Pseudocarbynes,
defined as linear carbon chains stabilized by noncovalent
bonding to a metal cluster, were synthesized via laser ablation of
a liquid/metal interface, in this case, gold (Au) in ethanol. We present
UV–vis, Raman, and IR spectra that collectively demonstrate
the formation of Au-pseudocarbynes. The Au-pseudocarbynes presented
here likely consist of polyynes containing fewer than 16 carbon atoms
associated with subnanometer Au clusters. Their characteristic spectral
signatures are supported by density functional theory calculations
that highlight the interaction between the Au clusters and the π
network of −CC– chains. This class of molecules
represents a synergy between sp-hybridized carbon chains and small
metal clusters that stabilize one another.