Low rank representations for quantum simulation of electronic structure (2021)

Abstract The quantum simulation of quantum chemistry is a promising application of quantum computers. However, for N molecular orbitals, the $${\mathcal{O}}({N}^{4})$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mi>O</mml:mi> <mml:mrow> <mml:mo>(</mml:mo> <mml:mrow> <mml:msup> <mml:mrow> <mml:mi>N</mml:mi> </mml:mrow> <mml:mrow> <mml:mn>4</mml:mn> </mml:mrow> </mml:msup> </mml:mrow> <mml:mo>)</mml:mo> </mml:mrow> </mml:mrow> </mml:math> gate complexity of performing Hamiltonian and unitary Coupled Cluster Trotter steps makes simulation based on such primitives challenging. We substantially reduce the gate complexity of such primitives through a two-step low-rank factorization of the Hamiltonian and cluster operator, accompanied by truncation of small terms. Using truncations that incur errors below chemical accuracy allow one to perform Trotter steps of the arbitrary basis electronic structure Hamiltonian with $${\mathcal{O}}({N}^{3})$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mi>O</mml:mi> <mml:mrow> <mml:mo>(</mml:mo> <mml:mrow> <mml:msup> <mml:mrow> <mml:mi>N</mml:mi> </mml:mrow> <mml:mrow> <mml:mn>3</mml:mn> </mml:mrow> </mml:msup> </mml:mrow> <mml:mo>)</mml:mo> </mml:mrow> </mml:mrow> </mml:math> gate complexity in small simulations, which reduces to $${\mathcal{O}}({N}^{2})$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mi>O</mml:mi> <mml:mrow> <mml:mo>(</mml:mo> <mml:mrow> <mml:msup> <mml:mrow> <mml:mi>N</mml:mi> </mml:mrow> <mml:mrow> <mml:mn>2</mml:mn> </mml:mrow> </mml:msup> </mml:mrow> <mml:mo>)</mml:mo> </mml:mrow> </mml:mrow> </mml:math> gate complexity in the asymptotic regime; and unitary Coupled Cluster Trotter steps with $${\mathcal{O}}({N}^{3})$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mi>O</mml:mi> <mml:mrow> <mml:mo>(</mml:mo> <mml:mrow> <mml:msup> <mml:mrow> <mml:mi>N</mml:mi> </mml:mrow> <mml:mrow> <mml:mn>3</mml:mn> </mml:mrow> </mml:msup> </mml:mrow> <mml:mo>)</mml:mo> </mml:mrow> </mml:mrow> </mml:math> gate complexity as a function of increasing basis size for a given molecule. In the case of the Hamiltonian Trotter step, these circuits have $${\mathcal{O}}({N}^{2})$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mi>O</mml:mi> <mml:mrow> <mml:mo>(</mml:mo> <mml:mrow> <mml:msup> <mml:mrow> <mml:mi>N</mml:mi> </mml:mrow> <mml:mrow> <mml:mn>2</mml:mn> </mml:mrow> </mml:msup> </mml:mrow> <mml:mo>)</mml:mo> </mml:mrow> </mml:mrow> </mml:math> depth on a linearly connected array, an improvement over the $${\mathcal{O}}({N}^{3})$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mi>O</mml:mi> <mml:mrow> <mml:mo>(</mml:mo> <mml:mrow> <mml:msup> <mml:mrow> <mml:mi>N</mml:mi> </mml:mrow> <mml:mrow> <mml:mn>3</mml:mn> </mml:mrow> </mml:msup> </mml:mrow> <mml:mo>)</mml:mo> </mml:mrow> </mml:mrow> </mml:math> scaling assuming no truncation. As a practical example, we show that a chemically accurate Hamiltonian Trotter step for a 50 qubit molecular simulation can be carried out in the molecular orbital basis with as few as 4000 layers of parallel nearest-neighbor two-qubit gates, consisting of fewer than 10 5 non-Clifford rotations. We also apply our algorithm to iron–sulfur clusters relevant for elucidating the mode of action of metalloenzymes.