Towards a unified picture of polarization transfer - pulsed DNP and chemically equivalent PHIP.

Nuclear spin hyperpolarization techniques, such as dynamic nuclear polarization (DNP) and parahydrogen-induced polarization (PHIP), have revolutionized nuclear magnetic resonance and magnetic resonance imaging. In these methods, a readily available source of high spin order, either electron spins in DNP or singlet states in hydrogen for PHIP, is brought into close proximity with nuclear spin targets, enabling efficient transfer of spin order under external quantum control. Despite vast disparities in energy scales and interaction mechanisms between electron spins in DNP and nuclear singlet states in PHIP, a pseudo-spin formalism allows us to establish an intriguing equivalence. As a result, the important low-field polarization transfer regime of PHIP can be mapped onto an analogous system equivalent to pulsed-DNP. This establishes a correspondence between key polarization transfer sequences in PHIP and DNP, facilitating the transfer of sequence development concepts. This promises fresh insights and significant cross-pollination between DNP and PHIP polarization sequence developers.

Systematic Coarse Graining of Environments for the Nonperturbative Simulation of Open Quantum Systems.

Conducting precise electronic-vibrational dynamics simulations of molecular systems poses significant challenges when dealing with realistic environments composed of numerous vibrational modes. Here, we introduce a technique for the construction of effective phonon spectral densities that capture accurately open-system dynamics over a finite time interval of interest. When combined with existing nonperturbative simulation tools, our approach can reduce significantly the computational costs associated with many-body open-system dynamics.

Unraveling Eumelanin Radical Formation by Nanodiamond Optical Relaxometry in a Living Cell.

Defect centers in a nanodiamond (ND) allow the detection of tiny magnetic fields in their direct surroundings, rendering them as an emerging tool for nanoscale sensing applications. Eumelanin, an abundant pigment, plays an important role in biology and material science. Here, for the first time, we evaluate the comproportionation reaction in eumelanin by detecting and quantifying semiquinone radicals through the nitrogen-vacancy color center. A thin layer of eumelanin is polymerized on the surface of nanodiamonds (NDs), and depending on the environmental conditions, such as the local pH value, near-infrared, and ultraviolet light irradiation, the radicals form and react in situ. By combining experiments and theoretical simulations, we quantify the local number and kinetics of free radicals in the eumelanin layer. Next, the ND sensor enters the cells via endosomal vesicles. We quantify the number of radicals formed within the eumelanin layer in these acidic compartments by applying optical relaxometry measurements. In the future, we believe that the ND quantum sensor could provide valuable insights into the chemistry of eumelanin, which could contribute to the understanding and treatment of eumelanin- and melanin-related diseases.

A quantum physics layer of epigenetics: a hypothesis deduced from charge transfer and chirality-induced spin selectivity of DNA.

BACKGROUND: Epigenetic mechanisms are informational cellular processes instructing normal and diseased phenotypes. They are associated with DNA but without altering the DNA sequence. Whereas chemical processes like DNA methylation or histone modifications are well-accepted epigenetic mechanisms, we herein propose the existence of an additional quantum physics layer of epigenetics. RESULTS: We base our hypothesis on theoretical and experimental studies showing quantum phenomena to be active in double-stranded DNA, even under ambient conditions. These phenomena include coherent charge transfer along overlapping pi-orbitals of DNA bases and chirality-induced spin selectivity. Charge transfer via quantum tunneling mediated by overlapping orbitals results in charge delocalization along several neighboring bases, which can even be extended by classical (non-quantum) electron hopping. Such charge transfer is interrupted by flipping base(s) out of the double-strand e.g., by DNA modifying enzymes. Charge delocalization can directly alter DNA recognition by proteins or indirectly by DNA structural changes e.g., kinking. Regarding sequence dependency, charge localization, shown to favor guanines, could influence or even direct epigenetic changes, e.g., modification of cytosines in CpG dinucleotides. Chirality-induced spin selectivity filters electrons for their spin along DNA and, thus, is not only an indicator for quantum coherence but can potentially affect DNA binding properties. CONCLUSIONS: Quantum effects in DNA are prone to triggering and manipulation by external means. By the hypothesis put forward here, we would like to foster research on "Quantum Epigenetics" at the interface of medicine, biology, biochemistry, and physics to investigate the potential epigenetic impact of quantum physical principles on (human) life.

Asymptotic State Transformations of Continuous Variable Resources.

