Recently we demonstrated how the exchange dynamics of gas atoms localized near the openings of self-assembled L-alanyl-L-valine (AC) nanotubes can be studied by continuous-flow hyperpolarized xenon-129 two-dimensional NMR exchange spectroscopy (2D-EXSY). We noted that the finite residence time of the hyperpolarized gas inside the sample space suppresses the cross-peak signals associated with any exchange processes involving the free gas. Here we demonstrate that the gas-phase diagonal-peak and exchange cross-peak signals in the hyperpolarized 2D-EXSY spectrum of Xe in AV are dramatically enhanced by interrupting the gas flow during the EXSY pulse sequence. This simple but highly effective modification of the standard continuous flow hyperpolarized 2D-EXSY method is expected to broaden the range of exchange and diffusion processes that can be interrogated in nanoporous materials.