Resonant vibrational-electronic coupling between photosynthetic excitons is inadequately described by reduced basis sets
Ultrafast internal conversion between excited states of photosynthetic pigments has been a subject of intense spectroscopic interest owing to its near unity quantum yield. Of particular interest is the possibility of strong non-adiabatic mixing between vibrational and electronic degrees of freedom,...
| Main Authors: | , |
|---|---|
| Andre forfattere: | |
| Format: | Conference Paper |
| Sprog: | English |
| Udgivet: |
2020
|
| Fag: | |
| Online adgang: | https://hdl.handle.net/10356/144228 |
| _version_ | 1826116262531432448 |
|---|---|
| author | Sahu, Amitav Tiwari, Vivek |
| author2 | Asian Spectroscopy Conference 2020 |
| author_facet | Asian Spectroscopy Conference 2020 Sahu, Amitav Tiwari, Vivek |
| author_sort | Sahu, Amitav |
| collection | NTU |
| description | Ultrafast internal conversion between excited states of photosynthetic pigments has been a subject of intense spectroscopic interest owing to its near unity quantum yield. Of particular interest is the possibility of strong non-adiabatic mixing between vibrational and electronic degrees of freedom, termed as vibronic mixing, caused by resonances between exciton energy gaps and dense low-frequency vibrational spectrum of photosynthetic pigments. Several reports have implicated coherent superpositions of vibronically mixed excitons to explain experimental signatures, and vibronic exciton quantum dynamical simulations have further suggested a possible functional role for quantum superpositions in enhancing the rates of energy and charge delocalization. A key question which arises in this context is -- what are the unique properties of excitons coupled through resonant vibronic coupling, and whether these properties could be well approximated in basis sets with reduced vibrational dimensionality without over-simplifying the expected excited state dynamics? The above question will be the main theme of this presentation. |
| first_indexed | 2024-10-01T04:08:28Z |
| format | Conference Paper |
| id | ntu-10356/144228 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T04:08:28Z |
| publishDate | 2020 |
| record_format | dspace |
| spelling | ntu-10356/1442282020-10-27T01:46:21Z Resonant vibrational-electronic coupling between photosynthetic excitons is inadequately described by reduced basis sets Sahu, Amitav Tiwari, Vivek Asian Spectroscopy Conference 2020 Institute of Advanced Studies Science::Chemistry Vibrational-electronic Coupling Photosynthesis Ultrafast internal conversion between excited states of photosynthetic pigments has been a subject of intense spectroscopic interest owing to its near unity quantum yield. Of particular interest is the possibility of strong non-adiabatic mixing between vibrational and electronic degrees of freedom, termed as vibronic mixing, caused by resonances between exciton energy gaps and dense low-frequency vibrational spectrum of photosynthetic pigments. Several reports have implicated coherent superpositions of vibronically mixed excitons to explain experimental signatures, and vibronic exciton quantum dynamical simulations have further suggested a possible functional role for quantum superpositions in enhancing the rates of energy and charge delocalization. A key question which arises in this context is -- what are the unique properties of excitons coupled through resonant vibronic coupling, and whether these properties could be well approximated in basis sets with reduced vibrational dimensionality without over-simplifying the expected excited state dynamics? The above question will be the main theme of this presentation. Published version 2020-10-21T06:55:36Z 2020-10-21T06:55:36Z 2020 Conference Paper Sahu, A., & Tiwaro V. (2020). Resonant vibrational-electronic coupling between photosynthetic excitons is inadequately described by reduced basis sets. Proc. Of the 7th Asian Spectroscopy Conference (ASC 2020). doi:10.32655/ASC_8-10_Dec2020.18 https://hdl.handle.net/10356/144228 10.32655/ASC_8-10_Dec2020.18 en © 2020 Nanyang Technological University. application/pdf |
| spellingShingle | Science::Chemistry Vibrational-electronic Coupling Photosynthesis Sahu, Amitav Tiwari, Vivek Resonant vibrational-electronic coupling between photosynthetic excitons is inadequately described by reduced basis sets |
| title | Resonant vibrational-electronic coupling between photosynthetic excitons is inadequately described by reduced basis sets |
| title_full | Resonant vibrational-electronic coupling between photosynthetic excitons is inadequately described by reduced basis sets |
| title_fullStr | Resonant vibrational-electronic coupling between photosynthetic excitons is inadequately described by reduced basis sets |
| title_full_unstemmed | Resonant vibrational-electronic coupling between photosynthetic excitons is inadequately described by reduced basis sets |
| title_short | Resonant vibrational-electronic coupling between photosynthetic excitons is inadequately described by reduced basis sets |
| title_sort | resonant vibrational electronic coupling between photosynthetic excitons is inadequately described by reduced basis sets |
| topic | Science::Chemistry Vibrational-electronic Coupling Photosynthesis |
| url | https://hdl.handle.net/10356/144228 |
| work_keys_str_mv | AT sahuamitav resonantvibrationalelectroniccouplingbetweenphotosyntheticexcitonsisinadequatelydescribedbyreducedbasissets AT tiwarivivek resonantvibrationalelectroniccouplingbetweenphotosyntheticexcitonsisinadequatelydescribedbyreducedbasissets |