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Variational quantum eigensolvers are touted as a near-term algorithm capable of impacting many applications. However, the potential has not yet been realized, with few claims of quantum advantage and high resource estimates, especially due to the need for optimization in the presence of noise. Finding algorithms and methods to improve convergence is important to accelerate the capabilities of near-term hardware for variational quantum eigensolver or more broad applications of hybrid methods in which optimization is required. To this goal, we look to use modern approaches developed in circuit simulations and stochastic classical optimization, which can be combined to form a surrogate optimization approach to quantum circuits. Using an approximate (classical central processing unit/graphical processing unit) state vector simulator as a surrogate model, we efficiently calculate an approximate Hessian, which is passed as input for a quantum processing unit or exact circuit simulator. This method will lend itself well to parallelization across quantum processing units. We demonstrate the capabilities of such an approach with and without sampling noise and a proof-of-principle demonstration on a quantum processing unit utilizing 40 qubits.
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http://dx.doi.org/10.1073/pnas.2408530122 | DOI Listing |
J Chem Theory Comput
September 2025
Donostia International Physics Center (DIPC), 20018 Donostia, Euskadi, Spain.
The adaptive derivative-assembled problem-tailored variational quantum eigensolver (ADAPT-VQE) is one of the most widely used algorithms for electronic structure calculations in quantum computers. It adaptively selects operators based on their gradient, constructing ansätze that continuously evolve to match the energy landscape, helping avoid local traps and barren plateaus. However, this flexibility in reoptimization can lead to the inclusion of redundant or inefficient operators that have almost zero parameter value, barely contributing to the ansatz.
View Article and Find Full Text PDFJ Chem Theory Comput
September 2025
Department of Chemistry, Virginia Tech, Blacksburg, Virginia 24061, United States.
In this work, we combine the recently developed double unitary coupled cluster (DUCC) theory with the adaptive, problem-tailored variational quantum eigensolver (ADAPT-VQE) to explore the accuracy of unitary downfolded Hamiltonians for quantum simulation of chemistry. We benchmark the ability of DUCC effective Hamiltonians to recover dynamical correlation energy outside of an active space. We consider the effects of strong correlation, commutator truncation, higher-body terms, and approximate external amplitudes on the accuracy of these effective Hamiltonians.
View Article and Find Full Text PDFJ Org Chem
September 2025
Department of Chemistry, University of San Francisco, 2130 Fulton St., San Francisco, California 94117, United States.
Understanding the kinetics of reactions in biosynthetic pathways requires accounting for the contribution of quantum mechanical tunneling to the rates. Whereas hydrogen tunneling in biology is well established, the extent of heavy-atom tunneling in biochemical reactions has been very little studied. We report computational results (M06-2X/cc-pVDZ) on rate constants for electrocyclic ring closures and [3,3] sigmatropic shifts, processes dominated by heavy-atom motions, that are proposed steps in the biosynthesis of four representative natural products.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
September 2025
Applied Physics Group, NASA Ames Research Center, Moffett Field, CA 94035.
Variational quantum eigensolvers are touted as a near-term algorithm capable of impacting many applications. However, the potential has not yet been realized, with few claims of quantum advantage and high resource estimates, especially due to the need for optimization in the presence of noise. Finding algorithms and methods to improve convergence is important to accelerate the capabilities of near-term hardware for variational quantum eigensolver or more broad applications of hybrid methods in which optimization is required.
View Article and Find Full Text PDFSci Rep
August 2025
Department of Computer Science, University of Tsukuba, Tsukuba, 3058577, Japan.
Deep learning has achieved significant success in pattern recognition, with convolutional neural networks (CNNs) serving as a foundational architecture for extracting spatial features from images. Quantum computing provides an alternative computational framework, a hybrid quantum-classical convolutional neural networks (QCCNNs) leverage high-dimensional Hilbert spaces and entanglement to surpass classical CNNs in image classification accuracy under comparable architectures. Despite performance improvements, QCCNNs typically use fixed quantum layers without incorporating trainable quantum parameters.
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