Tin-carbon clusters and the onset of microscopic level immiscibility: Experimental and computational study

Area of Science:

• Materials Science
• Physical Chemistry
• Computational Chemistry

Background:

• Bulk tin and carbon are immiscible.
• Producing novel metal-carbon species is challenging for non-carbide forming elements.

Purpose of the Study:

• To experimentally synthesize and computationally analyze binary tin-carbon gas phase species.
• To explore the potential for molecular-level miscibility between tin and carbon.

Main Methods:

• C60(-) anion impact on a tin target at kiloelectronvolt energies.
• Mass spectrometry for ion detection.
• Born-Oppenheimer molecular dynamics and density functional theory (DFT) for structure optimization.
• Coupled cluster singles, doubles, and perturbative triples [CCSD(T)] calculations for energy analysis.

Main Results:

• Positive tin-carbon ions (Sn(m)C(n)(+)) were detected, with Sn2C2(+) being the most abundant.
• Impact-induced mixing enabled the formation of novel species despite bulk immiscibility.
• Calculated structures revealed distinct binding tendencies: polyynic/cummulenic carbon chains capped by tin, or segregated tin and carbon moieties.
• CCSD(T) calculations were crucial for identifying the segregation effect.

Conclusions:

• C60(-) ion beam induced synthesis is effective for creating novel metal-carbon species with non-carbide forming elements.
• The study demonstrates the possibility of molecular-level miscibility.
• Calculated stabilities correlate with observed mass spectral abundances, rationalizing cluster ion formation.