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首页> 外文期刊>The Journal of Chemical Physics >Role of exchange and correlation in high-harmonic generation spectra of H-2, N-2, and CO2: Real-time time-dependent electronic-structure approaches
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Role of exchange and correlation in high-harmonic generation spectra of H-2, N-2, and CO2: Real-time time-dependent electronic-structure approaches

机译：H-2，N-2和CO2的高谐波生成光谱中的交换和相关性的作用：实时依赖的电子结构方法

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This study arises from the attempt to answer the following question: how different descriptions of electronic exchange and correlation affect the high-harmonic generation (HHG) spectroscopy of H-2, N-2, and CO2 molecules? We compare HHG spectra for H-2, N-2, and CO2 with different ab initio electronic structure methods: real-time time-dependent configuration interaction and real-time time-dependent density functional theory (RT-TDDFT) using truncated basis sets composed of correlated wave functions expanded on Gaussian basis sets. In the framework of RT-TDDFT, we employ Perdew-Burke-Ernzerhof (PBE) and long-range corrected Perdew-Burke-Ernzerhof (LC-omega PBE) functionals. We study HHG spectroscopy by disentangling the effect of electronic exchange and correlation. We first analyze the electronic exchange alone, and in the case of RT-TDDFT with LC-omega PBE, we use omega = 0.3 and omega = 0.4 to tune the percentage of long-range Hartree-Fock exchange and short-range exchange PBE. Then, we added the correlation as described by the PBE functional. All the methods give very similar HHG spectra, and they seem not to be particularly sensitive to the different description of exchange and correlation or to the correct asymptotic behavior of the Coulomb potential. Despite this general trend, some differences are found in the region connecting the cutoff and the background. Here, the harmonics can be resolved with different accuracy depending on the theoretical schemes used. We believe that the investigation of the molecular continuum and its coupling with strong fields merits further theoretical investigations in the near future.
机译：本研究试图回答以下问题：对电子交换和关联的不同描述如何影响H-2、N-2和CO2分子的高次谐波产生（HHG）光谱？我们用不同的从头算电子结构方法比较了H-2、N-2和CO2的HHG光谱：实时含时组态相互作用和实时含时密度泛函理论（RT-TDDFT），使用截断基集（由在高斯基集上展开的相关波函数组成）。在RT-TDDFT框架下，我们采用了Perdew-Burke-Ernzerhof（PBE）和长程修正的Perdew-Burke-Ernzerhof（LC-omega-PBE）泛函。我们通过解开电子交换和关联的影响来研究HHG光谱。我们首先单独分析电子交换，在RT-TDDFT和LC omega PBE的情况下，我们使用omega=0.3和omega=0.4来调整长程Hartree-Fock交换和短程交换PBE的百分比。然后，我们添加了PBE函数描述的相关性。所有的方法都给出了非常相似的HHG谱，它们似乎对交换和关联的不同描述或库仑势的正确渐近行为并不特别敏感。尽管有这种总体趋势，但在连接截止点和背景的区域中发现了一些差异。在这里，根据所使用的理论方案，可以以不同的精度解析谐波。我们相信，在不久的将来，分子连续体及其与强场耦合的研究值得进一步的理论研究。

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