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Emergent Decoherence Dynamics in Doubly Disordered Spin Networks
Authors:
Cooper M. Selco,
Christian Bengs,
Chaitali Shah,
Zhuorui Zhang,
Ashok Ajoy
Abstract:
Elucidating the emergence of irreversible macroscopic laws from reversible quantum many-body dynamics is a question of broad importance across all quantum science. Many-body decoherence plays a key role in this transition, yet connecting microscopic dynamics to emergent macroscopic behavior remains challenging. Here, in a doubly disordered electron-nuclear spin network, we uncover an emergent deco…
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Elucidating the emergence of irreversible macroscopic laws from reversible quantum many-body dynamics is a question of broad importance across all quantum science. Many-body decoherence plays a key role in this transition, yet connecting microscopic dynamics to emergent macroscopic behavior remains challenging. Here, in a doubly disordered electron-nuclear spin network, we uncover an emergent decoherence law for nuclear polarization, $e^{-\sqrt{R_{p}t}}e^{-R_{d}t}$, that is robust across broad parameter regimes. We trace its microscopic origins to two interdependent decoherence channels: long-range interactions mediated by the electron network and spin transport within the nuclear network exhibiting anomalous, sub-diffusive dynamics. We demonstrate the capacity to control--and even eliminate--either channel individually through a combination of Floquet engineering and (optical) environment modulation. We find that disorder, typically viewed as detrimental, here proves protective, generating isolated electron-free clusters that localize polarization and prolong coherence lifetimes. These findings establish a microscopic framework for manipulating decoherence pathways and suggests engineered disorder as a new design principle for realizing long-lived quantum memories and sensors.
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Submitted 10 November, 2025;
originally announced November 2025.
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Quantum computation of molecular geometry via many-body nuclear spin echoes
Authors:
C. Zhang,
R. G. Cortiñas,
A. H. Karamlou,
N. Noll,
J. Provazza,
J. Bausch,
S. Shirobokov,
A. White,
M. Claassen,
S. H. Kang,
A. W. Senior,
N. Tomašev,
J. Gross,
K. Lee,
T. Schuster,
W. J. Huggins,
H. Celik,
A. Greene,
B. Kozlovskii,
F. J. H. Heras,
A. Bengtsson,
A. Grajales Dau,
I. Drozdov,
B. Ying,
W. Livingstone
, et al. (298 additional authors not shown)
Abstract:
Quantum-information-inspired experiments in nuclear magnetic resonance spectroscopy may yield a pathway towards determining molecular structure and properties that are otherwise challenging to learn. We measure out-of-time-ordered correlators (OTOCs) [1-4] on two organic molecules suspended in a nematic liquid crystal, and investigate the utility of this data in performing structural learning task…
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Quantum-information-inspired experiments in nuclear magnetic resonance spectroscopy may yield a pathway towards determining molecular structure and properties that are otherwise challenging to learn. We measure out-of-time-ordered correlators (OTOCs) [1-4] on two organic molecules suspended in a nematic liquid crystal, and investigate the utility of this data in performing structural learning tasks. We use OTOC measurements to augment molecular dynamics models, and to correct for known approximations in the underlying force fields. We demonstrate the utility of OTOCs in these models by estimating the mean ortho-meta H-H distance of toluene and the mean dihedral angle of 3',5'-dimethylbiphenyl, achieving similar accuracy and precision to independent spectroscopic measurements of both quantities. To ameliorate the apparent exponential classical cost of interpreting the above OTOC data, we simulate the molecular OTOCs on a Willow superconducting quantum processor, using AlphaEvolve-optimized [5] quantum circuits and arbitrary-angle fermionic simulation gates. We implement novel zero-noise extrapolation techniques based on the Pauli pathing model of operator dynamics [6], to repeat the learning experiments with root-mean-square error $0.05$ over all circuits used. Our work highlights a computational protocol to interpret many-body echoes from nuclear magnetic systems using low resource quantum computation.
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Submitted 22 October, 2025;
originally announced October 2025.
