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We perform a comprehensive analysis of both the chemical and correlated electronic structure reconstruction of rhombohedral CrX3 (X=Br, Cl, I) van der Waals bulk crystals. Using the generalized gradient approximation (GGA) plus dynamical mean-field theory we explicitly demonstrate the importance of local dynamical correlations for a consistent understanding of emergent Kondo quasiparticles and Mott localized electronic states, showing the interplay between material-dependent one-electron GGA line-shape and multiorbital electronic interactions. To probe the correlated paramagnetic electronic state we performed x-ray absorption spectroscopy measurements for CrCl3 and CrBr3 bulk crystals. Our correlated many-body study is relevant to understanding the electronic structure reconstruction of paramagnetic Cr-trihalide crystals and should be widely applicable to other van der Waals magnetic materials.

We perform a comprehensive analysis of both the chemical and correlated electronic structure reconstruction of rhombohedral CrX3 (X=Br, Cl, I) van der Waals bulk crystals. Using the generalized gradient approximation (GGA) plus dynamical mean-field theory we explicitly demonstrate the importance of local dynamical correlations for a consistent understanding of emergent Kondo quasiparticles and Mott localized electronic states, showing the interplay between material-dependent one-electron GGA line-shape and multiorbital electronic interactions. To probe the correlated paramagnetic electronic state we performed x-ray absorption spectroscopy measurements for CrCl3 and CrBr3 bulk crystals. Our correlated many-body study is relevant to understanding the electronic structure reconstruction of paramagnetic Cr-trihalide crystals and should be widely applicable to other van der Waals magnetic materials.

We perform a comprehensive analysis of both the chemical and correlated electronic structure reconstruction of rhombohedral CrX3 (X=Br, Cl, I) van der Waals bulk crystals. Using the generalized gradient approximation (GGA) plus dynamical mean-field theory we explicitly demonstrate the importance of local dynamical correlations for a consistent understanding of emergent Kondo quasiparticles and Mott localized electronic states, showing the interplay between material-dependent one-electron GGA line-shape and multiorbital electronic interactions. To probe the correlated paramagnetic electronic state we performed x-ray absorption spectroscopy measurements for CrCl3 and CrBr3 bulk crystals. Our correlated many-body study is relevant to understanding the electronic structure reconstruction of paramagnetic Cr-trihalide crystals and should be widely applicable to other van der Waals magnetic materials.

Using the generalized gradient approximation plus dynamical mean-field theory (GGA+DMFT) we confirm the importance of multi-orbital dynamical correlations in determining the paramagnetic insulating state of CrI3. While the ferromagnetic phase reveals weak electronic correlation effects due to strong spin-orbital polarization, the Mott insulating state of paramagnetic CrI3 crystal is shown to be driven by the interplay between orbital-dependent one-electron lineshape and multi-orbital electronic interactions. To probe the paramagnetic Mott insulating state we performed x-ray absorption spectroscopy (XAS) measurements for the two structural phases of CrI3. Our study is relevant to understanding the orbital-selective electronic structure reconstruction of Mott insulators and should be applicable to other van der Waals bonded materials from bulk to the ultrathin limit.

Using the generalized gradient approximation plus dynamical mean-field theory (GGA+DMFT) we confirm the importance of multi-orbital dynamical correlations in determining the paramagnetic insulating state of CrI3. While the ferromagnetic phase reveals weak electronic correlation effects due to strong spin-orbital polarization, the Mott insulating state of paramagnetic CrI3 crystal is shown to be driven by the interplay between orbital-dependent one-electron lineshape and multi-orbital electronic interactions. To probe the paramagnetic Mott insulating state we performed x-ray absorption spectroscopy (XAS) measurements for the two structural phases of CrI3. Our study is relevant to understanding the orbital-selective electronic structure reconstruction of Mott insulators and should be applicable to other van der Waals bonded materials from bulk to the ultrathin limit.

Using the generalized gradient approximation plus dynamical mean-field theory (GGA+DMFT) we confirm the importance of multi-orbital dynamical correlations in determining the paramagnetic insulating state of CrI3. While the ferromagnetic phase reveals weak electronic correlation effects due to strong spin-orbital polarization, the Mott insulating state of paramagnetic CrI3 crystal is shown to be driven by the interplay between orbital-dependent one-electron lineshape and multi-orbital electronic interactions. To probe the paramagnetic Mott insulating state we performed x-ray absorption spectroscopy (XAS) measurements for the two structural phases of CrI3. Our study is relevant to understanding the orbital-selective electronic structure reconstruction of Mott insulators and should be applicable to other van der Waals bonded materials from bulk to the ultrathin limit.

Using density functional dynamical mean-field theory we investigate the site-selective electronic structure of Ca[subscript 2]O[subscript 3]Fe[subscript 3]S[subscript 2]. We confirm that the parent compound with two distinct iron sites is a multiorbital Mott insulator similar to La[subscript 2]O[subscript 3]Fe[subscript 2]S[subscript 2]. Upon electron/hole doping, carrier localization is found to persist in the two active iron channels because the chemical potential lies in a gap structure with anisotropic and almost vanishing states near the Fermi energy. This emergent behavior stems from large electronic reconstruction caused by dynamical spectral weight transfer involving states with distinct d-shell occupancies and orbital character at low energies. We detail the implications of our microscopic analysis and discuss the underlying physics which will emerge in future experiments on Ca[subsccript 2]O[subscript 3]Fep[subscript 3]S[subscript 2]}.