20942
2020
eng
5531-5535
59
article
1
2020-07-30
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--
Tetraiododiborane(4) (B\(_2\)I\(_4\)) is a Polymer based on sp\(^3\) Boron in the Solid State
Herein we present the first solid‐state structures of tetraiododiborane(4) (B\(_2\)I\(_4\)), which was long believed to exist in all phases as discrete molecules with planar, tricoordinate boron atoms, like the lighter tetrahalodiboranes(4) B\(_2\)F\(_4\), B\(_2\)Cl\(_4\), and B\(_2\)Br\(_4\). Single‐crystal X‐ray diffraction, solid‐state NMR, and IR measurements indicate that B\(_2\)I\(_4\) in fact exists as two different polymeric forms in the solid state, both of which feature boron atoms in tetrahedral environments. DFT calculations are used to simulate the IR spectra of the solution and solid‐state structures, and these are compared with the experimental spectra.
Angewandte Chemie International Edition
10.1002/anie.201913590
urn:nbn:de:bvb:20-opus-209428
Angewandte Chemie International Edition 2020 , 59 , 5531-5535. DOI: 10.1002/anie.201913590
646737
CC BY: Creative-Commons-Lizenz: Namensnennung 4.0 International
Jonas H. Muessig
Polina Lisinetskaya
Rian D. Dewhurst
Rüdiger Bertermann
Melanie Thaler
Roland Mitric
Holger Braunschweig
eng
uncontrolled
boron tetraiodide
eng
uncontrolled
boron
eng
uncontrolled
density functional theory
eng
uncontrolled
diborane
eng
uncontrolled
halides
eng
uncontrolled
solid-state sturcture
Chemie und zugeordnete Wissenschaften
Anorganische Chemie
open_access
Institut für Anorganische Chemie
Institut für Physikalische und Theoretische Chemie
OpenAIRE
Universität Würzburg
https://opus.bibliothek.uni-wuerzburg.de/files/20942/Mitric_anie.201913590.pdf
15919
2016
eng
175
6
122
article
1
2018-03-16
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First-principles simulation of light propagation and exciton dynamics in metal cluster nanostructures
We present a theoretical approach for the simulation of the electric field and exciton propagation in ordered arrays constructed of molecular-sized noble metal clusters bound to organic polymer templates. In order to describe the electronic coupling between individual constituents of the nanostructure we use the ab initio parameterized transition charge method which is more accurate than the usual dipole-dipole coupling. The electronic population dynamics in the nanostructure under an external laser pulse excitation is simulated by numerical integration of the time-dependent Schrodinger equation employing the fully coupled Hamiltonian. The solution of the TDSE gives rise to time-dependent partial point charges for each subunit of the nanostructure, and the spatio-temporal electric field distribution is evaluated by means of classical electrodynamics methods. The time-dependent partial charges are determined based on the stationary partial and transition charges obtained in the framework of the TDDFT. In order to treat large plasmonic nanostructures constructed of many constituents, the approximate self-consistent iterative approach presented in (Lisinetskaya and Mitric in Phys Rev B 89:035433, 2014) is modified to include the transition-charge-based interaction. The developed methods are used to study the optical response and exciton dynamics of Ag-3(+) and porphyrin-Ag-4 dimers. Subsequently, the spatio-temporal electric field distribution in a ring constructed of ten porphyrin-Ag-4 subunits under the action of circularly polarized laser pulse is simulated. The presented methodology provides a theoretical basis for the investigation of coupled light-exciton propagation in nanoarchitectures built from molecular size metal nanoclusters in which quantum confinement effects are important.
Applied Physics B
10.1007/s00340-016-6436-6
https://doi.org/10.1007/s00340-016-6436-6
0946-2171
urn:nbn:de:bvb:20-opus-159193
This is a post-peer-review, pre-copyedit version of an article published in Apllied Physcis B. The final authenticated version is available online at: http://dx.doi.org/10.1007/s00340-016-6436-6
646737
Applied Physics B (2016) 122: 175. https://doi.org/10.1007/s00340-016-6436-6
Deutsches Urheberrecht
Polina Lisinetskaya
Merle I. S. Röhr
Roland Mitrić
eng
uncontrolled
metal-cluster hybrid systems
eng
uncontrolled
exciton transfer
eng
uncontrolled
optical response
eng
uncontrolled
transition density
eng
uncontrolled
total electric field
eng
uncontrolled
electric field distribution
eng
uncontrolled
transition dipole moment
eng
uncontrolled
transition charge
Physikalische Chemie
open_access
Institut für Physikalische und Theoretische Chemie
OpenAIRE
Universität Würzburg
https://opus.bibliothek.uni-wuerzburg.de/files/15919/Lisinetskaya_Roehr_Mitric_Firts-principles_simulation_Applied_Physics_B_Accepted_version.pdf
15917
2016
eng
6411-6419
9
18
article
1
2018-03-16
--
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Excited state nonadiabatic dynamics of bare and hydrated anionic gold clusters Au\(^−_3\)[H\(_2\)O]\(_n\) (n=0-2)
We present a joint theoretical and experimental study of excited state dynamics in pure and hydrated anionic gold clusters Au\(^-_3\)[H\(_2\)O]\(_n\) (n = 0-2). We employ mixed quantum-classical dynamics combined with femtosecond time-resolved photoelectron spectroscopy in order to investigate the influence of hydration on excited state lifetimes and photo-dissociation dynamics. A gradual decrease of the excited state lifetime with the number of adsorbed water molecules as well as gold cluster fragmentation quenching by two or more water molecules are observed both in experiment and in simulations. Non-radiative relaxation and dissociation in excited states are found to be responsible for the excited state population depletion. Time constants of these two processes strongly depend on the number of water molecules leading to the possibility to modulate excited state dynamics and fragmentation of the anionic cluster by adsorption of water molecules.
Physical Chemistry Chemical Physics
10.1039/c5cp04297f
https://doi.org/10.1039/C5CP04297F
1463-9076
26478260
urn:nbn:de:bvb:20-opus-159176
Accepted version
Fachbereich Physik, Universität Konstanz, D-78464 Konstanz, Germany
Department of Chemistry, Sungkyunkwan University, 440-746 Suwon, Republic of Korea
Physical Chemistry Chemical Physics, 2016, 18, 6411-6419. DOI: 10.1039/C5CP04297F
646737
Deutsches Urheberrecht
Polina Lisinetskaya
Christian Braun
Sebastian Proch
Young Dok Kim
Gerd Ganteför
Roland Mitrić
eng
uncontrolled
nonadiabatic dynamics
eng
uncontrolled
metal cluster
eng
uncontrolled
time-resolved photoelectron spectroscopy
Physikalische Chemie
open_access
Institut für Physikalische und Theoretische Chemie
OpenAIRE
Universität Würzburg
https://opus.bibliothek.uni-wuerzburg.de/files/15917/Lisinetskaya_Mitric_Gold_Clusters_PCCP_accepted_version.pdf