动力学模拟提供了对去杂化的随机性质的机械洞察，并证明了与稳态加热相比，激光脉冲加热期间金纳米粒子表面附近的碱基对分离增加。了解生物材料如何对金纳米粒子的飞秒激光脉冲光学加热所固有的短寿命和非均匀温度升高作出反应，对于提高该技术的功能和精度至关重要，以便将其实施到更复杂的生物系统中。

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Mechanistic Understanding of DNA Denaturation in Nanoscale Thermal Gradients Created by Femtosecond Excitation of Gold Nanoparticles

There is significant interest in developing photothermal systems that can precisely control the structure and function of biomolecules through local temperature modulation. One specific application is the denaturation of double-stranded (ds) DNA through femtosecond (fs) laser pulse optical heating of gold nanoparticles (AuNPs); however, the mechanism of DNA melting in these systems is not fully understood. Here, we utilize 55 nm AuNPs with surface-tethered dsDNA, which are locally heated using fs laser pulses to induce DNA melting. By varying the dsDNA distance from the AuNP surface and the laser pulse energy fluence, this system is used to study how the nanosecond duration temperature increase and the steep temperature gradient around the AuNP affect dsDNA dehybridization. Through modifying the distance between the dsDNA and AuNP surface by 3.8 nm in total and the pulse energy fluence from 7.1 to 14.1 J/m², the dehybridization rates ranged from 0.002 to 0.05 DNA per pulse, and the total amount of DNA released into solution was controlled over a range of 26–93% in only 100 s of irradiation. By shifting the dsDNA position as little as ∼1.1 nm, the average dsDNA dehybridization rate is altered up to 30 ± 2%, providing a high level of control over DNA melting and release. By comparing the theoretical temperature around the dsDNA to the experimentally derived temperature, we find that maximum or peak temperatures have a greater influence on the dehybridization rate when the dsDNA is closer to the AuNP surface and when lower laser pulse fluences are used. Furthermore, molecular dynamics simulations mimicking the photothermal heat pulse around a AuNP provide mechanistic insight into the stochastic nature of dehybridization and demonstrate increased base pair separation near the AuNP surface during laser pulse heating when compared to steady-state heating. Understanding how biological materials respond to the short-lived and non-uniform temperature increases innate to fs laser pulse optical heating of AuNPs is critical to improving the functionality and precision of this technique so that it may be implemented into more complex biological systems.

更新日期：2022-01-19

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