Investigation of crystal field effects for the spectral broadening of Yb3+-doped LuxY2−xO3 sesquioxide crystals

Abstract

The investigation of crystal field effects is significant for elucidating the spectral characteristics of Yb³⁺-doped sesquioxide crystals for ultrafast laser generation. The narrow spectra of Yb³⁺-doped single sesquioxide crystals limit the generation of ultrafast lasers; in this study, the Y³⁺ ions were introduced into Lu₂O₃ single crystals by the employment of ion replacement to broaden the spectra. To analyze the spectral broadening, the responsible crystal field parameters (CFPs) were calculated. The conversion of the host dominant ion and the distortion of the ligand affected the values and signs of the CFPs, and further determined the energy level splitting and fluorescence spectra. A linear relationship expressed by the semi-empirical equations for Yb³⁺-doped sesquioxide crystals was produced, which could be used for high throughput spectral prediction. Opposite variations of high- and low-frequency vibrational energies and the influence of the electron–phonon coupling on the spectra were also achieved. The redshift from the crystal field and the blueshift from the electron–phonon coupling make the optimal spectral broadening appear when x = 1.19 in the Yb:Lu_xY_2−xO₃ crystals. The results of these analyses could provide some key clues for the development of Yb³⁺-doped crystals for the generation and amplification of ultrafast lasers.