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

Terahertz harmonic generation across the Mott insulator-metal transition

G. L. Prajapati1,*, S. Ray2, I. Ilyakov1, A. N. Ponomaryov1, A. Arshad1,3, T. V. A. G. de Oliveira1, G. Dubey4, D. S. Rana4, J.-C. Deinert1 et al.

P. Werner2 and S. Kovalev5,†

  • *Contact author: g.prajapati@hzdr.de
  • †Contact author: sergey.kovalev@tu-dortmund.de

Phys. Rev. B 113, 045118 – Published 9 January, 2026

DOI: https://doi.org/10.1103/ydjj-xxcl

Abstract

High harmonic generation (HHG) in the terahertz (THz) regime is an emerging field that has already provided new insights into fundamental low-energy processes in Dirac materials and high-TC superconductors. Here, we demonstrate THz harmonic generation across the Mott insulator-metal transition in rare-earth nickelates (RNiO3, R = rare-earth atom). The THz harmonic signal shows distinct characteristics in the three different accessible phases: the intensity of harmonics increases upon cooling in both the low-temperature antiferromagnetic (AFM) insulating and high-temperature paramagnetic (PM) metallic phases, while this trend is reversed in the intermediate PM insulating phase. Using single- and two-band Hubbard models, we find different dominant origins of the THz harmonics in different phases: strong spin-charge and orbital-charge coupling in the AFM insulating phase, intraband currents from renormalized quasiparticles with temperature-dependent scattering rate in the PM metallic phase, and the reduction of the charge carrier density due to the opening of the Mott gap in the PM insulating phase. These results and mechanisms significantly differ from those observed upon excitation in the optical regime. Our study lays the foundation for THz HHG physics in Mott and other strongly correlated systems and offers design principles for efficient THz HHG from these systems.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (75)

