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Superatom spin-state dynamics of structurally precise metal monolayer-protected clusters (MPCs).

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Area of Science:

  • Nanomaterials Science
  • Quantum Chemistry
  • Spectroscopy

Background:

  • Monolayer-protected clusters (MPCs) like Au25(SC8H9)18^q and Au24Pd(SC8H9)18 exhibit unique electronic properties based on their oxidation states and electron configurations.
  • Understanding the spin dynamics in these superatomic systems is crucial for their application in nanoscale electronics and quantum information processing.
  • The difference between closed-shell (e.g., Au25(SC8H9)18^-1) and open-shell (e.g., Au25(SC8H9)18^0) configurations significantly impacts electronic behavior.

Purpose of the Study:

  • To investigate the electronic spin-state dynamics in Au25(SC8H9)18^q and Au24Pd(SC8H9)18 monolayer-protected clusters (MPCs) across different oxidation states.
  • To elucidate the role of superatomic orbital manifolds (P and D) and electron configuration (closed-shell vs. open-shell) in spin dynamics.
  • To explore the potential of these well-defined nanoclusters as model systems for studying spin and quantum state dynamics in nanoscale metals.

Main Methods:

  • Synthesis of Au25(SC8H9)18^q (q = -1, 0, +1) and Au24Pd(SC8H9)18^0 monolayer-protected clusters (MPCs).
  • Femtosecond time-resolved circularly polarized transient-absorption spectroscopy (fs-CPTA) was employed to probe carrier dynamics of electronic fine structure spin states.
  • Specific excitation energies (1.82 eV and 1.97 eV) were used to target transitions within the superatomic P- and D-orbital manifolds.

Main Results:

  • Neutral, open-shell Au25(SC8H9)18^0 exhibited multiple, persistent spin-polarized transient signals for several picoseconds after 1.82-eV excitation, with measured time constants of 5.03 ± 0.38 ps and 2.36 ± 0.59 ps.
  • Isoelectronic and closed-shell clusters, Au25(SC8H9)18^+1 and PdAu24(SC8H9)18^0, showed no spin-conversion dynamics, indicating a dependence on electron configuration.
  • The observed dynamics in the open-shell Au25 cluster are attributed to spin-polarized superatom P to D excitation involving an unpaired Pz electron.

Conclusions:

  • The spin dynamics are highly dependent on the electronic structure, specifically the presence of unpaired electrons in open-shell configurations of gold nanoclusters.
  • Closed-shell, isoelectronic gold nanoclusters do not display spin-conversion dynamics under the studied conditions.
  • Well-defined monolayer-protected clusters serve as valuable prototypes for understanding fundamental spin and quantum state dynamics in nanoscale metallic systems.