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Direct Observation of Transient Ligand-Field Changes in Transition Metal Complexes via Time-Resolved Soft X-ray Spectroscopy

등록일
2009년 8월 21일 15시 15분 45초
접수번호
1520
발표코드
34P165포 이곳을 클릭하시면 발표코드에 대한 설명을 보실 수 있습니다.
발표시간
목 <발표Ⅱ>
발표형식
포스터
발표분야
물리화학
저자 및
공동저자
조하나, 홍기룡, 김태규
부산대학교 화학과, Korea
Here we report the first time-resolved soft x-ray spectroscopy of electron and spin dynamics in solvated molecules. We observe changes in ligand-field splitting, spin-state and orbital populations, and electron delocalization in the studied Fe2+ spin-crossover complex by probing photo-initiated transient absorption changes of the iron L2,3-edges. The large shift of the L2,3-edges to lower energies upon spin crossover is not only caused by a reduction in ligand-field splitting and changes Fe-3d orbital occupancy but necessitates a strong reduction in Fe-3d electron interaction with the π-electron system of the ligands. Upon spin crossover, the ligand-field splitting reduces by more than 1 eV while the iron 3d metal character increases through changes in metal-ligand orbital covalency with indications for spin-orbit quenching in the high-spin state. Our time-resolved measurements directly capture the transients valence-orbital structure in a solvated system, offering future opportunities to investigate important classes of transition metal compounds such as protein co-factors (e.g. metalloporphyrins in Myoglobin and Hemoglobin) or mixed-valence compounds, and more generally the solvent influence on ultrafast dynamics of electronic and spin states.

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