Distributed quantum computing (DQC) has been proposed as a way to scale quantum algorithms for practical applications beyond monolithic quantum processor architectures. Among these applications, quantum chemistry is widely regarded as one of the most promising use cases for quantum computing. In this work, we estimate the distributed-resource requirements of unitary coupled-cluster (UCC) ansätze for quantum chemistry, focusing on unitary coupled-cluster singles and doubles (UCCSD), unitary pair coupled-cluster doubles (UpCCD), and unitary pair coupled-cluster with generalized singles and doubles (UpCCGSD) circuits for hydrogen chains. We focus on a teleportation-based approach to DQC, quantitatively comparing a naive distribution method to the output of the TeleSABRE algorithm. For both approaches, we estimate the cost of handling nonlocal two-qubit gates across a fixed midpoint or quarter-point partition, reporting Bell-pair/classical-communication costs in teleportation. Across Jordan-Wigner and Bravyi-Kitaev, we find that UpCCD with spin-blocked Jordan-Wigner ordering gives the most favorable scaling, while UCCSD incurs substantially larger distributed-resource requirements.
Distributed quantum computing (DQC) has been proposed as a way to scale quantum algorithms for practical applications beyond monolithic quantum processor architectures. Among these applications, quantum chemistry is widely regarded as one of the most promising use cases for quantum computing. In this work, we estimate the distributed-resource requirements of unitary coupled-cluster (UCC) ansätze for quantum chemistry, focusing on unitary coupled-cluster singles and doubles (UCCSD), unitary pair coupled-cluster doubles (UpCCD), and unitary pair coupled-cluster with generalized singles and doubles (UpCCGSD) circuits for hydrogen chains. We focus on a teleportation-based approach to DQC, quantitatively comparing a naive distribution method to the output of the TeleSABRE algorithm. For both approaches, we estimate the cost of handling nonlocal two-qubit gates across a fixed midpoint or quarter-point partition, reporting Bell-pair/classical-communication costs in teleportation. Across Jordan-Wigner and Bravyi-Kitaev, we find that UpCCD with spin-blocked Jordan-Wigner ordering gives the most favorable scaling, while UCCSD incurs substantially larger distributed-resource requirements.
To move towards the utility era of quantum computing, many corporations have posed distributed quantum computing (DQC) as a framework for scaling the current generation of devices for practical applications. One of these applications is quantum chemistry, also known as electronic structure theory, which has been poised as a “killer application” of quantum computing. To this end, we analyze five electronic structure methods, including the unitary coupled-cluster singles and doubles (UCCSD), unitary pair coupled-cluster doubles (UpCCD), unitary pair coupled-cluster with generalized singles and doubles (UpCCGSD), separable pair approximation plus generalized singles (SPA+GS), and local unitary cluster Jastrow (LUCJ) ansätze. The key benefit of these methods is that they can be found in common packages, such as Tequila and ffsim, that interface easily with the Qiskit Circuit Cutting addon. Herein, we highlight the challenges and aptitude of the aforementioned electronic structure methods for distribution using quasiprobability simulation with local operations (LO). The key findings of our work are that many of these algorithms cannot be efficiently parallelized using LO, and new methods must be developed to apply electronic structure theory within a DQC framework.
Quantum chemistry calculations of large, strongly correlated systems are typically limited by the computation cost that scales exponentially with the size of the system. Quantum algorithms, designed specifically for quantum computers, can alleviate this, but the resources required are still too large for today's quantum devices. Here we present a quantum algorithm that combines a localization of multireference wave functions of chemical systems with quantum phase estimation (QPE) and variational unitary coupled cluster singles and doubles (UCCSD) to compute their ground state energy. Our algorithm, termed "local active space unitary coupled cluster" (LAS-UCC), scales linearly with system size for certain geometries, providing a polynomial reduction in the total number of gates compared with QPE, while providing accuracy above that of the variational quantum eigensolver using the UCCSD ansatz and also above that of the classical local active space self-consistent field. The accuracy of LAS-UCC is demonstrated by dissociating (H2)2 into two H2 molecules and by breaking the two double bonds in trans-butadiene and resources estimates are provided for linear chains of up to 20 H2 molecules.
