Because of their unique physicochemical integration mode, energetic host–guest solvates provide a balanced method to expand CL-20 high explosives. CL-20/hydrogen peroxide (H₂O₂) energetic solvates maintain their detonation performance by combining H₂O₂ molecules into a lattice akin to hydrate CL-20/H₂O solvate (α-CL-20). Herein, using periodic density functional theory (DFT) calculation and molecular dynamics simulation, the structural evolution and intermolecular interaction mechanism of orthorhombic CL-20/H₂O₂ (o-CL-20/H₂O₂), monoclinic CL-20/H₂O₂ (m-CL-20/H₂O₂) and CL-20/H₂O solvates were monitored by the vibrational spectrum and vibrational density of states (VDOS) in the THz region when the temperature was increased from 298 K to 558 K. There was greater similarity in the vibrational characteristics of THz spectra for o-CL-20/H₂O₂ and CL-20/H₂O solvates that was supported by the thermal expansion anisotropy of lattice parameters and that of difference for the m-CL-20/H₂O₂ solvate. With increased temperature, spectral signals in the power spectrum of VDOS reflected the conformational evolution of CL-20 molecules in o-CL-20/H₂O₂ solvate and structural insensitivity of m-CL-20/H₂O₂ solvate. THz peaks of CL-20/H₂O revealed the weakening of intermolecular interactions of CL-20 and H₂O molecules, which were in agreement with the fact that H₂O molecules more easily escape from host–guest solvates, whereas the H₂O₂ molecule was restricted in a cage of CL-20 molecules for the m-CL-20/H₂O₂ solvate. RDF and hydrogen bond (H-bond) interaction analyses were performed to further clarify stronger intermolecular H-bond interactions in the o-CL-20/H₂O₂ solvate as compared to that of the other two combined with H₂O₂ or H₂O solvates. This finding introduces new insights into clarifying the formation mechanism of hydroxide with CL-20-based energetic host–guest solvates.

中文翻译：

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根据太赫兹光谱的感知，基于 CL-20 的高能主客体溶剂化物在分解温度下的结构演化

由于其独特的物理化学整合模式，高能主客体溶剂化物提供了一种平衡的方法来膨胀CL-20高能炸药。 CL-20/过氧化氢 (H ₂ O _{2 ) 高能溶剂化物通过将 H 2} O ₂分子结合成类似于水合 CL-20/H ₂ O 溶剂化物 (α-CL-20) 的晶格来保持其爆炸性能。本文利用周期密度泛函理论（DFT）计算和分子动力学模拟，研究了斜方晶系CL-20/H ₂ O ₂（o-CL-20/H ₂ O ₂）、单斜晶系CL-20的结构演化和分子间相互作用机制。_当温度从_​​_​​_​​_​​ 298 K 至 558 K。 o-CL-20/H ₂ O ₂和 CL-20/H ₂ O 溶剂化物的太赫兹光谱振动特征具有更大的相似性，这得到了晶格参数的热膨胀各向异性的支持，并且m-CL-20/H ₂ O ₂溶剂化物的差异。随着温度升高，VDOS功率谱中的光谱信号反映了o-CL-20/H ₂ O ₂溶剂化物中CL-20分子的构象演化和m-CL-20/H ₂ O ₂溶剂化物的结构不敏感性。 CL-20/H ₂ O的太赫兹峰揭示了CL-20和H ₂ O分子间相互作用的减弱，这与H ₂ O分子更容易从主客体溶剂化物中逃逸的事实相一致，而H ₂ O _{2分子被限制在m-CL-20/H 2} O ₂溶剂化物的CL-20分子笼中。进行 RDF 和氢键 (H-bond) 相互作用分析，以进一步阐明 o-CL-20/H ₂ O ₂溶剂化物中的分子间氢键相互作用比其他两种与 H 2 O 2或H ₂ O ₂组合的溶剂化物更强。 H ₂ O溶剂化物。这一发现为阐明基于 CL-20 的高能主客体溶剂化物形成氢氧化物的机制提供了新的见解。