Structural observation of the primary isomerization in vision with femtosecond-stimulated Raman. Local vibrational coherences drive the primary photochemistry of vision. Nodeless vibrational amplitudes and quantum nonadiabatic dynamics in the nested funnel for a pseudo Jahn-Teller molecule or homodimer. Quantum mechanical wave packet dynamics at a conical intersection with strong vibrational dissipation. Direct mapping of curve-crossing dynamics in IBr by attosecond transient absorption spectroscopy. Selective excitation of vibrational wave packet motion using chirped pulses. Rapid acquisition of broadband two-dimensional electronic spectra by continuous scanning with conventional delay lines. Theoretical study of pyrazolate-bridged dinuclear platinum(II) complexes: interesting potential energy curve of the lowest energy triplet excited state and phosphorescence spectra. Ultrafast excited-state dynamics of photoluminescent Pt(II) dimers probed by a coherent vibrational wavepacket. Excited-state processes of cyclometalated platinum(II) charge-transfer dimers bridged by hydroxypyridines. Vibrational coherence transfer in the ultrafast intersystem crossing of a diplatinum complex in solution. Interplays of excited state structures and dynamics in copper(I) diimine complexes: implications and perspectives. The origin of efficient triplet state population in sulfur-substituted nucleobases. Intersystem crossing driven by vibronic spin–orbit coupling: a case study on psoralen. Spin-vibronic mechanism for intersystem crossing. Delayed fluorescence from a zirconium(IV) photosensitizer with ligand-to-metal charge-transfer excited states. The merger of transition metal and photocatalysis. Organic light-emitting diodes employing efficient reverse intersystem crossing for triplet-to-singlet state conversion. Light harvesting for organic photovoltaics. Interplay of vibrational wavepackets during an ultrafast electron transfer reaction. Dinitrogen coupling to a terpyridine-molybdenum chromophore is switched on by Fermi resonance. Vibrational coherences in manganese single-molecule magnets after ultrafast photoexcitation. Leveraging excited-state coherence for synthetic control of ultrafast dynamics. Revealing the spin–vibronic coupling mechanism of thermally activated delayed fluorescence. Sub-50-fs photoinduced spin crossover in 2+. The role of spin in the kinetic control of recombination in organic photovoltaics. Organic light emitters exhibiting very fast reverse intersystem crossing. Wada, Y., Nakagawa, H., Matsumoto, S., Wakisaka, Y. Stabilizing triplet excited states for ultralong organic phosphorescence. This work demonstrates the viability of using vibronic coherences as probes 6, 7, 8, 9 to clarify the interplay among spin, electronic and nuclear dynamics in spin-conversion processes, and this could inspire new modular designs to tailor the properties of excited states.Īn, Z. We find that vectorial motion along the Pt–Pt stretching coordinates tunes the singlet and intermediate-state energy gap irreversibly towards the conical intersection and subsequently drives formation of the lowest stable triplet state in a ratcheting fashion. The molecular-structure-dependent decoherence and recoherence dynamics of this wavepacket resolve the spin–vibronic mechanism. Photoexcitation activates the formation of a Pt–Pt bond, launching a stretching vibrational wavepacket. Here we present coherence spectroscopy experiments that reveal the interplay between the spin, electronic and vibrational degrees of freedom that drive efficient singlet–triplet conversion in four structurally related dinuclear Pt(II) metal–metal-to-ligand charge-transfer (MMLCT) complexes. However, it has been difficult to identify precise experimental manifestations of the spin–vibronic mechanism. Previous studies have indicated that the combination of spin–orbit and vibronic effects, collectively termed the spin–vibronic effect, can accelerate quantum-mechanically forbidden transitions at non-adiabatic crossings 4, 5. Design-specific control over the transitions between excited electronic states with different spin multiplicities is of the utmost importance in molecular and materials chemistry 1, 2, 3.
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