Nonlinear spectroscopy employs a series of laser pulses to interrogate dynamics in large interacting many-body systems, and it has become a highly successful method for experiments in chemical physics. Current quantum optical experiments approach system sizes and levels of complexity that require the development of efficient techniques to assess spectral and dynamical features with scalable experimental overhead. However, established methods from optical spectroscopy of macroscopic ensembles cannot be applied straightforwardly to few-atom systems. Based on the ideas proposed in M. Gessner, (arXiv:1312.3365), we develop a diagrammatic approach to construct nonlinear measurement protocols for controlled quantum systems, and we discuss experimental implementations with trapped ion technology in detail. These methods, in combination with distinct features of ultracold-matter systems, allow us to monitor and analyze excitation dynamics in both the electronic and vibrational degrees of freedom. They are independent of system size, and they can therefore reliably probe systems in which, e.g., quantum state tomography becomes prohibitively expensive. We propose signals that can probe steady-state currents, detect the influence of anharmonicities on phonon transport, and identify signatures of chaotic dynamics near a quantum phase transition in an Ising-type spin chain. © 2014 American Physical Society.

We establish a novel approach to probing spatially resolved multitime correlation functions of interacting many-body systems, with scalable experimental overheads. Specifically, designing nonlinear measurement protocols for multidimensional spectra in a chain of trapped ions with single-site addressability enables us, for example, to distinguish coherent from incoherent transport processes, to quantify potential anharmonicities, and to identify decoherence-free subspaces.

The detailed characterization of non-trivial coherence properties of composite quantum systems of increasing size is an indispensable prerequisite for scalable quantum computation, as well as for understanding non-equilibrium many-body physics. Here, we show how autocorrelation functions in an interacting system of phonons as well as the quantum discord between distinct degrees of freedoms can be extracted from a small controllable part of the system. As a benchmark, we show this in chains of up to 42 trapped ions, by tracing a single phonon excitation through interferometric measurements of only a single ion in the chain. We observe the spreading and partial refocusing of the excitation in the chain, even on a background of thermal excitations. We further show how this local observable reflects the dynamical evolution of quantum discord between the electronic state and the vibrational degrees of freedom of the probe ion.

Coherence phenomena arise from interference, or the addition, of wave-like amplitudes with fixed phase differences. Although coherence has been shown to yield transformative ways for improving function, advances have been confined to pristine matter and coherence was considered fragile. However, recent evidence of coherence in chemical and biological systems suggests that the phenomena are robust and can survive in the face of disorder and noise. Here we survey the state of recent discoveries, present viewpoints that suggest that coherence can be used in complex chemical systems, and discuss the role of coherence as a design element in realizing function.