2014
DOI: 10.1002/anie.201310884
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Abstract: Light-induced excited spin-state trapping (LIESST) in iron(II) spin-crossover compounds, that is, the light-induced population of the high-spin (S=2) state below the thermal transition temperature, was discovered thirty years ago. For irradiation into metal-ligand charge transfer (MLCT) bands of the low-spin (S=0) species the acknowledged sequence takes the system from the initially excited (1) MLCT to the high-spin state via the (3) MLCT state within ca. 150 fs, thereby bypassing low-lying ligand-field (LF) s… Show more

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Cited by 70 publications
(108 citation statements)
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References 35 publications
(16 reference statements)
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“…193 The intersystem crossing (ISC) dynamics was then explored with the use of complementary probes, sensitive to different degrees of freedom, which strongly help investigating both ultrafast electronic and structural dynamics. 97,113,192,[194][195][196][197][198] A generic diagram of the potential energy curves of the various states of Fe(II)-based complexes is shown in Figure 9, as a function of the Fe-N bond length, which is supposed to be the reactive coordinate of the spin transition. 171 The MLCT states have nearly the same equilibrium distance as the ground state, in agreement with the results on Ru(II) complexes discussed above, 159 while the ligand field states 1,3 T, 5 T and 5 E have their equilibrium distances elongated by ~0.1 Å, ~0.2 Å, and ~0.3 Å, respectively, relative to the ground state bond distance.…”
Section: Photoinduced Spin Cross-over Dynamicsmentioning
confidence: 99%
“…193 The intersystem crossing (ISC) dynamics was then explored with the use of complementary probes, sensitive to different degrees of freedom, which strongly help investigating both ultrafast electronic and structural dynamics. 97,113,192,[194][195][196][197][198] A generic diagram of the potential energy curves of the various states of Fe(II)-based complexes is shown in Figure 9, as a function of the Fe-N bond length, which is supposed to be the reactive coordinate of the spin transition. 171 The MLCT states have nearly the same equilibrium distance as the ground state, in agreement with the results on Ru(II) complexes discussed above, 159 while the ligand field states 1,3 T, 5 T and 5 E have their equilibrium distances elongated by ~0.1 Å, ~0.2 Å, and ~0.3 Å, respectively, relative to the ground state bond distance.…”
Section: Photoinduced Spin Cross-over Dynamicsmentioning
confidence: 99%
“…It is also possible to trigger the change of spin state by light excitation [5]: this is the socalled Light-Induced Excited Spin State Trapping (LIESST) effect, easily observed at low temperature (typically below 100 K) where the photoinduced HS state is long-lived. At higher temperature, the use of time-resolved technique is required for observing transient LIESST and reverse LIESST with a ms or shorter life-time [6]. There are many SCO systems in the literature undergoing a first-order phase transition between LS and HS states and describing a thermal hysteresis.…”
Section: Fementioning
confidence: 99%
“…In crystals, the photoinduced out-of-equilibrium dynamics initiated by a laser pulse involves several steps [13][14][15][16][17][18]. First the LS to HS photoswitching occurs [6,[19][20]: the photoexcited molecules are trapped within less than 200 femtoseconds in the HS potential by the ultrafast activation and damping of the molecular breathing phonon, through a coherent structural reorganization [21][22][23]. The consecutive volume expansion drives additional conversion to the HS state during the socalled elastic step on nanosecond time scale [16,17].…”
Section: Fementioning
confidence: 99%
“…This is one of the reasons why more than twenty years after its discovery, LIESST e↵ect is still at the very center of the SCO research. The advances in short pulsed lasers enables researchers to extract information on the deactivation mechanism [15][16][17][18][19][20][21][22][23] and theoretical studies also contributed to the understanding of LIESST in octhedral Fe(II) complexes [60][61][62]. For Fe(III) complexes, the light irradiation induces ligand-tometal charge transfer transition (LMCT).…”
Section: Liesstmentioning
confidence: 99%
“…Therefore, the synthesis of systems with bistability under standard conditions for which switching is fast and both states are su ciently long-lived (i.e., persistent) has become increasingly important over the last 50 years. In this area of research, the interconversion between two di↵erent spin states that can be triggered by light irradiation is especially important [15][16][17][18][19][20][21][22][23]. The bistability in molecular magnets involves the M S components of a given spin state and the population of the bistable states can be controlled by the application of an external magnetic field.…”
mentioning
confidence: 99%