Abstract Bond relaxation from one equilibrium to another under perturbation matters uniquely the performance of a substance and thus it has enormous impact to materials science and engineering. However, the basic rules for the perturbation-bond-property correlation and efficient probing strategies for high-resolution detection stay yet great challenge. This treatise features recent progress in this regard with focus on the multifield bond oscillation notion and the theory-enabled phonon spectrometrics. From the perspective of Fourier transformation and the Taylor series of the potentials, we correlate the phonon spectral signatures directly to the transition of the characteristic bonds in terms of stiffness (frequency shift), number fraction (integral of the differential spectral peak), structure fluctuation (linewidth), and the macroscopic properties of the substance. A systematic examination of the spectral feature evolution for group IV, III-V, II-VI crystals, layered graphene nanoribbons, black phosphor, (W, Mo)(S2, Se2) flakes, typical nanocrystals, and liquid water and aqueous solutions under perturbation has enabled the ever-unexpected information on the perturbation-bond-property regulations. Consistency between predictions and measurements of the crystal size-resolved phonon frequency shift clarifies that atomic dimer oscillation dictates the vibration modes showing blueshift while the collective vibration of oscillators formed between a certain atom and its nearest neighbors governs the modes of redshift when the sample size is reduced. Theoretical matching to the phonon frequency shift due to atomic undercoordination, mechanical and thermal activation, and aqueous charge injection by solvation has been realized. The reproduction of experimental measurements has turned out quantitative information of bond length, bond energy, single bond force constant, binding energy density, vibration mode activation energy, Debye temperature, elastic modulus, and the number and stiffness transition of bonds from the mode of references to the conditioned upon perturbation. Findings prove not only the essentiality of the multifield lattice oscillating dynamics but also the immense power of the phonon spectrometrics in revealing the bond-phonon-property correlation of solid and liquid substance.

中文翻译：

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结构晶体和水相液体键合能量和性质的多场介导

摘要 扰动下从一个平衡到另一个平衡的键弛豫对物质的性能具有独特的影响，因此它对材料科学和工程具有巨大的影响。然而，微扰-键-性质相关的基本规则和高分辨率检测的有效探测策略仍然存在巨大挑战。本论文重点介绍了这方面的最新进展，重点是多场键振荡概念和支持理论的声子光谱学。从傅里叶变换和势的泰勒级数的角度来看，我们将声子光谱特征直接与刚度（频移）、数分数（微分谱峰的积分）、结构波动方面的特征键的转变相关联（行宽），以及物质的宏观性质。对 IV、III-V、II-VI 族晶体、层状石墨烯纳米带、黑色磷光体、(W、Mo)(S2、Se2) 薄片、典型纳米晶体以及液态水和水溶液的光谱特征演变进行系统检查扰动使有关扰动债券财产法规的信息变得出乎意料。晶体尺寸分辨声子频移的预测和测量之间的一致性阐明了原子二聚体振荡决定了显示蓝移的振动模式，而当样本大小为减少。由于原子配位不足，机械和热激活，与声子频移的理论匹配，并且实现了溶剂化的水性电荷注入。实验测量的再现已经从参考模式得到了键长、键能、单键力常数、结合能密度、振动模式活化能、德拜温度、弹性模量以及键的数量和刚度转变的定量信息到条件扰动。研究结果不仅证明了多场晶格振荡动力学的重要性，而且证明了声子光谱学在揭示固体和液体物质的键 - 声子 - 性质相关性方面的巨大力量。结合能密度、振动模式激活能、德拜温度、弹性模量，以及从参考模式到扰动条件的键的数量和刚度转变。研究结果不仅证明了多场晶格振荡动力学的重要性，而且证明了声子光谱学在揭示固体和液体物质的键 - 声子 - 性质相关性方面的巨大力量。结合能密度、振动模式激活能、德拜温度、弹性模量，以及从参考模式到扰动条件的键的数量和刚度转变。研究结果不仅证明了多场晶格振荡动力学的重要性，而且证明了声子光谱学在揭示固体和液体物质的键 - 声子 - 性质相关性方面的巨大力量。