Manifestation of incoherent-coherent crossover and non-Stoner magnetism in the electronic structure of Fe$_3$GeTe$_2$

Abstract: Two-dimensional (2D) van der Waals ferromagnets have potential applications as next-generation spintronic devices and provide a platform to explore the fundamental physics behind 2D magnetism. The dual nature (localized and itinerant) of electrons adds further complexity to the understanding of correlated magnetic materials. Here, we present the temperature evolution of electronic structure in 2D van der Waals ferromagnet, Fe${3}$GeTe${2}$, using photoemission spectroscopy in conjunction with density functional theory (DFT) plus dynamical mean field theory (DMFT). With the appearance of quasiparticle peak and its evolution in the vicinity of Fermi energy, we unveil empirical evidences of incoherent-coherent crossover at around 125 K. DFT+DMFT results show that the quasiparticle lifetime surpasses thermal energy for temperature below 150 K, confirming incoherent-coherent crossover in the system. No appreciable change in the Fe 2$p$ core level, overall valence band spectra across the magnetic transition, and temperature dependent ferromagnetic DFT+DMFT results, provide substantial evidence for non-stoner magnetism in Fe${3}$GeTe${2}$. We elucidate the temperature dependent intimate relation between magnetism and electronic structure in Fe${3}$GeTe${2}$. Sommerfeld coefficient of $\sim$ 104 mJ mol$^{-1}$ K$^{-2}$ obtained in the low temperature limit from DFT+DMFT calculations resolve the long standing issue of large Sommerfeld coefficient ($\sim$ 110 mJ mol$^{-1}$ K$^{-2}$) obtained from specific heat measurements.