We report herein the synthesis of new dioxopiperazine isoquinolines using the Pictet– Spengler cyclisation. Our synthetic strategy for the preparation of two new compounds (,), with a tetrahydro-6H-pyrazino [1, 2-b] isoquinoline-1, 4-dione moiety was developed in only four steps. To understand better the crucial step of the synthesis reported here, theoretical calculations using semiempirical (PM3), ab initio and DFT computations were carried out ...