White Light Snapshot of Non-Equilibrium High-Spin State in a Molecular Crystal

Molecular compounds with photoswitchable magnetic properties have been intensively investigated over the last decades due to their prospective applications in nanoelectronics, sensing and magnetic data storage. The family of coppernitroxide-based molecular magnets represents a new promising type of photoswitchable compounds. We report the first study of these appealing systems using femtosecond optical spectroscopy. We unveil the mechanism of ultrafast (< 50 fs) spin state photoswitching and establish its principal differences compared to other photoswitchable magnets. On this basis, we propose potential advantages of copper-nitroxide-based molecular magnets for the future design of ultrafast magnetic materials.Among various photoswitchable materials, special attention has been given to spin-crossover (SCO) compounds and the light-induced excited spin state trapping (LIESST) phenomenon, which allow optical manipulation of the magnetization by switching the molecules between high-and low-spin states. [1, 2] In the solid state it is also possible to reach new phases through light-control of structural order between SCO molecules. [3] LIESST has been extensively investigated in common SCO compounds, with the complete photocycle revealed and dynamics of photoswitching studied on femtosecond timescale in solution [4] and the solid state. [5] More recently, another type of promising spin-crossover-like compounds has emerged. These copper-nitroxide-based molec-

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Ultrafast Photoswitching in a Copper‐Nitroxide‐Based Molecular Magnet

Kaszub

Marino

Lorenc

et al. 2014

Angewandte Chemie

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Ultrafast Photoswitching in a Copper‐Nitroxide‐Based Molecular Magnet

et al. 2014

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Spin‐State Ordering on One Sub‐lattice of a Mononuclear Iron(III) Spin Crossover Complex Exhibiting LIESST and TIESST

Murnaghan

Carbonera

Toupet

et al. 2014

Chemistry A European J

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The two-step spin crossover in mononuclear iron(III) complex [Fe(salpm)2 ]ClO4 ⋅0.5 EtOH (1) is shown to be accompanied by a structural phase transition as concluded from (57) Fe Mössbauer spectroscopy and single crystal X-ray diffraction, with spin-state ordering on just one of two sub-lattices in the intermediate magnetic and structural phase. The complex also exhibits thermal- and light-induced spin-state trapping (TIESST and LIESST), and relaxation from the LIESST and TIESST excited states occurs via the broken symmetry intermediate phase. Two relaxation events are evident in both experiments, that is, two T(LIESST) and two T(TIESST) values are recorded. The change in symmetry which accompanies the TIESST effect was followed in real time using single crystal diffraction. After flash freezing at 15 K the crystal was warmed to 40 K at which temperature superstructure reflections were observed to appear and disappear within a 10 000 s time range. In the frame of the international year of crystallography, these results illustrate how X-ray diffraction makes it possible to understand complex ordering phenomena.

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White Light Snapshot of Non-Equilibrium High-Spin State in a Molecular Crystal

Cited by 4 publications

References 13 publications

Ultrafast Photoswitching in a Copper‐Nitroxide‐Based Molecular Magnet

Ultrafast Photoswitching in a Copper‐Nitroxide‐Based Molecular Magnet

Ultrafast Photoswitching in a Copper‐Nitroxide‐Based Molecular Magnet

Spin‐State Ordering on One Sub‐lattice of a Mononuclear Iron(III) Spin Crossover Complex Exhibiting LIESST and TIESST

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