Sample-based Quantum Diagonalization (SQD) is a hybrid quantum-classical method that replaces variational optimization with a self-consistent recovery loop over QPU samples. Although SQD is considered robust to noisy samples and imperfect classical inputs, its robustness across practical deployment choices has not been systematically analyzed. As a result, shot budgets, qubit layouts, noise mitigation strategies, and the coupled-cluster singles and doubles (CCSD) amplitudes that initialize the ansatz are often chosen without clear empirical guidance. We analyze SQD robustness on IBM Heron hardware across these dimensions. Structured CCSD-amplitude perturbations, including complete zeroing, produce only modest energy shifts from the clean baseline. Differences across layouts and noise-mitigation settings are large in the first recovery iteration but narrow within a few iterations. Accuracy saturates at moderate shot budgets, while very large budgets slightly worsen recovered energies, likely because working-set selection limits the value of additional samples. These results identify where SQD provides genuine deployment robustness and where its limits remain.
Sample-based Quantum Diagonalization (SQD) is a hybrid quantum-classical method that replaces variational optimization with a self-consistent recovery loop over QPU samples. Although SQD is considered robust to noisy samples and imperfect classical inputs, its robustness across practical deployment choices has not been systematically analyzed. As a result, shot budgets, qubit layouts, noise mitigation strategies, and the coupled-cluster singles and doubles (CCSD) amplitudes that initialize the ansatz are often chosen without clear empirical guidance. We analyze SQD robustness on IBM Heron hardware across these dimensions. Structured CCSD-amplitude perturbations, including complete zeroing, produce only modest energy shifts from the clean baseline. Differences across layouts and noise-mitigation settings are large in the first recovery iteration but narrow within a few iterations. Accuracy saturates at moderate shot budgets, while very large budgets slightly worsen recovered energies, likely because working-set selection limits the value of additional samples. These results identify where SQD provides genuine deployment robustness and where its limits remain.
Sampling-based quantum diagonalization method exploits Quantum-centric supercomputing platforms to sample bitstrings for Hamiltonian projection on a quantum computer, and then classically diagonalize the Hamiltonian to estimate the eigenvalues and eigenvectors. In current quantum devices an algorithm is useful when shallow quantum circuits with error mitigation support can discover better results while having either a proof of convergence or some method to explain trust in experiment. In this paper, we introduce DF-SQD, a hybrid algorithm that derives deterministic auxiliary-field circuits from selected double-factorization leaves of the two-electron tensor. The circuits propose occupation-number configurations, while selected configuration interaction evaluates the original active-space Hamiltonian and can recentre subsequent proposal rounds. On N2 (32 qubits; 6-31G basis) and a 40-qubit [Fe2S2(SCH3)4]2- active-space Hamiltonian, we show that DF-SQD improves the energy obtained from sampled determinant spaces while using shallow number-preserving circuits in both simulator and hardware runs. For N2, DF-SQD is 45x more accurate with a 11.23\% smaller subspace, and due to its ability to sample better bitstrings at lesser shots it is 2.93x faster than SQD in quantum devices. For the iron-sulfur cluster, DF-SQD generated a subspace dimension of 221M with 400K shots, while SQD needed 1.5M shots to generate a 238M subspace, thus we have better subspace recovery evident from the hardware at 3.75x reduced shots. At a matched 50M subspace dimension, DF-SQD is 1.32x more accurate (achieves a 24.5\% relative error reduction over standard SQD). So overall, our method is able to discover better results with shallower circuits, is sample efficient, uses configuration recovery (so has targeted error mitigation) and we have empirical convergence observation.
Near-term quantum devices provide only finite-shot measurements and prepare imperfect, contaminated states. This motivates algorithms that convert samples into reliable low-energy estimates without full tomography or exhaustive measurements. We propose Active Sampling Sample-based Quantum Diagonalization (AS-SQD), framing SQD as an active learning problem: given measured bitstrings, which additional basis states should be included to efficiently recover the ground-state energy? SQD restricts the Hamiltonian to a selected set of basis states and classically diagonalizes the restricted matrix. However, naive SQD using only sampled states suffers from bias under finite-shot sampling and excited-state contamination, while blind random expansion is inefficient as system size grows. We introduce a perturbation-theoretic acquisition function based on Epstein--Nesbet second-order energy corrections to rank candidate basis states connected to the current subspace. At each iteration, AS-SQD diagonalizes the restricted Hamiltonian, generates connected candidates, and adds the most valuable ones according to this score. We evaluate AS-SQD on disordered Heisenberg and Transverse-Field Ising (TFIM) spin chains up to 16 qubits under a preparation model mixing 80\% ground state and 20\% first excited state. Furthermore, we validate its robustness against real-world state preparation and measurement (SPAM) errors using physical samples from an IBM Quantum processor. Across simulated and hardware evaluations, AS-SQD consistently achieves substantially lower absolute energy errors than standard SQD and random expansion. Detailed ablation studies demonstrate that physics-guided basis acquisition effectively concentrates computation on energetically relevant directions, bypassing exponential combinatorial bottlenecks.
