Ultrafast non-radiative dynamics of atomically thin MoSe2
Abstract Photo-induced non-radiative energy dissipation is a potential pathway to induce structural-phase transitions in two-dimensional materials. For advancing this field, a quantitative understanding of real-time atomic motion and lattice temperature is required. However, this understanding has b...
| Main Authors: | , , , , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2017-11-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-017-01844-2 |
| _version_ | 1797699179489787904 |
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| author | Ming-Fu Lin Vidya Kochat Aravind Krishnamoorthy Lindsay Bassman Oftelie Clemens Weninger Qiang Zheng Xiang Zhang Amey Apte Chandra Sekhar Tiwary Xiaozhe Shen Renkai Li Rajiv Kalia Pulickel Ajayan Aiichiro Nakano Priya Vashishta Fuyuki Shimojo Xijie Wang David M. Fritz Uwe Bergmann |
| author_facet | Ming-Fu Lin Vidya Kochat Aravind Krishnamoorthy Lindsay Bassman Oftelie Clemens Weninger Qiang Zheng Xiang Zhang Amey Apte Chandra Sekhar Tiwary Xiaozhe Shen Renkai Li Rajiv Kalia Pulickel Ajayan Aiichiro Nakano Priya Vashishta Fuyuki Shimojo Xijie Wang David M. Fritz Uwe Bergmann |
| author_sort | Ming-Fu Lin |
| collection | DOAJ |
| description | Abstract Photo-induced non-radiative energy dissipation is a potential pathway to induce structural-phase transitions in two-dimensional materials. For advancing this field, a quantitative understanding of real-time atomic motion and lattice temperature is required. However, this understanding has been incomplete due to a lack of suitable experimental techniques. Here, we use ultrafast electron diffraction to directly probe the subpicosecond conversion of photoenergy to lattice vibrations in a model bilayered semiconductor, molybdenum diselenide. We find that when creating a high charge carrier density, the energy is efficiently transferred to the lattice within one picosecond. First-principles nonadiabatic quantum molecular dynamics simulations reproduce the observed ultrafast increase in lattice temperature and the corresponding conversion of photoenergy to lattice vibrations. Nonadiabatic quantum simulations further suggest that a softening of vibrational modes in the excited state is involved in efficient and rapid energy transfer between the electronic system and the lattice. |
| first_indexed | 2024-03-12T04:05:18Z |
| format | Article |
| id | doaj.art-11a6c585dac54cefb1b01e08c61b5dd5 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-12T04:05:18Z |
| publishDate | 2017-11-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-11a6c585dac54cefb1b01e08c61b5dd52023-09-03T11:19:55ZengNature PortfolioNature Communications2041-17232017-11-01811810.1038/s41467-017-01844-2Ultrafast non-radiative dynamics of atomically thin MoSe2Ming-Fu Lin0Vidya Kochat1Aravind Krishnamoorthy2Lindsay Bassman Oftelie3Clemens Weninger4Qiang Zheng5Xiang Zhang6Amey Apte7Chandra Sekhar Tiwary8Xiaozhe Shen9Renkai Li10Rajiv Kalia11Pulickel Ajayan12Aiichiro Nakano13Priya Vashishta14Fuyuki Shimojo15Xijie Wang16David M. Fritz17Uwe Bergmann18Linac Coherent Light Source, SLAC National Accelerator LaboratoryDepartment of Materials Science and NanoEngineering, Rice UniversityCollaboratory for Advanced Computing and Simulations, Department of Physics & Astronomy, Department of Computer Science, Department of Chemical Engineering & Materials Science, Department of Biological Sciences, University of Southern CaliforniaCollaboratory for Advanced Computing and Simulations, Department of Physics & Astronomy, Department of Computer Science, Department of Chemical Engineering & Materials Science, Department of Biological Sciences, University of Southern CaliforniaLinac Coherent Light Source, SLAC National Accelerator LaboratorySLAC National Accelerator LaboratoryDepartment of Materials Science and NanoEngineering, Rice UniversityDepartment of Materials Science and NanoEngineering, Rice UniversityDepartment of Materials Science and NanoEngineering, Rice UniversitySLAC National Accelerator LaboratorySLAC National Accelerator LaboratoryCollaboratory for Advanced Computing and Simulations, Department of Physics & Astronomy, Department of Computer Science, Department of Chemical Engineering & Materials Science, Department of Biological Sciences, University of Southern CaliforniaDepartment of Materials Science and NanoEngineering, Rice UniversityCollaboratory for Advanced Computing and Simulations, Department of Physics & Astronomy, Department of Computer Science, Department of Chemical Engineering & Materials Science, Department of Biological Sciences, University of Southern CaliforniaCollaboratory for Advanced Computing and Simulations, Department of Physics & Astronomy, Department of Computer Science, Department of Chemical Engineering & Materials Science, Department of Biological Sciences, University of Southern CaliforniaDepartment of Physics, Kumamoto UniversitySLAC National Accelerator LaboratoryLinac Coherent Light Source, SLAC National Accelerator LaboratoryStanford PULSE Institute, SLAC National Accelerator LaboratoryAbstract Photo-induced non-radiative energy dissipation is a potential pathway to induce structural-phase transitions in two-dimensional materials. For advancing this field, a quantitative understanding of real-time atomic motion and lattice temperature is required. However, this understanding has been incomplete due to a lack of suitable experimental techniques. Here, we use ultrafast electron diffraction to directly probe the subpicosecond conversion of photoenergy to lattice vibrations in a model bilayered semiconductor, molybdenum diselenide. We find that when creating a high charge carrier density, the energy is efficiently transferred to the lattice within one picosecond. First-principles nonadiabatic quantum molecular dynamics simulations reproduce the observed ultrafast increase in lattice temperature and the corresponding conversion of photoenergy to lattice vibrations. Nonadiabatic quantum simulations further suggest that a softening of vibrational modes in the excited state is involved in efficient and rapid energy transfer between the electronic system and the lattice.https://doi.org/10.1038/s41467-017-01844-2 |
| spellingShingle | Ming-Fu Lin Vidya Kochat Aravind Krishnamoorthy Lindsay Bassman Oftelie Clemens Weninger Qiang Zheng Xiang Zhang Amey Apte Chandra Sekhar Tiwary Xiaozhe Shen Renkai Li Rajiv Kalia Pulickel Ajayan Aiichiro Nakano Priya Vashishta Fuyuki Shimojo Xijie Wang David M. Fritz Uwe Bergmann Ultrafast non-radiative dynamics of atomically thin MoSe2 Nature Communications |
| title | Ultrafast non-radiative dynamics of atomically thin MoSe2 |
| title_full | Ultrafast non-radiative dynamics of atomically thin MoSe2 |
| title_fullStr | Ultrafast non-radiative dynamics of atomically thin MoSe2 |
| title_full_unstemmed | Ultrafast non-radiative dynamics of atomically thin MoSe2 |
| title_short | Ultrafast non-radiative dynamics of atomically thin MoSe2 |
| title_sort | ultrafast non radiative dynamics of atomically thin mose2 |
| url | https://doi.org/10.1038/s41467-017-01844-2 |
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