Direct femtosecond laser writing of ferroelectric domain structures has been an indispensable technique for engineering the second-order optical nonlinearity of materials in three dimensions. It utilizes localized thermoelectric field motivated by nonlinear absorption at the position of laser focus to manipulate domains. However, the impact of laser wavelengths, which is pivotal in nonlinear absorption, on the inverted domains is still sketchy. Herein, the light-induced ferroelectric domain inversion is experimentally studied. It is shown that the domain inversions can be achieved over a broad spectral range, but the optical threshold for domain inversion varies dramatically with the laser wavelength, which can be explained by considering the physical mechanism of femtosecond laser poling and nonlinear absorption properties of the crystal. Meanwhile, the effects of other laser processing parameters are also experimentally investigated. Our findings are useful to guide the fabrication of high-performance optical and electronic devices based on ferroelectric domains.

Nonlinear frequency conversion via three-dimensional (3D) quasi-phase matching (QPM) process is experimentally realized based on a Ba_0.77Ca_0.23TiO₃ (BCT) crystal. The ferroelectric domains in BCT crystal are observed, and the results reveal that the antiparallel domains distribute in three dimensions and can provide 3D reciprocal lattice vectors for QPM processes. Broadband petal-like second-harmonic patterns are achieved, which are well consistent with the theoretical quasi-cubic model of 3D nonlinear photonic crystals. Our work not only promotes the development of QPM technique but also builds a platform for 3D nonlinear optics and quantum optics.

Nonlinear wavefront shaping in periodically poled ferroelectric crystals has received great attention because it offers a convenient way to generate a structured light beam at new frequencies. In contrast to structurally uniform beams like Laguerre–Gaussian or Hermite–Gaussian modes, here we demonstrate the possibility to generate a spatially varied optical bottle beam via a frequency doubling process in a domain-engineered Sr_0.61Ba_0.39Nb₂O₆ (SBN) crystal. The nonlinear holography method was employed to design the modulation pattern of the second-order nonlinear coefficient χ⁽²⁾, and the femtosecond laser poling was used to imprint the χ⁽²⁾ pattern into the SBN crystal via ferroelectric domain inversion. The second harmonic bottle beam with zero intensity in its center that is surrounded in all three dimensions by light was observed with the incidence of a fundamental Gaussian beam. These results are useful for nonlinear generation and control of structured light at new frequencies, which has important applications in nonlinear photonics and quantum optics.

Quasi‐phase matching (QPM) is a technique in nonlinear optics for achieving efficient energy exchange among optical waves at different frequencies, by spatially modulating the quadratic nonlinearity (χ ⁽²⁾) of the medium. To realize the full potential of QPM, 3D spatial modulation of χ ⁽²⁾ is required. This has become experimentally feasible recently thanks to the invention of femtosecond laser‐based nonlinearity engineering in ferroelectric crystals. Herein, the first experimental demonstration of QPM second harmonic generation (SHG) in a nonlinear cubic crystal system is presented, in which χ ⁽²⁾ modulations form simple cubic, body‐centered cubic, face‐centered cubic, and diamond cubic lattices, respectively. The experimental results indicate that these nonlinear cubic structures share the same primary reciprocal lattice vectors (RLVs), but possess different Fourier coefficients (in conventional cells), leading to SHG with similar angular resonances but various intensity distributions in the far field. This work contributes to a comprehensive understanding of nonlinear optical processes in 3D periodic media, and thus sheds light on the development of high‐performance QPM devices.

Femtosecond laser-induced crystallization and ablation of Ge₂Sb₂Te₅ (GST) phase change film is investigated by reflectivity pump-probing technology. Below the ablation threshold, the face-centered cubic structure (FCC) state in the central area can be formed, and cylindrical rims are formed in the peripheral dewetting zone due to the solidification of transported matter. The time of surface temperature dropping to the crystallization point needs about 30 ps for 5.86 mJ/cm² and 82 ps for 7.04 mJ/cm², respectively. At higher laser fluence, crystallization GST island structures appear in the central ablation region due to the extremely short heating time (100 ps). Furthermore, crystallization rate is faster than the ablation rate of the GST film, which is caused by different reflectivity.