  1. M. Ferray, A. L'Huillier, X. F. Li, L. A. Lompre, G. Mainfray, and C. Manus, Multiple-harmonic conversion of 1064 nm radiation in rare gases, J. Phys. B: At. Mol. Opt. Phys. 21, L31 (1988).
  2. C. Lyngå, A. L'Huillier, and C.-G. Wahlström, High-order harmonic generation in molecular gases, J. Phys. B: At. Mol. Opt. Phys. 29, 3293 (1996).
  3. T. T. Luu, Z. Yin, A. Jain, T. Gaumnitz, Y. Pertot, J. Ma, and H. J. Wörner, Extreme–ultraviolet high–harmonic generation in liquids, Nat. Commun. 9, 3723 (2018).
  4. S. Ghimire and D. A. Reis, High-harmonic generation from solids, Nat. Phys. 15, 10 (2019).
  5. S. Ghimire, A. D. DiChiara, E. Sistrunk, G. Ndabashimiye, U. B. Szafruga, A. Mohammad, P. Agostini, L. F. DiMauro, and D. A. Reis, Generation and propagation of high-order harmonics in crystals, Phys. Rev. A 85, 043836 (2012).
  6. G. Vampa, C. R. McDonald, G. Orlando, D. D. Klug, P. B. Corkum, and T. Brabec, Theoretical analysis of high-harmonic generation in solids, Phys. Rev. Lett. 113, 073901 (2014).
  7. R. E. F. Silva, I. V. Blinov, A. N. Rubtsov, O. Smirnova, and M. Ivanov, High-harmonic spectroscopy of ultrafast many-body dynamics in strongly correlated systems, Nat. Photon. 12, 266 (2018).
  8. S. Imai, A. Ono, and S. Ishihara, High harmonic generation in a correlated electron system, Phys. Rev. Lett. 124, 157404 (2020).
  9. S. de Vega, J. D. Cox, F. Sols, and F. J. Garcia de Abajo, Strong-field-driven dynamics and high-harmonic generation in interacting one dimensional systems, Phys. Rev. Res. 2, 013313 (2020).
  10. C. Shao, H. Lu, X. Zhang, C. Yu, T. Tohyama, and R. Lu, High-harmonic generation approaching the quantum critical point of strongly correlated systems, Phys. Rev. Lett. 128, 047401 (2022).
  11. O. Neufeld and O. Cohen, Probing ultrafast electron correlations in high harmonic generation, Phys. Rev. Res. 2, 033037 (2020).
  12. T. Hansen, S. V. B. Jensen, and L. B. Madsen, Correlation effects in high-order harmonic generation from finite systems, Phys. Rev. A 105, 053118 (2022).
  13. S. Takayoshi, Y. Murakami, and P. Werner, High-harmonic generation in quantum spin systems, Phys. Rev. B 99, 184303 (2019).
  14. M. Lysne, Y. Murakami, M. Schüler, and P. Werner, High-harmonic generation in spin-orbit coupled systems, Phys. Rev. B 102, 081121(R) (2020).
  15. P. Werner, M. Lysne1, and Y. Murakami, High harmonic generation in altermagnets, Phys. Rev. B 110, 235101 (2024).
  16. R. Geneaux, H. J. Marroux, A. Guggenmos, D. M. Neumark, and S. R. Leone, Transient absorption spectroscopy using high harmonic generation: A review of ultrafast x-ray dynamics in molecules and solids, Philos. Trans. R. Soc. A 377, 20170463 (2019).
  17. O. Smirnova, Y. Mairesse, S. Patchkovskii, N. Dudovich, D. Villeneuve, P. Corkum, and M. Y. Ivanov, High harmonic interferometry of multi-electron dynamics in molecules, Nature (London) 460, 972 (2009).
  18. G. Vampa, T. J. Hammond, N. Thiré, B. E. Schmidt, F. Légaré, C. R. McDonald, T. Brabec, D. D. Klug, and P. B. Corkum, All-optical reconstruction of crystal band structure, Phys. Rev. Lett. 115, 193603 (2015).
  19. A. A. Lanin, E. A. Stepanov, A. B. Fedotov, and A. M. Zheltikov, Mapping the electron band structure by intraband high-harmonic generation in solids, Optica 4, 516 (2017).
  20. T. T. Luu and H. J. Wörner, Measurement of the Berry curvature of solids using high-harmonic spectroscopy, Nat. Commun. 9, 916 (2018).
  21. F. Krausz and M. Ivanov, Attosecond physics, Rev. Mod. Phys. 81, 163 (2009).
