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

Abstract

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.

References in corpus (3)

• Environment-Assisted Quantum Walks in Photosynthetic Energy Transfer
• Coherent Excitonic Coupling in an Asymmetric Double InGaAs Quantum Well Arises from Many-Body Effects
• Disentangling electronic and vibrational coherence in the Phycocyanin-645 light-harvesting complex

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• Revealing and Characterizing Dark Excitons Through Coherent Multidimensional Spectroscopy
• Two-dimensional double-quantum spectroscopy: peak shapes as a sensitive probe of carrier interactions in quantum wells
• Separating Pathways in Double-Quantum Optical Spectroscopy Reveals Excitonic Interactions
• Direct Measurement of Biexcitons in Monolayer WS2
• Persistent coherence of quantum superpositions in an optimally doped cuprate revealed by 2D spectroscopy
• Probing exciton dynamics with spectral selectivity through the use of quantum entangled photons
• Multi-color quantum control for suppressing ground state coherences in two-dimensional electronic spectroscopy
• Background-free time-resolved coherent Raman spectroscopy (CSRS and CARS): heterodyne detection of low-energy vibrations and recognition of excited-state contributions
• Excitation-pulse intensity mediated control of coherent nonlinear optical response of a V-type system