In the context of quantum computing, efficient resource management is crucial for optimizing throughput on cloud-based platforms and maximizing hardware utilization. In the present work, we propose an approach to tackle quantum chemistry problems via quantum multi-programming of the Local Unitary Cluster Jastrow (LUCJ) ansätze. The ground-state energy of the molecular system is obtained via Sample-based quantum diagonalization (SQD), further refined by its extended version (ext-SQD). Building upon the Qiskit Experiments package, which already supports parallel execution functionality for general tasks, we developed a novel parallel experiment class tailored for quantum chemistry problems. Cross-talk is a known issue in the multi-programming frameworks and can corrupt the ground-energy estimation of the simulated systems. To assess its impact within our approach, we simulated two conformations of the ethanol molecule: one at the equilibrium state (EtOH$_{Eq}$), and one with the O-H bond stretched to 1.2 ${Å}$ (EtOH$_{1.2}$). We defined three different layouts that we executed in a randomized fashion, alternating serial and parallel execution within 10 independent replicates. The single modality of each circuit was kept as a baseline to evaluate the effect of cross-talk induced by quantum multi-programming. The energies obtained at the first-, last- and ext-SQD iteration were compared to the classical Heat-bath Configuration Interaction (HCI) reference. Our findings highlight the viability of a quantum multi-programming workflow for quantum chemistry as the robust post-processing protocol effectively mitigates possible cross-talk induced noise. At the final step of the configuration recovery process, the energy difference relative to the HCI reference is negligible, within 0.001 kcal/mol.
In the context of quantum computing, efficient resource management is crucial for optimizing throughput on cloud-based platforms and maximizing hardware utilization. In the present work, we propose an approach to tackle quantum chemistry problems via quantum multi-programming of the Local Unitary Cluster Jastrow (LUCJ) ansätze. The ground-state energy of the molecular system is obtained via Sample-based quantum diagonalization (SQD), further refined by its extended version (ext-SQD). Building upon the Qiskit Experiments package, which already supports parallel execution functionality for general tasks, we developed a novel parallel experiment class tailored for quantum chemistry problems. Cross-talk is a known issue in the multi-programming frameworks and can corrupt the ground-energy estimation of the simulated systems. To assess its impact within our approach, we simulated two conformations of the ethanol molecule: one at the equilibrium state (EtOHEq), and one with the O-H bond stretched to 1.2 A˚ (EtOH1.2). We defined three different layouts that we executed in a randomized fashion, alternating serial and parallel execution within 10 independent replicates. The single modality of each circuit was kept as a baseline to evaluate the effect of cross-talk induced by quantum multi-programming. The energies obtained at the first-, last- and ext-SQD iteration were compared to the classical Heat-bath Configuration Interaction (HCI) reference. Our findings highlight the viability of a quantum multi-programming workflow for quantum chemistry as the robust post-processing protocol effectively mitigates possible cross-talk induced noise. At the final step of the configuration recovery process, the energy difference relative to the HCI reference is negligible, within 0.001 kcal/mol.
We present a large-scale experimental study of quantum-computing-based molecular simulation carried out on IQM's Sirius 24-qubit superconducting processor, utilizing up to 16 operational qubits. The work employs Sample-based Quantum Diagonalization (SQD) together with the Local Unitary Cluster Jastrow (LUCJ) ansatz to estimate ground-state energies for a set of benchmark molecules, including H2, LiH, BeH2, H2O, and NH3. In addition, we introduce a Linear-CNOT variant of the Unitary Coupled-Cluster Singles and Doubles (LCNot-UCCSD) ansatz within the SQD workflow, trading higher circuit depth for reduced classical preprocessing. A comparison between these ansätze is provided, clarifying their respective strengths, limitations, and suitability for near-term quantum hardware. We further explore potential energy landscapes through 1D scans for H2 and HeH+ using both STO-3G and 6-31G basis sets, and for LiH and BeH2 in STO-3G. Extending beyond this, we demonstrate the experimental construction of a full 2D potential energy surface for the water molecule on quantum hardware, mapped over a 32 × 32 grid in bond length and bond angle. To move beyond small benchmark systems, we combine SQD(LUCJ) with Density Matrix Embedding Theory (DMET) to compute active-space energies for a set of ligand-like molecules, as well as the pharmacologically relevant amantadine system. Across all studies, the majority of quantum-computed energies agree with reference FCI results, as well as with DMET-CASCI energies for embedded systems, to within chemical accuracy for the chosen basis sets. These results demonstrate the reliability of sample-based diagonalization approaches and underscore the potential of hybrid embedding strategies for extending quantum simulations to increasingly complex molecular systems, while also highlighting their practicality on current IQM quantum hardware.
Recent experiments on quantum computers have challenged the limits of classical computation in chemistry, simulating ground states of strongly correlated molecules. Many of these experiments have utilized the unitary cluster Jastrow ansatz, a quantum circuit inspired by the unitary coupled cluster ansatz that can be tailored to current quantum hardware. Notably, the largest experiment in Sci. Adv. 11, 25 (2025) executed a quantum circuit with 77 qubits and 10,570 gates on an IBM quantum computer and performed classical post-processing with up to 6400 nodes on Fugaku to compute ground state energies better than Hartree-Fock. In this work, we present a polynomial time classical algorithm to compute the energy of any single-layer unitary cluster Jastrow circuit, independent of locality constraints for quantum hardware. Our algorithm can reproduce the largest experiment from Sci. Adv. 11, 25 (2025) in less than a minute on a laptop, and through circuit optimization enabled by fast simulation we achieve a lower ground state energy than the experiment.
