The rational design of materials requires an understanding
of the
relationships between structure and properties. In some fields, advances
in computational tools and modeling have mapped out many of these
connections. In the realm of intermetallics, however, principles for
such relationships are still needed. Recently, we illustrated how
the DFT–Chemical Pressure (CP) analysis can link geometrical
motifs within crystalline arrangements to the phonon band structures
of intermetallics and thus the physical properties related to vibrations
and atomic motion. The key indicators here are quadrupolar CP featuresdistributions
in which positive and negative interatomic pressures are oriented
perpendicular to one another. These quadrupoles then create low energy
paths of motion for the atoms that can be linked to various structural
phenomena, such as anisotropic vibrations and incommensurate modulations.
In this article, we survey the presence of CP quadrupoles in a collection
of TE2 structures (T = transition metal and E = main group
element) and the roles they play in the behavior observed for these
compounds. We begin by developing a metric for CP quadrupolar character,
which can be calculated from the output of CP analysis. After compiling
these metrics for 17 TE2 structure types, we delve deeper
into four systems detected as exhibiting atomic sites with quadrupolar
character: (1) the Co–Sn binary system, where the quadrupoles
on the Co atoms in CuAl2-type CoSn2 direct the
features of its superstructure in CoSn3; (2) arsenopyrite-type
CoSb2, in which the highly quadrupolar CP distributions
on the Sb atoms correlate with the motions followed during the phase
transition to its high-temperature marcasite-type form; (3) the CrSi2 structure, in which the expansion of the lattice is predicted
to open a helical path of potential soft motion analogous to that
underlying the Nowotny Chimney Ladder series; and (4) the CdAs2 type, whose CP features anticipate the ability to incorporate
Li atoms as guests. Together, these case studies highlight the potential
for CP quadrupoles to link local atomic arrangements with a variety
of emergent properties in intermetallic phases.