Local Chemistry Engineering in Doped Photonic Glass for Optical Pulse Generation

Abstract The control of the optical response of multicomponent photonic glass through short‐ to medium‐range chemistry design has led to the development of high‐performance devices with efficient stimulated radiation, broadband optical amplification, and sensitive optical sensing. However, the success of optical modulation with an all‐fiber configuration is limited by the difficulty in creating smart structural units that can dynamically switch light–matter interactions. Here, a local chemistry design strategy is reported that can help realize dynamic energy storage and its controllable release, based on the simultaneous management of the chemical state and ligand field of transition‐metal dopant through glass crystallization. The theoretical analysis indicates that a four‐level configuration, such as that of tetrahedral Cr⁴⁺, can enable efficient photon–electron–photon conversion. Experimental data further reveal that this configuration can be stable in nanostructured glass. A nanostructured fiber with perfect core‐clad configuration is successfully fabricated by the melt‐in‐tube approach. The optical modulation function in bulk glass with estimated σ_gs and σ_es values of (1.39 ± 0.03) × 10⁻¹⁶ and (1.20 ± 0.02) × 10⁻¹⁶ cm², respectively, is also demonstrated. Therefore, a principle pulse laser device with operation wavelength at 1.06 µm and pulse duration of 176 ns is fabricated for the first time.