Plasser Felix, Lischka Hans, Shepard Ron, Szalay Péter G, Pitzer Russell M, Alves Rodolpho L R, Aquino Adelia J A, Autschbach Jochen, Barbatti Mario, Carvalho Jhonatas R, Chagas Julio C V, González Leticia, Hansen Andreas, Jayee Bhumika, Kertesz Miklos, Machado Francisco B C, Matsika Spiridoula, do Monte Silmar A, Mukherjee Saikat, Nachtigallová Dana, Nieman Reed, Oliveira Vytor P, Oppel Markus, Parish Carol A, Pittner Jiri, F Dos Santos Luan G, Scrinzi Armin, Sit Mahesh K, Spada Rene F K, Thodika Mushir, Valente Daniel C A, Vázquez-Mayagoitia Álvaro, Ventura Elizete, Westermayr Julia, Zaichenko Aleksandr, Zhang Zhiyong
Department of Chemistry, Loughborough University, Loughborough LE11 3TU, United Kingdom.
Department of Chemistry and Biochemistry, Texas Tech University, Lubbock, Texas 79409, United States.
J Phys Chem A. 2025 Jul 17;129(28):6482-6517. doi: 10.1021/acs.jpca.5c02047. Epub 2025 Jul 8.
The COLUMBUS program system provides the tools for performing high-level multireference (MR) computations, including the multireference configuration interaction (MRCI) method and its multireference averaged quadratic coupled cluster (MR-AQCC) extension, allowing computations on a wide range of fascinating atomic and molecular systems, including the treatment of open-shells and complicated excited state phenomena. The inclusion of spin-orbit coupling (SOC) directly within the MRCI step enables the description of systems containing heavy elements, such as lanthanides and actinides, whose properties are strongly influenced by SOC. Analytic energy gradients and nonadiabatic couplings at the correlated MRCI level provide the foundation for a variety of dynamics studies, giving insight into ultrafast photochemistry. New and ongoing method developments in COLUMBUS include the computation of spin densities, improved descriptions of ionic states, enhancements to the AQCC method, and the porting of COLUMBUS to graphical processing units (GPUs). New external interfaces enable an enhanced description of electronic resonances and molecules in strong laser fields. This work highlights these new developments while providing a detailed account of the diverse applications of COLUMBUS in recent years.
COLUMBUS程序系统提供了用于执行高级多参考（MR）计算的工具，包括多参考组态相互作用（MRCI）方法及其多参考平均二次耦合簇（MR-AQCC）扩展，可对广泛的有趣原子和分子系统进行计算，包括开壳层处理和复杂的激发态现象。在MRCI步骤中直接纳入自旋轨道耦合（SOC），能够描述包含重元素（如镧系元素和锕系元素）的系统，这些元素的性质会受到SOC的强烈影响。相关MRCI水平下的解析能量梯度和非绝热耦合为各种动力学研究奠定了基础，有助于深入了解超快光化学。COLUMBUS中正在进行的新方法开发包括自旋密度的计算、离子态的改进描述、AQCC方法的增强以及COLUMBUS向图形处理单元（GPU）的移植。新的外部接口能够增强对强激光场中电子共振和分子的描述。这项工作突出了这些新进展，同时详细介绍了COLUMBUS近年来的各种应用。
