Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Open Access

Ultrafast electronic structure engineering in 1T−TaS2: Role of doping and amplitude mode dynamics

J. Jayabalan1, Jiyu Chen2, Laura Pätzold3, Francesco Petocchi2,4, Florian K. Diekmann5, Negar Najafianpour1, Ping Zhou1, Walter Schnelle6, Gesa-R. Siemann7 et al.

Philip Hofmann7, Kai Rossnagel5,8, Tim Wehling3,9, Martin Eckstein3, Philipp Werner2, and Uwe Bovensiepen1,*

  • *Contact author: uwe.bovensiepen@uni-due.de

Phys. Rev. B 113, 245107 – Published 1 June, 2026

DOI: https://doi.org/10.1103/yc4p-y1xg

Abstract

In strongly correlated transition metal dichalcogenides, an intricate interplay of polaronic distortions, stacking arrangement, and electronic correlations determines the nature of the insulating state. Transient changes in pristine and Mo-doped 1T−TaS2 are measured by femtosecond time-resolved photoelectron spectroscopy and modeled using nonequilibrium dynamical mean-field theory complemented by density functional theory. Inspired by vibrational spectroscopy we analyze real-time oscillatory spectral changes induced by the charge density wave amplitude mode through modulations of electronic interactions. We distinguish effects induced by electron doping and structural disorder which can modify the layer stacking and conclude that doped crystals might feature an enhanced fraction of monolayers. Our work establishes substitutional doping as a pathway to engineer the dynamic electronic structure in correlated transition metal dichalcogenides.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (48)

