The spontaneous symmetry breaking in Ta2NiSe5 is structural in nature
The excitonic insulator is an electronically driven phase of matter that emerges upon the spontaneous formation and Bose condensation of excitons. Detecting this exotic order in candidate materials is a subject of paramount importance, as the size of the excitonic gap in the band structure establish...
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Published in | Proceedings of the National Academy of Sciences - PNAS Vol. 120; no. 17; p. e2221688120 |
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Main Authors | , , , , , , , , , , , , , , , , , , , |
Format | Journal Article |
Language | English |
Published |
Washington
National Academy of Sciences
25.04.2023
|
Subjects | |
Online Access | Get full text |
ISSN | 0027-8424 1091-6490 1091-6490 |
DOI | 10.1073/pnas.2221688120 |
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Abstract | The excitonic insulator is an electronically driven phase of matter that emerges upon the spontaneous formation and Bose condensation of excitons. Detecting this exotic order in candidate materials is a subject of paramount importance, as the size of the excitonic gap in the band structure establishes the potential of this collective state for superfluid energy transport. However, the identification of this phase in real solids is hindered by the coexistence of a structural order parameter with the same symmetry as the excitonic order. Only a few materials are currently believed to host a dominant excitonic phase, Ta2NiSe5 being the most promising. Here, we test this scenario by using an ultrashort laser pulse to quench the broken-symmetry phase of this transition metal chalcogenide. Tracking the dynamics of the material's electronic and crystal structure after light excitation reveals spectroscopic fingerprints that are compatible only with a primary order parameter of phononic nature. We rationalize our findings through state-of-the-art calculations, confirming that the structural order accounts for most of the gap opening. Our results suggest that the spontaneous symmetry breaking in Ta2NiSe5 is mostly of structural character, hampering the possibility to realize quasi-dissipationless energy transport. |
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AbstractList | In the quest for collective phases of matter that can lead to novel quantum properties, a long-sought example is the excitonic insulator—an exotic state where excitons spontaneously form in thermodynamic equilibrium and undergo Bose–Einstein condensation. In the past decades, Ta
2
NiSe
5
has been identified as the most promising candidate to host this electronically driven phase at a critical temperature of 328 K, which makes it ideal for the coherent control of an exciton condensate in ambient conditions. Here, we use nonequilibrium spectroscopy tools and first-principles calculations to show that the spontaneous symmetry breaking in Ta
2
NiSe
5
has a predominantly structural rather than electronic character. Our results establish a protocol to clarify elusive phase transitions in solids with intricate electron–phonon couplings.
The excitonic insulator is an electronically driven phase of matter that emerges upon the spontaneous formation and Bose condensation of excitons. Detecting this exotic order in candidate materials is a subject of paramount importance, as the size of the excitonic gap in the band structure establishes the potential of this collective state for superfluid energy transport. However, the identification of this phase in real solids is hindered by the coexistence of a structural order parameter with the same symmetry as the excitonic order. Only a few materials are currently believed to host a dominant excitonic phase, Ta
2
NiSe
5
being the most promising. Here, we test this scenario by using an ultrashort laser pulse to quench the broken-symmetry phase of this transition metal chalcogenide. Tracking the dynamics of the material’s electronic and crystal structure after light excitation reveals spectroscopic fingerprints that are compatible only with a primary order parameter of phononic nature. We rationalize our findings through state-of-the-art calculations, confirming that the structural order accounts for most of the gap opening. Our results suggest that the spontaneous symmetry breaking in Ta
2
NiSe
5
