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K. Birgitta Whaley

Publications and source records attributed to K. Birgitta Whaley.

At least 19 recordsLinked to original sources
arXiv2026

Reduced scaling implementation of the coupled cluster-based static embedding method, MPCC with density fitting

An improved algorithm to implement our previously proposed static quantum embedding method MPCC (J. Chem. Phys. 161, 164107 (2024)) is presented. It uses the density-fitting (DF) approximation for the electron-repulsion integrals (ERIs) across all layers of the embedding method: the low-level method, the screened interaction, and the high-level method. Additionally, an approximate factorized solution of the Sylvester equation is employed based on the Laplace transformation for the low-level method. To build the screened interaction, we have explored an approximate construction of it based on the distinguishable cluster approximation (DCA) by Kats and Manby (J. Chem. Phys. 141, 061101 (2014)), which amounts to neglecting certain higher-order exchange and ladder diagrams. Combining all these techniques, we have obtained an $\mathcal{O}(N^4)$ algorithm for the low-level method; a non-iterative $N_{\rm frag} \mathcal{O}(N^4)$ algorithm for the screened interaction; and an iterative $\mathcal{O}(N_{\rm frag}^6)$ algorithm for the fragment solver, where $N_{\rm frag}$ is the number of fragment orbitals and $N$ is the total number of orbitals. The resulting low-scaling implementation of the MPCC method is applied to trans polyacetylenes, that is, C$_{2n}$H$_{2n+2}$ molecules for chain lengths $n=1-8$, and the timing and accuracy of the method are compared to the original unfactorized implementation. Moreover, the approximations are further validated by applying the method to the potential energy surface of the \ce{O3} molecule. Finally, we apply the method to the selected molecules in the S22 dataset for which the performance of the MP2 method is known to be poor. The results demonstrate that the DF-based implementation of the MPCC method provides a significant reduction in computational cost while maintaining accuracy comparable to that of the original implementation.

physics.chem-ph↗
arXiv2026

Input-output formulation of quantum light spectroscopy

We develop an input-output formulation of quantum light spectroscopy (QLS) by combining the input-output theory, commonly used in quantum optics, with the perturbative expansion method for nonlinear spectroscopy, commonly used in chemical physics. The use of the input-output relation provides physical intuition for how matter systems alter the photon input field. As examples, we consider linear spectroscopy, fluorescence, intra-beam $G^{(2)}$, and Hong-Ou-Mandel correlation. For certain initial photon states, we show that signal expectation values can be evaluated non-perturbatively. For general initial photon states, the signals can be computed via a perturbative expansion of the input-output relation. The input-output relation reduces the work needed to perturbatively expand the optical signal, allowing for cleaner derivations and clearer physical interpretations.

quant-ph↗
arXiv2026

Normal-ordered perturbative expansion for matter systems interacting with continuous-mode quantum photon fields

We develop a normal-ordered perturbative expansion method to compute the reduced dynamics of a matter system interacting with a general continuous-mode photon field state. In this expansion, all field correlation functions are automatically normal-ordered, while the free evolution is modified by spontaneous emission. Our normal-ordered expansion elucidates the physical meaning of non-normal-ordered correlation terms in the conventional expansion. Furthermore, under intermediate coupling strengths, the normal-ordered expansion converges significantly faster than the conventional expansion, allowing one to extend the applicability of perturbative expansion to much larger matter-light coupling strengths. Interestingly, given an $m$-photon Fock state input, the normal-ordered expansion truncates exactly at the $2m$-th order. For special classes of input states, we show the normal-ordered expansion is consistent with the corresponding master equations. We demonstrate the normal-ordered expansion numerically for a two-level system interacting with coherent state, $m$-photon Fock state, and cat state inputs.

quant-ph↗
arXiv2026

ML-Powered FPGA-based Real-Time Quantum State Discrimination Enabling Mid-circuit Measurements

