Huels Michael A, Boudaïffa Badia, Cloutier Pierre, Hunting Darel, Sanche Leon
Canadian Institutes of Health Research Group in Radiation Sciences, Department of Nuclear Medicine and Radiobiology, Faculty of Medicine, University of Sherbrooke, Québec, Canada J1H 5N4.
J Am Chem Soc. 2003 Apr 16;125(15):4467-77. doi: 10.1021/ja029527x.
Nonthermal secondary electrons with initial kinetic energies below 100 eV are an abundant transient species created in irradiated cells and thermalize within picoseconds through successive multiple energy loss events. Here we show that below 15 eV such low-energy electrons induce single (SSB) and double (DSB) strand breaks in plasmid DNA exclusively via formation and decay of molecular resonances involving DNA components (base, sugar, hydration water, etc.). Furthermore, the strand break quantum yields (per incident electron) due to resonances occur with intensities similar to those that appear between 25 and 100 eV electron energy, where nonresonant mechanisms related to excitation/ionizations/dissociations are shown to dominate the yields, although with some contribution from multiple scattering electron energy loss events. We also present the first measurements of the electron energy dependence of multiple double strand breaks (MDSB) induced in DNA by electrons with energies below 100 eV. Unlike the SSB and DSB yields, which remain relatively constant above 25 eV, the MDSB yields show a strong monotonic increase above 30 eV, however with intensities at least 1 order of magnitude smaller than the combined SSB and DSB yields. The observation of MDSB above 30 eV is attributed to strand break clusters (nano-tracks) involving multiple successive interactions of one single electron at sites that are distant in primary sequence along the DNA double strand, but are in close contact; such regions exist in supercoiled DNA (as well as cellular DNA) where the double helix crosses itself or is in close proximity to another part of the same DNA molecule.
初始动能低于100电子伏特的非热二次电子是受辐照细胞中产生的大量瞬态粒子,通过连续的多次能量损失事件在皮秒内热化。我们在此表明,在15电子伏特以下,这种低能电子仅通过涉及DNA成分(碱基、糖、水化水等)的分子共振的形成和衰减,在质粒DNA中诱导单链(SSB)和双链(DSB)断裂。此外,由于共振导致的链断裂量子产率(每入射电子)出现的强度与25至100电子伏特电子能量之间出现的强度相似,在该能量范围内,与激发/电离/解离相关的非共振机制被证明主导了产率,尽管多次散射电子能量损失事件也有一定贡献。我们还首次测量了能量低于100电子伏特的电子在DNA中诱导的多个双链断裂(MDSB)的电子能量依赖性。与25电子伏特以上相对保持恒定的SSB和DSB产率不同,MDSB产率在30电子伏特以上呈现强烈的单调增加,然而其强度至少比SSB和DSB产率之和小1个数量级。在30电子伏特以上观察到的MDSB归因于链断裂簇(纳米径迹),其涉及单个电子在沿着DNA双链一级序列上距离较远但紧密接触的位点的多次连续相互作用;这种区域存在于超螺旋DNA(以及细胞DNA)中,其中双螺旋自身交叉或与同一DNA分子的另一部分紧密相邻。