arXivDaily arXiv每日学术速递 周一至周五更新
arXiv周末暂无论文更新,休息一下吧,周末愉快~~

通过太赫兹光谱和低温量热法探测硅酸钙水合物中的玻色子峰和中程弹性非均匀性

Boson peak and medium-range elastic heterogeneity in calcium silicate hydrate probed by terahertz spectroscopy and low-temperature calorimetry

Xiangyu Li, Ying Chen, Jipeng Luo, Ya Chen, Linhao Wang, Lidan Tian, Gan Ding, Zeyu Lu, Zhangli Hu, Biqin Dong, Yue Li, Zongjin Li

arXiv 2607.14764首次发表:更新:

AI 中文总结

研究通过太赫兹光谱和低温量热法,对不同Ca/Si比的硅酸钙水合物中玻色子峰进行表征。经校正后两种方法定位BP频率一致但强度不同,还获得相关长度和参数等。该双探针方法可用于其他无定形固体,为研究C-S-H性能提供新途径。

AI 中文摘要

玻色子峰(BP)是无序固体的一种普遍振动异常,在硬化水泥的粘结相硅酸钙水合物(C-S-H)中已被预测但未系统表征。基于初步的太赫兹调查,我们使用太赫兹时域光谱(THz-TDS)和低温量热法,对五个Ca/Si比(0.5-1.7)的BP进行了表征,这两种振动动力学探针补充了传统结构方法的静态图像。经布鲁格曼校正结晶杂质后,两种探针都将BP定位在1 THz附近;它们在频率上一致,但强度不同。太赫兹积分光谱权重和量热Cp/T3峰均随Ca/Si单调下降,而表观太赫兹峰高在Ca/Si = 1.0时最大,此时阻尼低且振子强度仍很大。这种解耦标志着硅酸盐链解聚和层间钙填充之间的结构转变。从BP我们获得了约1 nm(0.3-2 nm)的中程动力学相关长度和一个相干势弹性非均匀性参数,随着Ca/Si升高,该参数从γ = 0.98降至0.48;德拜归一化的BP频率(ν_BP/ν_D = 0.15-0.17)将C-S-H置于硅酸盐玻璃报道的范围内。因为γ控制局部结构重排的能垒分布,它提供了一个与C-S-H的固有蠕变和热传输相关的定量、成分分辨描述符,将纳米级振动动力学与混凝土的宏观耐久性联系起来。双探针玻色子峰方法可转移到其他无定形固体,包括低碳水泥的辅助胶凝材料。

英文摘要

The boson peak (BP), a universal vibrational anomaly of disordered solids, has been predicted but not systematically characterized in calcium silicate hydrate (C-S-H), the binding phase of hardened cement. Building on a preliminary terahertz survey, we characterize the BP across five Ca/Si ratios (0.5-1.7) using terahertz time-domain spectroscopy (THz-TDS) and low-temperature calorimetry, two probes of vibrational dynamics that complement the static picture of conventional structural methods. After Bruggeman correction for crystalline impurities, both probes locate the BP near 1 THz; they agree on frequency but diverge in intensity. The terahertz integrated spectral weight and the calorimetric Cp/T3 peak both fall monotonically with Ca/Si, whereas the apparent terahertz peak height is maximal at Ca/Si = 1.0, where damping is low and oscillator strength still substantial. This decoupling marks a structural crossover between silicate-chain depolymerization and interlayer calcium filling. From the BP we obtain a medium-range dynamical correlation length of order 1 nm (0.3-2 nm) and a coherent-potential elastic-heterogeneity parameter that decreases from gamma = 0.98 to 0.48 as Ca/Si rises; the Debye-normalized BP frequency (nu_BP/nu_D = 0.15-0.17) places C-S-H within the range reported for silicate glasses. Because gamma governs the distribution of energy barriers for local structural rearrangements, it provides a quantitative, composition-resolved descriptor relevant to the intrinsic creep and thermal transport of C-S-H, linking nanoscale vibrational dynamics to the macroscopic durability of concrete. The dual-probe boson-peak approach is transferable to other amorphous solids, including the supplementary cementitious materials of low-carbon cements.

论文原文

arXiv 摘要页 · PDF 原文 · HTML 原文

↑