Analysis of vibronic coupling in a 4f molecular magnet with FIRMS

2021 ◽  
Author(s):  
Jon G. C. Kragskow ◽  
Jonathan Marbey ◽  
Christian Dirk Buch ◽  
Joscha Nehrkorn ◽  
Mykhaylo Ozerov ◽  
...  
Keyword(s):  
Magnetic Relaxation ◽  
Electronic States ◽  
Far Infrared ◽  
Vibronic Coupling ◽  
Chemical Processes ◽  
Molecular Magnets ◽  
Molecular Magnet ◽  
Magnetic Memory ◽  
Vibrational Modes ◽  
Phonon Coupling

<p><b>Vibronic coupling, the interaction between molecular vibrations and electronic states, is a pervasive effect that profoundly affects chemical processes. In the case of molecular magnetic materials, vibronic, or spin-phonon, coupling leads to magnetic relaxation, which equates to loss of magnetic memory and loss of phase coherence in molecular magnets and qubits, respectively. The study of vibronic coupling is challenging, and most experimental evidence is indirect. Here we employ far-infrared magnetospectroscopy to probe vibronic transitions in in [Yb(trensal)] (where H<sub>3</sub>trensal = 2,2,2-tris(salicylideneimino)trimethylamine). We find intense signals near electronic states, which we show arise due to an “envelope effect” in the vibronic coupling Hamiltonian, and we calculate the vibronic coupling fully <i>ab initio</i> to simulate the spectra. We subsequently show that vibronic coupling is strongest for vibrational modes that simultaneously distort the first coordination sphere and break the C<sub>3</sub> symmetry of the molecule. With this knowledge, vibrational modes could be identified and engineered to shift their energy towards or away from particular electronic states to alter their impact. Hence, these findings provide new insights towards developing general guidelines for the control of vibronic coupling in molecules.</b></p>

scholarly journals Vibronic Coupling in a Molecular 4f Qubit

2021 ◽  
Author(s):  
Jonathan Marbey ◽  
Jon G. C. Kragskow ◽  
Christian Dirk Buch ◽  
Joscha Nehrkorn ◽  
Mykhaylo Ozerov ◽  
...  
Keyword(s):  
Experimental Evidence ◽  
Magnetic Relaxation ◽  
Electronic States ◽  
Far Infrared ◽  
Vibronic Coupling ◽  
Chemical Processes ◽  
Molecular Magnets ◽  
Magnetic Memory ◽  
Vibrational Modes ◽  
Phonon Coupling

<p><b>Vibronic coupling, the interaction between molecular vibrations and electronic states, is a pervasive effect that profoundly affects chemical processes. In the case of molecular magnetic materials, vibronic, or spin-phonon, coupling leads to magnetic relaxation, which equates to loss of magnetic memory and loss of phase coherence in molecular magnets and qubits, respectively. The study of vibronic coupling is challenging, and most experimental evidence is indirect. Here we employ far-infrared magnetospectroscopy to probe vibronic transitions in a Yb<sup>III</sup> molecular qubit directly. We find intense signals near electronic states, which we show arise due to an “envelope effect” in the vibronic coupling Hamiltonian, and we calculate the vibronic coupling fully <i>ab initio</i> to simulate the spectra. We subsequently show that vibronic coupling is strongest for vibrational modes that simultaneously distort the first coordination sphere and break the C<sub>3</sub> symmetry of the molecule. With this knowledge, vibrational modes could be identified and engineered to shift their energy towards or away from particular electronic states to alter their impact. Hence, these findings provide new insights towards developing general guidelines for the control of vibronic coupling in molecules.</b></p>

scholarly journals Vibronic Coupling in a Molecular 4f Qubit

2021 ◽  
Author(s):  
Jonathan Marbey ◽  
Jon G. C. Kragskow ◽  
Christian Dirk Buch ◽  
Joscha Nehrkorn ◽  
Mykhaylo Ozerov ◽  
...  
Keyword(s):  
Experimental Evidence ◽  
Magnetic Relaxation ◽  
Electronic States ◽  
Far Infrared ◽  
Vibronic Coupling ◽  
Chemical Processes ◽  
Molecular Magnets ◽  
Magnetic Memory ◽  
Vibrational Modes ◽  
Phonon Coupling

<p><b>Vibronic coupling, the interaction between molecular vibrations and electronic states, is a pervasive effect that profoundly affects chemical processes. In the case of molecular magnetic materials, vibronic, or spin-phonon, coupling leads to magnetic relaxation, which equates to loss of magnetic memory and loss of phase coherence in molecular magnets and qubits, respectively. The study of vibronic coupling is challenging, and most experimental evidence is indirect. Here we employ far-infrared magnetospectroscopy to probe vibronic transitions in a Yb<sup>III</sup> molecular qubit directly. We find intense signals near electronic states, which we show arise due to an “envelope effect” in the vibronic coupling Hamiltonian, and we calculate the vibronic coupling fully <i>ab initio</i> to simulate the spectra. We subsequently show that vibronic coupling is strongest for vibrational modes that simultaneously distort the first coordination sphere and break the C<sub>3</sub> symmetry of the molecule. With this knowledge, vibrational modes could be identified and engineered to shift their energy towards or away from particular electronic states to alter their impact. Hence, these findings provide new insights towards developing general guidelines for the control of vibronic coupling in molecules.</b></p>

scholarly journals Theoretical Basis for Switching a Kramers Single Molecular Magnet by Circularly-Polarized Radiation