  1. H. Yang, S. Kim, M. Chhowalla, and Y. H. Lee, Structural and quantum-state phase transitions in van der Waals layered materials, Nat. Phys. 13, 931 (2017).
  2. B. Sipos, A. F. Kusmartseva, A. Akrap, H. Berger, L. Forró, and E. Tutiš, From Mott state to superconductivity in 1T−TaS2, Nat. Mater. 7, 960 (2008).
  3. C. Giannetti, M. Capone, D. Fausti, M. Fabrizio, F. Parmigiani, and D. Mihailovic, Ultrafast optical spectroscopy of strongly correlated materials and high-temperature superconductors: A non-equilibrium approach, Adv. Phys. 65, 58 (2016).
  4. A. de la Torre, D. M. Kennes, M. Claassen, S. Gerber, J. W. McIver, and M. A. Sentef, Colloquium: Nonthermal pathways to ultrafast control in quantum materials, Rev. Mod. Phys. 93, 041002 (2021).
  5. N. Hua, F. Petocchi, H. G. Bell, G. Aeppli, P. Werner, and S. Gerber, Interlayer stacking controls the electronic properties of the van der Waals material 1T−TaS2, Phys. Rev. Res. 8, L012047 (2026).
  6. P. Fazekas and E. Tosatti, Electrical, structural and magnetic properties of pure and doped 1T−TaS2, Philos. Mag. B 39, 229 (1979).
  7. L. Perfetti, P. A. Loukakos, M. Lisowski, U. Bovensiepen, H. Berger, S. Biermann, P. S. Cornaglia, A. Georges, and M. Wolf, Time evolution of the electronic structure of 1T−TaS2 through the insulator-metal transition, Phys. Rev. Lett. 97, 067402 (2006).
  8. T. Ritschel, J. Trinckauf, K. Koepernik, B. Büchner, M. v. Zimmermann, H. Berger, Y. I. Joe, P. Abbamonte, and J. Geck, Orbital textures and charge density waves in transition metal dichalcogenides, Nat. Phys. 11, 328 (2015).
  9. T. Ritschel, H. Berger, and J. Geck, Stacking-driven gap formation in layered 1T−TaS2, Phys. Rev. B 98, 195134 (2018).
  10. S.-H. Lee, J. S. Goh, and D. Cho, Origin of the insulating phase and first-order metal-insulator transition in 1T−TaS2, Phys. Rev. Lett. 122, 106404 (2019).
  11. Y. D. Wang, W. L. Yao, Z. M. Xin, T. T. Han, Z. G. Wang, L. Chen, C. Cai, Y. Li, and Y. Zhang, Band insulator to Mott insulator transition in 1T−TaS2, Nat. Commun. 11, 4215 (2020).
  12. J. Dong, W. Qi, D. Shin, L. Cario, Z. Chen, R. Grasset, D. Boschetto, M. Weis, P. Lample, E. Pastor, T. Ritschel, M. Marsi, A. Taleb, N. Park, A. Rubio, E. Papalazarou, and L. Perfetti, Dynamics of electronic states in the insulating intermediate surface phase of 1T−TaS2, Phys. Rev. B 108, 155145 (2023).
  13. J. Jung, K.-H. Jin, J. Kim, and H. W. Yeom, Control over a wide phase diagram of 2D correlated electrons by surface doping; K/1T−TaS2, Nano Lett. 23, 8029 (2023).
  14. C. J. Butler, M. Yoshida, T. Hanaguri, and Y. Iwasa, Mottness versus unit-cell doubling as the driver of the insulating state in 1T−TaS2, Nat. Commun. 11, 2477 (2020).
  15. Y. Liu, R. Ang, W. J. Lu, W. H. Song, L. J. Li, and Y. P. Sun, Superconductivity induced by Se-doping in the layered charge-density-wave system 1T−TaS2−xSex, Appl. Phys. Lett. 102, 192602 (2013).
  16. S. Qiao, X. Li, N. Wang, W. Ruan, C. Ye, P. Cai, Z. Hao, H. Yao, X. Chen, J. Wu, Y. Wang, and Z. Liu, Mottness collapse in 1T−TaS2−xSex transition-metal dichalcogenide: An interplay between localized and itinerant orbitals, Phys. Rev. X 7, 041054 (2017).
  17. W. Zhang, J. Gao, L. Cheng, K. Bu, Z. Wu, Y. Fei, Y. Zheng, L. Wang, F. Li, X. Luo, Z. Liu, Y. Sun, and Y. Yin, Visualizing the evolution from Mott insulator to Anderson insulator in Ti-doped 1T−TaS2, npj Quantum Mater. 7, 8 (2023).
  18. J. Demsar, L. Forró, H. Berger, and D. Mihailovic, Femtosecond snapshots of gap-forming charge-density-wave correlations in quasi-two-dimensional dichalcogenides 1T−TaS2 and 2H−TaSe2, Phys. Rev. B 66, 041101(R) (2002).
  19. M. Eichberger, H. Schäfer, M. Krumova, M. Beyer, J. Demsar, H. Berger, G. Moriena, G. Sciaini, and R. J. D. Miller, Snapshots of cooperative atomic motions in the optical suppression of charge density waves, Nature (London) 468, 799 (2010).
  20. N. Dean, J. C. Petersen, D. Fausti, R. I. Tobey, S. Kaiser, L. V. Gasparov, H. Berger, and A. Cavalleri, Polaronic conductivity in the photoinduced phase of 1T−TaS2, Phys. Rev. Lett. 106, 016401 (2011).
  21. J. C. Petersen, S. Kaiser, N. Dean, A. Simoncig, H. Y. Liu, A. L. Cavalieri, C. Cacho, I. C. E. Turcu, E. Springate, F. Frassetto, L. Poletto, S. S. Dhesi, H. Berger, and A. Cavalleri, Clocking the melting transition of charge and lattice order in 1T−TaS2 with ultrafast extreme-ultraviolet angle-resolved photoemission spectroscopy, Phys. Rev. Lett. 107, 177402 (2011).
  22. S. Hellmann, T. Rohwer, M. Kalläne, K. Hanff, C. Sohrt, A. Stange, A. Carr, M. M. Murnane, H. C. Kapteyn, L. Kipp, M. Bauer, and K. Rossnagel, Time-domain classification of charge-density-wave insulators, Nat. Commun. 3, 1069 (2012).
  23. C. J. Butler, M. Yoshida, T. Hanaguri, and Y. Iwasa, Doublonlike excitations and their phononic coupling in a Mott charge-density-wave system, Phys. Rev. X 11, 011059 (2021).
