Department Physik, Universität Siegen, Walter-Flex-Str. 3, 57072, Siegen, Germany.
Deutsches Elektronen-Synchrotron DESY, Notkestr. 85, 22607, Hamburg, Germany.
Sci Rep. 2023 Jul 8;13(1):11048. doi: 10.1038/s41598-023-38059-z.
We use X-ray photon correlation spectroscopy to investigate how structure and dynamics of egg white protein gels are affected by X-ray dose and dose rate. We find that both, changes in structure and beam-induced dynamics, depend on the viscoelastic properties of the gels with soft gels prepared at low temperatures being more sensitive to beam-induced effects. Soft gels can be fluidized by X-ray doses of a few kGy with a crossover from stress relaxation dynamics (Kohlrausch-Williams-Watts exponents [Formula: see text] to 2) to typical dynamical heterogeneous behavior ([Formula: see text]1) while the high temperature egg white gels are radiation-stable up to doses of 15 kGy with [Formula: see text]. For all gel samples we observe a crossover from equilibrium dynamics to beam induced motion upon increasing X-ray fluence and determine the resulting fluence threshold values [Formula: see text]. Surprisingly small threshold values of [Formula: see text] s[Formula: see text] nm[Formula: see text] can drive the dynamics in the soft gels while for stronger gels this threshold is increased to [Formula: see text] s[Formula: see text] nm[Formula: see text]. We explain our observations with the viscoelastic properties of the materials and can connect the threshold dose for structural beam damage with the dynamic properties of beam-induced motion. Our results suggest that soft viscoelastic materials can display pronounced X-ray driven motion even for low X-ray fluences. This induced motion is not detectable by static scattering as it appears at dose values well below the static damage threshold. We show that intrinsic sample dynamics can be separated from X-ray driven motion by measuring the fluence dependence of the dynamical properties.
我们使用 X 射线光子相关光谱来研究卵清蛋白凝胶的结构和动力学如何受到 X 射线剂量和剂量率的影响。我们发现,结构和束致动力学的变化都取决于凝胶的粘弹性性质,低温下制备的软凝胶对束致效应更为敏感。软凝胶可以通过几 kGy 的 X 射线剂量流化,从应力松弛动力学(Kohlrausch-Williams-Watts 指数 [公式:见文本] 变为 2)到典型的动态多相行为 [公式:见文本] 1),而高温卵清蛋白凝胶在 15 kGy 剂量下具有辐射稳定性,[公式:见文本]。对于所有凝胶样品,我们观察到从平衡动力学到增加 X 射线通量时的束致运动的转变,并确定了由此产生的通量阈值[公式:见文本]。令人惊讶的是,软凝胶中可以驱动动力学的小阈值值[公式:见文本] s[公式:见文本] nm[公式:见文本],而对于更强的凝胶,该阈值增加到[公式:见文本] s[公式:见文本] nm[公式:见文本]。我们用材料的粘弹性性质来解释我们的观察结果,并可以将结构束损伤的阈值剂量与束致运动的动态性质联系起来。我们的结果表明,即使在低 X 射线通量下,软粘弹性材料也可以显示出明显的 X 射线驱动的运动。这种诱导的运动不能通过静态散射来检测,因为它出现在低于静态损伤阈值的剂量值下。我们通过测量动态特性的通量依赖性来证明可以将固有样品动力学与 X 射线驱动的运动分离。