Phonon engineering in Yb:La₂CaB₁₀O₁₉ crystal for extended lasing beyond the fluorescence spectrum

Since the first invention of the laser in 1960, direct lasing outside the fluorescence spectrum is deemed impossible owing to the "zero-gain" cross-section. However, when electron-phonon coupling meets laser oscillation, an energy modulation by the quantized phonon can tailor the electronic transitions, thus directly creating some unprecedented lasers with extended wavelengths by phonon engineering. Here, we demonstrate a broadband lasing (1000-1280 nm) in a Yb-doped La₂CaB₁₀O₁₉ (Yb:LCB) crystal, far beyond its spontaneous fluorescence spectrum. Numerical calculations and in situ Raman verify that such a substantial laser emission is devoted to the multiphonon coupling to lattice vibrations of a dangling "quasi-free-oxygen" site, with the increasing phonon numbers step-by-step (n = 1-6). This new structural motif provides more alternative candidates with strong-coupling laser materials. Moreover, the quantitative relations between phonon density distribution and laser wavelength extension are discussed. These results give rise to the search for on-demand lasers in the darkness and pave a reliable guideline to study those intriguing electron-phonon-photon coupled systems for integrated photonic applications.