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Constructive interference at the edge of quantum ergodic dynamics
Authors:
Dmitry A. Abanin,
Rajeev Acharya,
Laleh Aghababaie-Beni,
Georg Aigeldinger,
Ashok Ajoy,
Ross Alcaraz,
Igor Aleiner,
Trond I. Andersen,
Markus Ansmann,
Frank Arute,
Kunal Arya,
Abraham Asfaw,
Nikita Astrakhantsev,
Juan Atalaya,
Ryan Babbush,
Dave Bacon,
Brian Ballard,
Joseph C. Bardin,
Christian Bengs,
Andreas Bengtsson,
Alexander Bilmes,
Sergio Boixo,
Gina Bortoli,
Alexandre Bourassa,
Jenna Bovaird
, et al. (240 additional authors not shown)
Abstract:
Quantum observables in the form of few-point correlators are the key to characterizing the dynamics of quantum many-body systems. In dynamics with fast entanglement generation, quantum observables generally become insensitive to the details of the underlying dynamics at long times due to the effects of scrambling. In experimental systems, repeated time-reversal protocols have been successfully imp…
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Quantum observables in the form of few-point correlators are the key to characterizing the dynamics of quantum many-body systems. In dynamics with fast entanglement generation, quantum observables generally become insensitive to the details of the underlying dynamics at long times due to the effects of scrambling. In experimental systems, repeated time-reversal protocols have been successfully implemented to restore sensitivities of quantum observables. Using a 103-qubit superconducting quantum processor, we characterize ergodic dynamics using the second-order out-of-time-order correlators, OTOC$^{(2)}$. In contrast to dynamics without time reversal, OTOC$^{(2)}$ are observed to remain sensitive to the underlying dynamics at long time scales. Furthermore, by inserting Pauli operators during quantum evolution and randomizing the phases of Pauli strings in the Heisenberg picture, we observe substantial changes in OTOC$^{(2)}$ values. This indicates that OTOC$^{(2)}$ is dominated by constructive interference between Pauli strings that form large loops in configuration space. The observed interference mechanism endows OTOC$^{(2)}$ with a high degree of classical simulation complexity, which culminates in a set of large-scale OTOC$^{(2)}$ measurements exceeding the simulation capacity of known classical algorithms. Further supported by an example of Hamiltonian learning through OTOC$^{(2)}$, our results indicate a viable path to practical quantum advantage.
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Submitted 11 June, 2025;
originally announced June 2025.
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Fundamental bounds on many-body spin cluster intensities
Authors:
Christian Bengs,
Chongwei Zhang,
Ashok Ajoy
Abstract:
Multiple-quantum coherence (MQC) spectroscopy is a powerful technique for probing spin clusters, offering insights into diverse materials and quantum many-body systems. However, prior experiments have revealed a rapid decay in MQC intensities as the coherence order increases, restricting observable cluster sizes to the square root of the total system size. In this work, we establish fundamental bo…
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Multiple-quantum coherence (MQC) spectroscopy is a powerful technique for probing spin clusters, offering insights into diverse materials and quantum many-body systems. However, prior experiments have revealed a rapid decay in MQC intensities as the coherence order increases, restricting observable cluster sizes to the square root of the total system size. In this work, we establish fundamental bounds on observable MQC intensities in the thermodynamic limit outside the weak polarisation limit. We identify a sharp transition point in the observable MQC intensities as the coherence order grows. This transition points fragments the state space into two components consisting of observable and unobservable spin clusters. Notably, we find that this transition point is directly proportional to the size $N$ and polarization $p$ of the system, suggesting that the aforementioned square root limitation can be overcome through hyperpolarization techniques. Our results provide important experimental guidelines for the observation of large spin cluster phenomena.
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Submitted 11 December, 2024;
originally announced December 2024.
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Anomalously extended Floquet prethermal lifetimes and applications to long-time quantum sensing
Authors:
Kieren A. Harkins,
Cooper Selco,
Christian Bengs,
David Marchiori,
Leo Joon Il Moon,
Zhuo-Rui Zhang,
Aristotle Yang,
Angad Singh,
Emanuel Druga,
Yi-Qiao Song,
Ashok Ajoy
Abstract:
Floquet prethermalization is observed in periodically driven quantum many-body systems where the system avoids heating and maintains a stable, non-equilibrium state, for extended periods. Here we introduce a novel quantum control method using off-resonance and short-angle excitation to significantly extend Floquet prethermal lifetimes. This is demonstrated on randomly positioned, dipolar-coupled,…
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Floquet prethermalization is observed in periodically driven quantum many-body systems where the system avoids heating and maintains a stable, non-equilibrium state, for extended periods. Here we introduce a novel quantum control method using off-resonance and short-angle excitation to significantly extend Floquet prethermal lifetimes. This is demonstrated on randomly positioned, dipolar-coupled, 13C nuclear spins in diamond, but the methodology is broadly applicable. We achieve a lifetime $T_2'~800 s at 100 K while tracking the transition to the prethermal state quasi-continuously. This corresponds to a >533,000-fold extension over the bare spin lifetime without prethermalization, and constitutes a new record both in terms of absolute lifetime as well as the total number of Floquet pulses applied (here exceeding 7 million). Using Laplace inversion, we develop a new form of noise spectroscopy that provides insights into the origin of the lifetime extension. Finally, we demonstrate applications of these extended lifetimes in long-time, reinitialization-free quantum sensing of time-varying magnetic fields continuously for ~10 minutes at room temperature. Our work facilitates new opportunities for stabilizing driven quantum systems through Floquet control, and opens novel applications for continuously interrogated, long-time responsive quantum sensors.
