Over the years, an enormous effort has been made to establish nitrogen vacancy (N-) centers in diamond as easily accessible and precise magnetic field sensors. However, most of their sensing protocols rely on the application of bias magnetic fields, preventing their usage in zero- or low-field experiments. We overcome this limitation by exploiting the full spin nature of the N- center, allowing us to detect nuclear spin signals at zero and low field with a linearly polarized microwave field. As conventional dynamical decoupling protocols fail in this regime, we develop robust pulse sequences and optimize pulse pairs, which allow us to sense temperature and weak ac magnetic fields and achieve an efficient decoupling from environmental noise. Our work allows for much broader and simpler applications of N- centers as magnetic field sensors in the zero- and low-field regime and can be further extended to three-level systems in ions and atoms.
Non-Markovian effects in the evolution of open quantum systems have recently attracted widespread interest, particularly in the context of assessing the efficiency of energy and charge transfer in nanoscale biomolecular networks and quantum technologies. With the aid of many-body simulation methods, we uncover and analyze an ultrafast environmental process that causes energy relaxation in the reduced system to depend explicitly on the phase relation of the initial-state preparation. Remarkably, for particular phases and system parameters, the net energy flow is uphill, transiently violating the principle of detailed balance, and implying that energy is spontaneously taken up from the environment. A theoretical analysis reveals that nonsecular contributions, significant only within the environmental correlation time, underlie this effect. This suggests that environmental energy harvesting will be observable across a wide range of coupled quantum systems.
4 June 2018 in The Journal of Physical Chemistry Letters
Charge separation is a critical process for achieving high efficiencies in organic photovoltaic cells. The initial tightly bound excitonic electron-hole pair has to dissociate fast enough in order to avoid photocurrent generation and thus power conversion efficiency loss via geminate recombination. Such process takes place assisted by transitional states that lie between the initial exciton and the free charge state. Due to spin conservation rules these intermediate charge transfer states typically have singlet character. Here we propose a donor-acceptor model for a generic organic photovoltaic cell in which the process of charge separation is modulated by a magnetic field which tunes the energy levels. The impact of a magnetic field is to intensify the generation of charge transfer states with triplet character via inter-system crossing. As the ground state of the system has singlet character, triplet states are recombination-protected, thus leading to a higher probability of successful charge separation. Using the open quantum systems formalism we demonstrate that the population of triplet charge transfer states grows in the presence of a magnetic field, and discuss the impact on carrier population and hence photocurrent, highlighting its potential as a tool for research on charge transfer kinetics in this complex systems.
Conventional control strategies for nitrogen-vacancy centers in quantum sensing are based on a two-level model of their triplet ground state. However, this approach fails in regimes of weak bias magnetic fields or strong microwave pulses, as we demonstrate. To overcome this limitation, we propose a novel control sequence that exploits all three levels by addressing a hidden Raman configuration with microwave pulses tuned to the zero-field transition. We report excellent performance in typical dynamical decoupling sequences, opening up the possibility for nano-NMR operation in low field environments.
Diffusion noise is a major source of spectral line broadening in liquid state nano-scale nuclear magnetic resonance with shallow nitrogen-vacancy centres, whose main consequence is a limited spectral resolution. This limitation arises by virtue of the widely accepted assumption that nuclear spin signal correlations decay exponentially in nano-NMR. However, a more accurate analysis of diffusion shows that correlations survive for a longer time due to a power-law scaling, yielding the possibility for improved resolution and altering our understanding of diffusion at the nano-scale. Nevertheless, such behaviour remains to be demonstrated in experiments. Using three different experimental setups and disparate measurement techniques, we present overwhelming evidence of power-law decay of correlations. These result in sharp-peaked spectral lines, for which diffusion broadening need not be a limitation to resolution.