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dc.contributor.authorZhang, Wen
dc.contributor.authorMaul, Jen
dc.contributor.authorVulpe, Dianaen
dc.contributor.authorMoghadam, PZen
dc.contributor.authorFairen Jimenez, Daviden
dc.contributor.authorMittleman, DMen
dc.contributor.authorZeitler, Axelen
dc.contributor.authorErba, Aen
dc.contributor.authorRuggiero, MTen
dc.date.accessioned2018-12-20T00:30:22Z
dc.date.available2018-12-20T00:30:22Z
dc.date.issued2018-12-06en
dc.identifier.issn1932-7447
dc.identifier.urihttps://www.repository.cam.ac.uk/handle/1810/287207
dc.description.abstractThe identification and characterization of low-frequency vibrational motions of metal-organic frameworks (MOFs) allows for a better understanding of their mechanical and structural response upon perturbation by external stimuli such as temperature, pressure, and adsorption. Here, we describe the combination of an experimental temperature- and pressure-dependent terahertz spectroscopy system with quantum mechanical simulations to measure and assign specific low-frequency vibrational modes that directly drive the mechanochemical properties of this important class of porous materials. More specifically, those intense spectral features in the terahertz region of the vibrational spectrum of ZIF-8 are identified, which are directly connected to its mechanochemical response. In particular, the mechanical compressibility of pristine ZIF-8 is found to follow a peculiar non-linear trend upon pressure: its bulk modulus initially increases up to 0.1 GPa and decreases at higher pressures, which is simultaneously reflected in the terahertz vibrational spectra. This work highlights the interplay between structural, vibrational, and mechanochemical phenomena, all of which are key to the effective exploitation of MOFs. The importance of terahertz vibrational motions on the function of MOFs is demonstrated, and a method presented for their measurement and interpretation, which can be applied widely to any supramolecular material.
dc.publisherAmerican Chemical Society (ACS)
dc.titleProbing the Mechanochemistry of Metal-Organic Frameworks with Low-Frequency Vibrational Spectroscopyen
dc.typeArticle
prism.endingPage27450
prism.issueIdentifier48en
prism.publicationDate2018en
prism.publicationNameJournal of Physical Chemistry Cen
prism.startingPage27442
prism.volume122en
dc.identifier.doi10.17863/CAM.34514
dcterms.dateAccepted2018-11-06en
rioxxterms.versionofrecord10.1021/acs.jpcc.8b08334en
rioxxterms.versionAM
rioxxterms.licenseref.urihttp://www.rioxx.net/licenses/all-rights-reserveden
rioxxterms.licenseref.startdate2018-12-06en
dc.contributor.orcidMaul, J [0000-0002-4920-1001]
dc.contributor.orcidFairen-Jimenez, David [0000-0002-5013-1194]
dc.contributor.orcidMittleman, DM [0000-0003-4277-7419]
dc.contributor.orcidZeitler, Jochen [0000-0002-4958-0582]
dc.contributor.orcidErba, A [0000-0002-2986-4254]
dc.contributor.orcidRuggiero, MT [0000-0003-1848-2565]
dc.identifier.eissn1932-7455
rioxxterms.typeJournal Article/Reviewen
pubs.funder-project-idEPSRC (1198)
pubs.funder-project-idEuropean Commission Horizon 2020 (H2020) ERC (726380)
rioxxterms.freetoread.startdate2019-11-06


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