Sample-based Quantum Diagonalization (SQD) recovers ground-state energies by classically diagonalizing a Hamiltonian in the subspace spanned by quantum samples, requiring only bitstrings with sufficient ground-state overlap rather than an accurate variational energy. We reveal and exploit this underexplored robustness property: how much non-Clifford and variational expressivity can be removed from the sampling circuit before SQD accuracy degrades? We answer through two complementary compression techniques: gradient-based operator pruning, which discards low-impact excitation operators, and Clifford rounding, which snaps remaining parameters to the nearest Clifford angle. Both of these techniques can be applied to a VQE ansatz on a qubit-reduced Hamiltonian. A systematic ablation study across 21 molecules shows that median SQD error stays within chemical accuracy even at 50\% compression on both axes, while simulation speedup reaches 33×. Hardware validation on 6 molecules on IBM quantum hardware confirms up to 2.8× transpiled-depth reduction with zero loss in SQD accuracy. Our implementation can be found at: https://github.com/zkysfls/cs-vqe-sqd
Sample-based quantum diagonalization (SQD) is a hybrid quantum-classical algorithm for estimating ground-state energies in electronic-structure calculations. It uses a quantum processor as a sampler to construct a variational subspace, with Hamiltonian projection and diagonalization performed classically. A critical step in SQD is self-consistent particle-number recovery guided by a global reference occupancy vector. In strongly correlated systems, however, dominant determinants can be distributed across regions of determinant space, causing this reference to become mixture-averaged and biasing recovery toward mean occupations. Here, we introduce cluster-adaptive SQD (CSQD), which clusters pooled single-spin strings and performs particle-number recovery using cluster-specific reference occupancy vectors. Under a matched variational budget, CSQD lowers ground-state energies relative to SQD by up to 15.95 mHa for stretched N2 in a (10e,26o) active space and 57.82 mHa for [2Fe-2S] in a (30e,20o) active space. These results suggest that CSQD better captures dispersed occupation structure in strongly correlated systems.
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
A previous report (Okuda, Zenodo DOI: 10.5281/zenodo.22469203) identified a discrete failure mode in sample-based quantum diagonalization (SQD): at low shot counts, classical configuration recovery can lock onto a reproducible but incorrect "wrong attractor," and injecting a single correct configuration into the raw sample can trigger a discrete escape from it. That finding was established on a shallow circuit (N2, CAS(6,6), 166 two-qubit gates) where the wrong-attractor structure itself was directly observable. Here we address two questions left open by that work. First, was the original demonstration merely a sample-size artifact rather than evidence that the specific injected configuration mattered? We answer this with a controlled random-injection experiment (Fe2S2, CAS(12,12), 2053 two-qubit gates, 76-80 independent trials per condition): recovery probability rises from 14.5% with no injection to 100.0% with one pre-specified escape configuration, while a random single-configuration injection of the same size produces only 15.0% recovery, and the escape itself is discrete while the residual energy error continues to improve smoothly with further injected configurations. Second, at circuit depths beyond roughly 1000 two-qubit gates, the wrong-attractor structure itself often becomes too noise-dominated to observe directly, so a practical recovery procedure cannot simply look for and inject "the" known wrong-attractor escape configuration. We present such a procedure: a small set of chemically motivated candidate configurations is generated and injected, and the best candidate is selected using one of three answer-free criteria (variational energy, escape rate from a known baseline attractor, or seed-to-seed energy variance), chosen by a cheap upfront classification of the target system. Across 23 independent hardware-data trials spanning two IBM Quantum backends and 21 distinct molecular systems and active-space combinations, this decision rule selected the correct candidate in all 23 trials, including one case improving accuracy by approximately 1000x. We report this as validation of the decision framework across a broad range of hardware and chemical conditions, not as evidence of answer-free prediction for arbitrary, genuinely unknown multi-reference chemistry, and report the framework's limitations candidly. Open-source implementation: https://github.com/okudat9/escape-config-predictor