Inhomogeneous broadening in disordered
crystals has been
widely
recognized as a successful approach to enhance the spectral bandwidth
of rare earth ions in optical spectra, and the Yb3+-doped
mixed laser crystals are known as ultrafast pulse materials and have
emerged as a hotspot recently. In this study, mixed sodium gadolinium/lanthanum
double molybdate disordered laser crystals NaGd(1–x)La(x)(MoO4)2 with x = 0.3, 0.5, and 0.9 were grown
by the Czochralski (Cz) method. The structure of as-grown crystals
was investigated by XRD, SEM, FT-IR, and Raman experiments. The spectroscopic
properties, including absorption, emission, and fluorescence decay
characteristics, were investigated thoroughly. The NaGd0.5La0.5(MoO4)2 (NGLM) composite crystal
exhibited an exceptionally broad absorption which reaches 70 nm (fwhm)
at 980 nm, exceeding those of NaGd(MoO4)2 (NGM)
and NaLa(MoO4)2 (NLM). Additionally, the electronic
structures (band structure and density of states) of NGM, NGLM, and
NLM were determined from the first-principles method combined with
the PBE function. The calculations of defect formation energies under
O-poor and O-rich conditions demonstrate that the +2 defects are easily
generated in the undoped NGM crystal prepared under reducing atmospheres,
and the calculation of absorption properties reveals that the black
color of NGM without annealing is mainly attributed to intraband transitions
between defect induction states and VBM or CBM. Moreover, the lifetimes
of excited energy level 2F5/2 of Yb3+ were examined under different experimental environments to obtain
the intrinsic radiative lifetime, and the emission cross section was
calculated as 2.25 × 10–20 cm2 at
1016 nm. The features of the Yb3+:NaGd(1–x)La(x)(MoO4)2 crystal indicate the potential applications for ultrafast
and broad tunable laser through slight regulation of the composite
engineering strategy.