  22. P. B. Corkum and F. Krausz, Attosecond science, Nat. Phys. 3, 381 (2007).
  23. R. Matsunaga, N. Tsuji, H. Fujita, A. Sugioka, K. Makise, Y. Uzawa, H. Terai, Z. Wang, H. Aoki, and R. Shimano, Light-induced collective pseudospin precession resonating with Higgs mode in a superconductor, Science 345, 1145 (2014).
  24. B. Green, S. Kovalev, V. Asgekar, G. Geloni, U. Lehnert, T. Golz, M. Kuntzsch, C. Bauer, J. Hauser, J. Voigtlaender, et al., High-field high-repetition-rate sources for the coherent thz control of matter, Sci. Rep. 6, 22256 (2016).
  25. H. A. Hafez, S. Kovalev, J.-C. Deinert, Z. Mics, B. Green, N. Awari, M. Chen, S. Germanskiy, U. Lehnert, J. Teichert, et al., Extremely efficient terahertz high-harmonic generation in graphene by hot Dirac fermions, Nature (London) 561, 507 (2018).
  26. S. Kovalev, R. M. A. Dantas, S. Germanskiy, J.-C. Deinert, B. Green, I. Ilyakov, N. Awari, M. Chen, M. Bawatna, J. Ling, et al., Non-perturbative terahertz high-harmonic generation in the three-dimensional Dirac semimetal Cd3As2, Nat. Commun. 11, 2451 (2020).
  27. B. Cheng, N. Kanda, T. N. Ikeda, T. Matsuda, P. Xia, T. Schumann, S. Stemmer, J. Itatani, N. P. Armitage, and R. Matsunaga, Efficient terahertz harmonic generation with coherent acceleration of electrons in the Dirac semimetal Cd3As2, Phys. Rev. Lett. 124, 117402 (2020).
  28. K.-J. Tielrooij, A. Principi, D. S. Reig, A. Block, S. Varghese, S. Schreyeck, K. Brunner, G. Karczewski, I. Ilyakov, O. Ponomaryov, et al., Milliwatt terahertz harmonic generation from topological insulator metamaterials, Light Sci. Appl. 11, 315 (2022).
  29. S. Kovalev, K.-J. Tielrooij, J.-C. Deinert, I. Ilyakov, N. Awari, M. Chen, A. Ponomaryov, M. Bawatna, T. V. A. G. de Oliveira, L. M. Eng, K. A. Kuznetsov, et al., Terahertz signatures of ultrafast Dirac fermion relaxation at the surface of topological insulators, npj Quantum Mater., 6, 84 (2021).
  30. I. Ilyakov, A. Ponomaryov, D. S. Reig, C. Murphy, J. D. Mehew, T. de Oliveira, G. L. Prajapati, A. Arshad, J.-C. Deinert, M. F. Craciun, et al., Ultrafast tunable terahertz-to-visible light conversion through thermal radiation from graphene metamaterials, Nano Lett. 23, 3872 (2023).
  31. A. Arshad, H. N. Koyun, R. Salikhov, M. Gensch, I. Ilyakov, A. Ponomaryov, G. L. Prajapati, T. V. A. G. de Oliveira, K. Mavridou, J. Lindner, et al., Terahertz harmonic generation from graphite pencil drawings, Adv. Photon. Res. 4, 2300088 (2023).
  32. N. Tsuji and H. Aoki, Theory of Anderson pseudospin resonance with Higgs mode in superconductors, Phys. Rev. B 92, 064508 (2015).
  33. R. Matsunaga, N. Tsuji, K. Makise, H. Terai, H. Aoki, and R. Shimano, Polarization-resolved terahertz third-harmonic generation in a single-crystal superconductor nbn: Dominance of the Higgs mode beyond the BCS approximation, Phys. Rev. B 96, 020505(R) (2017).
  34. H. Chu, M.-J. Kim, K. Katsumi, S. Kovalev, R. D. Dawson, L. Schwarz, N. Yoshikawa, G. Kim, D. Putzky, Z. Z. Li, et al., Phase-resolved Higgs response in superconducting cuprates, Nat. Commun. 11, 1793 (2020).
  35. M. Udina, J. Fiore, T. Cea, C. Castellani, G. Seibold, and L. Benfatto, THz non-linear optical response in cuprates: Predominance of the BCS response over the Higgs mode, Faraday Discuss. 237, 168 (2022).
  36. M. Puviani, R. Haenel, and D. Manske, Quench-drive spectroscopy and high-harmonic generation in BCS superconductors, Phys. Rev. B 107, 094501 (2023).
