The Variational Quantum Eigensolver (VQE) is a leading algorithm for noisy intermediate-scale quantum (NISQ) devices, but its adaptive variants (e.g., ADAPT-VQE) suffer from severe classical simulation bottlenecks during the ansatz growth phase. Representing and exponentiating pool operators for multi-qubit systems constructs massive sparse matrices that quickly scale to millions of elements, choking classical memory bandwidth and CPU/GPU cycle capacity. In this work, we present a resource-efficient software-layer framework that completely bypasses dense matrix exponentiation by evaluating state updates through a deterministic fifth-order (O(5)) Taylor series expansion. This approach reframes the costly unitary evolution into a chained sequence of five lightweight, successive sparse matrix-vector multiplications scaling strictly as O(Nz), where Nz is the number of non-zero elements. We validate our framework using equilibrium BeH2 (14 qubits), equilibrium H2O (12 qubits), and strongly correlated asymmetrically stretched H2O molecular profiles under both Jordan-Wigner (JW) and Bravyi-Kitaev (BK) transformations. The simulation results demonstrate that the O(5) truncation maintains exceptional numerical fidelity, retaining a state fidelity > 0.999999 and matching absolute ground state energies down to subchemical accuracy, while effortlessly navigating matrix spaces exceeding 268 million structural elements. This framework provides a scalable, high-performance pathway for executing deep variational simulations on hardware platforms with constrained computational budgets.
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7 pages, submitted to IEEE Transactions on Quantum Engineering
The Variational Quantum Eigensolver (VQE) is a leading algorithm for noisy intermediate-scale quantum (NISQ) devices, but its adaptive variants (e.g., ADAPT-VQE) suffer from severe classical simulation bottlenecks during the ansatz growth phase. Representing and exponentiating pool operators for multi-qubit systems constructs massive sparse matrices that quickly scale to millions of elements, choking classical memory bandwidth and CPU/GPU cycle capacity. In this work, we present a resource-efficient software-layer framework that completely bypasses dense matrix exponentiation by evaluating state updates through a deterministic fifth-order (O(5)) Taylor series expansion. This approach reframes the costly unitary evolution into a chained sequence of five lightweight, successive sparse matrix-vector multiplications scaling strictly as O(Nz), where Nz is the number of non-zero elements. We validate our framework using equilibrium BeH2 (14 qubits), equilibrium H2O (12 qubits), and strongly correlated asymmetrically stretched H2O molecular profiles under both Jordan-Wigner (JW) and Bravyi-Kitaev (BK) transformations. The simulation results demonstrate that the O(5) truncation maintains exceptional numerical fidelity, retaining a state fidelity > 0.999999 and matching absolute ground state energies down to subchemical accuracy, while effortlessly navigating matrix spaces exceeding 268 million structural elements. This framework provides a scalable, high-performance pathway for executing deep variational simulations on hardware platforms with constrained computational budgets.
The Variational Quantum Eigensolver (VQE) and its adaptive variants, such as ADAPT-VQE, are central to the study of strongly correlated quantum systems. However, the classical simulation of the ansatz growth process remains constrained by the exponential scaling of operator space and the associated computational cost of unitary evolution. We introduce the Greedy Operator Commutativity Partitioning (GOCP) framework, an analytical methodology designed to optimize both operator selection and state evolution. By reformulating complex unitary rotations as a chained sequence of fifth-order O(5) Taylor series expansions, GOCP bypasses the need for explicit matrix exponentiation, reducing the computational task to a sequence of sparse matrix-vector operations. We evaluate the performance of this framework across diverse molecular systems, including BeH2 and strongly correlated H2O geometries, utilizing both Jordan-Wigner and Bravyi-Kitaev mappings. Our results demonstrate that the GOCP framework maintains exceptional numerical fidelity-exceeding 1 - 10^-6 in state fidelity-while achieving sub-chemical accuracy in ground-state energy calculations. By enabling the simulation of operator manifolds exceeding 2.68 x 10^8 elements with high efficiency, this approach provides a scalable and rigorous pathway for exploring deep variational circuits in complex quantum many-body systems.
Fixed-ansatz Variational Quantum Eigensolvers (VQE), such as the Unitary Coupled Cluster with Singles and Doubles (UCCSD) framework, frequently suffer from severe initialization paralyzation and zero-gradient traps when evaluated using the non-local Bravyi-Kitaev (BK) fermion-to-qubit mapping. In this work, we systematically demonstrate how the Adaptive Derivative-Assembled Pseudo-Trotter (ADAPT-VQE) framework shatters these structural limitations across three distinct electronic and geometric molecular pillars: Lithium Hydride (LiH), Hydrogen Fluoride (HF), and Water (H2O), under heavily stretched or asymmetric multi-reference configurations. While conventional UCCSD-VQE flatlines completely at a zero energy shift (0.000000~Ha) due to global phase cancellations inherent to the BK tree structures, our dynamic ADAPT-VQE loop successfully isolates the dominant symmetry-breaking operators using analytical commutator gradients. To bypass the severe O(N3) computational bottlenecks of dense matrix exponentiation and Singular Value Decomposition on larger registers, we implement a highly optimized, vector-based Taylor series expansion state-evolution engine. Our numerical results show that the accelerated ADAPT-VQE framework achieves instant, exact Full Configuration Interaction (FCI) convergence within the very first macro-cycle across all three molecular systems, maintaining absolute numerical stability up to a 12-qubit register space. This study establishes a robust, hardware-efficient path for simulating strongly correlated, highly polarized triatomic chemical environments on near-term local architectures.
