Nonlinear
optical experiments, especially the second-harmonic generation
(SHG) of topological insulators (TIs) such as Bi2Te3 and Bi2Se3, provide significant insights
into the second-order nonlinear susceptibility (χ(2)) of the topological surface states (TSS) and the DC electric field
(E
dc), formed by the intrinsic band bending
between the surface and bulk states. Importantly, by selectively tuning
the polarization of the incident laser field from linear to circular,
second-harmonic measurements in TIs enable us to extract these explicit
contributions from the band bending (E
dc) and metallic surface states (χ(2)), respectively.
In this work, we report the relaxation dynamics of the differential
change in SHG intensity (ΔI(τpp) = I
shg
pump on(τpp) – I
shg
pump off) with respect to the pump–probe delay time (τpp) in Bi2Te3 crystal, mainly emphasizing on
different pump–probe polarization configurations to provide
an understanding of the temporal evolution of ΔE
dc(τpp) and Δχ(2)(τpp). Upon photoexcitation, ΔI(τpp) with linearly polarized pump–probe
configuration, we observe two opposing contributions to ΔE
dc, namely, the depletion electric field (DEF)
and surface photovoltage (SPV) that effectively determine the spatial
distribution of the bulk and surface carrier densities. However, on
switching the probe polarization from linear to circular, we show
that the SHG response has a predominant contribution from χ(2), thereby extracting the time evolution of Δχ(2) arising from the TSS after photoexcitation, observed as
an additional positive enhancement of ΔI(τpp). This is analytically understood by opening a band gap
of ∼48 meV at the Dirac point due to the breaking of time reversal
symmetry using circularly polarized light.