Laser-induced spectral broadening and hole-burning in rare earth doped crystals and coherent optical spectroscopy for frequency upconversion

The excitation spectra for linear fluorescence and for frequency upconversion are recorded in Er³⁺ doped crystal Er:YAG. An excitation induced spectral broadening and hole-burning are shown to appear at the resonant frequency of the linear fluorescence excitation spectrum, where the upconversion is simultaneously enhanced. Rate equation analysis is applied to model the optical pumping processes in the crystal. We present evidence that the induced resonance broadening and hole-burning are the result of excitation competition between the linear absorption and the excited state absorption. Femtosecond pulse pairs are applied to excite the linear and nonlinear frequency conversion, resulting in coherent controlled branching ratio between the linear and nonlinear frequency conversion. The experimental reasults are in good agreement with the numerical evaluation based on optical Bloch equation. PACS 78.47.+p; 42.65.Re; 78.20.Ci