Issue 35, 2023

Exploring fingerprints of ultrafast structural dynamics in molecular solutions with an X-ray laser

Abstract

We apply ultrashort X-ray laser pulses to track optically excited structural dynamics of [Ir2(dimen)4]2+ molecules in solution. In our exploratory study we determine angular correlations in the scattered X-rays, which comprise a complex fingerprint of the ultrafast dynamics. Model-assisted analysis of the experimental correlation data allows us to elucidate various aspects of the photoinduced changes in the excited molecular ensembles. We unambiguously identify that in our experiment the photoinduced transition dipole moments in [Ir2(dimen)4]2+ molecules are oriented perpendicular to the Ir–Ir bond. The analysis also shows that the ground state conformer of [Ir2(dimen)4]2+ with a larger Ir–Ir distance is mostly responsible for the formation of the excited state. We also reveal that the ensemble of solute molecules can be characterized with a substantial structural heterogeneity due to solvent influence. The proposed X-ray correlation approach offers an alternative path for studies of ultrafast structural dynamics of molecular ensembles in the liquid and gas phases.

Graphical abstract: Exploring fingerprints of ultrafast structural dynamics in molecular solutions with an X-ray laser

Supplementary files

Article information

Article type
Paper
Submitted
20 Mar 2023
Accepted
28 Jun 2023
First published
24 Jul 2023

Phys. Chem. Chem. Phys., 2023,25, 23417-23434

Author version available

Exploring fingerprints of ultrafast structural dynamics in molecular solutions with an X-ray laser

R. P. Kurta, T. B. van Driel, A. O. Dohn, T. B. Berberich, S. Nelson, I. A. Zaluzhnyy, N. Mukharamova, D. Lapkin, D. B. Zederkof, M. Seaberg, K. S. Pedersen, K. S. Kjær, G. I. Rippy, E. Biasin, K. B. Møller, L. Gelisio, K. Haldrup, I. A. Vartanyants and M. M. Nielsen, Phys. Chem. Chem. Phys., 2023, 25, 23417 DOI: 10.1039/D3CP01257C

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