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Recent observations of oscillatory features in the optical response of photosynthetic complexes have revealed evidence for surprisingly long-lasting electronic coherences which can coexist with energy transport. These observations have ignited multidisciplinary interest in the role of quantum effects in biological systems, including the fundamental question of how electronic coherence can survive in biological surroundings. Here we show that the non-trivial spectral structures of protein fluctuations can generate non-equilibrium processes that lead to the spontaneous creation and sustenance of electronic coherence, even at physiological temperatures. Developing new advanced simulation tools to treat these effects, we provide a firm microscopic basis to successfully reproduce the experimentally observed coherence times in the Fenna–Matthews–Olson complex, and illustrate how detailed quantum modelling and simulation can shed further light on a wide range of other non-equilibrium processes which may be important in different photosynthetic systems. Photosynthesis is remarkably efficient. The transport of optically generated excitons from absorbing pigments, through protein complexes, to reaction centres is nearly perfect. Simulations now uncover the microscopic mechanism that drives this coherent behaviour: interactions between the excitons and the vibrational modes of the pigment-protein complex.

The electrical control and readout of single two-level state defects in a defective oxide film grown directly on the channel of a thin-film FET allow for the extraction of individual long relaxation times. Electronic defect states at material interfaces provide highly deleterious sources of noise in solid-state nanostructures, and even a single trapped charge can qualitatively alter the properties of short one-dimensional nanowire field-effect transistors (FET) and quantum bit (qubit) devices 1 , 2 , 3 , 4 , 5 . Understanding the dynamics of trapped charge is thus essential for future nanotechnologies, but their direct detection and manipulation is rather challenging 2 , 4 , 5 . Here, a transistor-based set-up is used to create and probe individual electronic defect states that can be coherently driven with microwave (MW) pulses. Strikingly, we resolve a large number of very high quality ( Q ∼ 1 × 10 5 ) resonances in the transistor current as a function of MW frequency and demonstrate both long decoherence times (∼1 μs—40 μs) and coherent control of the defect-induced dynamics. Efficiently characterizing over 800 individually addressable resonances across two separate defect-hosting materials, we propose that their properties are consistent with weakly driven two-level systems.

The quantum dynamics of transport networks in the presence of noisy environments has recently received renewed attention with the discovery of long-lived coherences in different photosynthetic complexes. This experimental evidence has raised two fundamental questions: firstly, what are the mechanisms supporting long-lived coherences; and, secondly, how can we assess the possible functional role that the interplay of noise and quantum coherence might play in the seemingly optimal operation of biological systems under natural conditions? Here, we review recent results, illuminate them by means of two paradigmatic systems (the Fenna-Matthew-Olson complex and the light-harvesting complex LHII) and present new progress on both questions.

Understanding the charge-separation mechanism in organic photovoltaic cells (OPVs) could facilitate optimization of their overall efficiency. Here we report the time dependence of the separation of photogenerated electron hole pairs across the donor-acceptor heterojunction in OPV model systems. By tracking the modulation of the optical absorption due to the electric field generated between the charges, we measure ∼200 millielectron volts of electrostatic energy arising from electron-hole separation within 40 femtoseconds of excitation, corresponding to a charge separation distance of at least 4 nanometers. At this separation, the residual Coulomb attraction between charges is at or below thermal energies, so that electron and hole separate freely. This early time behavior is consistent with charge separation through access to delocalized π-electron states in ordered regions of the fullerene acceptor material.

Chain-mapping techniques combined with the time-dependent density matrix renormalization group are powerful tools for simulating the dynamics of open quantum systems interacting with structured bosonic environments. Most interestingly, they leave the degrees of freedom of the environment open to inspection. In this work, we fully exploit the access to environmental observables to illustrate how the evolution of the open quantum system can be related to the detailed evolution of the environment it interacts with. In particular, we give a precise description of the fundamental physics that enables the finite temperature chain-mapping formalism to express dynamical equilibrium states. Furthermore, we analyze a two-level system strongly interacting with a super-Ohmic environment, where we discover a change in the spin-boson ground state that can be traced to the formation of polaronic states.

Nature Materials 16, 208–213 (2017); published online 19 September 2016; corrected after print 30 June 2017 In this work we reported the development of a rigorous mathematical and physical framework in order to model the detailed time-resolved behaviour of over 800 resonances that we studied, through continuous-wave and single-pulse microwave spectroscopy measurements in a field-effect transistor.

Engineering and harnessing coherent excitonic transport in organic nanostructures has recently been suggested as a promising way towards improving man-made light harvesting materials. However, realising and testing the dissipative system-environment models underlying these proposals is presently very challenging in supramolecular materials. A promising alternative is to use simpler and highly tunable quantum simulators built from programmable qubits, as recently achieved in a superconducting circuit by Potocnik et al. In this article, we simulate the real-time dynamics of an exciton coupled to a quantum bath as it moves through a network based on the quantum circuit of Potocnik et al. Using the numerically exact hierarchical equations of motion to capture the open quantum system dynamics, we find that an ultrafast but completely incoherent relaxation from a high-lying bright exciton into a doublet of closely spaced dark excitons can spontaneously generate electronic coherences and oscillatory real-space motion across the network (quantum beats). Importantly, we show that this behaviour also survives when the environmental noise is classically stochastic (effectively high temperature), as in present experiments, and also leads to a novel, transient violation of detailed balance in the population relaxation. These predictions highlight the possibilities of designing matched electronic and spectral noise structures for robust coherence generation that does not require coherent excitation or cold environments.