Fault-Tolerant Quantum Simulations of Chemistry in First Quantization

Abstract

Quantum simulations of chemistry in first quantization offer some important advantages over approaches in second quantization including faster convergence to the continuum limit and the opportunity for practical simulations outside of the Born-Oppenheimer approximation. However, since all prior work on quantum simulation of chemistry in first quantization has been limited to asymptotic analysis, it has been impossible to directly compare the resources required for these approaches to those required for the more commonly studied algorithms in second quantization. Here, we compile, optimize, and analyze the finite resources required to implement two first quantized quantum algorithms for chemistry from Babbush et al. [Npj Quantum Inf. 5, 92 (2019)] that realize block encodings for the qubitization and interaction-picture frameworks of Low et al. [Quantum 3, 163 (2019), arXiv:1805.00675 (2018)]. The two algorithms we study enable simulation with gate complexities of O~(η8/3N1/3t+η4/3N2/3t) and O~(η8/3N1/3t) where η is the number of electrons, N is the number of plane-wave basis functions, and t is the duration of time evolution (t is linearly inverse to target precision when the goal is to estimate energies). In addition to providing the first explicit circuits and constant factors for any first quantized simulation, and then introducing improvements, which reduce circuit complexity by about a thousandfold over naive implementations for modest sized systems, we also describe new algorithms that asymptotically achieve the same scaling in a real-space representation. Finally, we assess the resources required to simulate various molecules and materials and conclude that the qubitized algorithm will often be more practical than the interaction-picture algorithm. We demonstrate that our qubitization algorithm often requires much less surface-code space-time volume for simulating millions of plane waves than the best second quantized algorithms require for simulating hundreds of Gaussian orbitals.