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gamma radiation induced self-assembly of fluorescent molecules into nanofibers: a stimuli-responsive sensing

机译:γ辐射诱导荧光分子自组装成纳米纤维:刺激响应感应

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Low dose detection of gamma radiation remains critical for radiology therapy and nuclear security. We report herein on a novel dual-band fluorescence sensor system based on a molecule, 4-(1H-phenanthro[9,10-d]-imidazol-2-yl)-N,N-diphenylaniline (PI-DPA), which can be dissolved into halogenated solvents to enable expedient detection of gamma radiation. The limit of detection was projected down to 0.006 Gy. Exposure to gamma radiation decomposes CHCl3 into small radicals, which then combine to produce HCl. Strong interaction of HCl with the imidazole group of PI-DPA converts it into a PI-DPA-HCl adduct, which self-assembles into nanofibers, quenching the fluorescence of the pristine PI-DPA molecule, while producing new fluorescent emission at longer wavelength. Such dual-band emission response provides improved sensing reliability compared to single band response. Systematic investigations based on acid titration, H-1 NMR spectral measurements and time-course SEM imaging suggest that the observed new fluorescence band is due to pi-pi stacking of the PI-DPA-HCl adduct, which is facilitated by the formation of hydrogen bonded cluster units. The nanofibers exhibited high and reversible photoconductivity. Combining with the sensitive fluorescence response, the photoconductive nanofibers will enable development of a multimode stimuli-responsive sensor system that is suited for small, low cost dosimetry of gamma radiation with improved sensitivity and detection reliability.
机译:低剂量γ射线检测对于放射治疗和核安全仍然至关重要。我们在此报告基于分子4-(1H-菲[9,10-d]-咪唑-2-基)-N,N-二苯基苯胺(PI-DPA)的新型双频荧光传感器系统,该系统可以溶解在卤化溶剂中,以方便地检测伽玛射线。检出限预计降至0.006 Gy。暴露于伽玛射线会分解CHCl3为小自由基,然后结合生成HCl。 HCl与PI-DPA的咪唑基团的强相互作用将其转化为PI-DPA-HCl加合物,该加合物可自组装成纳米纤维,从而淬灭了原始PI-DPA分子的荧光,同时在更长的波长处产生了新的荧光发射。与单频带响应相比,这种双频带发射响应提供了改进的感测可靠性。基于酸滴定,H-1 NMR光谱测量和时程SEM成像的系统研究表明,观察到的新荧光带归因于PI-DPA-HCl加合物的pi-pi堆积,这通过氢的形成得以促进绑定集群单元。纳米纤维表现出高且可逆的光电导性。与敏感的荧光响应相结合,光电导纳米纤维将使多模刺激响应传感器系统的开发成为可能,该传感器系统适用于伽马辐射的小型,低成本剂量测定,并具有更高的灵敏度和检测可靠性。

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