We propose an efficient O( N 2 )-parameter ansatz that consists of a sequence of exponential operators, each of which is a unitary variant of Neuscamman’s cluster Jastrow operator. The ansatz can also be derived as a decomposition of T 2 amplitudes of the unitary coupled cluster with generalized singles and doubles, which gives a near full-CI energy. The proposed ansatz therefore can reproduce the uCCGSD energy, or rather will reach the exact full-CI energy because of the exponential operator product form. Because the cluster Jastrow operators are expressed by a product of number operators and the derived Pauli operator products, namely, the Jordan–Wigner strings, are all commutative, it does not require the Trotter approximation to implement to a quantum circuit and should be a good candidate for the variational quantum eigensolver algorithm of a near-term quantum computer. The accuracy of the ansatz was examined for dissociation of a nitrogen dimer, and compared with other existing O( N 2 )-parameter ansatzs. Not only the original ansatzs defined in the second-quantization form but also their Trotter-splitting variants, in which the cluster amplitudes are optimized to minimize the energy obtained with a few, typically single, Trotter steps, were examined by quantum circuit simulators.
We propose an efficient O( N 2 )-parameter ansatz that consists of a sequence of exponential operators, each of which is a unitary variant of Neuscamman’s cluster Jastrow operator. The ansatz can also be derived as a decomposition of T 2 amplitudes of the unitary coupled cluster with generalized singles and doubles, which gives a near full-CI energy. The proposed ansatz therefore can reproduce the uCCGSD energy, or rather will reach the exact full-CI energy because of the exponential operator product form. Because the cluster Jastrow operators are expressed by a product of number operators and the derived Pauli operator products, namely, the Jordan–Wigner strings, are all commutative, it does not require the Trotter approximation to implement to a quantum circuit and should be a good candidate for the variational quantum eigensolver algorithm of a near-term quantum computer. The accuracy of the ansatz was examined for dissociation of a nitrogen dimer, and compared with other existing O( N 2 )-parameter ansatzs. Not only the original ansatzs defined in the second-quantization form but also their Trotter-splitting variants, in which the cluster amplitudes are optimized to minimize the energy obtained with a few, typically single, Trotter steps, were examined by quantum circuit simulators.
Near-term quantum devices require wavefunction ansätze that are expressive while also of shallow circuit depth in order to both accurately and efficiently simulate molecular electronic structure. While unitary coupled cluster (e.g., UCCSD) has become a standard, the high gate count associated with the implementation of this limits its feasibility on noisy intermediate-scale quantum (NISQ) hardware. K-fold unitary cluster Jastrow (uCJ) ansätze mitigate this challenge by providing O(kN2) circuit scaling and favorable linear depth circuit implementation. Previous work has focused on the real orbital-rotation (Re-uCJ) variant of uCJ, which allows an exact (Trotter-free) implementation. Here we extend and generalize the k-fold uCJ framework by introducing two new variants, Im-uCJ and g-uCJ, which incorporate imaginary and fully complex orbital rotation operators, respectively. Similar to Re-uCJ, both of the new variants achieve quadratic gate-count scaling. Our results focus on the simplest k=1 model, and show that the uCJ models frequently maintain energy errors within chemical accuracy. Both g-uCJ and Im-uCJ are more expressive in terms of capturing electron correlation and are also more accurate than the earlier Re-uCJ ansatz. We further show that Im-uCJ and g-uCJ circuits can also be implemented exactly, without any Trotter decomposition. Numerical tests using k=1 on H2, H3+, Be2, C2H4, C2H6 and C6H6 in various basis sets confirm the practical feasibility of these shallow Jastrow-based ansätze for applications on near-term quantum hardware.
