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Characterizing Ultrafast Intersystem Crossing Pathways in Molecular Pt Dimers Using Time-Resolved Wide-Angle X-ray

Michael W Mara¹, Denis Leshchev², Nicholas P Weingartz²

¹Chemical Sciences and Engineering, Argonne National Laboratory, Lemont, Illinois 60439, United States.

The Journal of Physical Chemistry Letters

|July 3, 2025

Summary

This summary is machine-generated.

Vibronic coupling, driven by platinum-dimer vibrations, enhances intersystem crossing (ISC) rates. Ultrafast X-ray scattering reveals how bridging ligands influence these dynamics and ISC mechanisms.

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Published on: August 22, 2017

Area of Science:

Photochemistry and Photophysics
Inorganic Chemistry
Materials Science

Background:

Vibronic coupling is a key mechanism influencing charge transfer states and intersystem crossing (ISC) rates in transition metal complexes.
Previous studies have observed vibronic coupling-driven ISC in platinum(II) dimer complexes, where Pt-Pt stretching vibrations tune excited-state pathways.

Purpose of the Study:

To investigate the role of vibronic coupling in enhancing intersystem crossing (ISC) rates in platinum(II) dimer complexes.
To quantify the Pt-Pt bond contraction and coherent vibrational wavepackets (CVWPs) dynamics following MMLCT excitation.
To elucidate the influence of different bridging ligands on the ISC mechanism via ultrafast TR-WAXS analysis.

Main Methods:

Time-resolved wide-angle X-ray scattering (TR-WAXS) was employed to probe ultrafast structural dynamics.
TR-WAXS was used to measure Pt-Pt distance changes and analyze coherent vibrational wavepackets (CVWPs) in Pt dimers.
Analysis of interference patterns between CVWPs was performed to track excited-state trajectories.

Main Results:

Both Pt dimer complexes exhibited Pt-Pt bond formation (contraction of ~0.25 Å) and encoded CVWPs upon MMLCT excitation.
The time-dependent evolution of CVWPs differed between the two complexes, indicating ligand-dependent dynamics.
Interference patterns in CVWPs provided indirect information about electronic excited-states and the ISC mechanism.

Conclusions:

The study demonstrates that vibronic coupling plays a crucial role in the ISC mechanism of Pt(II) dimers.
Ultrafast TR-WAXS is a powerful tool for revealing excited-state dynamics and ligand effects on ISC.
The interference of CVWPs offers insights into the bridge-dependent nature of ISC in these systems.