*J Phys Chem Lett ; 14(2): 340-346, 2023 Jan 19.*

##### RESUMO

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.

*Phys Rev Lett ; 129(14): 140604, 2022 Sep 30.*

##### RESUMO

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.

*Phys Rev Lett ; 129(15): 150501, 2022 Oct 07.*

##### RESUMO

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.

*Phys Rev Lett ; 129(12): 120501, 2022 Sep 16.*

##### RESUMO

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.

*J Am Chem Soc ; 144(28): 12642-12651, 2022 07 20.*

##### RESUMO

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.

##### Assuntos

Nanodiamantes , Peróxido de Hidrogênio , Nitrogênio*Phys Rev Lett ; 128(11): 110401, 2022 Mar 18.*

##### RESUMO

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.

*J Phys Chem Lett ; 13(7): 1791-1796, 2022 Feb 24.*

##### RESUMO

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.

*J Am Chem Soc ; 144(6): 2511-2519, 2022 02 16.*

##### RESUMO

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.

*Phys Rev Lett ; 126(19): 193602, 2021 May 14.*

##### RESUMO

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.

*J Magn Reson ; 322: 106860, 2021 01.*

##### RESUMO

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.

*Phys Rev Lett ; 125(13): 130401, 2020 Sep 25.*

##### RESUMO

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.

*Phys Rev Lett ; 125(11): 110504, 2020 Sep 11.*

##### RESUMO

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.

*Phys Rev Lett ; 125(6): 060404, 2020 Aug 07.*

##### RESUMO

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.

*Nat Commun ; 11(1): 3900, 2020 Aug 06.*

##### RESUMO

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.

*ACS Nano ; 14(10): 12938-12950, 2020 10 27.*

##### RESUMO

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 â¼10 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.

*Phys Rev Lett ; 125(2): 023602, 2020 Jul 10.*

##### RESUMO

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.

*Phys Rev Lett ; 124(23): 230602, 2020 Jun 12.*

##### RESUMO

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.

*Angew Chem Int Ed Engl ; 59(38): 16455-16458, 2020 09 14.*

##### RESUMO

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.

##### Assuntos

Carbocianinas/metabolismo , Corantes/metabolismo , Complexos de Proteínas Captadores de Luz/metabolismo , Nanopartículas/metabolismo , Porfirinas/metabolismo , Rotaxanos/metabolismo , Carbocianinas/química , Corantes/química , Complexos de Proteínas Captadores de Luz/química , Modelos Moleculares , Nanopartículas/química , Porfirinas/química , Rotaxanos/química*Natl Sci Rev ; 7(2): 254-260, 2020 Feb.*

##### RESUMO

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 13C 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.

*Phys Rev Lett ; 123(10): 100502, 2019 Sep 06.*

##### RESUMO

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.