Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Article
  • Published:

Multiple mobile excitons manifested as sidebands in quasi-one-dimensional metallic TaSe3

Nature Materials volume 21, pages 423–429 (2022)Cite this article

Subjects

Abstract

Charge neutrality and their expected itinerant nature makes excitons potential transmitters of information. However, exciton mobility remains inaccessible to traditional optical experiments that only create and detect excitons with negligible momentum. Here, using angle-resolved photoemission spectroscopy, we detect dispersing excitons in the quasi-one-dimensional metallic trichalcogenide, TaSe3. The low density of conduction electrons and the low dimensionality in TaSe3 combined with a polaronic renormalization of the conduction band and the poorly screened interaction between these polarons and photo-induced valence holes leads to various excitonic bound states that we interpret as intrachain and interchain excitons, and possibly trions. The thresholds for the formation of a photo-hole together with an exciton appear as side valence bands with dispersions nearly parallel to the main valence band, but shifted to lower excitation energies. The energy separation between side and main valence bands can be controlled by surface doping, enabling the tuning of certain exciton properties.

This is a preview of subscription content, access via your institution

Access options

Buy this article

  • Purchase on Springer Link
  • Instant access to full article PDF
Buy now

Prices may be subject to local taxes which are calculated during checkout

Fig. 1: The crystalline and electronic structures of TaSe3 at 15 K.
Fig. 2: SVBs and polarons in pristine sample.
Fig. 3: Dependence on potassium doping of the electronic structure of TaSe3.
Fig. 4: Schematic of how mobile excitons show up in the form of SVBs in photoemission.

Similar content being viewed by others

Data availability

The data that support the findings of this study are available in the MARVEL public repository (MARVEL Materials Cloud Archive: https://archive.materialscloud.org) with the same title as this paper.

References

  1. Nagaosa, N. Quantum Field Theory in Strongly Correlated Electronic Systems. Theoretical and Mathematical Physics (Springer, 1999).

  2. Giamarchi, T. Quantum Physics in One Dimension (Clarendon Press, 2004).

  3. Frenkel, J. On the transformation of light into heat in solids. I. Phys. Rev. 37, 17–44 (1931).

    Article  CAS  Google Scholar 

  4. Wannier, G. H. The structure of electronic excitation levels in insulating crystals. Phys. Rev. 52, 191–197 (1937).

    Article  CAS  Google Scholar 

  5. Kasha, M. Relation between exciton bands and conduction bands in molecular lamellar systems. Rev. Mod. Phys. 31, 162–169 (1959).

    Article  CAS  Google Scholar 

  6. Knox, R. S. Introduction to Exciton Physics 183–245 (Springer, 1983).

  7. Combescot, M. & Shiau, S. Excitons and Cooper Pairs: Two Composite Bosons in Many-Body Physics (Oxford Univ. Press, 2016).

  8. Wang, G. et al. Colloquium: excitons in atomically thin transition metal dichalcogenides. Rev. Mod. Phys. 90, 021001 (2018).

    Article  CAS  Google Scholar 

  9. Hong, J., Senga, R., Pichler, T. & Suenaga, K. Probing exciton dispersions of freestanding monolayer WSe2 by momentum-resolved electron energy-loss spectroscopy. Phys. Rev. Lett. 124, 087401 (2020).

    Article  CAS  Google Scholar 

  10. Seki, K. Excitonic Bose–Einstein condensation in Ta2NiSe5 above room temperature. Phys. Rev. B. 90, 155116 (2014).

    Article  Google Scholar 

  11. Sugawara, K. et al. Unconventional charge-density-wave transition in monolayer 1T-TiSe2. ACS Nano 10, 1341–1345 (2016).

    Article  CAS  Google Scholar 

  12. Srivastava, S. K. & Avasthi, B. N. Preparation, structure and properties of transition metal trichalcogenides. J. Mater. Sci. 27, 3693 (1992).

