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 inProceedings of the National Academy of Sciences - PNAS Vol. 120; no. 17; p. e2221688120
Main Authors Baldini, Edoardo, Zong, Alfred, Choi, Dongsung, Lee, Changmin, Michael, Marios H, Windgaetter, Lukas, Mazin, Igor I, Latini, Simone, Azoury, Doron, Lv, Baiqing, Kogar, Anshul, Su, Yifan, Wang, Yao, Lu, Yangfan, Takayama, Tomohiro, Takagi, Hidenori, Millis, Andrew J, Rubio, Angel, Demler, Eugene, Gedik, Nuh
Format Journal Article
LanguageEnglish
Published Washington National Academy of Sciences 25.04.2023
Subjects
Online AccessGet full text
ISSN0027-8424
1091-6490
1091-6490
DOI10.1073/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.
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
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Edited by Stuart Rice, University of Chicago, James Franck Institute, Chicago, IL; received December 21, 2022; accepted February 24, 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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StartPage e2221688120
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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