Vibrational coherences in manganese single-molecule magnets after ultrafast photoexcitation.
Florian LiedyJulien EngRobbie McNabRoss InglisThomas J PenfoldEuan K BrechinJ Olof JohanssonPublished in: Nature chemistry (2020)
Magnetic recording using femtosecond laser pulses has recently been achieved in some dielectric media, showing potential for ultrafast data storage applications. Single-molecule magnets (SMMs) are metal complexes with two degenerate magnetic ground states and are promising for increasing storage density, but remain unexplored using ultrafast techniques. Here we have explored the dynamics occurring after photoexcitation of a trinuclear µ3-oxo-bridged Mn(III)-based SMM, whose magnetic anisotropy is closely related to the Jahn-Teller distortion. Ultrafast transient absorption spectroscopy in solution reveals oscillations superimposed on the decay traces due to a vibrational wavepacket. Based on complementary measurements and calculations on the monomer Mn(acac)3, we conclude that the wavepacket motion in the trinuclear SMM is constrained along the Jahn-Teller axis due to the µ3-oxo and µ-oxime bridges. Our results provide new possibilities for optical control of the magnetization in SMMs on femtosecond timescales and open up new molecular-design challenges to control the wavepacket motion in the excited state of polynuclear transition-metal complexes.
Keyphrases
- single molecule
- energy transfer
- transition metal
- molecularly imprinted
- density functional theory
- atomic force microscopy
- living cells
- molecular dynamics simulations
- high speed
- quantum dots
- electron transfer
- room temperature
- molecular dynamics
- high resolution
- solid phase extraction
- machine learning
- electronic health record
- mass spectrometry
- big data
- risk assessment
- cerebral ischemia
- raman spectroscopy
- brain injury
- blood brain barrier
- climate change
- data analysis
- human health
- oxide nanoparticles