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Electronic coherence signatures can be directly identified in the time–frequency maps measured in two-dimensional electronic spectroscopy (2DES). Here, we demonstrate the theory and discuss the advantages of this approach via the detailed application to the fast-femtosecond beatings of a wide variety of electronic coherences in ensemble dimers of quantum dots (QDs), assembled from QDs of 3 nm in diameter, with 8% size dispersion in diameter. The observed and computed results can be consistently characterized directly in the time–frequency domain by probing the polarization in the 2DES setup. The experimental and computed time–frequency maps are found in very good agreement, and several electronic coherences are characterized at room temperature in solution, before the extensive dephasing due to the size dispersion begins. As compared to the frequency–frequency maps that are commonly used in 2DES, the time–frequency maps allow exploiting electronic coherences without additional post-processing and with fewer 2DES measurements. Towards quantum technology applications, we also report on the modeling of the time–frequency photocurrent response of these electronic coherences, which paves the way to integrating QD devices with classical architectures, thereby enhancing the quantum advantage of such technologies for parallel information processing at room temperature.

Given their importance, hydrogen bonds (H-bonds) have been the subject of intense investigation since their discovery. Indeed, H-bonds play a fundamental role in determining the structure, the electronic properties, and the dynamics of complex systems, including biologically relevant materials such as DNA and proteins. While H-bonds have been largely investigated for systems in their electronic ground state, fewer studies have focused on how the presence of H-bonds could affect the static and dynamic properties of electronic excited states. This review presents an overview of the more relevant progress in studying the role of H-bond interactions in modulating excited-state features in multichromophoric biomimetic complex systems. The most promising spectroscopic techniques that can be used for investigating the H-bond effects in excited states and for characterizing the ultrafast processes associated with their dynamics are briefly summarized. Then, experimental insights into the modulation of the electronic properties resulting from the presence of H-bond interactions are provided, and the role of the H-bond in tuning the excited-state dynamics and the related photophysical processes is discussed.

The ability to control the light–matter interaction in nanosystems is a major challenge in the field of innovative photonics applications. In this framework, plexcitons are promising hybrid light–matter states arising from the strong coupling between plasmonic and excitonic materials. However, strategies to precisely control the formation of plexcitons and to modulate the coupling between the plasmonic and molecular moieties are still poorly explored. In this work, the attention is focused on suspensions of hybrid nanosystems prepared by coupling cationic gold nanoparticles to tetraphenyl porphyrins in different aggregation states. The role of crucial parameters such as the dimension of nanoparticles, the pH of the solution, and the ratio between the nanoparticles and dye concentration was systematically investigated. A variety of structures and coupling regimes were obtained. The rationalization of the results allowed for the suggestion of important guidelines towards the control of plexcitonic systems.

Energy transfer from carotenoids to chlorophylls in light-harvesting is still not fully understood, especially in the ultrafast regime. Here, the authors investigate the coherent dynamics of this process in peridinin-chlorophyll a-protein complex via 2D electronic spectroscopy and quantum chemical calculations.

Bacteriochlorophyll is the primary pigment in the light-harvesting pigment-protein complexes (PPCs) of the bacterial photosynthetic apparatus. 2D electronic spectroscopy (2DES) represents one of the most exploited and powerful techniques to characterize the ultrafast relaxation dynamics in PPCs, in particular, to assess the presence of coherent mechanisms during energy transport.The data reported in this work and the associated research article, “Characterization of the coherent dynamics of bacteriochlorophyll a in solution” [Meneghin et al., 2019] are an important contribution to the literature on coherent dynamics of light-harvesting complexes and can be useful in the interpretation of coherent motion in more complex systems with bacteriochlorophyll a (BChla) as a basic unit. The analysis of the provided data allows the identification of vibrational coherences associated with several Franck-Condon active modes and the characterization of their frequencies and dephasing times.Here we report additional data analysis and additional measures that complement the associated research article [Meneghin et al., 2019] and support its main conclusions. In particular, we compare vibrational coherences extracted from 2DES response with Raman modes detected for BChla powders at cryogenic temperature in resonant and non-resonant conditions. Finally, we show the time-resolved fluorescence decay of the chromophore to support the interpretation of non-coherent dynamics discussed in Ref. [Meneghin et al., 2019].