Hunting for quantum advantage in electronic structure calculations is a highly non-trivial task

In light of major developments over the past decades in both quantum computing and simulations on classical hardware, it is a serious challenge to identify a real-world problem where quantum advantage is expected to appear. In quantum chemistry, electronic structure calculations of strongly correlated, i.e. multi-reference problems, are often argued to fall into such category because of their intractability with standard methods based on mean-field theory. Therefore, providing state-of-the-art benchmark data by classical algorithms is necessary to make a decisive conclusion when such competing development directions are compared. We report cutting-edge performance results together with high accuracy ground state energy for the Fe$_4$S$_4$ molecular cluster on a CAS(54,36) model space, a problem that has been included quite recently among the list of systems in the {\it Quantum Advantage Tracker} webpage maintained by IBM and RIKEN. Pushing the limits even further, we also present CAS-SCF based orbital optimizations for unprecedented CAS sizes of up to 89 electrons in 102 orbitals [CAS(89,102)] for the Fe$_5$S$_{12}$H$_4^{5-}$ molecular system comprising twenty five open shell orbitals in its sextet ground state and an active spaces size of 331 electrons in 451 orbitals. We have achieved our results via mixed-precision spin-adapted \textit{ab initio} Density Matrix Renormalization Group (DMRG) electronic structure calculations interfaced with the ORCA program package and utilizing the NVIDIA Blackwell graphics processing unit (GPU) platform. We argue that DMRG benchmark data should be taken as a classical reference when quantum advantage is reported. In addition, full exploitation of classical hardware should also be considered since even the most advanced DMRG implementations are still in a premature stage regarding utilization of all the benefits of GPU technology.

Source: arXiv:2603.28648v1 - http://arxiv.org/abs/2603.28648v1 PDF: https://arxiv.org/pdf/2603.28648v1 Original Link: http://arxiv.org/abs/2603.28648v1