Optical Properties of Colloidal II-VI and III-V Semiconductor Nanocrystals: Single Nanocrystal Photon Correlation Spectroscopy
Colloidal nanocrystals (NCs), also known as quantum dots, are nanometer-sized semiconductor crystalline structures comprised of thousands to tens of thousands of atoms placing them in a world between the molecular-sized and the bulk-sized world, allowing them to harness unique qualities from both. C...
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| Format: | Thesis |
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Massachusetts Institute of Technology
2024
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| Online Access: | https://hdl.handle.net/1721.1/157111 https://orcid.org/0000-0002-7143-1073 |
| _version_ | 1824458247028867072 |
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| author | Berkinsky, David |
| author2 | Bawendi, Moungi G. |
| author_facet | Bawendi, Moungi G. Berkinsky, David |
| author_sort | Berkinsky, David |
| collection | MIT |
| description | Colloidal nanocrystals (NCs), also known as quantum dots, are nanometer-sized semiconductor crystalline structures comprised of thousands to tens of thousands of atoms placing them in a world between the molecular-sized and the bulk-sized world, allowing them to harness unique qualities from both. Colloidal NCs are used in many applications including light-emitting diodes (LEDs), photovoltaics (solar cells), lasers, transistors, photocatalysis, and many more. In this thesis, I investigate the optical properties of colloidal NCs, specifically InP/ZnSe/ZnS, CdSe/CdS/ZnS, and ZnSe/ZnS NCs using a combination of ensemble and single NC photon correlation spectroscopic techniques. In the first chapter, I introduce the photophysical properties of colloidal NCs and spectroscopic techniques relevant to my studies. In the second chapter, I determine the dominant photoluminescent line shape broadening mechanisms in single InP/ZnSe/ZnS and CdSe/CdS/ZnS NCs using temperature dependent photoluminescent spectroscopic techniques. In the third chapter, I investigate the coherent emissive properties of single InP/ZnSe/ZnS and CdSe/CdS/ZnS at cryogenic temperatures, demonstrating the longest coherence time measured in a colloidal NC system to date. In the fourth chapter, I develop an ensemble third-order correlation technique to elucidate the average single ZnSe/ZnS NC triexciton efficiency and dynamics. Finally, I propose future directions in the fifth chapter, including a fourth order correlation technique to resolve absolute energy information on timescales faster than CCDbase spectroscopic techniques, and an open-access photon correlation Monte Carlo toolkit with the aim of filling education gaps and provide the colloidal NC community with a database of analytical tools that will encourage a wider audience to engage with photon correlation spectroscopy. |
| first_indexed | 2025-02-19T04:22:51Z |
| format | Thesis |
| id | mit-1721.1/157111 |
| institution | Massachusetts Institute of Technology |
| last_indexed | 2025-02-19T04:22:51Z |
| publishDate | 2024 |
| publisher | Massachusetts Institute of Technology |
| record_format | dspace |
| spelling | mit-1721.1/1571112024-10-03T03:27:30Z Optical Properties of Colloidal II-VI and III-V Semiconductor Nanocrystals: Single Nanocrystal Photon Correlation Spectroscopy Berkinsky, David Bawendi, Moungi G. Massachusetts Institute of Technology. Department of Chemistry Colloidal nanocrystals (NCs), also known as quantum dots, are nanometer-sized semiconductor crystalline structures comprised of thousands to tens of thousands of atoms placing them in a world between the molecular-sized and the bulk-sized world, allowing them to harness unique qualities from both. Colloidal NCs are used in many applications including light-emitting diodes (LEDs), photovoltaics (solar cells), lasers, transistors, photocatalysis, and many more. In this thesis, I investigate the optical properties of colloidal NCs, specifically InP/ZnSe/ZnS, CdSe/CdS/ZnS, and ZnSe/ZnS NCs using a combination of ensemble and single NC photon correlation spectroscopic techniques. In the first chapter, I introduce the photophysical properties of colloidal NCs and spectroscopic techniques relevant to my studies. In the second chapter, I determine the dominant photoluminescent line shape broadening mechanisms in single InP/ZnSe/ZnS and CdSe/CdS/ZnS NCs using temperature dependent photoluminescent spectroscopic techniques. In the third chapter, I investigate the coherent emissive properties of single InP/ZnSe/ZnS and CdSe/CdS/ZnS at cryogenic temperatures, demonstrating the longest coherence time measured in a colloidal NC system to date. In the fourth chapter, I develop an ensemble third-order correlation technique to elucidate the average single ZnSe/ZnS NC triexciton efficiency and dynamics. Finally, I propose future directions in the fifth chapter, including a fourth order correlation technique to resolve absolute energy information on timescales faster than CCDbase spectroscopic techniques, and an open-access photon correlation Monte Carlo toolkit with the aim of filling education gaps and provide the colloidal NC community with a database of analytical tools that will encourage a wider audience to engage with photon correlation spectroscopy. Ph.D. 2024-10-02T17:31:13Z 2024-10-02T17:31:13Z 2024-05 2024-09-23T17:37:52.485Z Thesis https://hdl.handle.net/1721.1/157111 https://orcid.org/0000-0002-7143-1073 In Copyright - Educational Use Permitted Copyright retained by author(s) https://rightsstatements.org/page/InC-EDU/1.0/ application/pdf Massachusetts Institute of Technology |
| spellingShingle | Berkinsky, David Optical Properties of Colloidal II-VI and III-V Semiconductor Nanocrystals: Single Nanocrystal Photon Correlation Spectroscopy |
| title | Optical Properties of Colloidal II-VI and III-V Semiconductor Nanocrystals: Single Nanocrystal Photon Correlation Spectroscopy |
| title_full | Optical Properties of Colloidal II-VI and III-V Semiconductor Nanocrystals: Single Nanocrystal Photon Correlation Spectroscopy |
| title_fullStr | Optical Properties of Colloidal II-VI and III-V Semiconductor Nanocrystals: Single Nanocrystal Photon Correlation Spectroscopy |
| title_full_unstemmed | Optical Properties of Colloidal II-VI and III-V Semiconductor Nanocrystals: Single Nanocrystal Photon Correlation Spectroscopy |
| title_short | Optical Properties of Colloidal II-VI and III-V Semiconductor Nanocrystals: Single Nanocrystal Photon Correlation Spectroscopy |
| title_sort | optical properties of colloidal ii vi and iii v semiconductor nanocrystals single nanocrystal photon correlation spectroscopy |
| url | https://hdl.handle.net/1721.1/157111 https://orcid.org/0000-0002-7143-1073 |
| work_keys_str_mv | AT berkinskydavid opticalpropertiesofcolloidaliiviandiiivsemiconductornanocrystalssinglenanocrystalphotoncorrelationspectroscopy |