Quantum chemistry calculations of large, strongly correlated systems are typically limited by the computation cost that scales exponentially with the size of the system. Quantum algorithms, designed specifically for quantum computers, can alleviate this, but the resources required are still too large for today's quantum devices. Here, we present a quantum algorithm that combines a localization of multireference wave functions of chemical systems with quantum phase estimation (QPE) and variational unitary coupled cluster singles and doubles (UCCSD) to compute their ground-state energy. Our algorithm, termed "local active space unitary coupled cluster" (LAS-UCC), scales linearly with the system size for certain geometries, providing a polynomial reduction in the total number of gates compared with QPE, while providing accuracy above that of the variational quantum eigensolver using the UCCSD ansatz and also above that of the classical local active space self-consistent field. The accuracy of LAS-UCC is demonstrated by dissociating (H2)2 into two H2 molecules and by breaking the two double bonds in trans-butadiene, and resource estimates are provided for linear chains of up to 20 H2 molecules.
We introduce a unitary coupled-cluster (UCC) ansatz termed k -UpCCGSD that is based on a family of sparse generalized doubles operators, which provides an affordable and systematically improvable unitary coupled-cluster wave function suitable for implementation on a near-term quantum computer. k -UpCCGSD employs k products of the exponential of pair coupled-cluster double excitation operators (pCCD), together with generalized single excitation operators. We compare its performance in both efficiency of implementation and accuracy with that of the generalized UCC ansatz employing the full generalized single and double excitation operators (UCCGSD), as well as with the standard ansatz employing only single and double excitations (UCCSD). k -UpCCGSD is found to show the best scaling for quantum computing applications, requiring a circuit depth of, compared with for UCCGSD, and for UCCSD, where N is the number of spin orbitals and η is the number of electrons. We analyzed the accuracy of these three ansätze by making classical benchmark calculations on the ground state and the first excited state of H 4 (STO-3G, 6-31G), H 2 O (STO-3G), and N 2 (STO-3G), making additional comparisons to conventional coupled cluster methods. The results for ground states show that k -UpCCGSD offers a good trade-off between accuracy and cost, achieving chemical accuracy for lower cost of implementation on quantum computers than both UCCGSD and UCCSD. UCCGSD is also found to be more accurate than UCCSD but at a greater cost for implementation. Excited states are calculated with an orthogonally constrained variational quantum eigensolver approach. This is seen to generally yield less accurate energies than for the corresponding ground states. We demonstrate that using a specialized multideterminantal reference state constructed from classical linear response calculations allows these excited state energetics to be improved.
Quantum chemistry calculations of large, strongly correlated systems are typically limited by the computation cost that scales exponentially with the size of the system. Quantum algorithms, designed specifically for quantum computers, can alleviate this, but the resources required are still too large for today’s quantum devices. Here we present a quantum algorithm that combines a localization of multireference wave functions of chemical systems with quantum phase estimation (QPE) and variational unitary coupled cluster singles and doubles (UCCSD) to compute their ground state energy. Our algorithm, termed “local active space unitary coupled cluster” (LAS-UCC), scales linearly with system size for certain geometries, providing a polynomial reduction in the total number of gates compared with QPE, while providing accuracy above that of the variational quantum eigensolver using the UCCSD ansatz and also above that of the classical local active space self-consistent field. The accuracy of LAS-UCC is demonstrated by dissociating (H2)2 into two H2 molecules and by breaking the two double bonds in trans-butadiene and resources estimates are provided for linear chains of up to 20 H2 molecules.
Quantum chemistry calculations of large, strongly correlated systems are typically limited by the computation cost that scales exponentially with the size of the system. Quantum algorithms, designed specifically for quantum computers, can alleviate this, but the resources required are still too large for today’s quantum devices. Here we present a quantum algorithm that combines a localization of multireference wave functions of chemical systems with quantum phase estimation (QPE) and variational unitary coupled cluster singles and doubles (UCCSD) to compute their ground state energy. Our algorithm, termed “local active space unitary coupled cluster” (LAS-UCC), scales linearly with system size for certain geometries, providing a polynomial reduction in the total number of gates compared with QPE, while providing accuracy above that of the variational quantum eigensolver using the UCCSD ansatz and also above that of the classical local active space self-consistent field. The accuracy of LAS-UCC is demonstrated by dissociating (H2)2 into two H2 molecules and by breaking the two double bonds in trans-butadiene and resources estimates are provided for linear chains of up to 20 H2 molecules.