is mostly of structural character, hampering the possibility to realize quasi-dissipationless energy transport. The excitonic insulator is an electronically driven phase of matter that emerges upon the spontaneous formation and Bose condensation of excitons. Detecting this exotic order in candidate materials is a subject of paramount importance, as the size of the excitonic gap in the band structure establishes the potential of this collective state for superfluid energy transport. However, the identification of this phase in real solids is hindered by the coexistence of a structural order parameter with the same symmetry as the excitonic order. Only a few materials are currently believed to host a dominant excitonic phase, Ta2NiSe5 being the most promising. Here, we test this scenario by using an ultrashort laser pulse to quench the broken-symmetry phase of this transition metal chalcogenide. Tracking the dynamics of the material's electronic and crystal structure after light excitation reveals spectroscopic fingerprints that are compatible only with a primary order parameter of phononic nature. We rationalize our findings through state-of-the-art calculations, confirming that the structural order accounts for most of the gap opening. Our results suggest that the spontaneous symmetry breaking in Ta2NiSe5 is mostly of structural character, hampering the possibility to realize quasi-dissipationless energy transport.The excitonic insulator is an electronically driven phase of matter that emerges upon the spontaneous formation and Bose condensation of excitons. Detecting this exotic order in candidate materials is a subject of paramount importance, as the size of the excitonic gap in the band structure establishes the potential of this collective state for superfluid energy transport. However, the identification of this phase in real solids is hindered by the coexistence of a structural order parameter with the same symmetry as the excitonic order. Only a few materials are currently believed to host a dominant excitonic phase, Ta2NiSe5 being the most promising. Here, we test this scenario by using an ultrashort laser pulse to quench the broken-symmetry phase of this transition metal chalcogenide. Tracking the dynamics of the material's electronic and crystal structure after light excitation reveals spectroscopic fingerprints that are compatible only with a primary order parameter of phononic nature. We rationalize our findings through state-of-the-art calculations, confirming that the structural order accounts for most of the gap opening. Our results suggest that the spontaneous symmetry breaking in Ta2NiSe5 is mostly of structural character, hampering the possibility to realize quasi-dissipationless energy transport. The excitonic insulator is an electronically driven phase of matter that emerges upon the spontaneous formation and Bose condensation of excitons. Detecting this exotic order in candidate materials is a subject of paramount importance, as the size of the excitonic gap in the band structure establishes the potential of this collective state for superfluid energy transport. However, the identification of this phase in real solids is hindered by the coexistence of a structural order parameter with the same symmetry as the excitonic order. Only a few materials are currently believed to host a dominant excitonic phase, Ta2NiSe5 being the most promising. Here, we test this scenario by using an ultrashort laser pulse to quench the broken-symmetry phase of this transition metal chalcogenide. Tracking the dynamics of the material's electronic and crystal structure after light excitation reveals spectroscopic fingerprints that are compatible only with a primary order parameter of phononic nature. We rationalize our findings through state-of-the-art calculations, confirming that the structural order accounts for most of the gap opening. Our results suggest that the spontaneous symmetry breaking in Ta2NiSe5 is mostly of structural character, hampering the possibility to realize quasi-dissipationless energy transport. |
Author | Mazin, Igor I Millis, Andrew J Demler, Eugene Lee, Changmin Azoury, Doron Takayama, Tomohiro Takagi, Hidenori Zong, Alfred Kogar, Anshul Latini, Simone Windgaetter, Lukas Michael, Marios H Baldini, Edoardo Wang, Yao Gedik, Nuh Choi, Dongsung Su, Yifan Lv, Baiqing Lu, Yangfan Rubio, Angel |
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Copyright | Copyright National Academy of Sciences Apr 25, 2023 Copyright © 2023 the Author(s). Published by PNAS. 2023 |
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Snippet | The excitonic insulator is an electronically driven phase of matter that emerges upon the spontaneous formation and Bose condensation of excitons. Detecting... In the quest for collective phases of matter that can lead to novel quantum properties, a long-sought example is the excitonic insulator—an exotic state where... |
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SubjectTerms | Broken symmetry Coexistence Condensates Crystal structure Energy transfer Excitation spectra Excitons Fluids Materials selection Order parameters Physical Sciences Superfluidity Symmetry Transition metal compounds |
Title | The spontaneous symmetry breaking in Ta2NiSe5 is structural in nature |
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