While Variational Quantum Eigensolver (VQE) variants are among the leading candidates for electronic structure calculations on quantum computers, gradient-based operator selection limits their scalability. To solve this, we introduce the Hamiltonian-gradient-free VULCAN (Variational Upbuilding, Layered Compression, Adaptive N-body perturbation) layered VQE framework. Our method dynamically generates ansatz operators using Variational Double Bracket Flow (VDBF) equations. Combined with a linearly scaling minimal complete pool, it creates a pool 4-12 times smaller than QEB (Qubit-Excitation-Based) pools. By appending entire layers simultaneously, Hamiltonian gradient measurements are completely eliminated. Circuit depth is managed via a grow-then-compress scheme using efficient state-overlap measurements, and qubit requirements are reduced by projecting the Hamiltonian onto a dominant-determinant subspace. Using high-performance emulation up to 32 logical qubits, we achieve chemical accuracy at just 5-20% of the measurement cost of batched ADAPT-VQE for hydrogen chains, BeH2 and H2O. For the 32-qubit C3H6, where batched ADAPT-VQE does not reach chemical accuracy, a single VULCAN layer combined with a GPU-accelerated stochastic Epstein-Nesbet (ENPT2) correction does. This stochastic ENPT2 post-processing step enables early termination at chemical accuracy.
While fermion-to-qubit isomorphisms are mathematically invariant under exact unitary statevector transformations, their physical implementation on noisy intermediate-scale quantum (NISQ) devices introduces severe, practical measurement bottlenecks. In this work, we systematically investigate the measurement efficiency of adaptive derivative-assembled pseudo-trotter variational quantum eigensolver (ADAPT-VQE) algorithms across three critical molecular benchmarks (LiH, BeH2, and H2O) at stretched bond lengths (2xRe) covering distinct point-group symmetries. First, we establish exact representation invariance across all target multi-reference geometries, demonstrating that operator pool gradients and statevector electronic energies remain strictly isomorphic under exact mathematical execution (E(LiH) = -7.691469 Ha, E(BeH2) = -15.110110 Ha, and E(H2O) = -74.566874 Ha). Second, we quantify the hardware measurement overhead by partitioning operator pool observables into qubit-wise commuting (QWC) tensor-product basis (TPB) cliques. We reveal that while both Jordan-Wigner (JW) and Bravyi-Kitaev (BK) encodings yield identical total Pauli term counts across the singlet excitation manifold (128 terms for H2O and BeH2), the hierarchical binary-tree layout of the BK mapping dramatically compresses the required measurement circuits---achieving up to a 45.31% reduction in total hardware execution steps compared to 12.50% under JW. Our findings demonstrate that tree-structured mappers serve as implicit, highly efficient measurement-packing engines for adaptive quantum simulations without altering the underlying variational trajectory.
Simulating strongly correlated molecular systems on near-term quantum hardware remains challenging because current hardware offers limited quantum volume and moderate-fidelity qubits. One way to address this challenge is through bootstrap embedding (BE). Bootstrap embedding partitions molecules into smaller fragments that are then embedded in the ``bath'' of other fragments iteratively. Bootstrap embedding is appealing for quantum simulation because fragmentation reduces the qubit requirements of each fragment problem. In this work, we develop a quantum bootstrap embedding (QBE) workflow that uses variational quantum eigensolver (VQE) fragment solvers and examines the algorithmic choices that determine the success of the overall VQE-QBE procedure. To improve efficiency, we introduce FastAdaptVQE, a sparse-matrix-accelerated form of the adaptive variational quantum eigensolver (ADAPT-VQE) that replaces symbolic commutator evaluation with direct statevector calculations, and MatrixFreeAdaptVQE, a matrix-free extension that removes the sparse-matrix memory bottleneck that arises for larger fragments. We also explore modifying the ADAPT-VQE operator-selection step by replacing the purely greedy choice with a lookahead strategy. Benchmarks on H4, F2, and selected geometries of H6 reach chemical accuracy, within 1 kcal/mol of BE results obtained with a full configuration interaction (FCI) solver. For n-butane, density-matching residuals converged, but energy errors remained outside chemical accuracy. These results show that combining QBE with VQE can accurately compute molecular energies, while density convergence alone does not ensure energy accuracy. This work lays the foundation for extending these energy calculations to larger molecular systems and quantum materials on near-term quantum hardware.
We introduce the Cyclic Variational Quantum Eigensolver (CVQE), a hardware-efficient framework for accurate ground-state quantum simulation on noisy intermediate-scale quantum (NISQ) devices. CVQE departs from conventional VQE by incorporating a measurement-driven feedback cycle: Slater determinants with significant sampling probability are iteratively added to the reference superposition, while a fixed entangler (e.g., single-layer UCCSD) is reused throughout. This adaptive reference growth systematically enlarges the variational space in most promising directions, avoiding manual ansatz or operator-pool design, costly searches, and preserving compile-once circuits. The strategy parallels multi-reference methods in quantum chemistry, while remaining fully automated on quantum hardware. Remarkably, CVQE exhibits a distinctive staircase-like descent pattern, where successive energy drops sharply signal efficient escape from barren plateaus. Benchmarks show that CVQE consistently maintains chemical precision across correlation regimes, outperforms fixed UCCSD by several orders of magnitude, and achieves favorable accuracy-cost trade-offs compared to the Selected Configuration Interaction. These results position CVQE as a scalable, interpretable, and resource-efficient paradigm for near-term quantum simulation.