    Article  CAS  Google Scholar 

  13. Island, J. O. et al. Electronics and optoelectronics of quasi-1d layered transition metal trichalcogenides. 2D Materials 4, 022003 (2017).

    Article  Google Scholar 

  14. Sambongi, T. Superconductivity in one-dimensional TaSe3. J. Phys. Soc. Jpn 42, 1421–1422 (1977).

    Article  CAS  Google Scholar 

  15. Tsutsumi, K. Direct electron-diffraction evidence of charge-density-wave formation in NbSe3. Phys. Rev. Lett. 39, 1675–1676 (1977).

    Article  CAS  Google Scholar 

  16. Yamamoto, M. Superconducting properties of TaSe3. J. Phys. Soc. Jpn 45, 431–438 (1978).

    Article  CAS  Google Scholar 

  17. Haen, P., Lapierre, F., Monceau, P., Regueiro, M. N. & Richard, J. Low temperature phase transition in the chain-like compounds NbSe3 and TaSe3. Solid State Commun. 26, 725–730 (1978).

    Article  CAS  Google Scholar 

  18. Ekino, T. & Akimitsu, J. Electron tunneling study of NbSe3. Japn. J. Appl. Phys. 26, 625 (1987).

    Article  CAS  Google Scholar 

  19. Cava, R. J., Fleming, R. M., Dunn, R. G. & Rietman, E. A. Low-frequency dielectric response of the charge-density wave in orthorhombic TaSe3. Phys. Rev. B. 31, 8325–8328 (1985).

    Article  CAS  Google Scholar 

  20. Nagata, S., Kutsuzawa, H., Ebisu, S., Yamamura, H. & Taniguchi, S. Superconductivity in the quasi-one-dimensional conductor TaSe3. J. Phys. Chem. Solids 50, 703–707 (1989).

    Article  CAS  Google Scholar 

  21. Nomura, A. et al. Emergence of a resistance anomaly by cu-doping in TaSe3. Europhys. Lett. 119, 17005 (2017).

    Article  Google Scholar 

  22. Nomura, A., Yamaya, K., Takayanagi, S., Ichimura, K. & Tanda, S. Effect of Cu doping on superconductivity in TaSe3: relationship between superconductivity and induced charge density wave. Europhys. Lett. 124, 67001 (2019).

    Article  Google Scholar 

  23. Yang, J. Observation of charge density wave transition in TaSe3 mesowires. Appl. Phys. Lett. 115, 033102 (2019).

    Article  Google Scholar 

  24. Nie, S. et al. Topological phases in the TaSe3 compound. Phys. Rev. B. 98, 125143 (2018).

    Article  CAS  Google Scholar 

  25. Chen, C. et al. Observation of topological electronic structure in quasi-1D superconductor TaSe3. Matter 3, 2055–2065 (2020).

    Article  Google Scholar 

  26. Lin, C. et al. Visualization of the strain-induced topological phase transition in a quasi-one-dimensional superconductor TaSe3. Nat. Mater. 20, 1093–1099 (2021).

    Article  CAS  Google Scholar 

  27. Lampert, M. A. Mobile and immobile effective-mass-particle complexes in nonmetallic solids. Phys. Rev. Lett. 1, 450–453 (1958).

    Article  CAS  Google Scholar 

  28. Kheng, K. et al. Observation of negatively charged excitons x- in semiconductor quantum wells. Phys. Rev. Lett. 71, 1752–1755 (1993).

    Article  CAS  Google Scholar 

  29. Matsunaga, R., Matsuda, K. & Kanemitsu, Y. Observation of charged excitons in hole-doped carbon nanotubes using photoluminescence and absorption spectroscopy. Phys. Rev. Lett. 106, 037404 (2011).

    Article  Google Scholar 

  30. Efimkin, D. K. & MacDonald, A. H. Many-body theory of trion absorption features in two-dimensional semiconductors. Phys. Rev. B. 95, 035417 (2017).

