Real-time monitoring of plasmon induced dissociative electron transfer to the potential DNA radiosensitizer 8-bromoadenine.
Real-time monitoring of plasmon induced dissociative electron transfer to the potential DNA radiosensitizer 8-bromoadenine.
复制标题
实时监测等离激元诱导的解离电子转移至潜在的 DNA 放射增敏剂 8-溴腺嘌呤
作者：
R. Schürmann;I. Bald
在贵金属纳米颗粒（NP）中局部表面等离子体激元的激发导致不同的纳米尺度效应，例如电场增强、热电子的产生和NP表面附近的温度升高。这些效应通常在不同的领域中被利用，例如表面增强拉曼散射（Sers）、NP催化和光热疗法（PTT）。卤代核碱基由于其对二次电子的高反应性而被用作常规放射癌症治疗中的放射增敏剂。在这里，我们使用表面增强拉曼光谱（Sers）的研究转化为腺嘌呤的Au和银纳米粒子的表面上的8-溴腺嘌呤（8BrA）照射后，在532，633和785 nm，分别与低功率连续波激光。8BrA的解离归因于热电子转移反应，并仔细探索了潜在的动力学。反应在几秒钟甚至几毫秒内进行。类似的解离反应也可能发生与其他亲电分子，这必须考虑在各自的Sers光谱的解释。此外，我们建议，热电子转移诱导解离的放射增敏剂，如8BrA可以在未来应用于PTT，以增强照射后的肿瘤组织的损伤。
The excitation of localized surface plasmons in noble metal nanoparticles (NPs) results in different nanoscale effects such as electric field enhancement, the generation of hot electrons and a temperature increase close to the NP surface. These effects are typically exploited in diverse fields such as surface-enhanced Raman scattering (SERS), NP catalysis and photothermal therapy (PTT). Halogenated nucleobases are applied as radiosensitizers in conventional radiation cancer therapy due to their high reactivity towards secondary electrons. Here, we use SERS to study the transformation of 8-bromoadenine (8BrA) into adenine on the surface of Au and AgNPs upon irradiation with a low-power continuous wave laser at 532, 633 and 785 nm, respectively. The dissociation of 8BrA is ascribed to a hot-electron transfer reaction and the underlying kinetics are carefully explored. The reaction proceeds within seconds or even milliseconds. Similar dissociation reactions might also occur with other electrophilic molecules, which must be considered in the interpretation of respective SERS spectra. Furthermore, we suggest that hot-electron transfer induced dissociation of radiosensitizers such as 8BrA can be applied in the future in PTT to enhance the damage of tumor tissue upon irradiation.
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