- Open Access
Interplay between high-harmonic generation and photoluminescence in ZnO: Anisotropic spectral properties of harmonic emission and the role of excitons
Phys. Rev. B 112, 214311 – Published 8 December, 2025
DOI: https://doi.org/10.1103/b56l-hvgn
Abstract
We investigate the nonlinear optical response of bulk ZnO under intense short-wave infrared excitation, focusing on the interplay between high-harmonic generation (HHG) and photoluminescence (PL). While HHG exhibits nonperturbative intensity scaling and a spectral blueshift consistent with plasma-induced refractive index changes, the PL signal shows a pronounced superlinear increase and a redshift, attributed to a combination of exciton-exciton scattering and phonon-assisted exciton recombination emission. A similar PL response under above-bandgap excitation supports its intrinsic origin. Spectral analysis of the HHG emission reveals an intensity-driven transition in the characteristics of the fifth harmonic, indicating a change in the underlying generation mechanism. These findings establish PL and spectral HHG analysis as complementary probes of strong-field and many-body effects in wide-bandgap semiconductors.
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References (53)
- A. H. Chin, O. G. Calderón, and J. Kono, Extreme midinfrared nonlinear optics in semiconductors, Phys. Rev. Lett. 86, 3292 (2001).
- S. Ghimire, A. D. DiChiara, E. Sistrunk, P. Agostini, L. F. DiMauro, and D. A. Reis, Observation of high-order harmonic generation in a bulk crystal, Nat. Phys. 7, 138 (2011).
- J. Li, J. Lu, A. Chew, S. Han, J. Li, Y. Wu, H. Wang, S. Ghimire, and Z. Chang, Attosecond science based on high harmonic generation from gases and solids, Nat. Commun. 11, 2748 (2020).
- M. Ossiander, K. Golyari, K. Scharl, L. Lehnert, F. Siegrist, J. Bürger, D. Zimin, J. Gessner, M. Weidman, I. Floss, V. Smejkal, S. Donsa, C. Lemell, F. Libisch, N. Karpowicz, J. Burgdörfer, F. Krausz, and M. Schultze, The speed limit of optoelectronics, Nat. Commun. 13, 1620 (2022).
- C. Heide, P. D. Keathley, and M. F. Kling, Petahertz electronics, Nat. Rev. Phys. 6, 648 (2024).
- D. Zimin, M. Weidman, J. Schötz, M. F. Kling, V. S. Yakovlev, F. Krausz, and N. Karpowicz, Petahertz-scale nonlinear photoconductive sampling in air, Optica 8, 586 (2021).
- S. Sederberg, D. Zimin, S. Keiber, F. Siegrist, M. S. Wismer, V. S. Yakovlev, I. Floss, C. Lemell, J. Burgdörfer, M. Schultze, F. Krausz, and N. Karpowicz, Attosecond optoelectronic field measurement in solids, Nat. Commun. 11, 430 (2020).
- T. T. Luu, M. Garg, S. Y. Kruchinin, A. Moulet, M. T. Hassan, and E. Goulielmakis, Extreme ultraviolet high-harmonic spectroscopy of solids, Nature (London) 521, 498 (2015).
- A. Lanin, E. Stepanov, A. Fedotov, and A. Zheltikov, Mapping the electron band structure by intraband high-harmonic generation in solids, Optica 4, 516 (2017).
- B. Zaks, R.-B. Liu, and M. S. Sherwin, Experimental observation of electron–hole recollisions, Nature (London) 483, 580 (2012).
- K. Uchida and K. Tanaka, High harmonic Mach–Zehnder interferometer for probing sub-laser-cycle electron dynamics in solids, Optica 11, 1130 (2024).
- C. Heide, Y. Kobayashi, A. C. Johnson, F. Liu, T. F. Heinz, D. A. Reis, and S. Ghimire, Probing electron-hole coherence in strongly driven 2D materials using high-harmonic generation, Optica 9, 512 (2022).
- S. Gholam-Mirzaei, J. E. Beetar, A. Chacón, and M. Chini, High-harmonic generation in ZnO driven by self-compressed mid-infrared pulses, J. Opt. Soc. Am. B 35, A27 (2018).
- R. Hollinger, P. Herrmann, V. Korolev, M. Zapf, V. Shumakova, R. Röder, I. Uschmann, A. Pugžlys, A. Baltuška, M. Zürch, C. Ronning, C. Spielmann, and D. Kartashov, Polarization dependent excitation and high harmonic generation from intense mid-IR laser pulses in ZnO, Nanomaterials 11, 4 (2020).
- S. Jiang, S. Gholam-Mirzaei, E. Crites, J. E. Beetar, M. Singh, R. Lu, M. Chini, and C. Lin, Crystal symmetry and polarization of high-order harmonics in ZnO, J. Phys. B: At. Mol. Opt. Phys. 52, 225601 (2019).
- S. Gholam-Mirzaei, J. Beetar, and M. Chini, High harmonic generation in ZnO with a high-power mid-IR OPA, Appl. Phys. Lett. 110, 061101 (2017).
- W. Li, Z. Liu, B. Shao, J. Qian, Y. Li, Y. Peng, and Y. Leng, Angle-resolved high-order harmonics in wurtzite-type ZnO, J. Appl. Phys. 132, 123102 (2022).
- 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).
- S. Xu, H. Zhang, J. Yu, Y. Han, Z. Wang, and J. Hu, Ultrafast modulation of a high harmonic generation in a bulk ZnO single crystal, Opt. Express 30, 41350 (2022).
- Z. Nie, K. Murzyn, L. Guery, T. J. van den Hooven, and P. M. Kraus, Ultrafast permittivity engineering enables broadband enhancement and spatial emission control of harmonic generation in ZnO, ACS Photonics 11, 5084 (2024).
- Y. Liu, S. Gholam-Mirzaei, J. E. Beetar, J. Nesper, A. Yousif, M. Nrisimhamurty, and M. Chini, All-optical sampling of few-cycle infrared pulses using tunneling in a solid, Photon. Res. 9, 929 (2021).
- T.-C. Truong, Y. Liu, D. Khatri, Y. Zhang, B. Shim, and M. Chini, Scanless laser waveform measurement in the near-infrared, APL Photonics 10, 016101 (2025).
- P. Juergens, S. D. Roscam Abbing, M. Mero, C. L. Garcia, G. G. Brown, M. J. Vrakking, A. Mermillod-Blondin, P. M. Kraus, and A. Husakou, Linking high-harmonic generation and strong-field ionization in bulk crystals, ACS Photonics 11, 247 (2024).
- Ü. Özgür, Y. I. Alivov, C. Liu, A. Teke, M. A. Reshchikov, S. Doğan, V. C. S. J. Avrutin, S.-J. Cho, and H. Morkoç, A comprehensive review of ZnO materials and devices, J. Appl. Phys. 98, 041301 (2005).
- J. Q. Grim, K. B. Ucer, A. Burger, P. Bhattacharya, E. Tupitsyn, E. Rowe, V. M. Buliga, L. Trefilova, A. Gektin, G. A. Bizarri, W. W. Moses, and R. T. Williams, Nonlinear quenching of densely excited states in wide-gap solids, Phys. Rev. B 87, 125117 (2013).
- S. Jessen, A. Di Giacomo, I. Moreels, B. Julsgaard, and R. M. Turtos, Nonlinear quenching of excitonic emission from nanoplatelet films at high excitation densities, Sci. Rep. 15, 23423 (2025).
- D. Grojo, S. Leyder, P. Delaporte, W. Marine, M. Sentis, and O. Utéza, Long-wavelength multiphoton ionization inside band-gap solids, Phys. Rev. B 88, 195135 (2013).
- P. S. Sneftrup, P. Juergens, V. D. Michele, J. R. Andrade, M. J. Vrakking, P. Balling, and A. Mermillod-Blondin, Probing nonlinear excitation conditions: Photoluminescence and nonlinear absorption studies in laser-irradiated dielectrics, Appl. Phys. A 130, 175 (2024).
- T. Shubina, M. Glazov, N. A. Gippius, A. Toropov, D. Lagarde, P. Disseix, J. Leymarie, B. Gil, G. Pozina, J. P. Bergman et al., Delay and distortion of slow light pulses by excitons in ZnO, Phys. Rev. B 84, 075202 (2011).
- B. K. Meyer, H. Alves, D. M. Hofmann, W. Kriegseis, D. Forster, F. Bertram, J. Christen, A. Hoffmann, M. Straßburg, M. Dworzak, U. Haboeck, and A. V. Rodina, Bound exciton and donor–acceptor pair recombinations in ZnO, Phys. Status Solidi (b) 241, 231 (2004).
- J.-C. Deinert, D. Wegkamp, M. Meyer, C. Richter, M. Wolf, and J. Stähler, Ultrafast exciton formation at the surface, Phys. Rev. Lett. 113, 057602 (2014).
- C. J. Milne, N. Nagornova, T. Pope, H.-Y. Chen, T. Rossi, J. Szlachetko, W. Gawelda, A. Britz, T. B. van Driel, L. Sala et al., Disentangling the evolution of electrons and holes in photoexcited ZnO nanoparticles, Struct. Dyn. 10, 064501 (2023).
- G. Heiland, E. Mollwo, and F. Stöckmann, Electronic Processes in Zinc Oxide (Academic Press, New York, 1959), pp. 191–323.
- Y. Benkrima, S. Benhamida, and D. Belfennache, Theoretical study of structural and optical properties of ZnO in wurtzite phase, Digest J. Nanomater. Biostruct. 18, 11 (2023).
- M. Kirm, V. Nagirnyi, E. Feldbach, M. De Grazia, B. Carré, H. Merdji, S. Guizard, G. Geoffroy, J. Gaudin, N. Fedorov, P. Martin, A. Vasil'ev, and A. Belsky, Exciton-exciton interactions in irradiated by intense femtosecond vacuum ultraviolet pulses, Phys. Rev. B 79, 233103 (2009).
- D. Spassky, A. Vasil'ev, A. Belsky, N. Fedorov, P. Martin, S. Markov, O. Buzanov, N. Kozlova, and V. Shlegel, Excitation density effects in luminescence properties of and , Opt. Mater. (Amsterdam) 90, 7 (2019).
- Y. I. Alivov, E. Kalinina, A. Cherenkov, D. C. Look, B. Ataev, A. Omaev, M. Chukichev, and D. Bagnall, Fabrication and characterization of n-ZnO/p-AlGaN heterojunction light-emitting diodes on 6H-SiC substrates, Appl. Phys. Lett. 83, 4719 (2003).
- C. F. Klingshirn, Semiconductor Optics (Springer Science & Business Media, 2012).
- Y. Chen, N. T. Tuan, Y. Segawa, H.-j. Ko, S.-k. Hong, and T. Yao, Stimulated emission and optical gain in ZnO epilayers grown by plasma-assisted molecular-beam epitaxy with buffers, Appl. Phys. Lett. 78, 1469 (2001).
- J. B. Baxter and C. A. Schmuttenmaer, Conductivity of ZnO nanowires, nanoparticles, and thin films using time-resolved terahertz spectroscopy, J. Phys. Chem. B 110, 25229 (2006).
- K. Wei, D. Hei, Q. Xu, J. Liu, Q. Guo, X. Weng, X. Tan, and L. Sheng, Photoluminescence nonlinearity and picosecond transient absorption in an LYSO:Ce scintillator excited by a 266 nm ultraviolet laser, RSC Adv. 11, 17020 (2021).
- O. Sergaeva, V. Gruzdev, D. Austin, and E. Chowdhury, Ultrafast excitation of conduction-band electrons by high-intensity ultrashort laser pulses in band-gap solids: Vinogradov equation versus Drude model, J. Opt. Soc. Am. B 35, 2895 (2018).
- A. J. Verhoef, A. Mitrofanov, A. Zheltikov, and A. Baltuška, Plasma-blueshift spectral shear interferometry for characterization of ultimately short optical pulses, Opt. Lett. 34, 82 (2009).
- M. L. van der Geest, J. J. de Boer, K. Murzyn, P. Jürgens, B. Ehrler, and P. M. Kraus, Transient high-harmonic spectroscopy in an inorganic–organic lead halide perovskite, J. Phys. Chem. Lett. 14, 10810 (2023).
- L.-M. Koll, S. V. B. Jensen, P. J. van Essen, B. de Keijzer, E. Olsson, J. Cottom, T. Witting, A. Husakou, M. J. J. Vrakking, L. B. Madsen, P. M. Kraus, and P. Jürgens, Extreme ultraviolet high-harmonic interferometry of excitation-induced bandgap dynamics in solids, Optica 12, 1606 (2025).
- D. Reynolds, D. C. Look, and B. Jogai, Combined effects of screening and band gap renormalization on the energy of optical transitions in ZnO and GaN, J. Appl. Phys. 88, 5760 (2000).
- J. Dai, C. Xu, T. Nakamura, Y. Wang, J. Li, and Y. Lin, Electron–hole plasma induced band gap renormalization in ZnO microlaser cavities, Opt. Express 22, 28831 (2014).
- B. Ziaja, N. Medvedev, V. Tkachenko, T. Maltezopoulos, and W. Wurth, Time-resolved observation of band-gap shrinking and electron-lattice thermalization within x-ray excited gallium arsenide, Sci. Rep. 5, 18068 (2015).
- F. Liu, M. E. Ziffer, K. R. Hansen, J. Wang, and X. Zhu, Direct determination of band-gap renormalization in the photoexcited monolayer , Phys. Rev. Lett. 122, 246803 (2019).
- Y. Ren, Z. Huang, and Y. Wang, Dynamic and giant bandgap renormalization dictates the transient optical response in perovskite quantum dots, Appl. Phys. Lett. 121, 251103 (2022).
- G. Vampa, C. McDonald, G. Orlando, D. Klug, P. Corkum, and T. Brabec, Theoretical analysis of high-harmonic generation in solids, Phys. Rev. Lett. 113, 073901 (2014).
- L. Yue and M. B. Gaarde, Imperfect recollisions in high-harmonic generation in solids, Phys. Rev. Lett. 124, 153204 (2020).
- N. Garejev, I. Gražulevičiūtė, D. Majus, G. Tamošauskas, V. Jukna, A. Couairon, and A. Dubietis, Third-and fifth-harmonic generation in transparent solids with few-optical-cycle midinfrared pulses, Phys. Rev. A 89, 033846 (2014).