    Article  Google Scholar 

  31. Rivera, P. et al. Observation of long-lived interlayer excitons in monolayer MoSe2-WSe2 heterostructures. Nat. Commun. 6, 6242 (2015).

    Article  CAS  Google Scholar 

  32. Wilson, N. R. Determination of band offsets, hybridization, and exciton binding in 2D semiconductor heterostructures. Sci. Adv. 3, e1601832 (2017).

    Article  Google Scholar 

Download references

Acknowledgements

We acknowledge E. Rienks, H. Li, Y. Hu and V. Strokov for help during the ARPES experiments. We thank D. van der Marel for discussions. M.S., J.Z.M. and J.J. were supported by the Sino-Swiss Science and Technology Cooperation (grant no. IZLCZ2-170075). M.S. was supported by the Swiss National Science Foundation under grant no. 200021_188413. M.S., O.V.Y. and D.G.-M. were supported by the NCCR MARVEL funded by the Swiss National Science Foundation. M.R. and J.Z.M. were supported by the Swiss National Science Foundation under grant no. 200021_182695. M.M. was supported by the Swiss National Science Foundation under grant no. 200021_166271. M.N. and N.K. have received funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement no. 701647; and M.N. has received funding from the Swiss National Science Foundation under grant no. 200021_159678. J.Z.M. was supported by City University of Hong Kong through the start-up project (project no. 9610489), the National Natural Science Foundation of China (12104379) and Shenzhen Research Institute, City University of Hong Kong. M.A.S. is supported by Deutsche Forschungsgemeinschaft through the Emmy-Noether programme (SE 2558/2). J.L.Z. was supported by Excellence Program of Hefei Science Center CAS 2021HSC-UE011. W.W.X. was supported by Beckman Young Investigator Programme funded by Arnold and Mabel Beckman Foundation and US NSF DMR-1944965. X.G. was supported by the US Department of Energy Division of Basic Energy Sciences (DG-FG02-98ER45706).

Author information

Authors and Affiliations

  1. Department of Physics, City University of Hong Kong, Kowloon, Hong Kong, China

    Junzhang Ma

  2. Photon Science Division, Paul Scherrer Institute, Villigen, Switzerland

    Junzhang Ma, Muntaser Naamneh, Jasmin Jandke, Nicholas Clark Plumb, Milan Radovic & Ming Shi

  3. City University of Hong Kong Shenzhen Research Institute, Shenzhen, China

    Junzhang Ma

  4. Department of Materials Science and Engineering, Stanford University, Stanford, CA, USA

    Simin Nie

  5. Department of Chemistry, Princeton University, Princeton, NJ, USA

    Xin Gui

  6. Anhui Province Key Laboratory of Condensed Matter Physics at Extreme Conditions, High Magnetic Field Laboratory, HFIPS, Chinese Academy of Sciences, Hefei, China

    Chuanying Xi, Jinglei Zhang & Yimin Xiong

  7. Key Laboratory of Polar Materials and Devices, School of Physics and Electronic Science, East China Normal University, Shanghai, China

    Tian Shang

  8. Department of Quantum Matter Physics, University of Geneva, Geneva, Switzerland

    Itzik Kapon

  9. Paul Scherrer Institute, Villigen, Switzerland

    Neeraj Kumar & Yona Soh

  10. Institute of Physics, École Polytechnique Fédérale de Lausanne (EPFL), Lausanne, Switzerland

    Daniel Gosálbez-Martínez, Oleg V. Yazyev & Christopher Mudry

  11. Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences, Beijing, China

    Wenhui Fan & Zhijun Wang

  12. University of Chinese Academy of Sciences, Beijing, China

    Wenhui Fan & Zhijun Wang

  13. Max Planck Institute for the Structure and Dynamics of Matter, Hamburg, Germany

    Hannes Hübener, Umberto De Giovannini & Michael Andreas Sentef

  14. Department of Chemistry and Chemical Biology, Rutgers University, Piscataway, NJ, USA

    Weiwei Xie

  15. Condensed Matter Theory Group, Paul Scherrer Institute, Villigen, Switzerland

    Christopher Mudry & Markus Müller

Authors
  1. Junzhang Ma
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Simin Nie
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Xin Gui
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Muntaser Naamneh
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Jasmin Jandke
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Chuanying Xi
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Jinglei Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Tian Shang
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Yimin Xiong
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. Itzik Kapon
    View author publications