Accurate and timely quantum state discrimination is critical for quantum computing, particularly in protocols requiring mid-circuit measurement (MCM) and conditional feed-forward. While classical state readout in transistors is near-instantaneous, identifying the state of superconducting qubits remains latency-limited and error-prone. Existing approaches rely on post-processing measurement data transferred to host computers, introducing delays on the order of milliseconds -- vastly exceeding the coherence time of quantum states, which typically last only hundreds of microseconds. To bridge this latency gap, we present an in-situ machine learning (ML) inference engine implemented on a field-programmable gate array (FPGA), enabling real-time quantum state discrimination within 40 ns. Our system supports both two-level (qubit) and three-level (qutrit) systems and performs inference directly on digitized readout signals without host-side intervention. This low-latency operation facilitates mid-circuit measurements, where qubit states are measured and reused within a single quantum circuit, and enables real-time conditional operations essential for quantum error correction. Crucially, fast and accurate mid-circuit readout is a prerequisite for implementing practical fault-tolerant error correction, where errors must be detected and corrected within a single circuit cycle to preserve logical state coherence. We validate our system using superconducting transmon devices, demonstrating robust discrimination fidelity across multiple qubit and qutrit channels. Further, we implement a conditional qutrit logic protocol based on FPGA-resident state classification, highlighting the practical benefits of our approach for NISQ-era quantum algorithms and scalable fault-tolerant architectures.

quant-ph↗
arXiv2026

Improved Measurement Cost Scaling in the Nonorthogonal Quantum Eigensolver

Quantum subspace diagonalization methods are promising algorithms for quantum chemistry on near-term quantum computers. These methods can estimate low-lying energies of molecular systems using shallow quantum circuits, at the cost of many circuit repetitions to estimate the projected matrix elements. Errors in these matrix elements can be converted into much larger eigenvalue errors by an ill-conditioned overlap matrix. We study this bottleneck for the nonorthogonal quantum eigensolver (NOQE), which constructs a compact multireference subspace from dressed unrestricted Hartree-Fock states. We prove a finite-shot perturbation bound showing that, after overlap thresholding, the eigenvalue sensitivity is controlled by the condition number of the retained overlap matrix rather than by a worst-case dimension factor. With a scalable thresholding scheme, the upper bound on the per-matrix-element shot count required to reach a target accuracy scales as $\mathcal{O}(M)$, improving on the previously known $\mathcal{O}(M^3)$ bound, where $M$ is the number of reference states. Numerical experiments on hydrogen chains and rings suggest that, in practice, the measurement cost of structured NOQE instances can grow even more slowly than this linear bound.

quant-ph↗
arXiv2026

Optimal schedule of multi-channel quantum Zeno dragging with application to solving the k-SAT problem

Quantum Zeno dragging enables the preparation of common eigenstates of a set of observables by frequent measurement and adiabatic-like modulation of the measurement basis. In this work, we present a deeper analysis of multi-channel Zeno dragging using generalized measurements, i.e. simultaneously measuring a set of non-commuting observables that vary slowly in time, to drag the state towards a target subspace. For concreteness, we will focus on a measurement-driven approach to solving k-SAT problems as examples. We first compute some analytical upper bounds on the convergence time, including the effect of finite measurement time resolution. We then apply optimal control theory to obtain the optimal dragging schedule that lower bounds the convergence time, for low-dimensional settings. This study provides a theoretical foundation for multi-channel Zeno dragging and its optimization, and also serves as a guide for designing optimal dragging schedules for quantum information tasks including measurement-driven quantum algorithms.

quant-ph↗
arXiv2026

Provable Quantum Speedups for Reaction-Rate Estimation in High-Dimensional Fokker-Planck Dynamics

