Accurate Infrared Line Lists for 20 Isotopologues of Carbon Disulfide (CS2) at Room Temperature

First generation data product and IR line lists for Carbon Disulfide (CS2), including an isotopologue-independent ab initio PES of Carbon Disulfide refined with selected HITRAN energy levels below 7000 cm-1, an ab initio DMS fitted with CCSD(T)/aug-cc-pV(T/Q/5+d)Z dipoles computed up to 20,000 cm-1 above potential minimum and extrapolated to one-electron basis set limit, room temperature IR line lists for 20 individual isotopologues of 12/13C and 32/33/34/36S, denoted Ames-296K, and a "natural" CS2 list with intensities scaled by their terrestrial abundances. Line positions of the five most abundant isotopologues are further enhanced by more accurate energy levels in HITRAN2020 and Tashkun's global effective Hamiltonian (H_eff) model. This project is funded by NASA Grant 18-2XRP18_2-0046 through NASA/SETI Institute Co-operative Agreement 80NSSC19M0121. See https://huang.seti.org/CS2/cs2.html for data format and abundance information. Resources supporting this work were provided by the NASA High-End Computing (HEC) Program through the NASA Advanced Supercomputing (NAS) Division at Ames Research Center. The line profile parameters and room temperature simulations are supported through 80NSSC20K1596. List of Files, supplement to article " Accurate IR Line Lists for CS2 and Isotopologues at Room Temperature" Ames-1.PES.zip: Ames-0 and Ames-1 PES subroutine & coefficient files; PES.refinement.files.zip: PES refinement related files including reference energy level list and refinement output. J=0-200 energy level lists of 12C32S2 and 19 minor isotopologues, computed on the Ames-1 PES. The .zip file contains 20 compressed .tgz files. Ames-1.DMS.zip: Ames-1 DMS subroutine & coefficient files, and ab initio data; cs2.xxx.Ames-1.296K.1E-31.dat.tgz : 20 files, "xxx" is the S-C-S isotope mass unit number. These are the Ames-296K IR line lists for 12C32S2 and 19 minor isotopologues, each with 100% abundance. Computed using Ames-1 DMS and rovibrational wavefunctions for those energy levels acquired on Ames-1 PES; cs2.20iso.Ames.natural.296K.1E-31.10Kcm-1.dat.tgz: A "natural" Ames-296K IR line list for CS2, including 9,874,405 transitions from all 20 isotopologues with their 296K intensities scaled by terrestrial abundances, covering the range of 0 - 10,000 cm-1. Computed on the Ames-1 PES and DMS. cs2.222.AI-296K.ames+heff.natural.tgz: A+I.296K line list for the main isotopologue 222, with terrestrial abundance. Ames-296K intensity prediction is combined with the more accurate energy levels (and line positions) from Effective Hamiltonian model. [Note the "AI-296K" list has been renamed to "A+I.296K" list to avoid confusion in paper] cs2.iso2-20.Ames-1.natural.1E-31.dat.iso2-4_use_HITRAN2020_purified.tgz: the Ames "natural" line list for minor isotopologues #2 - #20, in which the energy levels of 224, 223 and 232 are replaced with reliable values in HITRAN2020. Therefore, the final composite line list = 6) + 7) Heff.and.HITRAN.energy.level.matches.and.line.list.update.zip: the short FORTRAN programs for energy level matches between Ames-1 PES levels and Heff model levels, and the subroutines to use Heff and HITRAN