Isolating quantum coherence with pathway-selective coherent multi-dimensional spectroscopy

Coherent coupling between spatially separated systems has long been explored as a necessary requirement for quantum information and cryptography. Recent discoveries suggest such phenomena appear in a much wider range of processes, including light-harvesting in photosynthesis. These discoveries have been facilitated by developments in coherent multi-dimensional spectroscopy (CMDS) that allow interactions between different electronic states to be identified in crowded spectra. For complex systems, however, spectral broadening and multiple overlapping peaks limit the ability to separate, identify and properly analyse all contributions. Here we demonstrate how pathway-selective CMDS can overcome these limitations to reveal, isolate and allow detailed analysis of weak coherent coupling between spatially separated excitons localised to different semiconductor quantum wells. Selective excitation of the coherence pathways, by spectrally shaping the laser pulses, provides access to previously hidden details and enables quantitative analysis that can facilitate precise and detailed understanding of interactions in this and other complex systems

Persistent coherence of quantum superpositions in an optimally doped cuprate revealed by 2D spectroscopy

Understanding of the precise mechanisms of high-temperature superconductivity is elusive. In particular, in order to solve the puzzle of the pairing mechanism, it is important to understand the detailed nature of the excitations at energies around the superconducting gap. While measurements of the dynamics of excited electronic populations have been able to give some insight, they have largely neglected the intricate dynamics of quantum coherence. Here, we apply multidimensional coherent spectroscopy for the first time to a prototypical cuprate and report unprecedented coherent dynamics persisting for ~500 fs, originating directly from the quantum superposition of optically excited states separated by 20 - 60 meV. These results reveal the correlation between high and low energy excitations, and indicate that the interplay between many-body states on different energy scales conserves phase coherence. In revealing these dynamics we demonstrate that multidimensional coherent spectroscopy can address electronic correlations and interrogate many-body quantum systems in unprecedented ways

Time-domain THz spectroscopy reveals coupled protein-hydration dielectric response in solutions of native and fibrils of human lyso-zyme

Here we reveal details of the interaction between human lysozyme proteins, both native and fibrils, and their water environment by intense terahertz time domain spectroscopy. With the aid of a rigorous dielectric model, we determine the amplitude and phase of the oscillating dipole induced by the THz field in the volume containing the protein and its hydration water. At low concentrations, the amplitude of this induced dipolar response decreases with increasing concentration. Beyond a certain threshold, marking the onset of the interactions between the extended hydration shells, the amplitude remains fixed but the phase of the induced dipolar response, which is initially in phase with the applied THz field, begins to change. The changes observed in the THz response reveal protein-protein interactions me-diated by extended hydration layers, which may control fibril formation and may have an important role in chemical recognition phenomena

Floquet engineering in the presence of optically excited carriers

Floquet engineering provides an optical means to manipulate electronic bandstructures, however, carriers excited by the pump field can lead to an effective heating, and can obscure measurement of the band changes. A recent demonstration of the effects of Floquet engineering on a coherent ensemble of excitons in monolayer WS$_2$ proved particularly sensitive to non-adiabatic effects, while still being able to accurately resolve bandstructure changes. Here, we drive an AC-Stark effect in monolayer WS$_2$ using pulses with constant fluence but varying pulse duration (from 25-235~fs). With shorter pump pulses, the corresponding increase in peak intensity introduces additional carriers via two-photon absorption, leading to additional decoherence and peak broadening (which makes it difficult to resolve the AC-Stark shift). We use multidimensional coherent spectroscopy to create a coherent ensemble of excitons in monolayer WS$_2$ and measure the evolution of the coherence throughout the duration of the Floquet pump pulse. Changes to the amplitude of the macroscopic coherence quantifies the additional broadening. At the same time, the evolution of the average phase allows the instantaneous changes to the bandstructure to be quantified, and is not impacted by the additional broadening. This approach to measuring the evolution of Floquet-Bloch states demonstrates a means to quantify effective heating and non-adiabaticity caused by excited carriers, while at the same time resolving the coherent evolution of the bandstructure

Investigating interoperability of the LSST Data Management software stack with Astropy

The Large Synoptic Survey Telescope (LSST) will be an 8.4m optical survey telescope sited in Chile and capable of imaging the entire sky twice a week. The data rate of approximately 15TB per night and the requirements to both issue alerts on transient sources within 60 seconds of observing and create annual data releases means that automated data management systems and data processing pipelines are a key deliverable of the LSST construction project. The LSST data management software has been in development since 2004 and is based on a C++ core with a Python control layer. The software consists of nearly a quarter of a million lines of code covering the system from fundamental WCS and table libraries to pipeline environments and distributed process execution. The Astropy project began in 2011 as an attempt to bring together disparate open source Python projects and build a core standard infrastructure that can be used and built upon by the astronomy community. This project has been phenomenally successful in the years since it has begun and has grown to be the de facto standard for Python software in astronomy. Astropy brings with it considerable expectations from the community on how astronomy Python software should be developed and it is clear that by the time LSST is fully operational in the 2020s many of the prospective users of the LSST software stack will expect it to be fully interoperable with Astropy. In this paper we describe the overlap between the LSST science pipeline software and Astropy software and investigate areas where the LSST software provides new functionality. We also discuss the possibilities of re-engineering the LSST science pipeline software to build upon Astropy, including the option of contributing affliated packages

Super-transport of Excitons in Atomically Thin Organic Semiconductors at the 2D Quantum Limit

Long-range and fast transport of coherent excitons is important for development of high-speed excitonic circuits and quantum computing applications. However, most of these coherent excitons have only been observed in some low-dimensional semiconductors when coupled with cavities, as there are large inhomogeneous broadening and dephasing effects on the exciton transport in their native states of the materials. Here, by confining coherent excitons at the 2D quantum limit, we firstly observed molecular aggregation enabled super-transport of excitons in atomically thin two-dimensional (2D) organic semiconductors between coherent states, with a measured a high effective exciton diffusion coefficient of 346.9 cm2/sec at room temperature. This value is one to several orders of magnitude higher than the reported values from other organic molecular aggregates and low-dimensional inorganic materials. Without coupling to any optical cavities, the monolayer pentacene sample, a very clean 2D quantum system (1.2 nm thick) with high crystallinity (J type aggregation) and minimal interfacial states, showed superradiant emissions from the Frenkel excitons, which was experimentally confirmed by the temperature-dependent photoluminescence (PL) emission, highly enhanced radiative decay rate, significantly narrowed PL peak width and strongly directional in-plane emission. The coherence in monolayer pentacene samples was observed to be delocalized over 135 molecules, which is significantly larger than the values (a few molecules) observed from other organic thin films. In addition, the super-transport of excitons in monolayer pentacene samples showed highly anisotropic behaviour. Our results pave the way for the development of future high-speed excitonic circuits, fast OLEDs, and other opto-electronic devices