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The combination of chain-mapping and tensor-network techniques provides a powerful tool for the numerically exact simulation of open quantum systems interacting with structured environments. However, these methods suffer from a quadratic scaling with the physical simulation time, and therefore, they become challenging in the presence of multiple environments. This is particularly true when fermionic environments, well-known to be highly correlated, are considered. In this work, we first illustrate how a thermo-chemical modulation of the spectral density allows replacing the original fermionic environments with equivalent, but simpler, ones. Moreover, we show how this procedure reduces the number of chains needed to model multiple environments. We then provide a derivation of the fermionic Markovian closure construction, consisting of a small collection of damped fermionic modes undergoing a Lindblad-type dynamics and mimicking a continuum of bath modes. We describe, in particular, how the use of the Markovian closure allows for a polynomial reduction of the time complexity of chain-mapping based algorithms when long-time dynamics are needed., (© 2024 Author(s). Published under an exclusive license by AIP Publishing.)

Parahydrogen-induced polarization (PHIP) is an inexpensive way to produce hyperpolarized molecules with polarization levels of >10 % in the solution-state, but is strongly limited in generality since it requires chemical reactions/ interactions with H 2 . Here we report a new method to widen the scope of PHIP hyperpolarization: a source molecule is produced via PHIP with high 13 C polarization, and precipitated out of solution together with a target species. Spin diffusion within the solid carries the polarization onto 13 C spins of the target, which can then be dissolved for solution-state applications. We name this method PHIP-SSD (PHIP with solid-state spin diffusion) and demonstrate it using PHIP-polarized [1- 13 C]-fumarate as the source molecule, to polarize different 13 C-labelled target molecules. 13 C polarizations of between 0.01 and 3 % were measured on [1- 13 C]-benzoic acid, depending on the molar ratio of fumarate:benzoate in the solid state. We also show that PHIP-SSD does not require specific co-crystallization conditions by grinding dry powders of target molecules together with solid fumarate crystals, and obtain 13 C signal enhancements of between 100 and 200 on [ 13 C, 15 N 2 ]-urea, [1- 13 C]-pyruvate, and [1- 13 C]-benzoic acid. This approach appears to be a promising new strategy for facile hyperpolarization based on PHIP., (© 2024 Wiley-VCH GmbH.)

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 target 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 due to the field produced by the sample magnetization during polarization transfer, which leads to complex dynamics and can severely affect the scalability of the technique. We address this challenge with a pulse sequence that suppresses 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.

We present a quantum sensing technique that utilizes a sequence of π pulses to cyclically drive the qubit dynamics along a geodesic path of adiabatic evolution. This approach effectively suppresses the effects of both decoherence noise and control errors while simultaneously removing unwanted resonance terms, such as higher harmonics and spurious responses commonly encountered in dynamical decoupling control. As a result, our technique offers robust, wide-band, unambiguous, and high-resolution quantum sensing capabilities for signal detection and individual addressing of quantum systems, including spins. To demonstrate its versatility, we showcase successful applications of our method in both low-frequency and high-frequency sensing scenarios. The significance of this quantum sensing technique extends to the detection of complex signals and the control of intricate quantum environments. By enhancing detection accuracy and enabling precise manipulation of quantum systems, our method holds considerable promise for a variety of practical applications.

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., Competing Interests: Declaration of competing interest The authors declare the following financial interests/personal relationships which may be considered as potential competing interests: Laurynas Dagys, Tim R. Eichhorn, Stefan Knecht, Christoph Müller, Alon Salhov, and Ilai Schwartz are employees of NVision Imaging Technologies GmbH (NVision). Martin B. Plenio and Ilai Schwartz are co-founders and shareholders of NVision. NVision is commercializing products in the field of magnetic resonance hyperpolarization. A patent application relating to the subject matter of this work has been filed under International Filing Number: PCT/IB2021/000202., (Copyright © 2024 The Author(s). Published by Elsevier Inc. All rights reserved.)

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.

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.

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., (© 2023. BioMed Central Ltd., part of Springer Nature.)