We study asymptotic state transformations in continuous variable quantum resource theories. In particular, we prove that monotones displaying lower semicontinuity and strong superadditivity can be used to bound asymptotic transformation rates in these settings. This removes the need for asymptotic continuity, which cannot be defined in the traditional sense for infinite-dimensional systems. We consider three applications, to the resource theories of (I) optical nonclassicality, (II) entanglement, and (III) quantum thermodynamics. In cases (II) and (III), the employed monotones are the (infinite-dimensional) squashed entanglement and the free energy, respectively. For case (I), we consider the measured relative entropy of nonclassicality and prove it to be lower semicontinuous and strongly superadditive. One of our main technical contributions, and a key tool to establish these results, is a handy variational expression for the measured relative entropy of nonclassicality. Our technique then yields computable upper bounds on asymptotic transformation rates, including those achievable under linear optical elements. We also prove a number of results which guarantee that the measured relative entropy of nonclassicality is bounded on any physically meaningful state and easily computable for some classes of states of interest, e.g., Fock diagonal states. We conclude by applying our findings to the problem of cat state manipulation and noisy Fock state purification.

Spin-Dependent Momentum Conservation of Electron-Phonon Scattering in Chirality-Induced Spin Selectivity.

The elucidation of the mechanisms underpinning chirality-induced spin selectivity remains an outstanding scientific challenge. Here we consider the role of delocalized phonon modes in electron transport in chiral structures and demonstrate that spin selectivity can originate from spin-dependent energy and momentum conservation in electron-phonon scattering events. While this mechanism is robust to the specific nature of the vibrational modes, the degree of spin polarization depends on environmental factors, such as the specific temperature and phonon relaxation rates, as well as the presence of external driving fields. This parametric dependence is used to present experimentally testable predictions of our model.

Fingerprint and Universal Markovian Closure of Structured Bosonic Environments.

We exploit the properties of chain mapping transformations of bosonic environments to identify a finite collection of modes able to capture the characteristic features, or fingerprint, of the environment. Moreover we show that the countable infinity of residual bath modes can be replaced by a universal Markovian closure, namely, a small collection of damped modes undergoing a Lindblad-type dynamics whose parametrization is independent of the spectral density under consideration. We show that the Markovian closure provides a quadratic speedup with respect to standard chain mapping techniques and makes the memory requirement independent of the simulation time, while preserving all the information on the fingerprint modes. We illustrate the application of the Markovian closure to the computation of linear spectra but also to nonlinear spectral response, a relevant experimentally accessible many body coherence witness for which efficient numerically exact calculations in realistic environments are currently lacking.

Scalable Generation of Multiphoton Entangled States by Active Feed-Forward and Multiplexing.

Multiphoton entangled quantum states are key to advancing quantum technologies such as multiparty quantum communications, quantum sensing, or quantum computation. Their scalable generation, however, remains an experimental challenge. Current methods for generating these states rely on stitching together photons from probabilistic sources, and state generation rates drop exponentially in the number of photons. Here, we implement a system based on active feed-forward and multiplexing that addresses this challenge. We demonstrate the scalable generation of four-photon and six-photon Greenberger-Horne-Zeilinger states, increasing generation rates by factors of 9 and 35, respectively. This is consistent with the exponential enhancement compared to the standard nonmultiplexed approach that is predicted by our theory. These results facilitate the realization of practical multiphoton protocols for photonic quantum technologies.

Coherence as a Resource for Shor's Algorithm.

Shor's factoring algorithm provides a superpolynomial speedup over all known classical factoring algorithms. Here, we address the question of which quantum properties fuel this advantage. We investigate a sequential variant of Shor's algorithm with a fixed overall structure and identify the role of coherence for this algorithm quantitatively. We analyze this protocol in the framework of dynamical resource theories, which capture the resource character of operations that can create and detect coherence. This allows us to derive a lower and an upper bound on the success probability of the protocol, which depend on rigorously defined measures of coherence as a dynamical resource. We compare these bounds with the classical limit of the protocol and conclude that within the fixed structure that we consider, coherence is the quantum resource that determines its performance by bounding the success probability from below and above. Therefore, we shine new light on the fundamental role of coherence in quantum computation.

Detection of Few Hydrogen Peroxide Molecules Using Self-Reporting Fluorescent Nanodiamond Quantum Sensors.

