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Sequential Infiltration Synthesis of Cadmium Sulfide Discrete Atom Clusters.

Nuwanthaka P Jayaweera¹, Shana Havenridge², Ashley R Bielinski¹

¹Material Science Division, Argonne National Laboratory, 9700 South Cass Avenue, Lemont, Illinois, 60439, United States.

Angewandte Chemie (International Ed. in English)

|January 13, 2025

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Sequential infiltration synthesis (SIS) successfully created cadmium sulfide (CdS) clusters within polymer films. This novel method offers precise control for developing advanced light-absorbing materials for solar energy applications.

Area of Science:

Materials Science
Nanotechnology
Chemical Engineering

Background:

Sequential infiltration synthesis (SIS) is analogous to atomic layer deposition (ALD) for creating inorganic materials within permeable templates.
Existing SIS processes primarily focus on metal oxides, with limited exploration of transition metal sulfides.
Developing new routes for transition metal sulfides is crucial for advanced material applications.

Purpose of the Study:

To report the first successful sequential infiltration synthesis (SIS) of a transition metal sulfide, cadmium sulfide (CdS).
To characterize the structure and properties of CdS clusters synthesized within polymer thin films.
To explore the potential of this method for creating precision architectures for light-absorbing materials.

Main Methods:

Keywords:

atomic layer deposition metal chalcogen semiconductors sequential infiltration synthesis thin films

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Utilized gas-phase dimethyl cadmium and hydrogen sulfide precursors to infiltrate poly(4-vinylpyridine) thin films.
Employed electronic and vibrational spectroscopy to analyze the synthesized CdS clusters.
Applied grazing-incidence total X-ray scattering and first principles modeling to determine cluster structure and properties.

Main Results:

Achieved 3D nucleation of CdS clusters with a cubane-type Cd4S4 core within polymer films.
Identified variable methyl, thiol, and hydroxy capping ligands on the CdS clusters.
Confirmed the formation of few-atom Cd-based clusters consistent with experimental spectroscopic and scattering data at 80°C.

Conclusions:

Successfully demonstrated a novel SIS process for synthesizing few-atom transition metal sulfide clusters.
The synthesized CdS clusters show promise for creating precision architectures for light-absorbing materials.
This method provides a versatile new route for applications in solar energy harvesting and conversion.