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dc.contributor.authorNayfeh, Munir H.
dc.contributor.authorMorgan, Huw
dc.contributor.authorNayfeh, Ammar
dc.contributor.authorBahçeci, Ersin
dc.contributor.authorAbuhassan, Laila
dc.date.accessioned2022-11-15T12:57:30Z
dc.date.available2022-11-15T12:57:30Z
dc.date.issued2022en_US
dc.identifier.citationNayfeh, M.H., Morgan, H., Nayfeh, A., Bahceci, E., Abuhassan, L. (2022). Time-thermo-dynamics of anti-Stokes and Stokes scattering and luminescence in 1-nm silicon nanoparticles: Toward an optical nanorefrigerator. AIP Advances, 12 (6), art. no. 065219. https://doi.org/10.1063/5.0091537en_US
dc.identifier.urihttps://doi.org/10.1063/5.0091537
dc.identifier.urihttps://aip.scitation.org/doi/10.1063/5.0091537
dc.identifier.urihttps://hdl.handle.net/20.500.12508/2254
dc.description.abstractThe thermodynamics of nanosystems is interesting, as they constitute the transition between the atomistic and solid states. This is empowered by the development of tools to manipulate individual atoms and perform atomistic simulations and fundamental thermos-science, such as microscopic time-symmetry and macroscopic time-asymmetry, the origin of time's arrow, and photo-cryo-refrigeration. We examine here the photo-thermo and time dynamics in 1-nm silicon nanoparticles with tetrahedral-molecular core-shell structure prepared ex situ and suspended in solvents or re-constituted in films. We examined the temperature dependence of the quantum efficiency and time-dynamics of the Stokes luminescence and its energy dependence across the band. With temperature, we get flat lifetimes but with delay in the onset in agreement with a model calculation of above barrier emission. Our atomistic time-dependent density functional theory shows that Stokes heating takes place in the molecular-like shell where the lifetime is in the nanosecond regime, whereas anti-Stokes cooling takes place in the tetrahedral core where the lifetime is in the ms regime. Unlike doped glasses, we observed a 2-order of magnitude increase in the quantum efficiency of the Stokes luminescence at 10 degrees K. The increase in the quantum efficiency at low temperature, the high quantum efficiency of stimulated anti-Stokes scattering and its anti-correlation with the luminescence, and the visible transparency/blindness due to quantum confinement are requirements for solid state photo-cooling, which may afford an all-silicon photo-cryo-refrigeration, with potential full integration into the CMOS silicon industry.en_US
dc.language.isoengen_US
dc.publisherAmerican Institute of Physics Inc.en_US
dc.relation.isversionof10.1063/5.0091537en_US
dc.rightsinfo:eu-repo/semantics/openAccessen_US
dc.subject.classificationSilicon
dc.subject.classificationNanocrystal
dc.subject.classificationPhotoluminescence
dc.subject.classificationScience & Technology - Other Topics
dc.subject.classificationMaterials Science
dc.subject.classificationPhysics
dc.subject.classificationPhysics - Semiconductor Physics - Optical Refrigeration
dc.subject.otherUp-conversion luminescence
dc.subject.otherSemiconductor
dc.subject.otherPhotoluminescence
dc.subject.otherFluorescence
dc.subject.otherEmission
dc.subject.otherState
dc.subject.otherFilms
dc.subject.otherDensity functional theory
dc.subject.otherDynamics
dc.subject.otherNanoparticles
dc.subject.otherQuantum efficiency
dc.subject.otherQuantum theory
dc.subject.otherRefrigeration
dc.subject.otherSilicon
dc.subject.otherTemperature distribution
dc.subject.otherAnti-Stokes
dc.subject.otherAtomistic simulations
dc.subject.otherAtomistics
dc.subject.otherCore shell structure
dc.subject.otherEx situ; Molecular core
dc.subject.other
dc.subject.otherOptical-
dc.subject.otherSilicon nanoparticles
dc.subject.otherThermo dynamics
dc.subject.otherTime dynamic
dc.titleTime-thermo-dynamics of anti-Stokes and Stokes scattering and luminescence in 1-nm silicon nanoparticles: Toward an optical nanorefrigeratoren_US
dc.typearticleen_US
dc.relation.journalAIP Advancesen_US
dc.contributor.departmentMühendislik ve Doğa Bilimleri Fakültesi -- Metalurji ve Malzeme Mühendisliği Bölümüen_US
dc.identifier.volume12en_US
dc.identifier.issue6en_US
dc.relation.publicationcategoryMakale - Uluslararası Hakemli Dergi - Kurum Öğretim Elemanıen_US
dc.contributor.isteauthorBahçeci, Ersin
dc.relation.indexWeb of Science - Scopusen_US
dc.relation.indexWeb of Science Core Collection - Science Citation Index Expanded


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