    You can also search for this author in PubMed Google Scholar

  11. Neeraj Kumar
    View author publications

    You can also search for this author in PubMed Google Scholar

  12. Yona Soh
    View author publications

    You can also search for this author in PubMed Google Scholar

  13. Daniel Gosálbez-Martínez
    View author publications

    You can also search for this author in PubMed Google Scholar

  14. Oleg V. Yazyev
    View author publications

    You can also search for this author in PubMed Google Scholar

  15. Wenhui Fan
    View author publications

    You can also search for this author in PubMed Google Scholar

  16. Hannes Hübener
    View author publications

    You can also search for this author in PubMed Google Scholar

  17. Umberto De Giovannini
    View author publications

    You can also search for this author in PubMed Google Scholar

  18. Nicholas Clark Plumb
    View author publications

    You can also search for this author in PubMed Google Scholar

  19. Milan Radovic
    View author publications

    You can also search for this author in PubMed Google Scholar

  20. Michael Andreas Sentef
    View author publications

    You can also search for this author in PubMed Google Scholar

  21. Weiwei Xie
    View author publications

    You can also search for this author in PubMed Google Scholar

  22. Zhijun Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  23. Christopher Mudry
    View author publications

    You can also search for this author in PubMed Google Scholar

  24. Markus Müller
    View author publications

    You can also search for this author in PubMed Google Scholar

  25. Ming Shi
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

J.Z.M. performed ARPES experiments with the help of M.N., J.J., N.C.P., M.R. and W.H.F. S.M.N. and Z.W. performed first-principles calculations of the band structure. J.Z.M. plotted all the figures. X.G. and W.W.X. synthesized the single crystals. C.Y.X. performed primary high magnetic field quantum oscillation measurements with the help of J.Z.M., J.L.Z., T.S. and Y.M.X. H.H. and U.D.G. analysed the possibility of boson driven band structures with the help of D.G.-M and O.V.Y. I.K. performed Raman measurements for checking the phonon energy. N.K. and Y.S. performed primary transport measurements with PPMS. M.A.S. helped by ruling out the bosonic strong coupling scenario. C.M. and M.M. analysed different physical scenarios on the basis of bound states and worked out the theory of excitonic sidebands. All authors contributed to the discussion of this project. J.Z.M., C.M., M.M. and M.S. wrote the paper.

Corresponding authors

Correspondence to Junzhang Ma, Markus Müller or Ming Shi.

Ethics declarations

Competing interests

The authors declare no competing interests.

Peer review

Peer review information

Nature Materials thanks the anonymous reviewers for their contribution to the peer review of this work.

Additional information

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

I. Features of metallic TaSe3 that favour the observation of mobile bound states. II. Ruling out standard scenarios for replica bands. III. EDCs identifying SVBs and the polaronic QPs. IV. Doping dependence of ARPES spectra. V. Soft-X-ray ARPES spectra and bulk doping by W. VI. Mobile excitons in a 1D metal. VII. The effect of screening on a Q1D exciton problem. VIII. Doping dependence of 1D exciton characteristics. IX. Summary.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Ma, J., Nie, S., Gui, X. et al. Multiple mobile excitons manifested as sidebands in quasi-one-dimensional metallic TaSe3. Nat. Mater. 21, 423–429 (2022). https://doi.org/10.1038/s41563-022-01201-9

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41563-022-01201-9

This article is cited by

Search

Advanced search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing