Time–thermo-dynamics of anti-Stokes and Stokes scattering and luminescence in 1-nm silicon nanoparticles: Toward an optical nanorefrigerator
The 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-symmetr...
| Main Authors: | , , , , |
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| Format: | Article |
| Language: | English |
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AIP Publishing LLC
2022-06-01
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| Series: | AIP Advances |
| Online Access: | http://dx.doi.org/10.1063/5.0091537 |
| _version_ | 1818114691664183296 |
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| author | Munir H. Nayfeh Huw Morgan Ammar Nayfeh Ersin Bahceci Laila Abuhassan |
| author_facet | Munir H. Nayfeh Huw Morgan Ammar Nayfeh Ersin Bahceci Laila Abuhassan |
| author_sort | Munir H. Nayfeh |
| collection | DOAJ |
| description | The 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° 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. |
| first_indexed | 2024-12-11T03:54:45Z |
| format | Article |
| id | doaj.art-9dae8ea29c784332a83d14a735030e73 |
| institution | Directory Open Access Journal |
| issn | 2158-3226 |
| language | English |
| last_indexed | 2024-12-11T03:54:45Z |
| publishDate | 2022-06-01 |
| publisher | AIP Publishing LLC |
| record_format | Article |
| series | AIP Advances |
| spelling | doaj.art-9dae8ea29c784332a83d14a735030e732022-12-22T01:21:49ZengAIP Publishing LLCAIP Advances2158-32262022-06-01126065219065219-1210.1063/5.0091537Time–thermo-dynamics of anti-Stokes and Stokes scattering and luminescence in 1-nm silicon nanoparticles: Toward an optical nanorefrigeratorMunir H. Nayfeh0Huw Morgan1Ammar Nayfeh2Ersin Bahceci3Laila Abuhassan4Department of Physics, University of Illinois at Urbana-Champaign, 1110 W. Green Street, Urbana, Illinois 61801, USADepartment of Physics, Aberystwyth University, Penglais, Aberystwyth, Ceredigion SY23 3BZ, United KingdomElectrical Engineering and Computer Science, Khalifa University, Abu Dhabi 127788, United Arab EmiratesDepartment of Metallurgical and Materials Engineering, Iskenderun Technical University, 31200 Hatay, TurkeyDepartment of Physics, University of Jordan, Amman, JordanThe 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° 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.http://dx.doi.org/10.1063/5.0091537 |
| spellingShingle | Munir H. Nayfeh Huw Morgan Ammar Nayfeh Ersin Bahceci Laila Abuhassan Time–thermo-dynamics of anti-Stokes and Stokes scattering and luminescence in 1-nm silicon nanoparticles: Toward an optical nanorefrigerator AIP Advances |
| title | Time–thermo-dynamics of anti-Stokes and Stokes scattering and luminescence in 1-nm silicon nanoparticles: Toward an optical nanorefrigerator |
| title_full | Time–thermo-dynamics of anti-Stokes and Stokes scattering and luminescence in 1-nm silicon nanoparticles: Toward an optical nanorefrigerator |
| title_fullStr | Time–thermo-dynamics of anti-Stokes and Stokes scattering and luminescence in 1-nm silicon nanoparticles: Toward an optical nanorefrigerator |
| title_full_unstemmed | Time–thermo-dynamics of anti-Stokes and Stokes scattering and luminescence in 1-nm silicon nanoparticles: Toward an optical nanorefrigerator |
| title_short | Time–thermo-dynamics of anti-Stokes and Stokes scattering and luminescence in 1-nm silicon nanoparticles: Toward an optical nanorefrigerator |
| title_sort | time thermo dynamics of anti stokes and stokes scattering and luminescence in 1 nm silicon nanoparticles toward an optical nanorefrigerator |
| url | http://dx.doi.org/10.1063/5.0091537 |
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