The Fokker-Planck equation models rare events across sciences, but blue{direct solution of the PDE is intractable for classical computers due to } its high-dimensional nature. Classical stochastic methods circumvent this curse-of-dimensionality, and serve as the de facto standard for practicing computational scientists. Quantum algorithms for such non-unitary dynamics often suffer from exponential decay in success probability. We introduce a quantum algorithm that overcomes this bottleneck for estimating reaction rates {and dynamical correlation functions more generally}. Using a sum-of-squares representation, we develop a Gaussian linear combination of Hamiltonian simulations (Gaussian-LCHS) to represent the non-unitary propagator with $O\left(\sqrt{t\|H\|\log(1/ε)}\right)$ queries to its block encoding. Crucially, we pair this with {a} novel technique to directly estimate matrix elements without exponential decay. For $η$ pairwise interacting particles discretized with $N$ plane waves per degree of freedom, we estimate reactive flux to error $ε$ using $\widetilde{O}\left((η^{5/2}\sqrt{tβ}α_V + η^{3/2}\sqrt{t/β}N)/ε\right)$ quantum gates, where $α_V = \max_{r}|V'(r)/r|$. We further prove that under comparable worst-case analytical guarantees, the sharpest classical bounds for estimating reaction rates via simulation of the associated overdamped Langevin dynamics scale as $O(tη^2 e^{Ω(η)}/ε^4)$, yielding an exponential improvement in $η$, a quartic speedup in $ε$, and quadratic speedup in the time horizon $t$. While classical algorithms may outperform these bounds in practice, this work demonstrates a rigorous route toward quantum advantage for high-dimensional dissipative dynamics.

quant-ph↗
arXiv2026

Efficient Quantum Error Mitigation for Unitary k-Designs

Quantum circuit ensembles that have the properties of unitary k-designs represent applications where there is no obvious bias toward any particular Pauli support, as is the case in simulating systems exhibiting ''quantum chaos,'' which range from quantum dynamics near black holes to gapless spin fluid analysis. However, noisy hardware makes quantum circuits prone to a myriad of error sources, of which depolarizing and coherent error can be particularly destructive. To combat depolarizing error, popular techniques typically involve circuit or gate folding, which can be time-intensive procedures due to increased circuit depth and shot overhead. Other tensor-network-based mitigation techniques suffer from intractability in high-entanglement regimes. In this work, we leverage the structure of unitary k-design Pauli support distributions by introducing a technique we name ''circuit balancing,'' along with gate benchmarking data, in order to estimate circuit-wide depolarization. We describe how to invert the diagnosed circuit depolarization even in the presence of coherent error, via Pauli twirling. We provide asymptotics to estimate the number of twirls needed to maintain a desired output fidelity. We test our method numerically in a variety of simulation settings and find that it can significantly reduce average random circuit infidelity. Further, we employ our methods to find significant infidelity reductions when running a random circuit ensemble on a contemporary superconducting quantum computer, IBM Fez. Overall, we show that the method effectively reduces gate-based error for unitary k-designs without incurring any two-qubit gate overhead.

quant-ph↗
arXiv2026

Towards Heisenberg Scaling: Measurement-Efficient Non-Orthogonal Quantum Eigensolver

The Non-Orthogonal Quantum Eigensolver (NOQE) provides an accurate framework for electronic-structure calculations, but the estimation of its Hamiltonian and overlap matrix elements relies on sampling and requires $O(1/\varepsilon^2)$ circuit repetitions to achieve additive precision $\varepsilon$. Here, we reformulate this matrix-element estimation step as a collection of amplitude-estimation tasks and integrate iterative quantum amplitude estimation into the NOQE workflow. The resulting protocol achieves near-Heisenberg query complexity $O(1/\varepsilon)$ for these estimation tasks, by replacing incoherent statistical averaging with coherent amplitude amplification. We present explicit circuit constructions and the corresponding implementation procedure. Numerical simulations for the electronic states of the hydrogen molecule show that the proposed method reaches chemical accuracy with substantially fewer total queries than the original sampling-based protocol. Overall, this work provides a measurement-efficient route to high-precision energy estimation and illustrates how sampling-limited quantum algorithms can be systematically reformulated to leverage quantum coherence and achieve lower measurement costs.

quant-ph↗
arXiv2026

Frequency- and time-resolved second order quantum coherence function of IDTBT single-molecule fluorescence

