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.
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.
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.
Sample-based quantum diagonalization (SQD), equivalently quantum-selected configuration interaction (QSCI), has become a centre of gravity of pre-fault-tolerant quantum chemistry: a processor samples electronic configurations and the Hamiltonian is diagonalized classically in the resulting subspace. Accuracy is governed entirely by which configurations enter it -- a machine-learning selection problem, made acute by a coupon-collector bottleneck. We review the generative and learned selectors by what each generates and the signal it exploits, and identify one gap: no reward-proportional generative-flow-network proposer has been built for tail discovery. On the field's central question -- whether the quantum sampler beats classical selected CI -- the negative verdict is not ours to claim: priority belongs to Reinholdt et al. [JCTC 21, 6811 (2025)], and polynomial-time classical estimation of the flagship circuits has reinforced it. We state that verdict at the precision a falsifiable claim requires -- it concerns reproducible, same-active-space comparisons on molecular electronic structure -- and weigh the claims outside those qualifiers. We show that alpha-string weights are not invariant under rotations inside degenerate orbital shells, so determinant counts are undefined until the orbital gauge is declared. We distil a ten-element benchmarking standard and apply it to our own deposit, which returned defects that changed numbers printed here and retracted one from v1. FCI-exact experiments confirm one prediction and refute another: the single generative advantage we find keeps no consistent sign along the dissociation coordinate at device-calibrated noise and reverses under a symmetric readout model. It does beat a noise-matched classical recovery loop on N2 by a margin five seeds cannot resolve, and loses by over a factor of two to a classical selector that needs no sampler.
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) 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.
Recently, sample-based quantum diagonalization (SQD) has emerged as a promising approach to compute ground and excited states of problem Hamiltonians.This method classically diagonalizes a Hamiltonian in a subspace that is spanned by samples obtained from a quantum computer. However, by its nature, SQD suffers from a fundamental sampling problem, as some basis states that are required for a targeted accuracy may only be sampled extremely rarely. To alleviate this limitation, we introduce the SQD-AA algorithm that combines SQD with amplitude amplification (AA). SQD-AA uses AA to sequentially reduce probabilities of already measured bitstrings, thus making the observation of new ones more likely. We observe a reduction in the total query complexity of more than a factor 100 for algebraically and exponentially decaying model distributions, and analytically show a quadratic advantage for the latter. Moreover, we evaluate real molecules in an early fault-tolerant scenario and compare SQD-AA to SQD and iterative quantum phase estimation (iQPE). For all considered examples, we observe the lowest total number of T-gates for SQD-AA while only requiring circuits that are 3-4 orders of magnitude shallower than those needed for iQPE. Given this substantial reduction in circuit depth compared to iQPE while saving 2 orders of magnitude in total runtime compared to SQD, we expect a significant regime in early fault-tolerance where SQD-AA runs feasibly, but iQPE circuits are too deep to execute confidently.
Subspace diagonalization techniques based on quantum sampling, such as quantum selected configuration interaction (QSCI) and sample-based quantum diagonalization (SQD), have recently emerged as promising quantum-centric approaches for approximating ground-state energies of many-body systems. However, their performance is fundamentally limited by an intrinsic trade-off between sampling efficiency and the sparsity of the ground-state wavefunction, which becomes particularly severe in strongly correlated systems. Here, we introduce a filter-assisted SQD protocol that engineers wavefunction sparsity via a quantum filter, i.e., a unitary transformation of the Hamiltonian designed to concentrate the ground-state weight onto a small number of computational basis states. Using the Gini coefficient as a robust sparsity measure, we establish a quantitative relationship between wavefunction sparsity and the resource requirements of SQD, providing theoretical bounds on the required subspace dimension and sampling cost. To realize the quantum filter, we employ a tensor-network-based circuit-encoding algorithm that maps target states to quantum circuits with controllable fidelity. We benchmark our approach on the quantum Ising model with transverse and longitudinal fields using both numerical simulations and quantum hardware experiments. Our results demonstrate that, compared with standard SQD, the proposed protocol significantly enhances wavefunction sparsity, reduces ground-state energy estimation errors by orders of magnitude, and substantially lowers sampling overhead. These findings establish filter-assisted subspace diagonalization as a powerful and scalable framework for quantum many-body calculations in the strongly correlated regime.