Hydrogen peroxide (H2O2) plays an important role in various signal transduction pathways and regulates important cellular processes. However, monitoring and quantitatively assessing the distribution of H2O2 molecules inside living cells requires a nanoscale sensor with molecular-level sensitivity. Herein, we show the first demonstration of sub-10 nm-sized fluorescent nanodiamonds (NDs) as catalysts for the decomposition of H2O2 and the production of radical intermediates at the nanoscale. Furthermore, the nitrogen-vacancy quantum sensors inside the NDs are employed to quantify the aforementioned radicals. We believe that our method of combining the peroxidase-mimicking activities of the NDs with their intrinsic quantum sensor showcases their application as self-reporting H2O2 sensors with molecular-level sensitivity and nanoscale spatial resolution. Given the robustness and the specificity of the sensor, our results promise a new platform for elucidating the role of H2O2 at the cellular level.

Enhancing Gravitational Interaction between Quantum Systems by a Massive Mediator.

In 1957 Feynman suggested that the quantum or classical character of gravity may be assessed by testing the gravitational interaction due to source masses in superposition. However, in all proposed experimental realizations using matter-wave interferometry, the extreme weakness of this interaction requires pure initial states with extreme squeezing to achieve measurable effects of nonclassical interaction for reasonable experiment durations. In practice, the systems that can be prepared in such nonclassical states are limited to small masses, which in turn limits the strength of their interaction. Here we address this key challenge-the weakness of gravitational interaction-by using a massive body as an amplifying mediator of gravitational interaction between two test systems. Our analysis shows that this results in an effective interaction between the two test systems that grows with the mass of the mediator, is independent of its initial state and, therefore, its temperature. This greatly reduces the requirement on the mass and degree of delocalization of the test systems and, while still highly challenging, brings experiments on gravitational source masses a step closer to reality.

Interface-Induced Conservation of Momentum Leads to Chiral-Induced Spin Selectivity.

We study the nonequilibrium dynamics of electron transmission from a straight waveguide to a helix with spin-orbit coupling. Transmission is found to be spin-selective and can lead to large spin polarizations of the itinerant electrons. The degree of spin selectivity depends on the width of the interface region, and no polarization is found for single-point couplings. We show that this is due to momentum conservation conditions arising from extended interfaces. We therefore identify interface structure and conservation of momentum as crucial ingredients for chiral-induced spin selectivity, and we confirm that this mechanism is robust against static disorder.

Hyperpolarized Solution-State NMR Spectroscopy with Optically Polarized Crystals.

Nuclear spin hyperpolarization provides a promising route to overcome the challenges imposed by the limited sensitivity of nuclear magnetic resonance. Here we demonstrate that dissolution of spin-polarized pentacene-doped naphthalene crystals enables transfer of polarization to target molecules via intermolecular cross-relaxation at room temperature and moderate magnetic fields (1.45 T). This makes it possible to exploit the high spin polarization of optically polarized crystals, while mitigating the challenges of its transfer to external nuclei. With this method, we inject the highly polarized mixture into a benchtop NMR spectrometer and observe the polarization dynamics for target 1H nuclei. Although the spectra are radiation damped due to the high naphthalene magnetization, we describe a procedure to process the data to obtain more conventional NMR spectra and extract the target nuclei polarization. With the entire process occurring on a time scale of 1 min, we observe NMR signals enhanced by factors between -200 and -1730 at 1.45 T for a range of small molecules.

Ground-State Cooling of Levitated Magnets in Low-Frequency Traps.

We present a ground-state cooling scheme for the mechanical degrees of freedom of mesoscopic magnetic particles levitated in low-frequency traps. Our method makes use of a binary sensor and suitably shaped pulses to perform weak, adaptive measurements on the position of the magnet. This allows us to precisely determine the position and momentum of the particle, transforming the initial high-entropy thermal state into a pure coherent state. The energy is then extracted by shifting the trap center. By delegating the task of energy extraction to a coherent displacement operation, we overcome the limitations associated with cooling schemes that rely on the dissipation of a two-level system coupled to the oscillator. We numerically benchmark our protocol in realistic experimental conditions, including heating rates and imperfect readout fidelities, showing that it is well suited for magnetogravitational traps operating at cryogenic temperatures. Our results pave the way for ground-state cooling of micron-scale particles.

Progress in miniaturization and low-field nuclear magnetic resonance.

In this paper, we review the latest developments in miniaturization of NMR systems with an emphasis on low-field NMR. We briefly cover the topics of magnet and coil miniaturization, elaborating on the advantages and disadvantages of miniaturized coils for different applications. The main part of the article is dedicated to progress in NMR electronics. Here, we touch upon software-defined radios as an emerging gadget for NMR before we provide a detailed discussion of NMR-on-a-chip transceivers as the ultimate solution in terms of miniaturization of NMR electronics. In addition to discussing the miniaturization capabilities of the NMR-on-a-chip approach, we also investigate the potential use of NMR-on-a-chip devices for an improved NMR system performance. Here, we also discuss the possibility of combining the NMR-on-a-chip approach with EPR-on-a-chip spectrometers to form compact DNP-on-a-chip systems that can provide a significant sensitivity boost, especially for low-field NMR systems.