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.

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., Competing Interests: Conflict of interestThe authors declare no competing interests., (© The Author(s) 2022.)

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.

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.

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.

Hydrogen peroxide (H 2 O 2 ) plays an important role in various signal transduction pathways and regulates important cellular processes. However, monitoring and quantitatively assessing the distribution of H 2 O 2 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 H 2 O 2 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 H 2 O 2 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 H 2 O 2 at the cellular level.

The primary steps of photosynthesis rely on the generation, transport, and trapping of excitons in pigment-protein complexes (PPCs). Generically, PPCs possess highly structured vibrational spectra, combining many discrete intra-pigment modes and a quasi-continuous of protein modes, with vibrational and electronic couplings of comparable strength. The intricacy of the resulting vibronic dynamics poses significant challenges in establishing a quantitative connection between spectroscopic data and underlying microscopic models. Here we show how to address this challenge using numerically exact simulation methods by considering two model systems, namely the water-soluble chlorophyll-binding protein of cauliflower and the special pair of bacterial reaction centers. We demonstrate that the inclusion of the full multi-mode vibronic dynamics in numerical calculations of linear spectra leads to systematic and quantitatively significant corrections to electronic parameter estimation. These multi-mode vibronic effects are shown to be relevant in the longstanding discussion regarding the origin of long-lived oscillations in multidimensional nonlinear spectra., (© 2022. The Author(s).)

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.

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.

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 1 H 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.

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.

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., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020. Published by Elsevier Inc.)

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 T 1 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 T 1 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.

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.

A nanoring-rotaxane supramolecular assembly with a Cy7 cyanine dye (hexamethylindotricarbocyanine) threaded along the axis of the nanoring was synthesized as a model for the energy transfer between the light-harvesting complex LH1 and the reaction center in purple bacteria photosynthesis. The complex displays efficient energy transfer from the central cyanine dye to the surrounding zinc porphyrin nanoring. We present a theoretical model that reproduces the absorption spectrum of the nanoring and quantifies the excitonic coupling between the nanoring and the central dye, thereby explaining the efficient energy transfer and demonstrating similarity with structurally related natural light-harvesting systems., (© 2020 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.)

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.

We employ spherical t-designs for the systematic construction of solids whose rotational degrees of freedom can be made robust to decoherence due to external fluctuating fields while simultaneously retaining their sensitivity to signals of interest. Specifically, the ratio of signal phase accumulation rate from a nearby source to the decoherence rate caused by fluctuating fields from more distant sources can be incremented to any desired level by using increasingly complex shapes. This allows for the generation of long-lived macroscopic quantum superpositions of rotational degrees of freedom and the robust generation of entanglement between two or more such solids with applications in robust quantum sensing and precision metrology as well as quantum registers.

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.

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.

We extend the concept of dynamical decoupling from spin to mechanical degrees of freedom of macroscopic objects, for application in interferometry. In this manner, the superposition of matter waves can be made resilient to many important sources of noise when these are driven along suitable paths in space. As a concrete implementation, we present the case of levitated (or free falling) nanodiamonds hosting a color center in a magnetic field gradient. We point out that these interferometers are inherently affected by diamagnetic forces, which restrict the separation of the superposed states to distances that scale with the inverse of the magnetic field gradient. Periodic forcing of the mechanical degree of freedom is shown to overcome this limitation, achieving a linear-in-time growth of the separation distance independent of the magnetic field gradient, while simultaneously protecting the coherence of the superposition from environmental perturbations.

We investigate the quench dynamics of an open quantum system involving a quantum phase transition. In the isolated case, the quench dynamics involving the phase transition exhibits a number of scaling relations with the quench rate as predicted by the celebrated Kibble-Zurek mechanism. In contact with an environment however, these scaling laws break down and one may observe an anti-Kibble-Zurek behavior: slower ramps lead to less adiabatic dynamics, increasing thus nonadiabatic effects with the quench time. In contrast to previous works, we show here that such anti-Kibble-Zurek scaling can acquire a universal form in the sense that it is determined by the equilibrium critical exponents of the phase transition, provided the excited states of the system exhibit singular behavior, as observed in fully connected models. This demonstrates novel universal scaling laws granted by a system-environment interaction in a critical system. We illustrate these findings in two fully connected models, namely, the quantum Rabi and the Lipkin-Meshkov-Glick models. In addition, we discuss the impact of nonlinear ramps and finite-size systems.

