Verdict: Time-Dependent Density Functional Theory "Not Guilty" of Large Errors for Cyanines
Verdict: Time-Dependent Density Functional Theory "Not Guilty" of Large Errors for Cyanines
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DOI：
10.1021/ct200721d
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发表时间：
2012-04-01
影响因子：
5.5
通讯作者：
Truhlar, Donald G.
中科院分区：
文献类型：
--
作者：
Jacquemin, Denis;Zhao, Yan;Truhlar, Donald G.
我们评估八明尼苏达密度泛函（M05至M08-SO）和其他两个（PBE和PBE 0）的准确性的一个家庭的四个花菁染料的电子激发能的预测。我们发现，含时密度泛函理论（TDDFT）与这些泛函中的五个最近的（从M06-HF到M08-SO）能够相对于最精确的可用量子蒙特卡罗计算在0.10-0.36 eV的精度内预测花青染料的激发能，提供与最新一代CASPT 2计算相当的精度，其具有0.16- 0.34eV的误差。因此，以前的结论，TDDFT不能合理准确地处理菁染料，必须加以修订。
We assess the accuracy of eight Minnesota density functionals (M05 through M08-SO) and two others (PBE and PBE0) for the prediction of electronic excitation energies of a family of four cyanine dyes. We find that time-dependent density functional theory (TDDFT) with the five most recent of these functionals (from M06-HF through M08-SO) is able to predict excitation energies for cyanine dyes within 0.10-0.36 eV accuracy with respect to the most accurate available Quantum Monte Carlo calculations, providing a comparable accuracy to the latest generation of CASPT2 calculations, which have errors of 0.16-0.34 eV. Therefore previous conclusions that TDDFT cannot treat cyanine dyes reasonably accurately must be revised.