The frequency- and time-resolved second order quantum coherence function (g(2)(τ)) of single-molecule fluorescence has recently been proposed as a powerful new quantum light spectroscopy that can reveal intrinsic quantum coherence in excitation energy transfer in molecular systems ranging from simple dimers to photosynthetic complexes. Yet, no experiments have been reported to date. Here, we have developed a single-molecule fluorescence g(2)(τ) quantum light spectroscopy (SMFg2-QLS) that can simultaneously measure the fluorescence intensity, lifetime, spectra, and g(2)(τ) with frequency resolution, for a single molecule in a controlled environment at both room temperature and cryogenic temperature. As a proof of principle, we have studied single molecules of IDTBT (indacenodithiophene-co-benzothiadiazole), a semiconducting donor-acceptor conjugated copolymer with a chain-like structure that shows a high carrier mobility and annihilation-limited long-range exciton transport. We have observed different g(2)(τ=0) values with different bands or bandwidths of the single molecule IDTBT fluorescence. The general features are consistent with theoretical predictions and suggest non-trivial excited state quantum dynamics, possibly showing quantum coherence, although further analysis and confirmation will require additional theoretical calculations that take into account the complexity and inhomogeneity of individual IDTBT single molecular chains. Our results demonstrate the feasibility and promise of frequency- and time-resolved SMFg2-QLS to provide new insights into molecular quantum dynamics and to reveal signatures of intrinsic quantum coherence in photosynthetic light harvesting that are independent of the nature of the light excitation.

cond-mat.mtrl-sci↗
arXiv2026

Experimental characterization of coherent and non-Markovian errors using tangent space decomposition

Accurate characterization of coherent and non-Markovian errors remains a central challenge in quantum information processing, as conventional benchmarking techniques typically rely on Markovian and time-independent noise assumptions. In practice, however, quantum devices exhibit both systematic coherent miscalibrations and temporally correlated fluctuations, which complicate error diagnosis and mitigation. Here, we apply a technique based on tangent-space decomposition to characterize such error in single-qubit quantum gates implemented on a trapped ion platform. Small imperfections in a quantum operation are treated as perturbations of the target quantum map, represented as tangent vectors in the space of quantum channels. This formulations enables a natural decomposition of the deviation into three components corresponding to coherent, Markovian and non-Markovian processes.The relative weights of these components provide a quantitative measure of the contribution from each type of error mechanism, directly from a single tomographic snapshot. We experimentally validate this method on a single-qubit gates implemented on a trapped $^{40}$Ca$^+$ ion, where control is achieved through laser-driven optical transitions. By analyzing experimentally reconstructed process matrices, expressed in the Pauli Transfer Matrix and Choi representations, we identify and quantify non-Markovian effects arising from controlled injection of slow fluctuations in the experimental environment. We also characterize deterministic coherent miscalibrations using the same technique. This approach provides a physically transparent and experimentally accessible tool for diagnosing complex error sources in quantum control systems.

quant-ph↗
arXiv2026

Consistent inclusion of triple substitutions within a coupled cluster based static quantum embedding theory

We incorporate a solver for the fragment problem with accuracy beyond coupled cluster singles and doubles (CCSD) into the previously proposed static embedding framework, MPCC. To this end, we employ a CCSDT solver for the fragment subsystem. For the environment subsystem, we construct a perturbative estimate of the triples amplitudes, explicitly accounting for feedback from all fragment amplitudes. The resulting approach is denoted MPCCSDT(pt). We further introduce a more complete formulation in which feedback from the environment amplitudes to the fragment amplitudes is also included. This scheme involves an iterative treatment of the environment triples amplitudes and is denoted MPCCSDT(it). In addition, we assess the accuracy of the previously proposed low-level method by introducing a modified low-level approach that incorporates a lowest-order treatment of selected long-range effects, including spin fluctuations and charge polarization. All resulting approaches may be viewed as post-CCSD(T) methods. We therefore consider test cases for which CCSD(T) exhibits substantial deviations from CCSDT. Our results demonstrate that inclusion of triples amplitudes at the fragment level alone is insufficient; a perturbative treatment of the environment triples amplitudes is required. For many energy-difference applications, feedback from the environment triples amplitudes to the fragment amplitudes, is not essential, but it does play a role in the very challenging molecules. A very interesting finding from our study is that in some challenging cases, we need an improved (second-order) perturbative method for the SD amplitudes, going beyond the first-order one used in our earlier work.

