Direct dynamics studies of a binuclear metal complex in solution: The interplay between vibrational relaxation, coherence, and solvent effects

Asmus Ougaard Dohn; Elvar Örn Jónsson; Kasper Skov Kjær; Tim Brandt Van Driel; Martin Meedom Nielsen; Karsten Wedel Jacobsen; Niels Engholm Henriksen; Klaus Braagaard Møller

doi:10.1021/jz500850s

Direct dynamics studies of a binuclear metal complex in solution: The interplay between vibrational relaxation, coherence, and solvent effects

Asmus Ougaard Dohn^*, Elvar Örn Jónsson, Kasper Skov Kjær, Tim Brandt Van Driel, Martin Meedom Nielsen, Karsten Wedel Jacobsen, Niels Engholm Henriksen, Klaus Braagaard Møller

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

28 Citations (Scopus)

Abstract

By using a newly implemented QM/MM multiscale MD method to simulate the excited state dynamics of the Ir₂(dimen)4₂₊ (dimen = 1,8-diisocyano-p-menthane) complex, we not only report on results that support the two experimentally observed coherent dynamical modes in the molecule but also reveal a third mode, not distinguishable by spectroscopic methods. We directly follow the channels of energy dissipation to the solvent and report that the main cause for coherence decay is the initial wide range of configurations in the excited state population. We observe that the solvent can actually extend the coherence lifetime by blocking channels for intramolecular vibrational energy redistribution (IVR).

Original language	English
Pages (from-to)	2414-2418
Number of pages	5
Journal	Journal of Physical Chemistry Letters
Volume	5
Issue number	14
DOIs	https://doi.org/10.1021/jz500850s
Publication status	Published - 17 Jul 2014

Other keywords

BOMD
Electronic Structure
Excited States
QM/MM MD
Solvation
Transition Metal Complexes
Ultrafast Dynamics

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10.1021/jz500850s

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Dohn, A. O., Jónsson, E. Ö., Kjær, K. S., Van Driel, T. B., Nielsen, M. M., Jacobsen, K. W., Henriksen, N. E., & Møller, K. B. (2014). Direct dynamics studies of a binuclear metal complex in solution: The interplay between vibrational relaxation, coherence, and solvent effects. Journal of Physical Chemistry Letters, 5(14), 2414-2418. https://doi.org/10.1021/jz500850s

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title = "Direct dynamics studies of a binuclear metal complex in solution: The interplay between vibrational relaxation, coherence, and solvent effects",

abstract = "By using a newly implemented QM/MM multiscale MD method to simulate the excited state dynamics of the Ir2(dimen)42+ (dimen = 1,8-diisocyano-p-menthane) complex, we not only report on results that support the two experimentally observed coherent dynamical modes in the molecule but also reveal a third mode, not distinguishable by spectroscopic methods. We directly follow the channels of energy dissipation to the solvent and report that the main cause for coherence decay is the initial wide range of configurations in the excited state population. We observe that the solvent can actually extend the coherence lifetime by blocking channels for intramolecular vibrational energy redistribution (IVR).",

keywords = "BOMD, Electronic Structure, Excited States, QM/MM MD, Solvation, Transition Metal Complexes, Ultrafast Dynamics",

author = "Dohn, {Asmus Ougaard} and J{\'o}nsson, {Elvar {\"O}rn} and Kj{\ae}r, {Kasper Skov} and {Van Driel}, {Tim Brandt} and Nielsen, {Martin Meedom} and Jacobsen, {Karsten Wedel} and Henriksen, {Niels Engholm} and M{\o}ller, {Klaus Braagaard}",

year = "2014",

month = jul,

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doi = "10.1021/jz500850s",

language = "English",

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journal = "Journal of Physical Chemistry Letters",

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publisher = "American Chemical Society",

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T2 - The interplay between vibrational relaxation, coherence, and solvent effects

AU - Dohn, Asmus Ougaard

AU - Jónsson, Elvar Örn

AU - Kjær, Kasper Skov

AU - Van Driel, Tim Brandt

AU - Nielsen, Martin Meedom

AU - Jacobsen, Karsten Wedel

AU - Henriksen, Niels Engholm

AU - Møller, Klaus Braagaard

PY - 2014/7/17

Y1 - 2014/7/17

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AB - By using a newly implemented QM/MM multiscale MD method to simulate the excited state dynamics of the Ir2(dimen)42+ (dimen = 1,8-diisocyano-p-menthane) complex, we not only report on results that support the two experimentally observed coherent dynamical modes in the molecule but also reveal a third mode, not distinguishable by spectroscopic methods. We directly follow the channels of energy dissipation to the solvent and report that the main cause for coherence decay is the initial wide range of configurations in the excited state population. We observe that the solvent can actually extend the coherence lifetime by blocking channels for intramolecular vibrational energy redistribution (IVR).

KW - BOMD

KW - Electronic Structure

KW - Excited States

KW - QM/MM MD

KW - Solvation

KW - Transition Metal Complexes

KW - Ultrafast Dynamics

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JO - Journal of Physical Chemistry Letters

JF - Journal of Physical Chemistry Letters

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ER -

Direct dynamics studies of a binuclear metal complex in solution: The interplay between vibrational relaxation, coherence, and solvent effects

Abstract

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