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.