physics.chem-ph↗
arXiv2026

Exponential quantum speedups for near-term molecular electronic structure methods

We prove classical simulation hardness, under the generalized $\mathsf{P}\neq\mathsf{NP}$ conjecture, for quantum circuit families with applications in near-term chemical ground state estimation. The proof exploits a connection to particle number conserving matchgate circuits with fermionic magic state inputs, which are shown to be universal for quantum computation under post-selection, and are therefore not classically simulable in the worst case, in either the strong (multiplicative) or weak (sampling) sense. We apply this result to quantum non-orthogonal multi-reference methods designed for near-term hardware by ruling out certain dequantization strategies for computing the off-diagonal matrix elements between reference states. We demonstrate these quantum speedups for two choices of ansatz that incorporate both static and dynamic correlations to model the electronic eigenstates of molecular systems: linear combinations of orbital-rotated matrix product states, which are preparable in linear depth, and linear combinations of states prepared by generalized UCCSD circuits of polynomial depth, for which computing the expectation values of local fermionic observables up to a constant additive error is $\mathsf{BQP}$-complete. We discuss the implications for achieving practical quantum advantage in resolving the electronic structure of catalytic systems composed from multivalent transition metal atoms using near-term quantum hardware.

quant-ph↗
arXiv2026

A quantum eigenvalue solver based on tensor networks

Electronic ground states are of central importance in chemical simulations, but have remained beyond the reach of efficient classical algorithms except in cases of weak electron correlation or one-dimensional spatial geometry. We introduce a hybrid quantum-classical eigenvalue solver that constructs a wavefunction ansatz from a linear combination of matrix product states in rotated orbital bases, enabling the characterization of strongly correlated ground states with arbitrary spatial geometry. The energy is converged via a gradient-free generalized sweep algorithm based on quantum subspace diagonalization, with a potentially exponential speedup in the off-diagonal matrix element contractions upon translation into compact quantum circuits of linear depth in the number of qubits. Chemical accuracy is attained in numerical experiments for both a stretched water molecule and an octahedral arrangement of hydrogen atoms, achieving substantially better correlation energies compared to a unitary coupled-cluster benchmark, with orders of magnitude reductions in quantum resource estimates and a surprisingly high tolerance to shot noise. This proof-of-concept study suggests a promising new avenue for scaling up simulations of strongly correlated chemical systems on near-term quantum hardware.

quant-ph↗
arXiv2025

Optimal sensing on an asymmetric exceptional surface

We study the connection between exceptional points (EPs) and optimal parameter estimation, in a simple system consisting of two counter-propagating traveling wave modes in a microring resonator. The unknown parameter to be estimated is the strength of a perturbing cross-coupling between the two modes. Partially reflecting the output of one mode into the other creates a non-Hermitian Hamiltonian which exhibits a family of EPs, creating an exceptional surface (ES). We use a fully quantum treatment of field inputs and noise sources to obtain a quantitative bound on the estimation error by calculating the quantum Fisher information (QFI) in the output fields, whose inverse gives the Cramér-Rao lower bound on the mean-squared-error of any unbiased estimator. We determine the bounds for two input states, namely, a semiclassical coherent state and a highly nonclassical NOON state. We find that the QFI is enhanced in the presence of an EP for both of these input states and that both states can saturate the Cramér-Rao bound. We then identify idealized yet experimentally feasible measurements that achieve the minimum bound for these two input states. We also investigate how the QFI changes for parameter values that do not lie on the ES, finding that these can have a larger QFI, suggesting alternative routes to optimize the parameter estimation for this problem.

quant-ph↗
arXiv2025

Quantum Sensing of Gravitational Frame-Dragging with a Superfluid $^4$He Gyrometer

