- Shen, L;
- Mack, SA;
- Dakovski, G;
- Coslovich, G;
- Krupin, O;
- Hoffmann, M;
- Huang, S-W;
- Chuang, Y-D;
- Johnson, JA;
- Lieu, S;
- Zohar, S;
- Ford, C;
- Kozina, M;
- Schlotter, W;
- Minitti, MP;
- Fujioka, J;
- Moore, R;
- Lee, W-S;
- Hussain, Z;
- Tokura, Y;
- Littlewood, P;
- Turner, JJ
In the mixed-valence manganites, a near-infrared laser typically melts the orbital and spin order simultaneously, corresponding to the photoinduced d1d0→d0d1 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 Nd1-xSr1+xMnO4(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 d1d0→d0d1 transition, a near-infrared pump in this compound promotes a fundamentally distinct mechanism of charge transfer, the d0→d1L, where L denotes a hole in the oxygen band. This finding may pave a different avenue for selectively manipulating specific types of order in complex materials of this class.