Open questions in attochemistry

Calegari, Francesca; Martin, Fernando

doi:10.1038/s42004-023-00989-0

Cited by 15 publications

(9 citation statements)

References 24 publications

(28 reference statements)

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“…Advancements in laser technology have recently enabled the development of intense and coherent ultraviolet (UV) light sources, opening up a variety of opportunities to conduct scientific research aiming to address fundamental questions of relevance in fields such as biology and atmospheric chemistry. Particularly, several phenomena occurring in nature involve the UV-excited dynamics of valence shell electrons in molecules, which are ultimately responsible for bond formation and breaking and therefore for the chemical changes that occur at longer time scales [1]. In this context, the engineering of novel UV light sources is constantly evolving towards the generation of temporally shorter and shorter light pulses with few-femtosecond duration [2].…”

Section: Introductionmentioning

confidence: 99%

Ultraviolet supercontinuum generation using a differentially-pumped integrated glass chip

Wanie,

Barbato,

Hahne

et al. 2024

J. Phys. Photonics

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We investigate the generation of ultrabroadband femtosecond ultraviolet (UV) radiation via third-order harmonic generation in highly confined gas media. A dual-stage differential-pumping scheme integrated into a glass microfluidic chip provides an exceptional gas confinement up to several bar and allows the apparatus to be operated under high-vacuum environment. UV pulses are generated both in argon and neon with up to ~0.8 µJ energy and 0.2% conversion efficiency for spectra that cover the UVB and UVC regions between 200 and 325 nm. Numerical simulations based on the unidirectional pulse propagation equation reveal that ionization plays a critical role for extending the spectral bandwidth of the generated third-harmonic pulse beyond the tripled 800 nm driving laser pulse bandwidth. By delivering UV supercontinua supporting Fourier transform limits below 2 fs, as well as comparable pulse energies with respect to capillary-based techniques that typically provide high spectral tunability but produce narrower bandwidths, our compact device makes a step forward towards the production and application of sub-fs ultraviolet pulses for the investigation of electron dynamics in neutral molecules.

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Section: Introductionmentioning

confidence: 99%

Ultraviolet supercontinuum generation using a differentially-pumped integrated glass chip

Wanie,

Barbato,

Hahne

et al. 2024

J. Phys. Photonics

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“…Exploring the extremely short and fast microscopic properties of matter with light has always been a great challenge, leading to the ever-expanding field of femtochemistry, and even attochemistry, − so far. The motivation at the heart of femtochemistry is devoted to revealing the elementary dynamical steps in all chemical transformations, − which are associated with molecular translations, molecular bond rotations, and vibrations, tending to occur on femtosecond time scales.…”

Section: Introductionmentioning

confidence: 99%

Probing and Steering Attosecond Electron Motion Using Tailored Ultrafast Laser Fields

Gong,

Zhang,

et al. 2024

J. Phys. Chem. A

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An ultrafast intense laser field is one of the most important tools to observe and manipulate electronic and nuclear dynamics with subcycle precision in highly nonlinear light−matter interactions, which provides access to attosecond chemistry and physics. In this review, we briefly summarize the protocol of attosecond chronoscopy and its application in probing the attosecond photoemission dynamics from atoms and molecules. We also review the control schemes of attosecond electron motion in atoms and molecules as well as molecular bond formation and cleavage with the assistance of tailored femtosecond laser fields.

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“…Attosecond chemistry is a rapidly evolving field aiming at visualizing electronic motion in molecules and eventually controlling that motion by acting on the electrons before the nuclei have time to respond. , In this way, one hopes to modify the chemical behavior of molecules, going beyond the usual approaches in femtochemistry. Controlling electronic motion requires an attosecond time resolution.…”

Section: Introductionmentioning

confidence: 99%

Tracing Photoinduced Hydrogen Migration in Alcohol Dications from Time-Resolved Molecular-Frame Photoelectron Angular Distributions

Kuraoka,

Goto,

Kanno

et al. 2024

J. Phys. Chem. A

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The recent implementation of attosecond and fewfemtosecond X-ray pump/X-ray probe schemes in large-scale freeelectron laser facilities has opened the way to visualize fast nuclear dynamics in molecules with unprecedented temporal and spatial resolution. Here, we present the results of theoretical calculations showing how polarization-averaged molecular-frame photoelectron angular distributions (PA-MFPADs) can be used to visualize the dynamics of hydrogen migration in methanol, ethanol, propanol, and isopropyl alcohol dications generated by X-ray irradiation of the corresponding neutral species. We show that changes in the PA-MFPADs with the pump−probe delay as a result of intramolecular photoelectron diffraction carry information on the dynamics of hydrogen migration in real space. Although visualization of this dynamics is more straightforward in the smaller systems, methanol and ethanol, one can still recognize the signature of that motion in propanol and isopropyl alcohol and assign a tentative path to it. A possible pathway for a corresponding experiment requires an angularly resolved detection of photoelectrons in coincidence with molecular fragment ions used to define a molecular frame of reference. Such studies have become, in principle, possible since the first XFELs with sufficiently high repetition rates have emerged. To further support our findings, we provide experimental evidence of H migration in ethanol−OD from ion− ion coincidence measurements performed with synchrotron radiation.

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Open questions in attochemistry

Cited by 15 publications

References 24 publications

Ultraviolet supercontinuum generation using a differentially-pumped integrated glass chip

Ultraviolet supercontinuum generation using a differentially-pumped integrated glass chip

Probing and Steering Attosecond Electron Motion Using Tailored Ultrafast Laser Fields

Tracing Photoinduced Hydrogen Migration in Alcohol Dications from Time-Resolved Molecular-Frame Photoelectron Angular Distributions

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