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Chemically reversible isomerization of inorganic clusters
Curtis B Williamson1, Douglas R Nevers1, Andrew Nelson2
1Robert F. Smith School of Chemical and Biomolecular Engineering, Cornell University, Ithaca, NY, USA.
Science (New York, N.Y.)
|February 16, 2019
Summary
Cadmium sulfide (CdS) clusters bridge molecular isomerization and solid-state transformations. These atomically precise clusters exhibit diffusionless reconfiguration, revealing intermediate states in structural changes.
Area of Science:
- Materials Science
- Nanotechnology
- Chemical Physics
Background:
- Structural transformations are typically studied in isolated molecular or solid systems.
- Intermediate states in these transformations have been difficult to characterize experimentally.
- Atomically precise clusters offer a potential platform for studying such phenomena.
Purpose of the Study:
- To investigate isomerization in well-defined, atomically precise cadmium sulfide (CdS) cluster systems.
- To bridge the study of molecular isomerization and solid-solid transformations.
- To characterize intermediate systems in structural transformations.
Main Methods:
- Utilized cadmium sulfide (CdS) cluster isomers as an experimental platform.
- Studied the coherent interconversion between cluster isomers.
- Analyzed the energy barrier and shift in excitonic energy gaps.
- Investigated the role of ligand-binding motifs and hydroxyl species.
Main Results:
- CdS cluster isomers coherently interconvert over a ~1-electron volt energy barrier.
- A 140-milli-electron volt shift in excitonic energy gaps was observed.
- A diffusionless, displacive reconfiguration of the inorganic core occurred, akin to a solid-solid transformation.
- Transformation kinetics were first-order, similar to molecular isomerization.
- Surface energy, influenced by hydroxyl species, dictates phase stability.
Conclusions:
- CdS clusters serve as an advantageous platform for studying isomerization across length scales.
- The observed transformation exhibits characteristics of both solid-solid transformations and molecular isomerizations.
- This work bridges the gap between molecular and solid-state structural changes.
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