The surface/interface species in perovskite oxides play an essential role in
many novel emergent physical phenomena and chemical processes. With low
eigen-energy in the terahertz region, such species at buried interfaces remain
poorly understood due to the lack of feasible experimental techniques. Here, we
show that vibrational resonances and two-dimensional electron gas at the
interface can be characterized using surface-specific nonlinear spectroscopy in
the terahertz range. This technique uses intra-pulse difference frequency
mixing (DFM) process, which is allowed only at surface/interface of a medium
with inversion symmetry. Sub-monolayer sensitivity can be achieved using the
state-of-the-art detection scheme for the terahertz emission from
surface/interface. As a demonstration, Drude-like nonlinear response from the
two-dimensional electron gas emerging at LaAlO3/SrTiO3 or Al2O3/ SrTiO3
interface was successfully observed. Meanwhile, the interfacial vibrational
spectrum of the ferroelectric soft mode of SrTiO3 at 2.8 THz was also obtained
that was polarized by the surface field in the interfacial region. The
corresponding surface/interface potential, which is a key parameter for
SrTiO3-based interface superconductivity and photocatalysis, can now be
determined optically via quantitative analysis on the polarized phonon
spectrum. The interfacial species with resonant frequencies in the THz region
revealed by our method provide more insights into the understanding of physical
properties of complex oxides.Comment: arXiv admin note: substantial text overlap with arXiv:2207.1461