Materials ◽  
2019 ◽  
Vol 12 (23) ◽  
pp. 3865
Author(s):  
Maryasov ◽  
Bowman ◽  
Fedin ◽  
Veber
Keyword(s):  
Double Resonance ◽  
Far Infrared ◽  
Molecular Magnets ◽  
Molecular Magnet ◽  
Zero Field ◽  
Zero Field Splitting ◽  
Circularly Polarized ◽  
Circularly Polarized Radiation ◽  
Alternating Magnetic Fields ◽  
Polarized Radiation

The d-group Kramers ions, having strong zero field splitting (ZFS) with axial symmetry and a negative D value for the ZFS Hamiltonian, are widely considered as candidates for use as single molecular magnets (SMMs). An important need is the means to switch the SMM between its states in a reasonably short and predictable period of time, which is generally not available. We propose an approach, Zeeman–far infrared (ZeFIR) double resonance, in which circularly polarized alternating magnetic fields in the far infrared (FIR) range induce selective magnetic dipole transitions between different Kramers doublets of the SMM and polarized microwave (mw) pulses transfer excitation inside the upper Kramers doublet. A combination of FIR and mw pulses allows unidirectional switching between +S and –S states of the ion. The proposed approach is considered for a model quartet system with total spin S = 3/2, which seems to be the most promising object for selective resonance manipulations of its states by circularly polarized radiation.

Identification of the Vibrational Modes in the Far-Infrared Spectra of Ruthenium Carbonyl Clusters and the Effect of Gold Substitution

2014 ◽  
Vol 53 (9) ◽  
pp. 4340-4349 ◽  
Author(s):  
Trystan Bennett ◽  
Rohul H. Adnan ◽  
Jason F. Alvino ◽  
Vladimir Golovko ◽  
Gunther G. Andersson ◽  
...  
Keyword(s):  
Infrared Spectra ◽  
Far Infrared ◽  
Vibrational Modes ◽  
Carbonyl Clusters ◽  
Ruthenium Carbonyl ◽  
Ruthenium Carbonyl Clusters ◽  
Far Infrared Spectra

scholarly journals Polar phonons and spin-phonon coupling inHgCr2S4andCdCr2S4studied with far-infrared spectroscopy

2007 ◽  
Vol 76 (17) ◽  
Author(s):  
T. Rudolf ◽  
Ch. Kant ◽  
F. Mayr ◽  
J. Hemberger ◽  
V. Tsurkan ◽  
...  
Keyword(s):  
Infrared Spectroscopy ◽  
Far Infrared ◽  
Far Infrared Spectroscopy ◽  
Phonon Coupling

Magnetic relaxation in Mn12-methanoate molecular magnet

2002 ◽  
Vol 242-245 ◽  
pp. 946-948
Author(s):  
D. Pajić ◽  
K. Zadro ◽  
T. Friščić ◽  
N. Judaš ◽  
E. Meštrović
Keyword(s):  
Magnetic Relaxation ◽  
Molecular Magnet

Directly monitoring the active sites of charge transfer in heterocycles in situ and in real time

2019 ◽  
Vol 55 (4) ◽  
pp. 541-544 ◽  
Author(s):  
Shuji Ye ◽  
Junjun Tan ◽  
Kangzhen Tian ◽  
Chuanzhao Li ◽  
Jiahui Zhang ◽  
...  
Keyword(s):  
Charge Transfer ◽  
Real Time ◽  
Vibrational Spectroscopy ◽  
Active Sites ◽  
Electronic States ◽  
Sum Frequency Generation ◽  
Vibrational Modes ◽  
Label Free ◽  
Sum Frequency

Coherent degenerate infrared-infrared-visible sum frequency generation vibrational spectroscopy provides a powerful label-free probe for identifying the vibrational modes that are coupled through the electronic states in situ and in real time.

Heterotrimetallic {LnOVPt} complexes with antiferromagnetic Ln–V coupling and magnetic memory

2020 ◽  
Vol 56 (75) ◽  
pp. 11062-11065
Author(s):  
Stephanie A. Beach ◽  
Jesse L. Guillet ◽  
Sydney P. Lagueux ◽  
Mauro Perfetti ◽  
Brooke N. Livesay ◽  
...  
Keyword(s):  
Magnetic Relaxation ◽  
Antiferromagnetic Coupling ◽  
Magnetic Memory ◽  
Slow Magnetic Relaxation

PtVO(SOCR)4 lantern complexes and Ce(OAr)3 or Nd(OAr)3 form heterotrimetallic [Ln(OAr)3{PtVO(SOCR)4}] with linear Ln–OVPt linkages; all four exhibit slow magnetic relaxation and likely antiferromagnetic coupling.

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