In this study, we analyze the choice of local unitary cluster Jastrow (LUCJ) ansatz initialization and sensitivity of the sample-based quantum diagonalization (SQD) algorithm within the quantum-centric supercomputing (QCSC) framework. We examine six initialization strategies, including those based on coupled-cluster singles and doubles (CCSD), Møller-Plesset second-order perturbation theory (MP2), data-driven coupled-cluster (DDCC), and trivial (zeroes and random) initializations, across twelve molecular systems and three basis sets (STO-3G, cc-pVDZ, and aug-cc-pVDZ). We find that while the mean absolute percentage errors (MAPEs) between the alternative and CCSD-initialized t2-amplitudes span many orders of magnitude, the resulting SQD energies are largely insensitive to this variation. In particular, most initializations recover energies within chemical accuracy (+/-1.6 mEh) of the CCSD reference, with convergence improving as the basis set size increases. Notably, random initialization achieves performance competitive with CCSD across all basis sets, while zeroes initialization, despite having smaller deviations from CCSD, yields the worst energy agreement. Our results highlight that the proximity to the CCSD initialization is not a reliable predictor of the quality of electronic energies. These findings establish that configuration recovery within SQD, rather than circuit initialization, is the dominant factor governing energy accuracy, and suggest that computationally cheaper initialization strategies are viable alternatives to CCSD for QCSC workflows
We demonstrate a quantum-classical workflow for ab initio molecular dynamics (AIMD) in which quantum measurements from a chemistry-inspired LUCJ ansatz are post-processed using Sample-based Quantum Diagonalization (SQD) to recover determinant subspaces and deliver energies and analytical nuclear gradients for dynamics. As an exact benchmark, we use full configuration interaction (FCI) in the STO-3G basis, enabling a direct assessment of the accuracy of SQD. In gas-phase benchmarks, SQD reproduces FCI energies and gradients to within 1 kcal mol−1 of the FCI reference and yields stable AIMD trajectories. In explicit-solvent QM/MM simulations, SQD retains this agreement, matching FCI energy fluctuations and RMS gradient profiles and reproducing solute-solvent structure as quantified by radial distribution functions. Overall, these benchmarks establish LUCJ+SQD as a practical route for integrating current quantum hardware into QM/MM molecular dynamics and provide an early demonstration of condensed-phase QM/MM dynamics driven by a quantum electronic-structure engine.
Sample-based quantum diagonalization (SQD) offers a powerful route to accurate quantum chemistry on noisy intermediate-scale quantum (NISQ) devices by combining quantum sampling with classical diagonalization. Here we introduce HSQD, a novel half-qubit SQD approach that halves the qubit requirement for simulating a chemical system and drastically reduces overall circuit depth and gate counts, suppressing hardware noise. When modeling the dissociation of the nitrogen molecule with a (10e, 26o) active space, HSQD matches the accuracy of SQD on IBM quantum hardware using only half the number of qubits and 40% fewer measurements. We further enhance HSQD with a heat-bath configuration interaction (HCI) inspired selection of the samples, forming HCI-HSQD. This yields sub-millihartree accuracy across the N2 potential energy surface and produces subspaces up to 39% smaller than those from classical HCI, showing a significant improvement in the compactness of the ground-state representation. Finally, we demonstrate the scalability of HCI-HSQD using iron-sulfur clusters, reaching active spaces of up to (54e, 36o) while using only half as many qubits as the original SQD. For these systems, HCI-HSQD reduces SQD energy errors by up to 76% for [2Fe-2S] and 26% for [4Fe-4S], while also reducing subspace sizes, halving measurement requirements, and eliminating expensive post-processing. Together, these results establish half-qubit SQD as a noise-resilient and resource-efficient pathway toward practical quantum advantage in strongly correlated chemistry.
The accurate treatment of electron correlation in extended molecular systems remains computationally challenging using classical electronic structure methods. Hybrid quantum-classical algorithms offer a potential route to overcome these limitations; however, their practical deployment on existing quantum computers requires strategies that both reduce problem size and mitigate hardware noise. In this work, we investigate ground-state energy calculations of ligand-like molecules using Sample-based Quantum Diagonalization (SQD) within the Density Matrix Embedding Theory (DMET) framework, focusing on low-symmetry systems with diverse bonding motifs that exhibit subsystem-dependent variations in fragment-environment entanglement. These entanglement-based variations directly influence bath orbital construction, impurity sizes, and the structure of the embedded Hamiltonians, posing nontrivial challenges for both embedding and quantum sampling. By combining DMET fragmentation with SQD-based construction of reduced configuration spaces through quantum sampling and iterative configuration recovery, we perform quantum simulations on IBM's Eagle R3 (IBM Sherbrooke) and IBM's Heron R3 (IBM Boston) superconducting quantum hardware thereby, showing that the entanglement structure across embedding subsystems plays a central role in determining the efficiency and accuracy of the simulations. Despite these complexities, we show that the DMET-SQD framework yields ground-state energies in strong agreement with DMET-FCI benchmarks, achieving chemical accuracy (1 kcal/mol) across all systems studied. These results demonstrate that SQD-based quantum simulations can be robustly extended to low-symmetry, chemically realistic, industry relevant molecules, and highlight the importance of entanglement-aware embedding strategies for scalable quantum electronic structure calculations.