Geometry and topology are fundamental concepts, which underlie a wide range of fascinating physical phenomena such as topological states of matter and topological defects. In quantum mechanics, the geometry of quantum states is fully captured by the quantum geometric tensor. Using a qubit formed by an NV center in diamond, we perform the first experimental measurement of the complete quantum geometric tensor. Our approach builds on a strong connection between coherent Rabi oscillations upon parametric modulations and the quantum geometry of the underlying states. We then apply our method to a system of two interacting qubits, by exploiting the coupling between the NV center spin and a neighboring 13 C nuclear spin. Our results establish coherent dynamical responses as a versatile probe for quantum geometry, and they pave the way for the detection of novel topological phenomena in solid state., (© The Author(s) 2019. Published by Oxford University Press on behalf of China Science Publishing & Media Ltd.)

The measured multidimensional spectral response of different light harvesting complexes exhibits oscillatory features which suggest an underlying coherent energy transfer. However, making this inference rigorous is challenging due to the difficulty of isolating excited state coherences in highly congested spectra. In this work, we provide a coherent control scheme that suppresses ground state coherences, thus making rephasing spectra dominated by excited state coherences. We provide a benchmark for the scheme using a model dimeric system and numerically exact methods to analyze the spectral response. We argue that combining temporal and spectral control methods can facilitate a second generation of experiments that are tailored to extract desired information and thus significantly advance our understanding of complex open many-body structure and dynamics.

Charge and energy transfer in biological and synthetic organic materials are strongly influenced by the coupling of electronic states to a highly structured dissipative environment. Nonperturbative simulations of these systems require a substantial computational effort, and current methods can only be applied to large systems if environmental structures are severely coarse grained. Time evolution methods based on tensor networks are fundamentally limited by the times that can be reached due to the buildup of entanglement in time, which quickly increases the size of the tensor representation, i.e., the bond dimension. In this Letter, we introduce a dissipation-assisted matrix product factorization (DAMPF) method that combines a tensor network representation of the vibronic state within a pseudomode description of the environment where a continuous bosonic environment is mapped into a few harmonic oscillators under Lindblad damping. This framework is particularly suitable for a tensor network representation, since damping suppresses the entanglement growth among oscillators and significantly reduces the bond dimension required to achieve a desired accuracy. We show that dissipation removes the "time-wall" limitation of existing methods, enabling the long-time simulation of large vibronic systems consisting of 10-50 sites coupled to 100-1000 underdamped modes in total and for a wide range of parameter regimes. For these reasons, we believe that our formalism will facilitate the investigation of spatially extended systems with applications to quantum biology, organic photovoltaics, and quantum thermodynamics.

Chain-mapping techniques in combination with the time-dependent density matrix renormalization group are a powerful tool for the simulation of open-system quantum dynamics. For finite-temperature environments, however, this approach suffers from an unfavorable algorithmic scaling with increasing temperature. We prove that the system dynamics under thermal environments can be nonperturbatively described by temperature-dependent system-environmental couplings with the initial environment state being in its pure vacuum state, instead of a mixed thermal state. As a consequence, as long as the initial system state is pure, the global system-environment state remains pure at all times. The resulting speed-up and relaxed memory requirements of this approach enable the efficient simulation of open quantum systems interacting with highly structured environments in any temperature range, with applications extending from quantum thermodynamics to quantum effects in mesoscopic systems.

