Dynamical Linear Response of TDDFT with LDA+U Functional: strongly hybridized Frenkel excitons in NiO

Abstract

Within the framework of time-dependent density-functional theory (TDDFT), we derive the dynamical linear response of LDA+U functional and benchmark it on NiO, a prototypical Mott insulator. Formulated using real-space Wannier functions, our computationally inexpensive framework gives detailed insights into the formation of tightly bound Frenkel excitons with reasonable accuracy. Specifically, a strong hybridization of multiple excitons is found to significantly modify the exciton properties. Furthermore, our study exposes a significant generic limitation of adiabatic approximation in TDDFT with hybrid functionals and in existing Bethe-Salpeter-equation approaches, advocating the necessity of strongly energy-dependent kernels in future development.

5 pages, 2 figures

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• First-principles method of propagation of tightly bound excitons: exciton band structure of LiF and verification with inelastic x-ray scattering
• Magnons from time-dependent density-functional perturbation theory and nonempirical Hubbard functionals
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