The nonlinear optical (NLO) properties of two-dimensional (2D) materials are fascinating for fundamental physics and optoelectronic device development. However, relatively few investigations have been conducted to establish the combined NLO activities of a 2D material. Herein, a study of numerous NLO properties of 2D gallium sulfide (GaS), including second-harmonic generation (SHG), two-photon excited fluorescence (TPEF), and NLO absorption are presented. The layer-dependent SHG response of 2D GaS identifies the noncentrosymmetric nature of the odd layers, and the second-order susceptibility (χ2) value of 47.98 pm/V (three-layers of GaS) indicates the superior efficiency of the SHG signal. In addition, structural deformation induces the symmetry breaking and facilitates the SHG in the bulk samples, whereas a possible efficient symmetry breaking in the liquid-phase exfoliated samples results in an enhancement of the SHG signal, providing prospective fields of investigation for researchers. The generation of TPEF from 800 to 860 nm depicts the two-photon absorption characteristics of 2D GaS material. Moreover, the saturable absorption characteristics of 2D GaS are realized from the largest nonlinear absorption coefficient (β) of −9.3 × 103, −91.0 × 103, and −6.05 × 103 cm/GW and giant modulation depths (T s ) of 24.4%, 35.3%, and 29.1% at three different wavelengths of 800, 1066, and 1560 nm, respectively. Hence, such NLO activities indicate that 2D GaS material can facilitate in the technical advancements of future nonlinear optoelectronic devices.

Fluorescent anti-counterfeiting materials have been widely studied due to their high resolution and convenient identification by direct visualization of the color output. To date, the anti-counterfeiting technology of single ultraviolet excitation mode still has security problems because the single mode could be imitated easily. Here, we have successfully developed four modes of anti-counterfeiting from Eu 2+ and Er 3+ co-doped Ba 2 Zr 2 Si 3 O 12 phosphors with photo, long persistent, photo-stimulated, and upconversion luminescence behavior. The as-fabricated phosphors can emit an intense blue-green luminescence originating from the characteristic transition of Eu 2+ ions and exhibit a blue-green long persistent luminescence phenomenon. Moreover, the enhancement of photo-stimulated luminescence that contributed to the effectively increased trap concentration is observed, along with the produced up-conversion phenomenon thanks to the introduction of Er 3+ ions. Notably, the fluorescence rapidly changes from blue-green to stable green luminescence with the delay of excitation time under the excitation of a 980 nm laser diode. Herein, this work realizes the fast down-to up-conversion luminescence output over time, which provides the basis for its possible application in advanced multi-mode anti-counterfeiting.

Two-dimensional Ruddlesden–Popper perovskites (RPPs) with multiple quantum well-like structures, strong excitonic quantum confinement, and high stability are promising optical gain media. However, the lasing from such material with a small number of inorganic well layers is difficult to achieve. Herein, we demonstrate the low-threshold upconversion lasing from the homologous RPP (PEA)2(MA) n −1Pb n I3 n +1 (n = 2 and 3) microflakes with wavelength varies from 598 to 637 nm under 800 nm laser excitation at low temperature (≤153 K). Using the micro Z-scan technique, we discovered that the RPP flakes have a giant two-photon absorption coefficient β as high as 3.6 × 103 cm GW–1, resulting in the effective upconversion transition under two-photon excitation. Furthermore, the self-formation of Fabry–Pérot microcavities provides the support for lasing emission from the n ≥ 2 RPP flakes. Calculation results and microscopic transient absorption measurements reveal that low-threshold lasing is due to the high differential gain coefficient and the suppressed nonradiative Auger recombination rate inside the quantum confinement structures. These properties enable RPPs as potential gain media for developing upconversion microcavity lasers.