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Submitted 11 October, 2024;
originally announced October 2024.
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Robust Parahydrogen-Induced Polarization at High Concentrations
Authors:
Laurynas Dagys,
Martin C. Korzeczek,
Anna J. Parker,
James Eills,
John W. Blanchard,
Christian Bengs,
Malcolm H. Levitt,
Stephan Knecht,
Ilai Schwartz,
M. B. Plenio
Abstract:
Parahydrogen-Induced Polarization (PHIP) is a potent technique for generating target molecules with high nuclear spin polarization. The PHIP process involves a chemical reaction between parahydrogen and a target molecule, followed by the transformation of nuclear singlet spin order into magnetization of a designated nucleus through magnetic field manipulations. Although the singlet-to-magnetizatio…
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Parahydrogen-Induced Polarization (PHIP) is a potent technique for generating target molecules with high nuclear spin polarization. The PHIP process involves a chemical reaction between parahydrogen and a target molecule, followed by the transformation of nuclear singlet spin order into magnetization of a designated nucleus through magnetic field manipulations. Although the singlet-to-magnetization polarization transfer process works effectively at moderate concentrations, it is observed to become much less efficient at high molar polarization, defined as the product of polarization and concentration. This strong dependence on the molar polarization is attributed to interference from the field produced by the sample's magnetization during polarization transfer, which leads to complex dynamics and can severely impact the scalability of the technique. We address this challenge with a pulse sequence that negates the influence of the distant dipolar field, while simultaneously achieving singlet-to-magnetization polarization transfer to the desired target spins, free from restrictions on the molar polarization.
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Submitted 14 January, 2024;
originally announced January 2024.
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Symmetry-Based Singlet-Triplet Excitation in Solution Nuclear Magnetic Resonance
Authors:
Mohamed Sabba,
Nino Wili,
Christian Bengs,
Lynda J. Brown,
Malcolm H. Levitt
Abstract:
Coupled pairs of spin-1/2 nuclei support one singlet state and three triplet states. In many circumstances the nuclear singlet order, defined as the difference between the singlet population and the mean of the triplet populations, is a long-lived state which persists for a relatively long time in solution. Various methods have been proposed for generating singlet order, starting from nuclear magn…
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Coupled pairs of spin-1/2 nuclei support one singlet state and three triplet states. In many circumstances the nuclear singlet order, defined as the difference between the singlet population and the mean of the triplet populations, is a long-lived state which persists for a relatively long time in solution. Various methods have been proposed for generating singlet order, starting from nuclear magnetization. This requires the stimulation of singlet-to-triplet transitions by modulated radiofrequency fields. We show that a recently described pulse sequence, known as PulsePol (Schwartz $\textit{et al.}$, Science Advances, $\textbf{4}$, eaat8978 (2018) and arXiv:1710.01508), is an efficient technique for converting magnetization into long-lived singlet order. We show that the operation of this pulse sequence may be understood by adapting the theory of symmetry-based recoupling sequences in magic-angle-spinning solid-state NMR. The concept of riffling allows PulsePol to be interpreted using the theory of symmetry-based pulse sequences, and explains its robustness. This theory is used to derive a range of new pulse sequences for performing singlet-triplet excitation and conversion in solution NMR. Schemes for further enhancing the robustness of the transformations are demonstrated.
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Submitted 14 June, 2022;
originally announced June 2022.
