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Solid-state optical absorption from optimally tuned time-dependent range-separated hybrid density functional theory

机译:最佳时变范围分离混合密度泛函理论的固态光吸收

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摘要

We present a framework for obtaining reliable solid-state charge and optical excitations and spectra from optimally tuned range-separated hybrid density functional theory. The approach, which is fully couched within the formal framework of generalized Kohn-Sham theory, allows for the accurate prediction of exciton binding energies. We demonstrate our approach through first principles calculations of one- and two-particle excitations in pentacene, a molecular semiconducting crystal, where our work is in excellent agreement with experiments and prior computations. We further show that with one adjustable parameter, set to produce the known band gap, this method accurately predicts band structures and optical spectra of silicon and lithium fluoride, prototypical covalent and ionic solids. Our findings indicate that for a broad range of extended bulk systems, this method may provide a computationally inexpensive alternative to many-body perturbation theory, opening the door to studies of materials of increasing size and complexity.
机译:我们提出了一个框架,用于从最佳调谐范围分离的混合密度泛函理论获得可靠的固态电荷,光学激发和光谱。该方法完全包含在广义Kohn-Sham理论的正式框架内,可精确预测激子结合能。我们通过并五苯(一种分子半导体晶体)中的一粒子和两粒子激发的第一原理计算来证明我们的方法,其中我们的工作与实验和先前的计算非常吻合。我们进一步表明,通过设置一个可调节参数以产生已知的带隙,该方法可以准确预测硅和氟化锂,典型共价和离子固体的能带结构和光谱。我们的发现表明,对于多种扩展的散装系统,该方法可能提供一种计算成本低廉的替代方法,代替了多体扰动理论,这为研究尺寸和复杂性不断增加的材料打开了大门。

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