High Resolution Image Download MS PowerPoint Slide Quantum computers have the potential to efficiently solve the electronic structure problem but are currently limited by noise and shallow circuits. We present an enhanced Variational Quantum Eigensolver (VQE) ansatz based on the Qubit Coupled Cluster (QCC) approach that requires optimization of only n parameters, where n is the number of Pauli string generators, rather than the typical n + 2 m parameters, where m is the number of qubits. We evaluate the ground state energies and molecular dissociation curves of strongly correlated molecules, namely O 3 and Li 4, using active spaces of varying sizes in conjunction with our enhanced QCC ansatz, Unitary Coupled Cluster Single–Double (UCCSD) ansatz, and the classical Coupled Cluster Singles and Doubles (CCSD) method. Compared to UCCSD, our approach significantly reduces the number of parameters while maintaining high accuracy. Numerical simulations demonstrate the effectiveness of our approach, and experiments on superconducting and trapped-ion quantum computers showcase its practicality on real hardware. By eliminating the need for symmetry-restoring gates and reducing the number of parameters, our enhanced QCC ansatz enables accurate quantum chemistry calculations on near-term quantum devices for strongly correlated systems.
The unitary cluster Jastrow (UCJ) ansatz and its variant known as local UCJ (LUCJ) are promising choices for variational quantum algorithms for chemistry due to their combination of physical motivation and hardware efficiency. The parameters of these ansatzes can be initialized from the output of a coupled cluster, singles and doubles (CCSD) calculation performed on a classical computer. However, truncating the number of repetitions of the ansatz, as well as discarding interactions to accommodate the connectivity constraints of near-term quantum processors, degrade the approximation to CCSD and the resulting energy accuracy. In this work, we propose two methods to improve the parameter initialization. The first method, which is applicable to both expectation value- and sample-based algorithms, uses compressed double factorization of the CCSD amplitudes to improve or recover the CCSD approximation. The second method, which is applicable to sample-based algorithms, uses approximate tensor network simulation to improve the quality of samples produced by the ansatz circuit. We validate our methods using exact state vector simulation on systems of up to 52 qubits, as well as experiments on superconducting quantum processors using up to 65 qubits. Our results indicate that our methods can significantly improve the output of both expectation value- and sample-based quantum algorithms.
The variational quantum eigensolver (VQE) has emerged as one of the most promising near-term quantum algorithms that can be used to simulate many-body systems such as molecular electronic structures. Serving as an attractive ansatz in the VQE algorithm, unitary coupled cluster (UCC) theory has seen a renewed interest in recent literature. However, unlike the original classical UCC theory, implementation on a quantum computer requires a finite-order Suzuki-Trotter decomposition to separate the exponentials of the large sum of Pauli operators. While previous literature has recognized the nonuniqueness of different orderings of the operators in the Trotterized form of UCC methods, the question of whether or not different orderings matter at the chemical scale has not been addressed. In this Letter, we explore the effect of operator ordering on the Trotterized UCCSD ansatz, as well as the much more compact k -UpCCGSD ansatz recently proposed by Lee et al. [ J. Chem. Theory Comput., 2019, 15, 311. arXiv, 2019, quant-ph:1909.09114. https://arxiv.org/abs/1909.09114 ]. We observe a significant, system-dependent variation in the energies of Trotterizations with different operator orderings. The energy variations occur on a chemical scale, sometimes on the order of hundreds of kcal/mol. This Letter establishes the need to define not only the operators present in the ansatz but also the order in which they appear. This is necessary for adhering to the quantum chemical notion of a “model chemistry”, in addition to the general importance of scientific reproducibility. As a final note, we suggest a useful strategy to select out of the combinatorial number of possibilities, a single well-defined and effective ordering of the operators.
The variational quantum eigensolver is one of the most promising algorithms for near-term quantum computers. It has the potential to solve quantum chemistry problems involving strongly correlated electrons with relatively low-depth circuits, which are otherwise difficult to solve on classical computers. The variational eigenstate is constructed from a number of factorized unitary coupled-cluster terms applied onto an initial (single-reference) state. Current algorithms for applying one of these operators to a quantum state require a number of operations that scale exponentially with the rank of the operator. We exploit a hidden SU(2) symmetry to allow us to employ the linear combination of unitaries approach, Our Prepare subroutine uses n+2 ancilla qubits for a rank-n operator. Our Select(U^) scheme uses O(n)Cnot gates. This results in a full algorithm that scales like the cube of the rank of the operator n3, a significant reduction in complexity for rank five or higher operators. This approach, when combined with other algorithms for lower-rank operators (when compared to the standard implementation), will make the factorized form of the unitary coupled-cluster approach much more efficient to implement on all types of quantum computers.
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.