Sottile Francesco, Olevano Valerio, Reining Lucia
Laboratoire des Solides Irradiés UMR 7642, CNRS-CEA/DSM, Ecole Polytechnique, F-91128 Palaiseau, France.
Phys Rev Lett. 2003 Aug 1;91(5):056402. doi: 10.1103/PhysRevLett.91.056402. Epub 2003 Jul 31.
We have established and implemented a fully ab initio method which allows one to calculate optical absorption spectra, including excitonic effects, without solving the cumbersome Bethe-Salpeter equation, but obtaining results of the same precision. This breakthrough has been achieved in the framework of time-dependent density-functional theory, using new exchange-correlation kernels f(xc) that are free of any empirical parameter. We show that the same excitonic effects in the optical spectra can be reproduced through different f(xc)'s, ranging from frequency-dependent ones to a static one, by varying the kernel's spatial degrees of freedom. This indicates that the key quantity is not f(xc), but f(xc) combined with a response function. We present results for the optical absorption of bulk Si and SiC in good agreement with experiment, almost indistinguishable from those of the Bethe-Salpeter approach.
我们已经建立并实施了一种完全从头算的方法,该方法无需求解繁琐的贝塞耳-萨尔皮特方程,就能计算包括激子效应在内的光吸收光谱,同时获得相同精度的结果。这一突破是在含时密度泛函理论框架内实现的,使用了不含任何经验参数的新型交换关联核f(xc)。我们表明,通过改变核的空间自由度,从频率相关的f(xc)到静态的f(xc),不同的f(xc)都能重现光谱中的相同激子效应。这表明关键量不是f(xc),而是f(xc)与响应函数的结合。我们给出了体硅和碳化硅光吸收的结果,与实验结果吻合良好,与贝塞耳-萨尔皮特方法的结果几乎无法区分。