Quantum adiabatic evolutions find a broad range of applications in quantum physics and quantum technologies. The traditional form of the quantum adiabatic theorem limits the speed of adiabatic evolution by the minimum energy gaps of the system Hamiltonian. Here, we experimentally show using a nitrogen-vacancy center in diamond that, even in the presence of vanishing energy gaps, quantum adiabatic evolution is possible. This verifies a recently derived necessary and sufficient quantum adiabatic theorem and offers paths to overcome the conventionally assumed constraints on adiabatic methods. By fast modulation of dynamic phases, we demonstrate near-unit-fidelity quantum adiabatic processes in finite times. These results challenge traditional views and provide deeper understanding on quantum adiabatic processes, as well as promising strategies for the control of quantum systems.

We develop theoretically and demonstrate experimentally a universal dynamical decoupling method for robust quantum sensing with unambiguous signal identification. Our method uses randomization of control pulses to simultaneously suppress two types of errors in the measured spectra that would otherwise lead to false signal identification. These are spurious responses due to finite-width π pulses, as well as signal distortion caused by π pulse imperfections. For the cases of nanoscale nuclear-spin sensing and ac magnetometry, we benchmark the performance of the protocol with a single nitrogen vacancy center in diamond against widely used nonrandomized pulse sequences. Our method is general and can be combined with existing multipulse quantum sensing sequences to enhance their performance.

In this Letter, we demonstrate initialization and readout of nuclear spins via a negatively charged silicon-vacancy (SiV) electron spin qubit. Under Hartmann-Hahn conditions the electron spin polarization is coherently transferred to the nuclear spin. The readout of the nuclear polarization is observed via the fluorescence of the SiV. We also show that the coherence time of the nuclear spin (6 ms) is limited by the electron spin-lattice relaxation due to the hyperfine coupling to the electron spin. This Letter paves the way toward realization of building blocks of quantum hardware with an efficient spin-photon interface based on the SiV color center coupled to a long lasting nuclear memory.

To describe certain facets of nonclassicality, it is necessary to quantify properties of operations instead of states. This is the case if one wants to quantify how well an operation detects nonclassicality, which is a necessary prerequisite for its use in quantum technologies. To do so rigorously, we build resource theories on the level of operations, exploiting the concept of resource destroying maps. We discuss the two basic ingredients of these resource theories, the free operations and the free superoperations, which are sequential and parallel concatenations with free operations. This leads to defining properties of functionals that are well suited to quantify the resources of operations. We introduce these concepts at the example of coherence. In particular, we present two measures quantifying the ability of an operation to detect, i.e., to use, coherence, one of them with an operational interpretation, and provide methods to evaluate them.

Nitrogen vacancy (NV) centers in diamond have been used as ultrasensitive magnetometers to perform nuclear magnetic resonance (NMR) spectroscopy of statistically polarized samples at 1-100 nm length scales. However, the spectral linewidth is typically limited to the kHz level, both by the NV sensor coherence time and by rapid molecular diffusion of the nuclei through the detection volume which in turn is critical for achieving long nuclear coherence times. Here we provide a blueprint supported by detailed theoretical analysis for a set-up that combines a sensitivity sufficient for detecting NMR signals from nano- to micron-scale samples with a spectral resolution that is limited only by the nuclear spin coherence, i.e. comparable to conventional NMR. Our protocol detects the nuclear polarization induced along the direction of an external magnetic field with near surface NV centers using lock-in detection techniques to enable phase coherent signal averaging. Using the NV centers in a dual role of NMR detector and optical hyperpolarization source to increase signal to noise, and in combination with Bayesian inference models for signal processing, nano/microscale NMR spectroscopy can be performed on sample concentrations in the micromolar range, several orders of magnitude better than the current state of the art.

