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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).)

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.

Methods to selectively detect and manipulate nuclear spins by single electrons of solid-state defects play a central role for quantum information processing and nanoscale nuclear magnetic resonance (NMR). However, with standard techniques, no more than eight nuclear spins have been resolved by a single defect centre. Here we develop a method that improves significantly the ability to detect, address and manipulate nuclear spins unambiguously and individually in a broad frequency band by using a nitrogen-vacancy (NV) centre as model system. On the basis of delayed entanglement control, a technique combining microwave and radio frequency fields, our method allows to selectively perform robust high-fidelity entangling gates between hardly resolved nuclear spins and the NV electron. Long-lived qubit memories can be naturally incorporated to our method for improved performance. The application of our ideas will increase the number of useful register qubits accessible to a defect centre and improve the signal of nanoscale NMR.

The optical excitation of organic semiconductors not only generates charge-neutral electron-hole pairs (excitons), but also charge-separated polaron pairs with high yield. The microscopic mechanisms underlying this charge separation have been debated for many years. Here we use ultrafast two-dimensional electronic spectroscopy to study the dynamics of polaron pair formation in a prototypical polymer thin film on a sub-20-fs time scale. We observe multi-period peak oscillations persisting for up to about 1 ps as distinct signatures of vibronic quantum coherence at room temperature. The measured two-dimensional spectra show pronounced peak splittings revealing that the elementary optical excitations of this polymer are hybridized exciton-polaron-pairs, strongly coupled to a dominant underdamped vibrational mode. Coherent vibronic coupling induces ultrafast polaron pair formation, accelerates the charge separation dynamics and makes it insensitive to disorder. These findings open up new perspectives for tailoring light-to-current conversion in organic materials.

Natural and artificial light-harvesting processes have recently gained new interest. Signatures of long-lasting coherence in spectroscopic signals of biological systems have been repeatedly observed, albeit their origin is a matter of ongoing debate, as it is unclear how the loss of coherence due to interaction with the noisy environments in such systems is averted. Here we report experimental and theoretical verification of coherent exciton-vibrational (vibronic) coupling as the origin of long-lasting coherence in an artificial light harvester, a molecular J-aggregate. In this macroscopically aligned tubular system, polarization-controlled 2D spectroscopy delivers an uncongested and specific optical response as an ideal foundation for an in-depth theoretical description. We derive analytical expressions that show under which general conditions vibronic coupling leads to prolonged excited-state coherence.

Nuclear magnetic resonance spectroscopy and magnetic resonance imaging at the ultimate sensitivity limit of single molecules or single nuclear spins requires fundamentally new detection strategies. The strong coupling regime, when interaction between sensor and sample spins dominates all other interactions, is one such strategy. In this regime, classically forbidden detection of completely unpolarized nuclei is allowed, going beyond statistical fluctuations in magnetization. Here we realize strong coupling between an atomic (nitrogen-vacancy) sensor and sample nuclei to perform nuclear magnetic resonance on four (29)Si spins. We exploit the field gradient created by the diamond atomic sensor, in concert with compressed sensing, to realize imaging protocols, enabling individual nuclei to be located with Angstrom precision. The achieved signal-to-noise ratio under ambient conditions allows single nuclear spin sensitivity to be achieved within seconds.

The ability to measure weak signals such as pressure, force, electric field and temperature with nanoscale devices and high spatial resolution offers a wide range of applications in fundamental and applied sciences. Here we present a proposal for a hybrid device composed of thin film layers of diamond with colour centres and piezoactive elements for the transduction and measurement of physical signals. The magnetic response of a piezomagnetic layer to an external stress or a stress induced by a signal is shown to affect significantly the spin properties of nitrogen-vacancy centres in diamond. Under ambient conditions, realistic environmental noise and material imperfections, we show that this hybrid device can achieve significant improvements in sensitivity over the pure diamond-based approach in combination with nanometre-scale spatial resolution. Furthermore, the proposed hybrid architecture offers novel possibilities for engineering strong coherent couplings between nanomechanical oscillator and solid state spin qubits.

Symmetry breaking phase transitions play an important role in nature. When a system traverses such a transition at a finite rate, its causally disconnected regions choose the new broken symmetry state independently. Where such local choices are incompatible, topological defects can form. The Kibble-Zurek mechanism predicts the defect densities to follow a power law that scales with the rate of the transition. Owing to its ubiquitous nature, this theory finds application in a wide field of systems ranging from cosmology to condensed matter. Here we present the successful creation of defects in ion Coulomb crystals by a controlled quench of the confining potential, and observe an enhanced power law scaling in accordance with numerical simulations and recent predictions. This simple system with well-defined critical exponents opens up ways to investigate the physics of non-equilibrium dynamics from the classical to the quantum regime.

Entanglement is a fundamental resource for quantum information processing, occurring naturally in many-body systems at low temperatures. The presence of entanglement and, in particular, its scaling with the size of system partitions underlies the complexity of quantum many-body states. The quantitative estimation of entanglement in many-body systems represents a major challenge, as it requires either full-state tomography, scaling exponentially in the system size, or the assumption of unverified system characteristics such as its Hamiltonian or temperature. Here we adopt recently developed approaches for the determination of rigorous lower entanglement bounds from readily accessible measurements and apply them in an experiment of ultracold interacting bosons in optical lattices of ~10(5) sites. We then study the behaviour of spatial entanglement between the sites when crossing the superfluid-Mott insulator transition and when varying temperature. This constitutes the first rigorous experimental large-scale entanglement quantification in a scalable quantum simulator.

Traversal of a symmetry-breaking phase transition at finite rates can lead to causally separated regions with incompatible symmetries and the formation of defects at their boundaries, which has a crucial role in quantum and statistical mechanics, cosmology and condensed matter physics. This mechanism is conjectured to follow universal scaling laws prescribed by the Kibble-Zurek mechanism. Here we determine the scaling law for defect formation in a crystal of 16 laser-cooled trapped ions, which are conducive to the precise control of structural phases and the detection of defects. The experiment reveals an exponential scaling of defect formation γ(β), where γ is the rate of traversal of the critical point and β=2.68±0.06. This supports the prediction of β=8/3≈2.67 for finite inhomogeneous systems. Our result demonstrates that the scaling laws also apply in the mesoscopic regime and emphasizes the potential for further tests of non-equilibrium thermodynamics with ion crystals.

Quantum state tomography--deducing quantum states from measured data--is the gold standard for verification and benchmarking of quantum devices. It has been realized in systems with few components, but for larger systems it becomes unfeasible because the number of measurements and the amount of computation required to process them grows exponentially in the system size. Here, we present two tomography schemes that scale much more favourably than direct tomography with system size. One of them requires unitary operations on a constant number of subsystems, whereas the other requires only local measurements together with more elaborate post-processing. Both rely only on a linear number of experimental operations and post-processing that is polynomial in the system size. These schemes can be applied to a wide range of quantum states, in particular those that are well approximated by matrix product states. The accuracy of the reconstructed states can be rigorously certified without any a priori assumptions.