Ultrafast Charge Dynamics in an Amino Acid Induced by Attosecond Pulses

Calegari, Francesca; Ayuso, David Fernández; Trabattoni, Andrea; Belshaw, Louise; Camillis, Simone De; Frassetto, Fabio; Poletto, Luca; Palacios, Alicia; Decleva, Piero; Greenwood, J. B.; Martín, Fernando; Nisoli, M.

doi:10.1109/jstqe.2015.2419218

Cited by 19 publications

(24 citation statements)

References 64 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…34,35,252,253 However, a correct theoretical description of the charge migration induced by attosecond pulses requires the explicit evaluation of all the ionization amplitudes that dene the coherent superposition of ionic states. 25,254 One can expect that the initial characteristics of this electronic wave packet, which in principle depend on the frequency, duration, and spectral phase of the attosecond pulse, will dictate the fate of the molecule, including its possible fragmentation at longer times.…”

Section: Molecular Ionizationmentioning

confidence: 99%

Attosecond Electron Dynamics in Molecules

et al. 2017

Self Cite

View full text Add to dashboard Cite

Advances in attosecond science have led to a wealth of important discoveries in atomic, molecular, and solid-state physics and are progressively directing their footsteps toward problems of chemical interest. Relevant technical achievements in the generation and application of extreme-ultraviolet subfemtosecond pulses, the introduction of experimental techniques able to follow in time the electron dynamics in quantum systems, and the development of sophisticated theoretical methods for the interpretation of the outcomes of such experiments have raised a continuous growing interest in attosecond phenomena, as demonstrated by the vast literature on the subject. In this review, after introducing the physical mechanisms at the basis of attosecond pulse generation and attosecond technology and describing the theoretical tools that complement experimental research in this field, we will concentrate on the application of attosecond methods to the investigation of ultrafast processes in molecules, with emphasis in molecules of chemical and biological interest. The measurement and control of electronic motion in complex molecular structures is a formidable challenge, for both theory and experiment, but will indubitably have a tremendous impact on chemistry in the years to come.

show abstract

Section: Molecular Ionizationmentioning

confidence: 99%

Attosecond Electron Dynamics in Molecules

et al. 2017

Self Cite

View full text Add to dashboard Cite

show abstract

“…t i and t r are the real components of the (complex) ionization and recombination times (see [74]), and a α n←m is the transition amplitude accounting for the laser-driven dynamics induced in the ion between ionization and recombination, which can be evaluated by propagating the initial wave function from t i to t r and projecting it onto the final state, i.e. a α n←m (t r , t i ) = n|U α (t r , t i )|m (14) where U α (t r , t i ) is the evolution operator acting on the electronic coordinates of the ion (see [74]). The dependence of ionization and recombination times on N and ε has been omitted for the sake of clarity.…”

Section: A Evaluation Of High-order Harmonic Spectramentioning

confidence: 99%

Strong-field control and enhancement of chiral response in bi-elliptical high-order harmonic generation: an analytical model

Ayuso

Decleva

Patchkovskii

et al. 2018

J. Phys. B: At. Mol. Opt. Phys.

Self Cite

View full text Add to dashboard Cite

The generation of high-order harmonics in a medium of chiral molecules driven by intense bielliptical laser fields can lead to strong chiroptical response in a broad range of harmonic numbers and ellipticities [D. Ayuso et al, J. Phys. B 51, 06LT01 (2018)]. Here we present a comprehensive analytical model that can describe the most relevant features arising in the high-order harmonic spectra of chiral molecules driven by strong bi-elliptical fields. Our model recovers the physical picture underlying chiral high-order harmonic generation based on ultrafast chiral hole motion and identifies the rotationally invariant molecular pseudoscalars responsible for chiral dynamics. Using the chiral molecule propylene oxide as an example, we show that one can control and enhance the chiral response in bi-elliptical high-order harmonic generation by tailoring the driving field, in particular by tuning its frequency, intensity and ellipticity, exploiting a suppression mechanism of achiral background based on the linear Stark effect. arXiv:1803.04952v2 [physics.optics]

show abstract

“…A significant probability for the hole to be located at the indole group is also in agreement with the observed fragmentation pattern (figure 1). The charge oscillations observed in Phe, instead, have been mainly assigned to periodic charge migration from the amine functional group to the carboxylic group [13,24]. The involvement of different functional groups for the two molecules may be the reason for the different features observed in the oscillatory patterns (figure 2).…”

Section: Numerical Results and Discussionmentioning

confidence: 99%

Charge migration in photo-ionized aromatic amino acids

Trabattoni

Galli

Lara-Astiaso

et al. 2019

Phil. Trans. R. Soc. A.

View full text Add to dashboard Cite

Attosecond pump–probe spectroscopy is a unique tool for the direct observation of the light-activated electronic motion in molecules and it offers the possibility to capture the first instants of a chemical reaction. Recently, advances in attosecond technology allowed the charge migration processes to be revealed in biochemically relevant molecules. Although this purely electronic process might be key for a future chemistry at the electron time scale, the influence of this ultrafast charge flow on the reactivity of a molecule is still debated. In this work, we exploit extreme ultraviolet attosecond pulses to activate charge migration in two aromatic amino acids, namely phenylalanine and tryptophan. Advanced numerical calculations are performed to interpret the experimental data and to discuss the effects of the nuclear dynamics on the activated quantum coherences. By comparing the experimental results obtained in the two molecules, we show that the presence of different functional groups strongly affects the fragmentation pathways, as well as the charge rearrangement. The observed charge dynamics indeed present peculiar aspects, including characteristic periodicities and decoherence times. Numerical results indicate that, even for a very large molecule such as tryptophan, the quantum coherences can survive the nuclear dynamics for several femtoseconds. These results open new and important perspectives for a deeper understanding of the photo-induced charge dynamics, as a promising tool to control the reactivity of bio-relevant molecules via photo-excitation. This article is part of the theme issue ‘Measurement of ultrafast electronic and structural dynamics with X-rays’.

show abstract

Ultrafast Charge Dynamics in an Amino Acid Induced by Attosecond Pulses

Cited by 19 publications

References 64 publications

Attosecond Electron Dynamics in Molecules

Attosecond Electron Dynamics in Molecules

Strong-field control and enhancement of chiral response in bi-elliptical high-order harmonic generation: an analytical model

Charge migration in photo-ionized aromatic amino acids

Contact Info

Product

Resources

About