Recent observation of quantum emitters in monolayers of hexagonal boron nitride (h-BN) has provided a novel platform for optomechanical experiments where the single-photon emitters can couple to the motion of a freely suspended h-BN membrane. Here, we propose a scheme where the electronic degree of freedom (d.o.f.) of an embedded color center is coupled to the motion of the hosting h-BN resonator via dispersive forces. We show that the coupling of membrane vibrations to the electronic d.o.f. of the emitter can reach the strong regime. By suitable driving of a three-level Λ-system composed of two spin d.o.f. in the electronic ground state as well as an isolated excited state of the emitter, a multiple electromagnetically induced transparency spectrum becomes available. The experimental feasibility of the efficient vibrational ground-state cooling of the membrane via quantum interference effects in the two-color drive scheme is numerically confirmed. More interestingly, the emission spectrum of the defect exhibits a frequency comb with frequency spacings as small as the fundamental vibrational mode, which finds applications in high-precision spectroscopy.

We develop energy efficient, continuous microwave schemes to couple electron and nuclear spins, using phase or amplitude modulation to bridge their frequency difference. These controls have promising applications in biological systems, where microwave power should be limited, as well as in situations with high Larmor frequencies due to large magnetic fields and nuclear magnetic moments. These include nanoscale NMR where high magnetic fields achieves enhanced thermal nuclear polarization and larger chemical shifts. Our controls are also suitable for quantum information processors and nuclear polarization schemes.

We experimentally observe Floquet Raman transitions in the weakly driven solid-state spin system of a nitrogen-vacancy center in diamond. The periodically driven spin system simulates a two-band Wannier-Stark ladder model and allows us to observe coherent spin state transfer arising from a Raman transition mediated by Floquet synthetic levels. It also leads to the prediction of an analog photon-assisted Floquet Raman transition and dynamical localization in a driven two-level quantum system. The demonstrated rich Floquet dynamics offers new capabilities to achieve effective Floquet coherent control of a quantum system with potential applications in various types of quantum technologies based on driven quantum dynamics. In particular, the Floquet Raman system may be used as a quantum simulator for the physics of periodically driven systems.

Ultra-thin layers of liquids on a surface behave differently from bulk liquids due to liquid-surface interactions. Some examples are significant changes in diffusion properties and the temperature at which the liquid-solid phase transition takes place. Indeed, molecular dynamics simulations suggest that thin layers of water on a diamond surface may remain solid even well above room temperature. However, because of the small volumes that are involved, it is exceedingly difficult to examine these phenomena experimentally with current technologies. In this context, shallow NV centres promise a highly sensitive tool for the investigation of magnetic signals emanating from liquids and solids that are deposited on the surface of a diamond. Moreover, NV centres are non-invasive sensors with extraordinary performance even at room-temperature. To that end, we present here a theoretical work, complemented with numerical evidence based on bosonization techniques, that predicts the measurable signal from a single NV centre when interacting with large spin baths in different configurations. In fact, by means of continuous dynamical decoupling, the polarization exchange between a single NV centre and the hydrogen nuclear spins from the water molecules is enhanced, leading to differences in the coherent dynamics of the NV centre that are interpreted as an unambiguous trace of the molecular structure. We therefore propose single NV centres as sensors capable to resolve structural water features at the nanoscale and even sensitive to phase transitions.

Dynamic nuclear polarization (DNP) is an important technique that uses polarization transfer from electron to nuclear spins to achieve nuclear hyperpolarization. Combining efficient DNP with optically polarized nitrogen-vacancy (NV) centers offers promising opportunities for novel technological applications, including nanoscale nuclear magnetic resonance spectroscopy of liquids, hyperpolarized nanodiamonds as magnetic resonance imaging contrast agents, and the initialization of nuclear spin-based diamond quantum simulators. However, none of the current realizations of polarization transfer are simultaneously robust and sufficiently efficient, making the realization of the applications extremely challenging. We introduce the concept of systematically designing polarization sequences by Hamiltonian engineering, resulting in polarization sequences that are robust and fast. We theoretically derive sequences and experimentally demonstrate that they are capable of efficient polarization transfer from optically polarized NV centers in diamond to the surrounding 13 C nuclear spin bath even in the presence of control errors, making the abovementioned novel applications possible.

