Huse Nils, Cho Hana, Hong Kiryong, Jamula Lindsey, de Groot Frank M F, Kim Tae Kyu, McCusker James K, Schoenlein Robert W
†Ultrafast X-ray Science Laboratory, Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.
‡Department of Chemistry and Chemistry Institute of Functional Materials, Pusan National University, Busan 609-735, Republic of Korea.
J Phys Chem Lett. 2011 Apr 21;2(8):880-4. doi: 10.1021/jz200168m. Epub 2011 Mar 30.
We present the first implementation of femtosecond soft X-ray spectroscopy as an ultrafast direct probe of the excited-state valence orbitals in solution-phase molecules. This method is applied to photoinduced spin crossover of Fe(tren(py)3), where the ultrafast spin-state conversion of the metal ion, initiated by metal-to-ligand charge-transfer excitation, is directly measured using the intrinsic spin-state selectivity of the soft X-ray L-edge transitions. Our results provide important experimental data concerning the mechanism of ultrafast spin-state conversion and subsequent electronic and structural dynamics, highlighting the potential of this technique to study ultrafast phenomena in the solution phase.
我们展示了飞秒软X射线光谱技术的首次应用,该技术可作为溶液相分子中激发态价轨道的超快直接探针。此方法应用于Fe(tren(py)3)的光致自旋交叉研究,其中由金属到配体的电荷转移激发引发的金属离子超快自旋态转换,利用软X射线L边跃迁的固有自旋态选择性进行直接测量。我们的结果提供了关于超快自旋态转换机制以及后续电子和结构动力学的重要实验数据,突出了该技术在研究溶液相中超快现象的潜力。