Issue 31, 2024

Sub-picosecond photodynamics of small neutral copper oxide clusters

Abstract

The ultrafast dynamics of neutral copper oxide clusters (CunOx, n < 5) are reported using femtosecond pump probe spectroscopy in the gas phase. The transient spectra recorded for each cluster demonstrate they relax on a 100s of fs timescale followed by a long-lived (>50 ps) response. Density functional theory calculations are performed to determine the lowest energy structures and spin states. Topological descripters for the excited states are calculated (time-dependent density functional theory) to relate the measured excited state dynamics to changes in the cluster's electronic structure with increasing oxidation. Strong field ionization is demonstrated here to be a soft form of ionization and able to record transient signals for clusters previously determined to be unstable to nanosecond multiphoton ionization. The relative cluster stability is further demonstrated by signal enhancement/depreciation that is recorded through the synergy from the two laser pulses. Once the oxygen atoms exceed the number of copper atoms, a weakly bound superoxide O2 unit forms, exhibiting a higher spin state. All clusters that are not in the lowest spin configuration demonstrate fragmentation.

Graphical abstract: Sub-picosecond photodynamics of small neutral copper oxide clusters

Supplementary files

Article information

Article type
Paper
Submitted
15 avr. 2024
Accepted
17 juil. 2024
First published
18 juil. 2024

Phys. Chem. Chem. Phys., 2024,26, 20937-20946

Sub-picosecond photodynamics of small neutral copper oxide clusters

C. H. Rotteger, C. K. Jarman, M. M. Sobol, S. F. Sutton and S. G. Sayres, Phys. Chem. Chem. Phys., 2024, 26, 20937 DOI: 10.1039/D4CP01544D

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