  Laser cooling is a powerful method to control molecules for applications in
precision measurement, as well as quantum information, many-body physics, and
fundamental chemistry. However, many optically-active metal centers in valence
states which are promising for these applications, especially precision
measurement, are difficult to laser cool. In order to extend the control
afforded by laser cooling to a wider array of promising atoms, we consider the
use of small, hypermetallic molecules that contain multiple metal centers. We
provide a detailed analysis of YbCCCa and YbCCAl as prototypical examples with
different spin multiplicities, and consider their feasibility for precision
measurements making use of the heavy Yb atom. We find that these molecules are
linear and feature metal-centered valence electrons, and study the complex
hybridization and spin structures that are relevant to photon cycling and laser
cooling. Our findings suggest that this hypermetallic approach may be a
versatile tool for experimental control of metal species that do not otherwise
efficiently cycle photons, and could present a new polyatomic platform for
state-of-the-art precision measurements.
