Volume 212, 2018

Multiple pulse coherent dynamics and wave packet control of the N2 a′′ 1Σ +g dark state by attosecond four-wave mixing

Abstract

Nonlinear multidimensional spectroscopy is ubiquitous in the optical and radio frequency regions as a powerful tool to access structure and dynamics. The extension of this technique into the extreme ultraviolet (XUV) region with attosecond pulses holds promise for probing electronic dynamics and correlations with unprecedented time and spatial resolution. In this work, we use noncollinear four-wave mixing of a weak XUV attosecond pulse train (11–17 eV) and few-femtosecond NIR pulses (800 nm) to spectroscopically and dynamically probe the dipole-forbidden double-well potential of the a′′ 1+g electronic state of nitrogen. The results demonstrate optical coupling of the inner and outer limits of the initial XUV-prepared vibrational wave packet in the valence character b′ 1+u state to the inner and outer wells, respectively, of the a′′ 1+g double well state by 800 nm light. Two four-wave mixing schemes with different pulse timing sequences and noncollinear beam geometries are used (one NIR pulse collinear and one NIR pulse noncollinear versus both NIR pulses noncollinear to the XUV beam) to measure the a′′ dark state energetic structure and to control the dynamical preparation and motion of a dark state wave packet by selective population of either the inner Rydberg or outer valence-character potential well. Experimental measurements of the a′′ 1+g outer well vibrational spacing and anharmonicity closely match the values theoretically predicted for this previously unobserved state.

Graphical abstract: Multiple pulse coherent dynamics and wave packet control of the N2 a′′ 1Σ+g dark state by attosecond four-wave mixing

Associated articles

Article information

Article type
Paper
Submitted
11 апр. 2018
Accepted
08 мај 2018
First published
08 мај 2018

Faraday Discuss., 2018,212, 157-174

Author version available

Multiple pulse coherent dynamics and wave packet control of the N2 a′′ 1Σ+g dark state by attosecond four-wave mixing

E. R. Warrick, A. P. Fidler, W. Cao, E. Bloch, D. M. Neumark and S. R. Leone, Faraday Discuss., 2018, 212, 157 DOI: 10.1039/C8FD00074C

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements