The
hollow cores and well-defined diameters of single-walled carbon
nanotubes (SWCNTs) allow for creation of one-dimensional hybrid structures
by encapsulation of various molecules. Absorption and near-infrared
photoluminescence-excitation (PLE) spectroscopy reveal that the absorption
spectrum of encapsulated 1,3-bis[4-(dimethylamino)phenyl]-squaraine
dye molecules inside SWCNTs is modulated by the SWCNT diameter, as
observed through excitation energy transfer (EET) from the encapsulated
molecules to the SWCNTs, implying a strongly diameter-dependent stacking
of the molecules inside the SWCNTs. Transient absorption spectroscopy,
simultaneously probing the encapsulated dyes and the host SWCNTs,
demonstrates this EET, which can be used as a route to diameter-dependent
photosensitization, to be fast (sub-picosecond). A wide series of
SWCNT samples is systematically characterized by absorption, PLE,
and resonant Raman scattering (RRS), also identifying the critical
diameter for squaraine filling. In addition, we find that SWCNT filling
does not limit the selectivity of subsequent separation protocols
(including polyfluorene polymers for isolating only semiconducting
SWCNTs and aqueous two-phase separation for enrichment of specific
SWCNT chiralities). The design of these functional hybrid systems,
with tunable dye absorption, fast and efficient EET, and the ability
to remove all metallic SWCNTs by subsequent separation, demonstrates
potential for implementation in photoconversion devices.