Iron
pyrite (FeS2) is an abundant natural mineral with
interesting physical and chemical properties, including its near IR
bandgap and extremely high absorption coefficient throughout the visible
range. The dynamics of photoinitiated carriers and their interactions
with intrinsic and surface defects are still not fully understood,
yet clearly are responsible for pyrite’s underwhelming photovoltaic
and photocatalytic performance. Here we report, to our knowledge for
the first time, broadband ultrafast transient reflection from single-crystal
natural iron pyrite with several excitation wavelengths both higher
and lower than the accepted nominal bandgap of pyrite. We also demonstrate
a method to transform transient reflection to transient absorption,
without requiring any assumptions regarding the magnitude of either
the absorption coefficient or the refractive index, allowing for a
more direct interpretation of our results. An important finding from
this work is the observation of a long-lived weak signal when pumping
with 0.58 eV, an energy well below the accepted bandgap, which may
be evidence for direct optical excitation of either intrinsic trailing
edges of the bands or midgap defect states. We identify that after
approximately 10 ps the transient spectra due to pumping at 2.59,
1.58, and 0.91 eV all appear qualitatively similar, suggesting relaxation
to a common carrier distribution. This common distribution appears
to decay on two time scales of about 30 and ≫200 ps. Our results
should play a role in understanding charge carrier dynamics within
the intricate and complex band structure of pyrite and hopefully provide
clarification and direction for future efforts in the development
of iron pyrite based technologies.