Kondo scenario of the {\gamma}-{\alpha} phase transition in single crystalline Cerium thin films

TL;DR

This study investigates the $ ext{γ}$-$ ext{α}$ phase transition in cerium thin films, combining experimental ARPES/XRD measurements with theoretical DFT+DMFT calculations, revealing a Kondo-driven transition influenced by substrate strain.

Contribution

It provides new insights into the Kondo scenario as a key mechanism for the $ ext{γ}$-$ ext{α}$ phase transition in cerium thin films, supported by both experimental and theoretical evidence.

Findings

$ ext{γ}$-$ ext{α}$ transition occurs around 50 K in thin films, lower than bulk.

Kondo singlet states form at approximately 80 K, indicating Kondo physics involvement.

Theoretical spectral functions agree with ARPES data, confirming the Kondo-driven transition.

Abstract

The physical mechanism driving the $\gamma$-$\alpha$ phase transition of face-centre-cubic (fcc) cerium (Ce) remains controversial until now. In this work, high quality single crystalline fcc-Ce thin films were grown on Graphene/6$H$-SiC(0001) substrate, and explored by XRD and ARPES measurement. XRD spectra showed a clear $\gamma$-$\alpha$ phase transition at $T_{\gamma-\alpha}\approx$ 50 K, which is retarded by strain effect from substrate comparing with $T_{\gamma-\alpha}$ (about 140 K) of the bulk Ce metal. However, APRES spectra did not show any signature of $\alpha$-phase emerging in the surface-layer from 300 K to 17 K, which implied that $\alpha$-phase might form at the bulk-layer of our Ce thin films. Besides, an evident Kondo dip near Fermi energy was observed in the APRES spectrum at 80 K, indicting the formation of Kondo singlet states in $\gamma$-Ce. Furthermore, the DFT+DMFT calculations were performed to simulate the electronic structures and the theoretical spectral functions agreed well with the experimental ARPES spectra. In $\gamma$-Ce, the behavior of the self-energy's imaginary part at low frequency not only confirmed that the Kondo singlet states emerged at $T_{\rm KS} \geq 80$ K, but also implied that they became coherent states at a lower characteristic temperature ($T_{\rm coh}\sim 40$ K) due to the indirect RKKY interaction among $f$-$f$ electrons. Besides, $T_{\rm coh}$ from the theoretical simulation was close to $T_{\gamma-\alpha}$ from the XRD spectra. These issues suggested that the Kondo scenario might play an important role in the $\gamma$-$\alpha$ phase transition of cerium thin films.