One-Dimensional Silver-Thiolate Cluster-Assembly: Effect of Argentophilic Interactions on Excited-State Dynamics
| Autor: | Anish Kumar Das, Amitava Patra, Shiv N. Khanna, Turbasu Sengupta, Sukhendu Mandal, Subarna Maity, Dinesh Bista, Arthur C. Reber |
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| Rok vydání: | 2021 |
| Předmět: |
Materials science
Relaxation (NMR) 02 engineering and technology Electronic structure Crystal structure 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences Molecular physics 0104 chemical sciences Excited state Ultrafast laser spectroscopy Cluster (physics) General Materials Science Physical and Theoretical Chemistry 0210 nano-technology Spectroscopy Absorption (electromagnetic radiation) |
| Zdroj: | The Journal of Physical Chemistry Letters. 12:2154-2159 |
| ISSN: | 1948-7185 |
| Popis: | We report the synthesis, crystal structure, and electronic structure calculations of a one-dimensional silver-thiolate cluster-assembled and its ultrafast spectroscopic investigation. Experiments and theory find the material to have a significant gap as the HOMO-LUMO absorption corresponds to 2.69 eV, and the defect-free structure is calculated to have a gap of 2.82 eV. Cluster models demonstrate that the gap energy is length-dependent. Theoretical studies identify a nonbonding metallophilic interaction that exists between two Ag atoms in adjacent strings that helps to stabilize the chain structure. Transient absorption spectroscopy reveals that the electron dynamics is a mixture of the behavior of cluster and nanoparticle, with the material having a 346 fs ground-state relaxation like a cluster, and the electron dynamics is dominated by electron-phonon coupling with a decay time of 1.5 ps, unlike the isolated cluster whose decay is mostly radiative. |
| Databáze: | OpenAIRE |
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