  In the mixed-valence manganites, a near-infrared laser typically melts the
orbital and spin order simultaneously, corresponding to the photoinduced
$d^{1}d^{0}$ $\xrightarrow{}$ $d^{0}d^{1}$ excitations in the Mott-Hubbard
bands of manganese. Here, we use ultrafast methods -- both femtosecond resonant
x-ray diffraction and optical reflectivity -- to demonstrate that the orbital
response in the layered manganite Nd$_{1-x}$Sr$_{1+x}$MnO$_{4}$ ($\it{x}$ =
2/3) does not follow this scheme. At the photoexcitation saturation fluence,
the orbital order is only diminished by a few percent in the transient state.
Instead of the typical $d^{1}d^{0}$ $\xrightarrow{}$ $d^{0}d^{1}$ transition, a
near-infrared pump in this compound promotes a fundamentally distinct mechanism
of charge transfer, the $d^{0}$ $ \xrightarrow{}$ $d^{1}L$, where $\it{L}$
denotes a hole in the oxygen band. This novel finding may pave a new avenue for
selectively manipulating specific types of order in complex materials of this
class.
