Two-dimensional UV spectroscopy: a new insight into the structure and dynamics of biomolecules

Borrego-Varillas, Rocío; Nenov, Artur; Ganzer, Lucia; Oriana, Aurelio; Manzoni, Cristian; Tolomelli, Alessandra; Rivalta, Ivan; Mukamel, Shaul; Garavelli, Marco; Cerullo, Giulio

doi:10.1039/c9sc03871j

Cited by 52 publications

(38 citation statements)

References 114 publications

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“…Unlike its steady-state analog, this technique allows for disentangling the contributions of different optical nonlinearities on the exciton peak, based on their characteristic timescale. In TiO 2 , this would require the simultaneous generation of intense pump and broadband probe pulses covering the elusive near-to-mid-ultravoilet (UV) range (3.20-4.50 eV), a technology that has long been limited by constraints in nonlinear optical conversion schemes [28][29][30][31].…”

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confidence: 99%

Giant Exciton Mott Density in Anatase TiO2

et al. 2020

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Elucidating the carrier density at which strongly bound excitons dissociate into a plasma of uncorrelated electron-hole pairs is a central topic in the many-body physics of semiconductors. However, there is a lack of information on the high-density response of excitons absorbing in the near-to-mid ultraviolet, due to the absence of suitable experimental probes in this elusive spectral range. Here, we present a unique combination of many-body perturbation theory and state-of-the-art ultrafast broadband ultraviolet spectroscopy to unveil the interplay between the ultraviolet-absorbing two-dimensional excitons of anatase TiO 2 and a sea of electron-hole pairs. We discover that the critical density for the exciton Mott transition in this material is the highest ever reported in semiconductors. These results deepen our knowledge of the exciton Mott transition and pave the route toward the investigation of the exciton phase diagram in a variety of wide-gap insulators.

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confidence: 99%

Giant Exciton Mott Density in Anatase TiO2

et al. 2020

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“…Multidimensionality is the natural development of the pump-probe spectroscopy. It has been implemented first in the Medium Infrared Region (MIR) [40,41] and more recently in the visible [42] and UV spectral regions [43]. Multidimensional optical spectroscopies have shown to be effective tools to understand the photophysics of a large set of extremely challenging phenomena such as quantum coherence in natural light harvesting, [42], structural dynamics [44], non-radiative relaxation, chemical reaction or solvation dynamics [45,46].…”

Section: Recent Advances In Multidimensional Ultrafast Spectroscopy Amentioning

confidence: 99%

“…Spectral interferometry between the nonlinear field and the LO allows full retrieval of the amplitude and phase of the nonlinear field Ẽ (3) (t 1 ,t 2 ,ω 3 ), and thus of the nonlinear polarization P (3) (t 1 ,t 2 ,ω 3 ). By performing another FT with respect to t 1 for a fixed value of the waiting time t 2 , the 2D map P (3) (ω 1 ,t 2 ,ω 3 ) is obtained, where ω 1 is the excitation frequency [43].…”

Section: Recent Advances In Multidimensional Ultrafast Spectroscopy Amentioning

confidence: 99%

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Synergistic Approach of Ultrafast Spectroscopy and Molecular Simulations in the Characterization of Intramolecular Charge Transfer in Push-Pull Molecules

et al. 2020

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The comprehensive characterization of Intramolecular Charge Transfer (ICT) stemming in push-pull molecules with a delocalized π-system of electrons is noteworthy for a bespoke design of organic materials, spanning widespread applications from photovoltaics to nanomedicine imaging devices. Photo-induced ICT is characterized by structural reorganizations, which allows the molecule to adapt to the new electronic density distribution. Herein, we discuss recent photophysical advances combined with recent progresses in the computational chemistry of photoactive molecular ensembles. We focus the discussion on femtosecond Transient Absorption Spectroscopy (TAS) enabling us to follow the transition from a Locally Excited (LE) state to the ICT and to understand how the environment polarity influences radiative and non-radiative decay mechanisms. In many cases, the charge transfer transition is accompanied by structural rearrangements, such as the twisting or molecule planarization. The possibility of an accurate prediction of the charge-transfer occurring in complex molecules and molecular materials represents an enormous advantage in guiding new molecular and materials design. We briefly report on recent advances in ultrafast multidimensional spectroscopy, in particular, Two-Dimensional Electronic Spectroscopy (2DES), in unraveling the ICT nature of push-pull molecular systems. A theoretical description at the atomistic level of photo-induced molecular transitions can predict with reasonable accuracy the properties of photoactive molecules. In this framework, the review includes a discussion on the advances from simulation and modeling, which have provided, over the years, significant information on photoexcitation, emission, charge-transport, and decay pathways. Density Functional Theory (DFT) coupled with the Time-Dependent (TD) framework can describe electronic properties and dynamics for a limited system size. More recently, Machine Learning (ML) or deep learning approaches, as well as free-energy simulations containing excited state potentials, can speed up the calculations with transferable accuracy to more complex molecules with extended system size. A perspective on combining ultrafast spectroscopy with molecular simulations is foreseen for optimizing the design of photoactive compounds with tunable properties.

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“…Femtosecond infrared laser pulses development came along with nonlinear two-dimensional infrared spectroscopy [70,71]. e experiment entails the first set of probe pulses useful to the sample, followed by a delay time for system relaxation [71][72][73]. e usual duration for the delay time requires zero to some picoseconds, which could be influenced by tens of femtosecond revolutions.…”

Section: Nonlinear Two-dimensional Infrared Spectroscopymentioning

confidence: 99%

Worthwhile Relevance of Infrared Spectroscopy in Characterization of Samples and Concept of Infrared Spectroscopy-Based Synchrotron Radiation

Odularu

2020

Journal of Spectroscopy

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The study explores the nitty-gritty of infrared spectroscopy. Firstly, the review gives a concise history of infrared discovery and its location in the electromagnetic spectrum. Secondly, the infrared spectroscopy is reported for its mechanism, principles, sample preparation, and application for absence and presence of functional groups determination in both ligands and coordination compounds. Thirdly, it helps in purity determination of unknown samples. Additional studies regarding this study entail infrared spectroscopy-based synchrotron radiation. It serves as a giant microscope to give detailed information of samples under investigation compared to the conventional infrared instrument. Infrared will continue to be useful to both chemical and pharmaceutical industries, in order to make chemical products and manufactured drugs put on wholesome integrity.

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Two-dimensional UV spectroscopy: a new insight into the structure and dynamics of biomolecules

Abstract: Two-dimensional ultraviolet spectroscopy has the potential to deliver rich structural and dynamical information on biomolecules such as DNA and proteins.

Cited by 52 publications

References 114 publications

Giant Exciton Mott Density in Anatase TiO2

Giant Exciton Mott Density in Anatase TiO2

Synergistic Approach of Ultrafast Spectroscopy and Molecular Simulations in the Characterization of Intramolecular Charge Transfer in Push-Pull Molecules

Worthwhile Relevance of Infrared Spectroscopy in Characterization of Samples and Concept of Infrared Spectroscopy-Based Synchrotron Radiation

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