  37. M. Mittendorff, S. Li, and T. E. Murphy, Graphene-based waveguide-integrated terahertz modulator, ACS Photonics 4, 316 (2017).
  38. I. Ilyakov, A. Brataas, T. V. A. G. de Oliveira, A. Ponomaryov, J.-C. Deinert, O. Hellwig, J. Faßbender, J. Lindner, R. Salikhov, and S. Kovalev, Efficient ultrafast field-driven spin current generation for spintronic terahertz frequency conversion, Nat. Commun. 14, 7010 (2023).
  39. T. N. Ikeda and M. Sato, High-harmonic generation by electric polarization, spin current, and magnetization, Phys. Rev. B 100, 214424 (2019).
  40. M. Yarmohammadi and M. H. Kolodrubetz, Terahertz high-harmonic generation in gapped antiferromagnetic chains, Phys. Rev. B 110, 134442 (2024).
  41. N. M. Allafi, M. H. Kolodrubetz, M. Bukov, V. Oganesyan, and M. Yarmohammadi, Spin high harmonic generation through terahertz laser-driven phonons, Phys. Rev. B 110, 064420 (2024).
  42. D. N. Basov, R. D. Averitt, D. van der Marel, M. Dressel, and K. Haule, Electrodynamics of correlated electron materials, Rev. Mod. Phys. 83, 471 (2011).
  43. C.-J. Yang, J. Li, M. Fiebig, and S. Pal, Terahertz control of many-body dynamics in quantum materials, Nat. Rev. Mater. 8, 518 (2023).
  44. Y. Murakami, M. Eckstein, and P. Werner, High-harmonic generation in Mott insulators, Phys. Rev. Lett. 121, 057405 (2018).
  45. M. Lysne, Y. Murakami, and P. Werner, Signatures of bosonic excitations in high-harmonic spectra of Mott insulators, Phys. Rev. B 101, 195139 (2020).
  46. Y. Murakami, S. Takayoshi, A. Koga, and P. Werner, High-harmonic generation in one-dimensional Mott insulators, Phys. Rev. B 103, 035110 (2021).
  47. Y. Murakami and P. Werner, Nonequilibrium steady states of electric field driven Mott insulators, Phys. Rev. B 98, 075102 (2018).
  48. Y. Murakami, K. Uchida, A. Koga, K. Tanaka, and P. Werner, Anomalous temperature dependence of high-harmonic generation in Mott insulators, Phys. Rev. Lett. 129, 157401 (2022).
  49. K. Uchida, G. Mattoni, S. Yonezawa, F. Nakamura, Y. Maeno, and K. Tanaka, High-order harmonic generation and its unconventional scaling law in the Mott-insulating Ca2RuO4, Phys. Rev. Lett. 128, 127401 (2022).
  50. M. R. Bionta, E. Haddad, A. Leblanc, V. Gruson, P. Lassonde, H. Ibrahim, J. Chaillou, N. Émond, M. R. Otto, Á. Jiménez-Galán, et al., Tracking ultrafast solid-state dynamics using high harmonic spectroscopy, Phys. Rev. Res. 3, 023250 (2021).
  51. C. Reinhoffer, S. Esser, S. Esser, E. A. Mashkovich, S. Germanskiy, P. Gegenwart, F. Anders, P. H. M. van Loosdrecht, and Z. Wang, Strong terahertz third-harmonic generation by kinetic heavy quasiparticles in CaRuO3, Phys. Rev. Lett. 132, 196501 (2024).
  52. R. Salikhov, M. Lysne, P. Werner, I. Ilyakov, M. Schüler, T. V. A. G. de Oliveira, A. Ponomaryov, A. Arshad, G. L. Prajapati, J.-C. Deinert, et al., Spin-orbit interaction driven terahertz nonlinear dynamics in transition metals, npj Spintronics 3, 3 (2025).
  53. S. Catalano, M. Gibert, J. Fowlie, J. Íñiguez, J.-M. Triscone, and J. Kreisel, Rare-earth nickelates RNiO3: Thin films and heterostructures, Rep. Prog. Phys. 81, 046501 (2018).
  54. S. Middey, J. Chakhalian, P. Mahadevan, J. W. Freeland, A. J. Millis, and D. D. Sarma, Physics of ultrathin films and heterostructures of rare-earth nickelates, Annu. Rev. Mater. Res. 46, 305 (2016).
  55. See Supplemental Material at http://link.aps.org/supplemental/10.1103/ydjj-xxcl for thin film growth, structural and electronic characterizations, THz THG experiment and numerical simulations.
