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E-mail: adarsh@iiserb.ac.in
Abstract
Nonlinear optical responses or Kerr nonlinearity of materials are of significant importance
in developing modern photonic and optoelectronic devices. Optical Kerr nonlinearity induced
by strong optical excitation in hybrid material can offer a larger amplitude, potentially helpful
in optical switching/limiting, all-optical signal processing, and quantum information. Here, we
demonstrate a remarkable, manifold increase in the magnitude of the third-order nonlinear optical
response (Kerr nonlinearity) of the donor-acceptor Ti3 C2 Tx (MXene)-VS2 hybrid in the strong
coupling regime compared to control systems in the femtosecond domain. Interestingly, we ob-
served a transition from reverse saturable absorption to saturable absorption and a change from
self-focusing to self-defocusing in the nonlinear optical behavior when moving from the MXene-
VS2 hybrid to control systems. Our four-level rate-equation model encapsulates the underlying
physics governing the unprecedented ultrafast nonlinear optical response observed in hybrid. The
enhanced Kerr nonlinearity of the hybrid is ascribed to charge transfer between MXene and VS2 .
Besides, First-principles calculations and the Bader charge study unveil strong electronic coupling
within the hybrid system, where the transfer of electrons from MXene to VS2 corroborated through
measurements of the steady-state and time-resolved photoluminescence. Finally, benefitting from
the high third-order nonlinear response, we present a propitious application of MXene-VS2 hybrid