energy levels and line positions. Lists of matched Ames vs HITRAN/H_eff levels are also included. ORIGIN project file for related analysis and figures. Use Origin Viewer to open on PC and MAC, https://www.originlab.com/viewer/dl.aspx a Python program to generate line-broadening parameters for rovibrational CS2 molecule CS2 cross-section data of PNNL, HITRAN and Ames line lists. # Iso #Lines #in"natural" abundance 1 222 1,903,882 1,856,648 0.892811 2 224 3,983,009 2,159,579 0.0792103 3 223 3,745,299 1,328,631 0.0140944 4 232 1,925,377 658,645 0.100306 5 424 1,940,490 439,254 1.207E-3 6 234 4,211,645 698,654 8.151E-4 7 324 3,671,708 589,323 6.510E-4 8 226 4,155,423 558,540 3.566E-4 9 233 3,918,753 410,542 1.439E-4 10 323 1,937,950 177,064 5.142E-5 11 434 2,080,912 138,209 1.692E-5 12 426 3,852,415 223,268 1.976E-5 13 334 4,062,765 172,858 6.773E-6 14 236 4,742,198 158,941 4.630E-6 15 326 4,113,292 137,128 3.075E-6 16 333 1,988,991 50,025 6.803E-7 17 436 4,434,008 58,478 1.361E-7 18 626 1,986,823 21,692 3.572E-8 19 336 4,613,173 32,681 3.528E-8 20 636 2,194,332 4,245 4.28E-10 Line List Data Format: (CS2 is the 53rd molecule in HITRAN, we use iso# from table below, e.g., 1 - 222; 2 - 224; ...; 10 - 323; ....; 20 - 636) in the original line list files: cs2.xxx.Ames-1.296K.1E-31.dat iso wavenumber S(Ames) A21(Ames) E"(cm-1) v1v2l2v3' v1v2l2v3" JPS' #root' JPS" #root" J' J" e/f_symmetry 2 6.165375 1.492856E-30 4.851961E-12 876.91172 0 2 2 0 0 2 2 0 29 1 2 4 28 2 2 4 29 28 e e in cs2.iso2-20.Ames-1.natural.1E-31.dat.iso2-4_use_HITRAN2020_purified.v4, original Ames-1 line position and the difference = Heff - Ames are appended to the end of each line of iso #2 (224), iso #3 (223), and iso #4 (232). in cs2.222.AI-296K.ames+heff.natural.dat.v3, two integers are added to each line to keep the record for the number of cycles after which a match (or no match) was made for upper and lower levels, "0-41" for "matched", '99' for "not matched", "-1" for out of range, i.e. > 9000 cm-1. The differences between the original Ames and corrected/replaced transition wavenumber, E', and E" are also appended at the end. The relation is wv/E'/E" (Heff) + diff = wv/E'/E" (Ames). For example, in the transition below, E''(Ames) = 3445.4018+0.7865 = 3446.1883 cm-1. 1 36.666580 1.538246E-31 2.306988E-07 3445.40177 0 4 2 1 1 6 2 0 57 1 2 31 58 2 2 34 57 58 e e 3 3 -0.7207 0.0658 0.7865本数据集为二硫化碳（Carbon Disulfide, CS₂）的初代数据产品与红外谱线列表，包含经7000 cm⁻¹以下精选HITRAN（High-resolution TRANsmission molecular absorption database, HITRAN）能级修正的、与同位素体（isotopologue）无关的二硫化碳从头算（ab initio）势能面（Potential Energy Surface, PES），以及基于CCSD(T)/aug-cc-pV(T/Q/5+d)Z偶极矩拟合的从头算偶极矩面（Dipole Moment Surface, DMS）：该偶极矩在势能极小值以上20000 cm⁻¹范围内计算，并外推至单电子基组极限。数据集包含12/13C与32/33/34/36S形成的20种独立同位素体的室温红外谱线列表，命名为Ames-296K，以及一份按地球丰度缩放强度的"天然"CS₂谱线列表。 针对五种丰度最高的同位素体，其谱线位置进一步通过HITRAN2020与塔什昆（Tashkun）全局有效哈密顿量（effective Hamiltonian, H_eff）模型中的高精度能级进行了优化。 本项目由美国国家航空航天局（National Aeronautics and Space Administration, NASA）资助项目18-2XRP18_2-0046通过NASA/地外智慧生命搜寻研究所（Search for Extraterrestrial Intelligence Institute, SETI Institute）合作协议80NSSC19M0121支持。数据格式与丰度信息可访问https://huang.seti.org/CS2/cs2.html 查询。本研究的计算资源由NASA先进超级计算部（Advanced Supercomputing Division, NAS）下属埃姆斯研究中心（Ames Research Center）的NASA高端计算（High-End Computing, HEC）项目提供。