  56. J. J. Peng, C. Song, M. Wang, F. Li, B. Cui, G. Y. Wang, P. Yu, and F. Pan, Manipulating the metal-to-insulator transition of NdNiO3 films by orbital polarization, Phys. Rev. B 93, 235102 (2016).
  57. M. Schüler, D. Golelez, Y. Murakami, N. Bittner, A. Herrmann, H. U. R. Strand, P. Werner, M. Eckstein, and NESSi: The non-equilibrium systems simulation package, Comput. Phys. Commun. 257, 107484 (2020).
  58. M. Kinha, G. L. Prajapati, M. Udeshi, P. Agarwal, N. B. Ram, and D. S. Rana, Ultrafast dynamical charge-lattice coupling in rare-earth nickelate thin films studied by time-resolved terahertz spectroscopy, J. Phys. D: Appl. Phys. 55, 225301 (2022).
  59. H. Yamakawa, et al., Mott transition by an impulsive dielectric breakdown, Nat. Mater. 16, 1100 (2017).
  60. G. L. Prajapati, S. Kovalev, I. Ilyakov, A. Arshad, G. Dubey, K. S. Navale, D. S. Rana, and J.-C. Deinert, Terahertz-driven ultrafast dynamics of rare-earth nickelates by controlling only the charge degree of freedom, Adv. Funct. Mater. 35, 2425867 (2025).
  61. Z. Wang, H. Park, Y. H. Lai, J. Xu, C. I. Blaga, F. Yang, P. Agostini, and L. F. DiMauro, The roles of photo-carrier doping and driving wavelength in high harmonic generation from a semiconductor, Nat. Commun. 8, 1686 (2017).
  62. 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).
  63. 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).
  64. P. Werner, H. U. R. Strand, S. Hoshino, and M. Eckstein, Ultrafast switching of composite order in A3C60, Phys. Rev. B 95, 195405 (2017).
  65. M. Schüler, M. Eckstein, and P. Werner, Truncating the memory time in nonequilibrium dynamical mean field theory calculations, Phys. Rev. B 97, 245129 (2018).
  66. C. Stahl, N. Dasari, J. Li, A. Picano, P. Werner, and M. Eckstein, Memory truncated Kadanoff-Baym equations, Phys. Rev. B 105, 115146 (2022).
  67. 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).
  68. M. Eckstein and P. Werner, Nonequilibrium dynamical mean-field calculations based on the noncrossing approximation and its generalizations, Phys. Rev. B 82, 115115 (2010).
  69. A. Hariki, M. Winder, T. Uozumi, and J. Kuneš, LDA DMFT approach to resonant inelastic x-ray scattering in correlated materials, Phys. Rev. B 101, 115130 (2020).
  70. T. Pruschke and N. Grewe, The Anderson model with finite Coulomb repulsion, Z. Phys. B 74, 439 (1989).
  71. V. E. Phanindra, P. Agarwal, and D. S. Rana, Terahertz spectroscopic evidence of non-Fermi-liquid-like behavior in structurally modulated PrNiO3 thin films, Phys. Rev. Mater. 2, 015001 (2018).
  72. G. L. Prajapati, S. Das, and D. S. Rana, Emergence of quenched disorder as a dominant control for complex phase diagram of rare-earth nickelates, J. Phys.: Condens. Matter 33, 415401 (2021).
  73. G. L. Prajapati, S. Das, R. Dagar, V. E. Phanindra, and D. S. Rana, Probing the evolution of electronic phase-coexistence in complex systems by terahertz radiation, Commun. Mater. 3, 49 (2022).
  74. G. L. Prajapati, S. Kundu, S. Das, T. Dev V. V., and D. S. Rana, Hysteresis dynamics of rare earth nickelates: Unusual scaling exponent and asymmetric spinodal decomposition, New J. Phys. 24, 103016 (2022).
  75. K. S. Kumar, G. L. Prajapati, R. Dagar, M. Vagadia, D. S. Rana, and M. Tonouchi, Terahertz electrodynamics in transition metal oxides, Adv. Opt. Mater. 8, 1900958 (2020).

Outline

Information

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation