On the feasibility of performing quantum chemistry calculations on quantum computers

Abstract: Quantum chemistry is envisioned as an early and disruptive application for quantum computers. Yet, closer scrutiny of the proposed algorithms shows that there are considerable difficulties along the way. Here, we propose two criteria for evaluating two leading quantum approaches for finding the ground state of molecules. The first criterion applies to the variational quantum eigensolver (VQE) algorithm. It sets an upper bound to the level of imprecision/decoherence that can be tolerated in quantum hardware as a function of the targeted precision, the number of gates and the typical energy contribution from states populated by decoherence processes. We find that decoherence is highly detrimental to the accuracy of VQE and performing relevant chemistry calculations would require performances that are expected for fault-tolerant quantum computers, not mere noisy hardware, even with advanced error mitigation techniques. Physically, the sensitivity of VQE to decoherence originates from the fact that, in VQE, the spectrum of the studied molecule has no correlation with the spectrum of the quantum hardware used to perform the computation. The second criterion applies to the quantum phase estimation (QPE) algorithm, which is often presented as the go-to replacement of VQE upon availability of (noiseless) fault-tolerant quantum computers. QPE requires an input state with a large enough overlap with the sought-after ground state. We provide a criterion to estimate quantitatively this overlap based on the energy and the energy variance of said input state. Using input states from a variety of state-of-the-art classical methods, we show that the scaling of this overlap with system size does display the standard orthogonality catastrophe, namely an exponential suppression with system size. This in turns leads to an exponentially reduced QPE success probability.