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Hyperpolarization read-out through rapidly rotating fields in the zero- and low-field regime
Authors:
Laurynas Dagys,
Christian Bengs
Abstract:
An integral part of para-hydrogen induced polarization (PHIP) methods is the conversion of nuclear singlet order into observable magnetization. In this study polarisation transfer to a heteronucleus is achieved through a selective rotation of the proton singlet-triplet states driven by a combination of a rotating magnetic field and a weak bias field. Surprisingly we find that efficient polarisatio…
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An integral part of para-hydrogen induced polarization (PHIP) methods is the conversion of nuclear singlet order into observable magnetization. In this study polarisation transfer to a heteronucleus is achieved through a selective rotation of the proton singlet-triplet states driven by a combination of a rotating magnetic field and a weak bias field. Surprisingly we find that efficient polarisation transfer driven by a STORM (Singlet-Triplet Oscillations through Rotating Magnetic fields) pulse in the presence of $μ$T bias fields requires rotation frequencies on the order of several kHz. The rotation frequencies therefore greatly exceed any of the internal frequencies of typical zero- to ultralow field experiments. We further show that the rotational direction of the rotating field is not arbitrary and greatly influences the final transfer efficiency. Some of these aspects are demonstrated experimentally by considering hyperpolarised (1-$^{13}$C)fumarate. In addition, we provide numerical simulations highlighting the resilience of the STORM pulse against disruptive quadrupolar coupling partners. In contrast to most of the existing methods, the STORM procedure therefore represents a promising candidate for quadrupolar decoupled polarisation transfer in PHIP experiments.
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Submitted 9 February, 2022;
originally announced February 2022.
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Low-Frequency Excitation of Singlet-Triplet Transitions. Application to Nuclear Hyperpolarization
Authors:
Laurynas Dagys,
Christian Bengs,
Malcolm H. Levitt
Abstract:
Coupled pairs of nuclear spins-1/2 support one singlet state and three triplet states. Transitions between the singlet state and one of the triplet states may be driven by an oscillating low-frequency magnetic field, in the presence of couplings to a third nuclear spin, and a weak bias magnetic field.This phenomenon allows the generation of strong nuclear hyperpolarization of ${}^{13}\mathrm{C}$ n…
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Coupled pairs of nuclear spins-1/2 support one singlet state and three triplet states. Transitions between the singlet state and one of the triplet states may be driven by an oscillating low-frequency magnetic field, in the presence of couplings to a third nuclear spin, and a weak bias magnetic field.This phenomenon allows the generation of strong nuclear hyperpolarization of ${}^{13}\mathrm{C}$ nuclei, starting from the nuclear singlet polarization of a ${}^{1}\mathrm{H}$ spin pair, associated with the enriched para spin isomer of hydrogen gas. Hyperpolarization is demonstrated for two molecular system.
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Submitted 22 July, 2021;
originally announced July 2021.
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Algorithmic Cooling of Nuclear Spin Pairs using a Long-Lived Singlet State
Authors:
Bogdan A. Rodin,
Christian Bengs,
Lynda J. Brown,
Kirill F. Sheberstov,
Alexey S. Kiryutin,
Richard C. D. Brown,
Alexandra V. Yurkovskaya,
Konstantin L. Ivanov,
Malcolm H. Levitt
Abstract:
Algorithmic cooling methods manipulate an open quantum system in order to lower its temperature below that of the environment. We show that significant cooling is achieved on an ensemble of spin-pair systems by exploiting the long-lived nuclear singlet state, which is an antisymmetric quantum superposition of the "up" and "down" qubit states. The effect is demonstrated by nuclear magnetic resonanc…
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Algorithmic cooling methods manipulate an open quantum system in order to lower its temperature below that of the environment. We show that significant cooling is achieved on an ensemble of spin-pair systems by exploiting the long-lived nuclear singlet state, which is an antisymmetric quantum superposition of the "up" and "down" qubit states. The effect is demonstrated by nuclear magnetic resonance (NMR) experiments on a molecular system containing a coupled pair of near-equivalent 13C nuclei. The populations of the system are subjected to a repeating sequence of cyclic permutations separated by relaxation intervals. The long-lived nuclear singlet order is pumped well beyond the unitary limit, and the nuclear magnetization is enhanced by 21% relative to its thermal equilibrium value. To our knowledge this is the first demonstration of algorithmic cooling using a quantum superposition state and without making a distinction between rapidly and slowly relaxing qubits.
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Submitted 31 December, 2019;
originally announced December 2019.