Abstract

2D electronic spectroscopy (2DES) techniques have gained particular interest given their capability of following ultrafast coherent and noncoherent processes in real-time. Although the fame of 2DES is still majorly linked to the investigation of energy and charge transport in biological light-harvesting complexes, 2DES is now starting to be recognized as a particularly valuable tool for studying transport processes in artificial nanomaterials and nanodevices. Particularly meaningful is the possibility of assessing coherent mechanisms active in the transport of excitation energy in these materials toward possible quantum technology applications. The diverse nature of these new target samples poses significant challenges and calls for a critical rethinking of the technique and its different realizations. With the confluence of promising new applications and rapidly developing technical capabilities, the enormous potential of 2DES techniques to impact the field of nanosystems, quantum technologies, and quantum devices is here delineated.

Highlights

  • The ability to spectroscopically probe ultrafast events in the femtoseconds time regime has been crucial for understanding fundamental scientific questions in biology, chemistry, and physics.[1]

  • New intra- and intermolecular ultrafast relaxation channels can be activated, mediated by the vibrational motions of the hydrogen donor and acceptor groups, when the coupled chromophores are at significant distances (Figure 7). These findings suggest that the design of H-bonded structures is a powerful tool to drive the ultrafast dynamics in complex materials

  • The sensitivity of the technique to interchromophore couplings, its capability of identifying with unprecedented clarity transport processes, and coherent dynamics have been crucial for the blossoming of the quantum biology discipline

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Summary

INTRODUCTION

The ability to spectroscopically probe ultrafast events in the femtoseconds (fs) time regime has been crucial for understanding fundamental scientific questions in biology, chemistry, and physics.[1] Examples of such investigations include transitionstate dynamics of chemical reactions, solute−solvent interactions, energy and charge transfer, excitonic interactions, and quantum coherence, just to cite a few.[2] Several ultrafast spectroscopy techniques have been developed to this aim, including pump−probe (probably the most famous and widespread among the fs techniques), various types of photon echo, transient grating, resonant coherent Raman, and holeburning spectroscopies, and optical Kerr spectroscopy. The medium’s response can be cast into 2D spectra, which provide more straightforward and direct access to signal contributions hidden within the broad lineshapes of 1D spectra This allows revealing with improved reliability details on molecular structure, vibrational and electronic motions, interactions, couplings, and relaxation processes.

ELECTRONIC TRANSITIONS IN 2DES SPECTRA
IMPLEMENTATIONS
CHARACTERIZATION OF COMPLEX DYNAMICS TOWARD QUANTUM TECHNOLOGY APPLICATIONS
CONCLUDING REMARKS
■ REFERENCES
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