Phase-cycling and double-quantum two-dimensional electronic spectroscopy using a common-path birefringent interferometer
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arXiv
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| Autori principali: | , , , , , , |
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| Natura: | Preprint |
| Pubblicazione: |
2024
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| author | Timmer, Daniel Lünemann, Daniel C. Gittinger, Moritz De Sio, Antonietta Manzoni, Cristian Cerullo, Giulio Lienau, Christoph |
| author_facet | Timmer, Daniel Lünemann, Daniel C. Gittinger, Moritz De Sio, Antonietta Manzoni, Cristian Cerullo, Giulio Lienau, Christoph |
| contents | Selecting distinct quantum pathways in two-dimensional electronic spectroscopy (2DES) can give particularly deep insights into coherent and incoherent interactions and quantum dynamics in various materials. This includes isolating rephasing and non-rephasing pathways for conventional single-quantum 2DES, but also the ability to record double- and zero-quantum spectra. Such advanced 2DES schemes usually require phase-cycling when performed in a partially or fully collinear geometry. A particularly simple and effective implementation of 2DES utilizes an in-line birefringent interferometer, the Translating-Wedge-based Identical pulses eNcoding System (TWINS), for the generation of an inherently phase-stable collinear excitation pulse pair. Here, we demonstrate how the TWINS can be adapted to allow for phase-cycling and experimental access to isolated quantum pathways. These new capabilities are demonstrated by recording rephasing, non-rephasing, zero-quantum and double-quantum 2DES on a molecular J-aggregate. This easy-to-implement extension opens up new experimental possibilities for TWINS-based 2DES in multidimensional all-optical and photoemission spectroscopy and microscopy. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2409_11959 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Phase-cycling and double-quantum two-dimensional electronic spectroscopy using a common-path birefringent interferometer Timmer, Daniel Lünemann, Daniel C. Gittinger, Moritz De Sio, Antonietta Manzoni, Cristian Cerullo, Giulio Lienau, Christoph Chemical Physics Mesoscale and Nanoscale Physics Selecting distinct quantum pathways in two-dimensional electronic spectroscopy (2DES) can give particularly deep insights into coherent and incoherent interactions and quantum dynamics in various materials. This includes isolating rephasing and non-rephasing pathways for conventional single-quantum 2DES, but also the ability to record double- and zero-quantum spectra. Such advanced 2DES schemes usually require phase-cycling when performed in a partially or fully collinear geometry. A particularly simple and effective implementation of 2DES utilizes an in-line birefringent interferometer, the Translating-Wedge-based Identical pulses eNcoding System (TWINS), for the generation of an inherently phase-stable collinear excitation pulse pair. Here, we demonstrate how the TWINS can be adapted to allow for phase-cycling and experimental access to isolated quantum pathways. These new capabilities are demonstrated by recording rephasing, non-rephasing, zero-quantum and double-quantum 2DES on a molecular J-aggregate. This easy-to-implement extension opens up new experimental possibilities for TWINS-based 2DES in multidimensional all-optical and photoemission spectroscopy and microscopy. |
| title | Phase-cycling and double-quantum two-dimensional electronic spectroscopy using a common-path birefringent interferometer |
| topic | Chemical Physics Mesoscale and Nanoscale Physics |
| url | https://arxiv.org/abs/2409.11959 |