Measurement-induced collective vibrational quantum coherence under spontaneous Raman scattering in a liquid
Abstract Spontaneous vibrational Raman scattering is a ubiquitous form of light–matter interaction whose description necessitates quantization of the electromagnetic field. It is usually considered as an incoherent process because the scattered field lacks any predictable phase relationship with the...
| Main Authors: | , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2023-05-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-38483-9 |
| _version_ | 1797822777824116736 |
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| author | Valeria Vento Santiago Tarrago Velez Anna Pogrebna Christophe Galland |
| author_facet | Valeria Vento Santiago Tarrago Velez Anna Pogrebna Christophe Galland |
| author_sort | Valeria Vento |
| collection | DOAJ |
| description | Abstract Spontaneous vibrational Raman scattering is a ubiquitous form of light–matter interaction whose description necessitates quantization of the electromagnetic field. It is usually considered as an incoherent process because the scattered field lacks any predictable phase relationship with the incoming field. When probing an ensemble of molecules, the question therefore arises: What quantum state should be used to describe the molecular ensemble following spontaneous Stokes scattering? We experimentally address this question by measuring time-resolved Stokes–anti-Stokes two-photon coincidences on a molecular liquid consisting of several sub-ensembles with slightly different vibrational frequencies. When spontaneously scattered Stokes photons and subsequent anti-Stokes photons are detected into a single spatiotemporal mode, the observed dynamics is inconsistent with a statistical mixture of individually excited molecules. Instead, we show that the data are reproduced if Stokes–anti-Stokes correlations are mediated by a collective vibrational quantum, i.e. a coherent superposition of all molecules interacting with light. Our results demonstrate that the degree of coherence in the vibrational state of the liquid is not an intrinsic property of the material system, but rather depends on the optical excitation and detection geometry. |
| first_indexed | 2024-03-13T10:14:10Z |
| format | Article |
| id | doaj.art-fd08a03b2d0644018e8487ca400dfdc0 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-13T10:14:10Z |
| publishDate | 2023-05-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-fd08a03b2d0644018e8487ca400dfdc02023-05-21T11:21:16ZengNature PortfolioNature Communications2041-17232023-05-011411710.1038/s41467-023-38483-9Measurement-induced collective vibrational quantum coherence under spontaneous Raman scattering in a liquidValeria Vento0Santiago Tarrago Velez1Anna Pogrebna2Christophe Galland3Institute of Physics, École polytechnique fédérale de Lausanne (EPFL)Institute of Physics, École polytechnique fédérale de Lausanne (EPFL)Institute of Physics, École polytechnique fédérale de Lausanne (EPFL)Institute of Physics, École polytechnique fédérale de Lausanne (EPFL)Abstract Spontaneous vibrational Raman scattering is a ubiquitous form of light–matter interaction whose description necessitates quantization of the electromagnetic field. It is usually considered as an incoherent process because the scattered field lacks any predictable phase relationship with the incoming field. When probing an ensemble of molecules, the question therefore arises: What quantum state should be used to describe the molecular ensemble following spontaneous Stokes scattering? We experimentally address this question by measuring time-resolved Stokes–anti-Stokes two-photon coincidences on a molecular liquid consisting of several sub-ensembles with slightly different vibrational frequencies. When spontaneously scattered Stokes photons and subsequent anti-Stokes photons are detected into a single spatiotemporal mode, the observed dynamics is inconsistent with a statistical mixture of individually excited molecules. Instead, we show that the data are reproduced if Stokes–anti-Stokes correlations are mediated by a collective vibrational quantum, i.e. a coherent superposition of all molecules interacting with light. Our results demonstrate that the degree of coherence in the vibrational state of the liquid is not an intrinsic property of the material system, but rather depends on the optical excitation and detection geometry.https://doi.org/10.1038/s41467-023-38483-9 |
| spellingShingle | Valeria Vento Santiago Tarrago Velez Anna Pogrebna Christophe Galland Measurement-induced collective vibrational quantum coherence under spontaneous Raman scattering in a liquid Nature Communications |
| title | Measurement-induced collective vibrational quantum coherence under spontaneous Raman scattering in a liquid |
| title_full | Measurement-induced collective vibrational quantum coherence under spontaneous Raman scattering in a liquid |
| title_fullStr | Measurement-induced collective vibrational quantum coherence under spontaneous Raman scattering in a liquid |
| title_full_unstemmed | Measurement-induced collective vibrational quantum coherence under spontaneous Raman scattering in a liquid |
| title_short | Measurement-induced collective vibrational quantum coherence under spontaneous Raman scattering in a liquid |
| title_sort | measurement induced collective vibrational quantum coherence under spontaneous raman scattering in a liquid |
| url | https://doi.org/10.1038/s41467-023-38483-9 |
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