arXiv subjects

Christian Bengs

Publications and source records attributed to Christian Bengs.

15 recordsLinked to original sources

arXiv2026

Continuous-Time Random Walk Description of Anomalous Spin Transport in Dilute Dipolar Networks

Nuclear spin diffusion is often summarized by a single diffusion coefficient, but this coarse-grained description can fail in dilute solids where positional disorder and long-range dipolar couplings generate a broad distribution of hopping rates. We develop a continuous-time random-walk (CTRW) description of $^{13}$C polarization transport in natural-abundance diamond (1.1%), constructing the rate matrix from dipolar-mediated flip-flop couplings and sampling exact continuous-time trajectories. Although site-to-site hopping is Markovian, the disorder-averaged dynamics give rise to emergent, anomalous transport. The empirical waiting-time distribution exhibits a heavy tail with exponent $\alpha=0.64$ and exponential cutoff $t_{\rm cutoff}=19$ s; the mean jump length becomes correlated with the waiting time $\tau$ for $\tau\gtrsim0.1$ s; and the mean-squared displacement grows sublinearly in both step number and physical time, with exponents $\gamma=0.56$ and $\delta=0.87$ respectively. We trace the microscopic origin of these signatures to geometric trapping: polarization can rapidly exchange within strongly coupled clusters, including dimers, while weak inter-cluster links control long-range exploration. A kinetic percolation construction links global transport to inter-cluster crossing times, and identifies a corresponding crossing time of $\sim20$ s, consistent with $t_{\rm cutoff}$. Finally, mapping paramagnetic impurities onto hard-sphere traps connects the CTRW framework to classic studies of trapping in reaction-diffusion theory and reproduces the qualitative timescale of experimentally measured relaxation, whereas a continuum diffusion equation description does not. These results show that dilute dipolar spin networks require a microscopic, network-resolved transport description beyond the Fickian diffusion equation.

cond-mat.stat-mech↗

arXiv2026

Breakdown of Disorder-Suppressed Floquet Heating under Two-Frequency Driving

Periodic (Floquet) driving enables Hamiltonian engineering and nonequilibrium phases, but interacting systems eventually heat by absorbing energy from the drive. Disorder can greatly delay this process, yielding long-lived prethermal plateaus. Here we show that this protection can fail when pulse-train control introduces a second driving frequency and when the disorder fluctuates. Using a natural-abundance 13C nuclear-spin network in diamond, we observe sharp peaks in the late-time heating rate at the double- and triple-spin-flip resonance conditions predicted by bimodal Floquet interference, and track their evolution with drive frequency. A switching-noise model attributes the resonant absorption to stochastic electron-spin dynamics that intermittently tune rare nuclear clusters into multi-photon resonance. Our results reveal a resonance-activated limit for disorder-stabilized Floquet phases and suggest new routes to DC-field quantum sensing based on an abrupt breakdown of prethermalization.

quant-ph↗

arXiv2026

Error compensation without a time penalty: robust spin-lock-induced crossing in solution NMR

A modification of the widely-used spin-lock-induced crossing (SLIC) procedure is proposed for the solution nuclear magnetic resonance (NMR) of strongly coupled nuclear spin systems, including singlet NMR and parahydrogen-enhanced hyperpolarised NMR experiments. The compensated-SLIC (cSLIC) scheme uses a repetitive sequence where the repeated element employs two different radiofrequency field amplitudes. Effective compensation for deviations in the radiofrequency field amplitude is achieved without increasing the overall duration of the SLIC sequence. The advantageous properties of cSLIC are demonstrated by numerical simulations and by representative experiments.

quant-ph↗

arXiv2026

Spinor Double-Quantum Excitation in the Solution NMR of Near-Equivalent Spin-1/2 Pairs

A family of double-quantum excitation schemes is described for the solution nuclear magnetic resonance (NMR) of near-equivalent spin-1/2 pairs. These new methods exploit the spinor behaviour of 2-level systems, whose signature is the change of sign of a quantum state upon a $2\pi$ rotation. The spinor behaviour is used to manipulate the phases of single-quantum coherences, in order to prepare a double-quantum precursor state which is rapidly converted into double-quantum coherence by a straightforward $\pi/2$ rotation. One set of spinor-based methods exploits symmetry-based pulse sequences, while the other set exploits SLIC (spin-lock-induced crossing), in which the nutation frequency under a resonant radiofrequency field is matched to the spin-spin coupling. A variant of SLIC is introduced which is well-compensated for deviations in the radiofrequency field amplitude. The methods are demonstrated by performing double-quantum-filtered $^{19}$F NMR on a molecular system containing a pair of diastereotopic $^{19}$F nuclei. The new methods are compared with existing techniques.

quant-ph↗

arXiv2025

Emergent Decoherence Dynamics in Doubly Disordered Spin Networks

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.

quant-ph↗

arXiv2025

Constructive interference at the edge of quantum ergodic dynamics

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.

quant-ph↗

arXiv2024

Fundamental bounds on many-body spin cluster intensities

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.

quant-ph↗

arXiv2024

Anomalously extended Floquet prethermal lifetimes and applications to long-time quantum sensing

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.

quant-ph↗

arXiv2024

Robust Parahydrogen-Induced Polarization at High Concentrations

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.

physics.chem-ph↗

arXiv2022

Cross-correlation effects in the solution NMR spectra of near-equivalent spin-1/2 pairs

The NMR spectra of spin-1/2 pairs contains four peaks, with two inner peaks much stronger than the outer peaks in the near-equivalence regime. We have observed that the strong inner peaks have significantly different linewidths, when measurements were performed on a 13C2-labelled triyne derivative. This linewidth difference may be attributed to strong cross-correlation effects. We develop the theory of cross-correlated relaxation in the case of near-equivalent homonuclear spin-1/2 pairs, in the case of a molecule exhibiting strongly anisotropic rotational diffusion. Good agreement is found with the experimental NMR lineshapes.

physics.chem-ph↗

arXiv2022

Symmetry-Based Singlet-Triplet Excitation in Solution Nuclear Magnetic Resonance

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.

quant-ph↗

arXiv2022

Hyperpolarization read-out through rapidly rotating fields in the zero- and low-field regime

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.

quant-ph↗

arXiv2021

Low-Frequency Excitation of Singlet-Triplet Transitions. Application to Nuclear Hyperpolarization

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.

quant-ph↗

arXiv2019

Algorithmic Cooling of Nuclear Spin Pairs using a Long-Lived Singlet State

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.

quant-ph↗

arXiv2018

Spin-isomer conversion of water at room temperature, and quantum-rotor-induced nuclear polarization, in the water-endofullerene H$_2$O@C$_{60}$

Water exists in two forms, para and ortho, that have nuclear spin states with different symmetries. Here we report the conversion of fullerene-encapsulated para-water to ortho-water. The enrichment of para-water at low temperatures is monitored via changes in the electrical polarizability of the material. Upon rapid dissolution of the material in toluene the excess para-water converts to ortho- water. In H$_2{}^{16}$O@C$_{60}$ the conversion leads to a slow increase in the NMR signal. In H$_2{}^{16}$O@C$_{60}$ the conversion gives rise to weak signal enhancements attributed to quantum-rotor-induced nuclear spin polarization. The time constants for the spin-isomer conversion of fullerene-encapsulated water in ambient temperature solution are estimated as 30$\pm$4 s for the $^{16}$O-isotopologue of water, and 16$\pm$3 s for the $^{17}$O isotopologue.

physics.chem-ph↗