We present a flexible scheme to realize non-Markovian dynamics of an electronic spin qubit, using a nitrogen-vacancy center in diamond where the inherent nitrogen spin serves as a regulator of the dynamics. By changing the population of the nitrogen spin, we show that we can smoothly tune the non-Markovianity of the electron spin's dynamics. Furthermore, we examine the decoherence dynamics induced by the spin bath to exclude other sources of non-Markovianity. The amount of collected measurement data is kept at a minimum by employing Bayesian data analysis. This allows for a precise quantification of the parameters involved in the description of the dynamics and a prediction of so far unobserved data points.

We propose a quantum control scheme aimed at interacting systems that gives rise to highly selective coupling among their near-to-resonance constituents. Our protocol implements temporal control of the interaction strength, switching it on and off again adiabatically. This soft temporal modulation significantly suppresses off-resonant contributions in the interactions. Among the applications of our method we show that it allows us to perform an efficient rotating-wave approximation in a wide parameter regime, the elimination of side peaks in quantum sensing experiments, and selective high-fidelity entanglement gates on nuclear spins with close frequencies. We apply our theory to nitrogen-vacancy centers in diamond and demonstrate the possibility for the detection of weak electron-nuclear coupling under the presence of strong perturbations.

Nonlinear spectroscopy has revealed long-lasting oscillations in the optical response of a variety of photosynthetic complexes. Different theoretical models that involve the coherent coupling of electronic (excitonic) or electronic-vibrational (vibronic) degrees of freedom have been put forward to explain these observations. The ensuing debate concerning the relevance of either mechanism may have obscured their complementarity. To illustrate this balance, we quantify how the excitonic delocalization in the LH2 unit of Rhodopseudomonas acidophila purple bacterium leads to correlations of excitonic energy fluctuations, relevant coherent vibronic coupling, and importantly, a decrease in the excitonic dephasing rates. Combining these effects, we identify a feasible origin for the long-lasting oscillations observed in fluorescent traces from time-delayed two-pulse single-molecule experiments performed on this photosynthetic complex and use this approach to discuss the role of this complementarity in other photosynthetic systems.

We devise an all-optical scheme for the generation of entangled multimode photonic states encoded in temporal modes of light. The scheme employs a nonlinear down-conversion process in an optical loop to generate one- and higher-dimensional tensor network states of light. We illustrate the principle with the generation of two different classes of entangled tensor network states and report on a variational algorithm to simulate the ground-state physics of many-body systems. We demonstrate that state-of-the-art optical devices are capable of determining the ground-state properties of the spin-1/2 Heisenberg model. Finally, implementations of the scheme are demonstrated to be robust against realistic losses and mode mismatch.

Efficient polarization of organic molecules is of extraordinary relevance when performing nuclear magnetic resonance (NMR) and imaging. Commercially available routes to dynamical nuclear polarization (DNP) work at extremely low temperatures, relying on the solidification of organic samples and thus bringing the molecules out of their ambient thermal conditions. In this work, we investigate polarization transfer from optically pumped nitrogen vacancy centers in diamond to external molecules at room temperature. This polarization transfer is described by both an extensive analytical analysis and numerical simulations based on spin bath bosonization and is supported by experimental data in excellent agreement. These results set the route to hyperpolarization of diffusive molecules in different scenarios and consequently, due to an increased signal, to high-resolution NMR.

We identify the conditions that guarantee equivalence of the reduced dynamics of an open quantum system (OQS) for two different types of environments-one a continuous bosonic environment leading to a unitary system-environment evolution and the other a discrete-mode bosonic environment resulting in a system-mode (nonunitary) Lindbladian evolution. Assuming initial Gaussian states for the environments, we prove that the two OQS dynamics are equivalent if both the expectation values and two-time correlation functions of the environmental interaction operators are the same at all times for the two configurations. Since the numerical and analytical description of a discrete-mode environment undergoing a Lindbladian evolution is significantly more efficient than that of a continuous bosonic environment in a unitary evolution, our result represents a powerful, nonperturbative tool to describe complex and possibly highly non-Markovian dynamics. As a special application, we recover and generalize the well-known pseudomodes approach to open-system dynamics.