{"title":"通过有效优化纠缠光操纵分子的双光子吸收","authors":"Sajal Kumar Giri, George C. Schatz","doi":"arxiv-2409.11368","DOIUrl":null,"url":null,"abstract":"We report how the unique temporal and spectral features of pulsed entangled\nphotons from a parametric downconversion source can be utilized for\nmanipulating electronic excitations through the optimization of their spectral\nphase. A new comprehensive optimization protocol based on Bayesian optimization\nhas been developed in this work to selectively excite electronic states\naccessible by two-photon absorption. Using our optimization method, the\nentangled two-photon absorption probability for a thiophene dendrimer can be\nenhanced by up to a factor of 20 while classical light turns out to be\nnonoptimizable. Moreover, the optimization involving photon entanglement\nenables selective excitation that would not be possible otherwise. In addition\nto optimization, we have explored entangled two-photon absorption in the small\nentanglement time limit showing that entangled light can excite molecular\nelectronic states that are vanishingly small for classical light. We\ndemonstrate these opportunities with an application to a thiophene dendrimer.","PeriodicalId":501226,"journal":{"name":"arXiv - PHYS - Quantum Physics","volume":null,"pages":null},"PeriodicalIF":0.0000,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Manipulating Two-Photon Absorption of Molecules through Efficient Optimization of Entangled Light\",\"authors\":\"Sajal Kumar Giri, George C. Schatz\",\"doi\":\"arxiv-2409.11368\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"We report how the unique temporal and spectral features of pulsed entangled\\nphotons from a parametric downconversion source can be utilized for\\nmanipulating electronic excitations through the optimization of their spectral\\nphase. A new comprehensive optimization protocol based on Bayesian optimization\\nhas been developed in this work to selectively excite electronic states\\naccessible by two-photon absorption. Using our optimization method, the\\nentangled two-photon absorption probability for a thiophene dendrimer can be\\nenhanced by up to a factor of 20 while classical light turns out to be\\nnonoptimizable. Moreover, the optimization involving photon entanglement\\nenables selective excitation that would not be possible otherwise. In addition\\nto optimization, we have explored entangled two-photon absorption in the small\\nentanglement time limit showing that entangled light can excite molecular\\nelectronic states that are vanishingly small for classical light. We\\ndemonstrate these opportunities with an application to a thiophene dendrimer.\",\"PeriodicalId\":501226,\"journal\":{\"name\":\"arXiv - PHYS - Quantum Physics\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2024-09-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"arXiv - PHYS - Quantum Physics\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/arxiv-2409.11368\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"arXiv - PHYS - Quantum Physics","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/arxiv-2409.11368","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Manipulating Two-Photon Absorption of Molecules through Efficient Optimization of Entangled Light
We report how the unique temporal and spectral features of pulsed entangled
photons from a parametric downconversion source can be utilized for
manipulating electronic excitations through the optimization of their spectral
phase. A new comprehensive optimization protocol based on Bayesian optimization
has been developed in this work to selectively excite electronic states
accessible by two-photon absorption. Using our optimization method, the
entangled two-photon absorption probability for a thiophene dendrimer can be
enhanced by up to a factor of 20 while classical light turns out to be
nonoptimizable. Moreover, the optimization involving photon entanglement
enables selective excitation that would not be possible otherwise. In addition
to optimization, we have explored entangled two-photon absorption in the small
entanglement time limit showing that entangled light can excite molecular
electronic states that are vanishingly small for classical light. We
demonstrate these opportunities with an application to a thiophene dendrimer.