We demonstrate a new method for populating line-by-line spectroscopic databases with beyond-Voigt line-shape parameters, which is based on ab initio quantum scattering calculations. We report a comprehensive dataset for the benchmark system of He-perturbed H${}_2$ (we cover all the rovibrational bands that are present in the HITRAN spectroscopic database). We generate the entire dataset of the line-shape parameters (broadening and shift, their speed dependence, and the complex Dicke parameter) from fully ab initio quantum-scattering calculations. We extend the previous calculations by taking into account the centrifugal distortion for all the bands and by including the hot bands. The results are projected on a simple structure of the quadratic speed-dependent hard-collision profile. We report a simple and compact formula that allows the speed-dependence parameters to be calculated directly from the generalized spectroscopic cross sections. For each line and each line-shape parameter, we provide a full temperature dependence within the double-power-law (DPL) representation, which makes the dataset compatible with the HITRAN database. The temperature dependences cover the range from 20 to 1000 K, which includes the low temperatures relevant for the studies of the atmospheres of giant planets. The final outcome from our dataset is validated on highly accurate experimental spectra collected with cavity ring-down spectrometers. The methodology can be applied to many other molecular species important for atmospheric and planetary studies.

我们演示了一种基于从头算量子散射计算的，具有超出Voit线形参数的逐行光谱数据库填充的新方法。我们报告了He扰动H基准系统的综合数据集${}_2$（我们涵盖了HITRAN光谱数据库中存在的所有振动带）。我们从头开始生成线形参数（扩展和平移，它们的速度依赖性以及复杂的Dicke参数）的整个数据集量子散射计算。我们通过考虑所有频段的离心失真并包括热频段来扩展先前的计算。将结果投影到一个与速度相关的二次硬碰撞轮廓的简单结构上。我们报告了一个简单而紧凑的公式，该公式允许直接从广义光谱截面中计算速度相关参数。对于每条线和每条线形参数，我们在双幂律（DPL）表示中提供了完全的温度依赖性，这使数据集与HITRAN数据库兼容。温度依赖性范围从20到1000 K，其中包括与研究巨型行星大气有关的低温。我们的数据集的最终结果在使用腔衰荡光谱仪收集的高精度实验光谱上得到了验证。该方法可以应用于对大气和行星研究重要的许多其他分子物种。