谱线轮廓参数与室温振转模拟得到项目80NSSC20K1596支持。 文件列表为论文"Accurate IR Line Lists for CS2 and Isotopologues at Room Temperature"的补充材料： 1. Ames-1.PES.zip：Ames-0与Ames-1势能面子程序及系数文件 2. PES.refinement.files.zip：与势能面修正相关的文件，包含参考能级列表与修正输出结果。基于Ames-1势能面计算的12C32S2与19种次要同位素体的J=0-200能级列表，该压缩包包含20个压缩后的.tgz文件 3. Ames-1.DMS.zip：Ames-1偶极矩面子程序及系数文件，以及从头算数据 4. cs2.xxx.Ames-1.296K.1E-31.dat.tgz：共20个文件，其中"xxx"为S-C-S同位素质量编号。该数据集为12C32S2与19种次要同位素体的Ames-296K红外谱线列表，每种同位素体的丰度均按100%处理，基于Ames-1偶极矩面与Ames-1势能面得到的振转波函数（rovibrational wavefunctions）计算得到 5. cs2.20iso.Ames.natural.296K.1E-31.10Kcm-1.dat.tgz：CS₂的"天然"Ames-296K红外谱线列表，包含9874405条来自全部20种同位素体的跃迁，其296K下的强度按地球丰度缩放，覆盖0~10000 cm⁻¹的波数范围，基于Ames-1势能面与偶极矩面计算得到 6. cs2.222.AI-296K.ames+heff.natural.tgz：针对主同位素体222的A+I.296K谱线列表，按地球丰度归一化。该数据集将Ames-296K的强度预测结果与有效哈密顿量模型得到的高精度能级（及谱线位置）相结合。【注：为避免论文中产生混淆，原"AI-296K"列表已更名为"A+I.296K"列表】 7. cs2.iso2-20.Ames-1.natural.1E-31.dat.iso2-4_use_HITRAN2020_purified.tgz：针对次要同位素体#2~#20的Ames"天然"谱线列表，其中224、223与232同位素体的能级替换为HITRAN2020中的可靠数值。因此最终复合谱线列表 = 第6项 + 第7项 8. Heff.and.HITRAN.energy.level.matches.and.line.list.update.zip：用于实现Ames-1势能面能级与有效哈密顿量模型能级匹配的简短Fortran子程序，以及调用有效哈密顿量与HITRAN能级、谱线位置的子程序，同时包含Ames与HITRAN/有效哈密顿量能级的匹配列表。此外还包含用于相关分析与绘图的ORIGIN项目文件，可在PC与Mac设备上通过Origin Viewer打开，下载地址为https://www.originlab.com/viewer/dl.aspx，以及用于生成二硫化碳振转分子谱线加宽参数的Python程序。 9. 二硫化碳的太平洋西北国家实验室（Pacific Northwest National Laboratory, PNNL）、HITRAN与Ames谱线列表的截面数据 # 同位素体编号（Iso） | #跃迁线数（Lines） | 自然丰度下的线数（#in"natural" abundance） | 地球丰度比例 1 | 222 | 1903882 | 1856648 | 0.892811 2 | 224 | 3983009 | 2159579 | 0.0792103 3 | 223 | 3745299 | 1328631 | 0.0140944 4 | 232 | 1925377 | 658645 | 0.100306 5 | 424 | 1940490 | 439254 | 1.207E-3 6 | 234 | 4211645 | 698654 | 8.151E-4 7 | 324 | 3671708 | 589323 | 6.510E-4 8 | 226 | 4155423 | 558540 | 3.566E-4 9 | 233 | 3918753 | 410542 | 1.439E-4 10 | 323 | 1937950 | 177064 | 5.142E-5 11 | 434 | 2080912 | 138209 | 1.692E-5 12 | 426 | 3852415 | 223268 | 1.976E-5 13 | 334 | 4062765 | 172858 | 6.773E-6 14 | 236 | 4742198 | 158941 | 4.630E-6 15 | 326 | 4113292 | 137128 | 3.075E-6 16 | 333 | 1988991 | 50025 | 6.803E-7 17 | 436 | 4434008 | 58478 | 1.361E-7 18 | 626 | 1986823 | 21692 | 3.572E-8 19 | 336 | 4613173 | 32681 | 3.528E-8 20 | 636 | 2194332 | 4245 | 4.28E-10 谱线列表数据格式： （CS₂是HITRAN数据库中的第53个分子，本文使用下表中的同位素体编号，例如1对应222；2对应224；……；10对应323；……；20对应636） 在原始谱线列表文件cs2.xxx.Ames-1.296K.1E-31.dat中，每行数据的字段依次为： 同位素体编号 | 波数 | Ames模型谱线强度S | Ames模型自发辐射爱因斯坦系数A₂₁ | 下能级能量E''(cm⁻¹) | 上振转量子数v1v2l2v3' | 下振转量子数v1v2l2v3" | 上能级总角动量J与宇称P' | 上能级根编号#root' | 下能级总角动量J与宇称P" | 下能级根编号#root" | 上能级总角动量量子数J' | 下能级总角动量量子数J" | 宇称对称性e/f 示例行：2 6.165375 1.492856E-30 4.851961E-12 876.91172 0 2 2 0 0 2 2 0 29 1 2 4 28 2 2 4 29 28 e e 在cs2.iso2-20.Ames-1.natural.1E-31.dat.iso2-4_use_HITRAN2020_purified.v4文件中，针对同位素体#2(224)、#3(223)与#4(232)的每一行数据末尾，会追加原始Ames-1谱线位置以及差值（差值=有效哈密顿量值 - Ames值）。 在cs2.222.AI-296K.ames+heff.natural.dat.v3文件中，每一行末尾会追加两个整数，用于记录上、下能级的匹配（或不匹配）所需的循环次数："0-41"表示匹配成功，"99"表示未匹配，"-1"表示超出范围（即波数>9000 cm⁻¹）。同时还会追加原始Ames值与修正/替换后的跃迁波数、E'与E''的差值。二者的关系为：wv/E'/E"(Heff) + 差值 = wv/E'/E"(Ames)。 例如在如下跃迁行中，E''(Ames) = 3445.4018 + 0.7865 = 3446.1883 cm⁻¹： 1 36.666580 1.538246E-31 2.306988E-07 3445.40177 0 4 2 1 1 6 2 0 57 1 2 31 58 2 2 34 57 58 e e 3 3 -0.7207 0.0658 0.7865