Identifying the role of terahertz vibrations in metal-organic frameworks: from gate-opening phenomenon to shear-driven structural destabilization.
We present an unambiguous identification of low-frequency terahertz vibrations in the archetypal imidazole-based metal-organic framework (MOF) materials: ZIF-4, ZIF-7, and ZIF-8, all of which adopt a zeolite-like nanoporous structure. Using inelastic neutron scattering and synchrotron radiation far-...
| Auteurs principaux: | , , , , , , , |
|---|---|
| Format: | Journal article |
| Langue: | English |
| Publié: |
American Physical Society
2014
|
| _version_ | 1826289851797864448 |
|---|---|
| author | Ryder, M Civalleri, B Bennett, T Henke, S Rudić, S Cinque, G Fernandez-Alonso, F Tan, J |
| author_facet | Ryder, M Civalleri, B Bennett, T Henke, S Rudić, S Cinque, G Fernandez-Alonso, F Tan, J |
| author_sort | Ryder, M |
| collection | OXFORD |
| description | We present an unambiguous identification of low-frequency terahertz vibrations in the archetypal imidazole-based metal-organic framework (MOF) materials: ZIF-4, ZIF-7, and ZIF-8, all of which adopt a zeolite-like nanoporous structure. Using inelastic neutron scattering and synchrotron radiation far-infrared absorption spectroscopy, in conjunction with density functional theory (DFT), we have pinpointed all major sources of vibrational modes.Ab initioDFT calculations revealed the complex nature of the collective THz modes, which enable us to establish detailed correlations with experiments. We discover that low-energy conformational dynamics offers multiple pathways to elucidate novel physical phenomena observed in MOFs. New evidence demonstrates that THz modes are intrinsically linked, not only to anomalous elasticity underpinning gate-opening and pore-breathing mechanisms, but also to shear-induced phase transitions and the onset of structural instability. |
| first_indexed | 2024-03-07T02:35:13Z |
| format | Journal article |
| id | oxford-uuid:a88c5a08-fb8e-498c-a483-a653e21c3ee2 |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-03-07T02:35:13Z |
| publishDate | 2014 |
| publisher | American Physical Society |
| record_format | dspace |
| spelling | oxford-uuid:a88c5a08-fb8e-498c-a483-a653e21c3ee22022-03-27T03:02:24ZIdentifying the role of terahertz vibrations in metal-organic frameworks: from gate-opening phenomenon to shear-driven structural destabilization.Journal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:a88c5a08-fb8e-498c-a483-a653e21c3ee2EnglishSymplectic Elements at OxfordAmerican Physical Society2014Ryder, MCivalleri, BBennett, THenke, SRudić, SCinque, GFernandez-Alonso, FTan, JWe present an unambiguous identification of low-frequency terahertz vibrations in the archetypal imidazole-based metal-organic framework (MOF) materials: ZIF-4, ZIF-7, and ZIF-8, all of which adopt a zeolite-like nanoporous structure. Using inelastic neutron scattering and synchrotron radiation far-infrared absorption spectroscopy, in conjunction with density functional theory (DFT), we have pinpointed all major sources of vibrational modes.Ab initioDFT calculations revealed the complex nature of the collective THz modes, which enable us to establish detailed correlations with experiments. We discover that low-energy conformational dynamics offers multiple pathways to elucidate novel physical phenomena observed in MOFs. New evidence demonstrates that THz modes are intrinsically linked, not only to anomalous elasticity underpinning gate-opening and pore-breathing mechanisms, but also to shear-induced phase transitions and the onset of structural instability. |
| spellingShingle | Ryder, M Civalleri, B Bennett, T Henke, S Rudić, S Cinque, G Fernandez-Alonso, F Tan, J Identifying the role of terahertz vibrations in metal-organic frameworks: from gate-opening phenomenon to shear-driven structural destabilization. |
| title | Identifying the role of terahertz vibrations in metal-organic frameworks: from gate-opening phenomenon to shear-driven structural destabilization. |
| title_full | Identifying the role of terahertz vibrations in metal-organic frameworks: from gate-opening phenomenon to shear-driven structural destabilization. |
| title_fullStr | Identifying the role of terahertz vibrations in metal-organic frameworks: from gate-opening phenomenon to shear-driven structural destabilization. |
| title_full_unstemmed | Identifying the role of terahertz vibrations in metal-organic frameworks: from gate-opening phenomenon to shear-driven structural destabilization. |
| title_short | Identifying the role of terahertz vibrations in metal-organic frameworks: from gate-opening phenomenon to shear-driven structural destabilization. |
| title_sort | identifying the role of terahertz vibrations in metal organic frameworks from gate opening phenomenon to shear driven structural destabilization |
| work_keys_str_mv | AT ryderm identifyingtheroleofterahertzvibrationsinmetalorganicframeworksfromgateopeningphenomenontosheardrivenstructuraldestabilization AT civallerib identifyingtheroleofterahertzvibrationsinmetalorganicframeworksfromgateopeningphenomenontosheardrivenstructuraldestabilization AT bennettt identifyingtheroleofterahertzvibrationsinmetalorganicframeworksfromgateopeningphenomenontosheardrivenstructuraldestabilization AT henkes identifyingtheroleofterahertzvibrationsinmetalorganicframeworksfromgateopeningphenomenontosheardrivenstructuraldestabilization AT rudics identifyingtheroleofterahertzvibrationsinmetalorganicframeworksfromgateopeningphenomenontosheardrivenstructuraldestabilization AT cinqueg identifyingtheroleofterahertzvibrationsinmetalorganicframeworksfromgateopeningphenomenontosheardrivenstructuraldestabilization AT fernandezalonsof identifyingtheroleofterahertzvibrationsinmetalorganicframeworksfromgateopeningphenomenontosheardrivenstructuraldestabilization AT tanj identifyingtheroleofterahertzvibrationsinmetalorganicframeworksfromgateopeningphenomenontosheardrivenstructuraldestabilization |