Quantifying Dynamical Coherence with Dynamical Entanglement.

Coherent superposition and entanglement are two fundamental aspects of nonclassicality. Here we provide a quantitative connection between the two on the level of operations by showing that the dynamical coherence of an operation upper bounds the dynamical entanglement that can be generated from it with the help of additional incoherent operations. In case a particular choice of monotones based on the relative entropy is used for the quantification of these dynamical resources, this bound can be achieved. In addition, we show that an analog to the entanglement potential exists on the level of operations and serves as a valid quantifier for dynamical coherence.

Bosonic Quantum Communication across Arbitrarily High Loss Channels.

A general attenuator Φ_{λ,σ} is a bosonic quantum channel that acts by combining the input with a fixed environment state σ in a beam splitter of transmissivity λ. If σ is a thermal state, the resulting channel is a thermal attenuator, whose quantum capacity vanishes for λ≤1/2. We study the quantum capacity of these objects for generic σ, proving a number of unexpected results. Most notably, we show that for any arbitrary value of λ>0 there exists a suitable single-mode state σ(λ) such that the quantum capacity of Φ_{λ,σ(λ)} is larger than a universal constant c>0. Our result holds even when we fix an energy constraint at the input of the channel, and implies that quantum communication at a constant rate is possible even in the limit of arbitrarily low transmissivity, provided that the environment state is appropriately controlled. We also find examples of states σ such that the quantum capacity of Φ_{λ,σ} is not monotonic in λ. These findings may have implications for the study of communication lines running across integrated optical circuits, of which general attenuators provide natural models.

Experimental Quantification of Coherence of a Tunable Quantum Detector.

Quantum coherence is a fundamental resource that quantum technologies exploit to achieve performance beyond that of classical devices. A necessary prerequisite to achieve this advantage is the ability of measurement devices to detect coherence from the measurement statistics. Based on a recently developed resource theory of quantum operations, here we quantify experimentally the ability of a typical quantum-optical detector, the weak-field homodyne detector, to detect coherence. We derive an improved algorithm for quantum detector tomography and apply it to reconstruct the positive-operator-valued measures of the detector in different configurations. The reconstructed positive-operator-valued measures are then employed to evaluate how well the detector can detect coherence using two computable measures. As the first experimental investigation of quantum measurements from a resource theoretical perspective, our work sheds new light on the rigorous evaluation of the performance of a quantum measurement apparatus.

On quantum gravity tests with composite particles.

Models of quantum gravity imply a fundamental revision of our description of position and momentum that manifests in modifications of the canonical commutation relations. Experimental tests of such modifications remain an outstanding challenge. These corrections scale with the mass of test particles, which motivates experiments using macroscopic composite particles. Here we consider a challenge to such tests, namely that quantum gravity corrections of canonical commutation relations are expected to be suppressed with increasing number of constituent particles. Since the precise scaling of this suppression is unknown, it needs to be bounded experimentally and explicitly incorporated into rigorous analyses of quantum gravity tests. We analyse this scaling based on data from past experiments involving macroscopic pendula, and provide tight bounds that exceed those of current experiments based on quantum mechanical oscillators. Furthermore, we discuss possible experiments that promise even stronger bounds thus bringing rigorous and well-controlled tests of quantum gravity closer to reality.

Nanoscale Dynamic Readout of a Chemical Redox Process Using Radicals Coupled with Nitrogen-Vacancy Centers in Nanodiamonds.

Biocompatible nanoscale probes for sensitive detection of paramagnetic species and molecules associated with their (bio)chemical transformations would provide a desirable tool for a better understanding of cellular redox processes. Here, we describe an analytical tool based on quantum sensing techniques. We magnetically coupled negatively charged nitrogen-vacancy (NV) centers in nanodiamonds (NDs) with nitroxide radicals present in a bioinert polymer coating of the NDs. We demonstrated that the T1 spin relaxation time of the NV centers is very sensitive to the number of nitroxide radicals, with a resolution down to ∼10 spins per ND (detection of approximately 10-23 mol in a localized volume). The detection is based on T1 shortening upon the radical attachment, and we propose a theoretical model describing this phenomenon. We further show that this colloidally stable, water-soluble system can be used dynamically for spatiotemporal readout of a redox chemical process (oxidation of ascorbic acid) occurring near the ND surface in an aqueous environment under ambient conditions.