We propose a laboratory-scale experiment to locally measure the general relativistic frame-dragging effect on Earth using the macroscopic quantum properties of a novel superfluid $^4$He single Josephson junction gyrometer. We derive the frame-dragging and related geodetic and Thomas effects in the superfluid gyrometer and present a procedure for their experimental measurement. We compute the expected thermal noise floor and find that very high sensitivity can be expected at millikelvin temperatures, where near-future Josephson junctions using nanoporous 2D materials are expected to operate. Assuming utilization of the lowest mechanical loss materials, we find a noise spectral density of $5\times 10^{-17}$ rads/s/$\sqrt{\mathrm{Hz}}$ at 10 mK, which is sufficient to resolve the frame-dragging rate to 0.2% within one second of measurement, giving a rotational sensitivity of 1 revolution in 4 Byrs. This extreme sensitivity to rotation corresponds to a measurement of proper time differences as small as $10^{-35}$ s.

quant-ph↗
arXiv2025

A Quantum Algorithm for the Finite Element Method

The finite element method (FEM) is a cornerstone numerical technique for solving partial differential equations (PDEs). Here, we present $\textbf{Qu-FEM}$, a fault-tolerant era quantum algorithm for the finite element method. In contrast to other quantum PDE solvers, Qu-FEM preserves the geometric flexibility of FEM by introducing two new primitives, the unit of interaction and the local-to-global indicator matrix, which enable the assembly of global finite element arrays with a constant-size linear combination of unitaries. We study the modified Poisson equation as an elliptic problem of interest, and provide explicit circuits for Qu-FEM in Cartesian domains. For problems with constant coefficients, our algorithm admits block-encodings of global arrays that require only $\tilde{\mathcal{O}}\left(d^2 p^2 n\right)$ Clifford+$T$ gates for $d$-dimensional, order-$p$ tensor product elements on grids with $2^n$ degrees of freedom in each dimension, where $n$ is the number of qubits representing the $N=2^n$ discrete grid points. For problems with spatially varying coefficients, we perform numerical integration directly on the quantum computer to assemble global arrays and force vectors. Dirichlet boundary conditions are enforced via the method of Lagrange multipliers, eliminating the need to modify the block-encodings that emerge from the assembly procedure. This work presents a framework for extending the geometric flexibility of quantum PDE solvers while preserving the possibility of a quantum advantage.

quant-ph↗
arXiv2025

Topological state permutations in time-modulated non-Hermitian multiqubit systems with suppressed non-adiabatic transitions

Non-Hermitian systems have been at the center of intense research for over a decade, partly due to their nontrivial energy topology formed by intersecting Riemann manifolds with branch points known as exceptional points (EPs). This spectral property can be exploited, e.g., to achieve topologically controlled state permutations that are necessary for implementing a wide class of classical and quantum information protocols. However, the complex-valued spectra of typical non-Hermitian systems lead to instabilities, losses, and breakdown of adiabaticity, which impedes the practical use of EP-induced energy topologies in quantum information protocols based on state permutation symmetries. Indeed, in a given non-Hermitian multiqubit system, the dynamical winding around EPs always results in a predetermined set of attenuated final eigenstates, due to the interplay of decoherence and non-adiabatic transitions, irrespective of the initial conditions. In this work, we address this long-standing problem by introducing a model of interacting qubits governed by an effective non-Hermitian Hamiltonian that hosts novel types of EPs while maintaining a completely real energy spectrum, ensuring the absence of losses in the system's dynamics. We demonstrate that such non-Hermitian Hamiltonians enable the realization of genuine, in general, non-Abelian permutation groups in the multiqubit system's eigenspace while dynamically encircling these EPs. Our findings indicate that, contrary to previous beliefs, non-Hermiticity can be utilized to achieve controlled topological state permutations in time-modulated multiqubit systems, thus paving the way for the advancement and development of novel quantum information protocols in real-world non-Hermitian quantum systems.

quant-ph↗