  24. J. Maklar, J. Sarkar, S. Dong, Y. A. Gerasimenko, T. Pincelli, S. Beaulieu, P. S. Kirchmann, J. A. Sobota, S. Yang, D. Leuenberger, R. G. Moore, Z.-X. Shen, M. Wolf, D. Mihailovic, R. Ernstorfer, and L. Rettig, Coherent light control of a metastable hidden state, Sci. Adv. 9, eadi4661 (2023).
  25. J. Zhang, C. Lian, M. Guan, W. Ma, H. Fu, H. Guo, and S. Meng, Photoexcitation induced quantum dynamics of charge density wave and emergence of a collective mode in 1T−TaS2, Nano Lett. 19, 6027 (2019).
  26. T. N. Ikeda, H. Tsunetsugu, and K. Yonemitsu, Photoinduced dynamics of commensurate charge density wave in 1T−TaS2 based on three-orbital Hubbard model, Appl. Sci. 9, 70 (2019).
  27. Q. Ren, T. Suzuki, T. Kanai, J. Itatani, S. Shin, and K. Okazaki, Phase-resolved frequency-domain analysis of the photoemission spectra for photoexcited 1T−TaS2 in the Mott insulating charge density wave state, Appl. Phys. Lett. 122, 221902 (2023).
  28. I. Avigo, P. Zhou, M. Kalläne, K. Rossnagel, U. Bovensiepen, and M. Ligges, Excitation and relaxation dynamics of the photo-perturbed correlated electron system 1T−TaS2, Appl. Sci. 9, 44 (2018).
  29. See Supplemental Material at http://link.aps.org/supplemental/10.1103/yc4p-y1xg for complementary experimental and theoretical data.
  30. A. J. H. Jones, P. Majchrzak, K. Volckaert, D. Biswas, J. Vad Andersen, S. V. Hoffmann, N. C. Jones, Z. Jiang, Y. P. Chen, M. L. Jensen, R. Ø. Stenshøj, M. Bianchi, P. Hofmann, S. Ulstrup, and J. A. Miwa, A spatial- and angle-resolved photoemission spectroscopy beamline based on capillary optics at ASTRID2, Rev. Sci. Instrum. 96, 025109 (2025).
  31. M. Ligges, I. Avigo, D. Golež, H. U. R. Strand, Y. Beyazit, K. Hanff, F. Diekmann, L. Stojchevska, M. Kalläne, P. Zhou, K. Rossnagel, M. Eckstein, P. Werner, and U. Bovensiepen, Ultrafast doublon dynamics in photoexcited 1T−TaS2, Phys. Rev. Lett. 120, 166401 (2018).
  32. I. Avigo, R. Cortés, L. Rettig, S. Thirupathaiah, H. S. Jeevan, P. Gegenwart, T. Wolf, M. Ligges, M. Wolf, J. Fink, and U. Bovensiepen, Coherent excitations and electron–phonon coupling in Ba/EuFe2As2 compounds investigated by femtosecond time- and angle-resolved photoemission spectroscopy, J. Phys.: Condens. Matter 25, 094003 (2013).
  33. M. Sandhofer, I. Sklyadneva, V. Sharma, V. M. Trontl, P. Zhou, M. Ligges, R. Heid, K.-P. Bohnen, E. Chulkov, and U. Bovensiepen, Unoccupied electronic structure and relaxation dynamics of Pb/Si(111), J. Electron Spectrosc. Relat. Phenom. 195, 278 (2014).
  34. A. Zong, X. Shen, A. Kogar, L. Ye, C. Marks, D. Chowdhury, T. Rohwer, B. Freelon, S. Weathersby, R. Li, J. Yang, J. Checkelsky, X. Wang, and N. Gedik, Ultrafast manipulation of mirror domain walls in a charge density wave, Sci. Adv. 4, eaau5501 (2018).
  35. P. Giannozzi et al., QUANTUM ESPRESSO: A modular and open-source software project for quantum simulations of materials, J. Phys.: Condens. Matter 21, 395502 (2009).
  36. J. P. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77, 3865 (1996).
  37. C. Hartwigsen, S. Goedecker, and J. Hutter, Relativistic separable dual-space Gaussian pseudopotentials from H to Rn, Phys. Rev. B 58, 3641 (1998).
  38. F. Petocchi, C. W. Nicholson, B. Salzmann, D. Pasquier, O. V. Yazyev, C. Monney, and P. Werner, Mott versus hybridization gap in the low-temperature phase of 1T−TaS2, Phys. Rev. Lett. 129, 016402 (2022).
  39. F. Petocchi, J. Chen, J. Li, M. Eckstein, and P. Werner, Photoinduced charge dynamics in 1T−TaS2, Phys. Rev. B 107, 165102 (2023).
  40. H. Aoki, N. Tsuji, M. Eckstein, M. Kollar, T. Oka, and P. Werner, Nonequilibrium dynamical mean-field theory and its applications, Rev. Mod. Phys. 86, 779 (2014).
  41. H. Keiter and J. C. Kimball, Diagrammatic perturbation technique for the Anderson Hamiltonian and relation to the s-d exchange Hamiltonian, Int. J. Magn. 1, 233 (1971).
  42. M. Eckstein and P. Werner, Nonequilibrium dynamical mean-field calculations based on the noncrossing approximation and its generalizations, Phys. Rev. B 82, 115115 (2010).
  43. A. Georges, G. Kotliar, W. Krauth, and M. J. Rozenberg, Dynamical mean-field theory of strongly correlated fermion systems and the limit of infinite dimensions, Rev. Mod. Phys. 68, 13 (1996).
  44. P. Werner, Hugo U. R. Strand, S. Hoshino, and M. Eckstein, Ultrafast switching of composite order in A3C60, Phys. Rev. B 95, 195405 (2017).
  45. J. Chen, F. Petocchi, V. Christiansson, and P. Werner, Nature of the photoinduced metallic state in monoclinic VO2, Phys. Rev. B 109, L201101 (2024).
  46. J. Chen, F. Petocchi, V. Christiansson, and P. Werner, Photoinduced insulator-metal transition in paramagnetic (V1−xCrx)2O3, Phys. Rev. B 110, 045117 (2024).
  47. A. I. Lichtenstein and M. I. Katsnelson, Antiferromagnetism and d-wave superconductivity in cuprates: A cluster dynamical mean-field theory, Phys. Rev. B 62, R9283 (2000).
  48. Note that in metallic Fe-122 an energy-dependent response similar to the one reported here for x>0 has been observed in trARPES experiments [32].

Outline

Information

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation