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Real-time simulations of laser-induced electron excitations in crystalline ZnO

Xiao Chen1,2,3,4, Thomas Lettau3, Ulf Peschel3, Nicolas Tancogne-Dejean1,2,4,5, and Silvana Botti1,2,3,4

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Phys. Rev. B 113, 085208 – Published 25 February, 2026

DOI: https://doi.org/10.1103/p3r8-6grq

Abstract

We investigate nonequilibrium electron dynamics in crystalline ZnO induced by ultrashort, relatively intense, infrared laser pulses. Our focus is on understanding the mechanism that facilitates efficient conduction band population in ZnO to enable optically pumped lasing. We consider two different pulse frequencies (in the near infrared and mid infrared) for which experimental data are available, and we calculate the electronic response of a ZnO crystal for a wide range of pulse intensities. We apply and compare three complementary theoretical approaches: the analytical Keldysh model, the numerical solution of the semiconductor Bloch equations, and real-time time-dependent density functional theory. We conclude that time-dependent density functional theory is a valid ab initio approach for predicting conduction band population, that offers an accurate enough description of static and transient optical properties of solids and provides physics insight into the intermediate excitation regime, where electronic excitations are determined by the interplay of intraband tunneling, a consequence of band bending, and interband multiphoton absorption.

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References (64)

  1. J. Kim, S. K. Lee, J.-H. Lee, H.-Y. Kim, N. H. Kim, C. H. Lee, C.-S. Lee, and H. G. Kim, ZnO nanowire-based early detection of SARS-CoV-2 antibody responses in asymptomatic patients with COVID-19, Adv. Mater. Interfaces 9, 2102046 (2022).
  2. S. Baruah, M. Jaisai, R. Imani, M. M. Nazhad, and J. Dutta, Photocatalytic paper using zinc oxide nanorods, Sci. Technol. Adv. Mater. 11, 055002 (2010).
  3. S. Tian, F. Yang, D. Zeng, and C. Xie, Solution-processed gas sensors based on ZnO nanorods array with an exposed (0001) facet for enhanced gas-sensing properties, J. Phys. Chem. C 116, 10586 (2012).
  4. X. Li, X. Liu, Y. Li, D. Gao, and L. Cao, Using novel semiconductor features to construct advanced ZnO nanowires-based ultraviolet photodetectors: A brief review, IEEE Access 9, 11954 (2021).
  5. F. H. Nicoll, Ultraviolet ZnO laser pumped by an electron beam, Appl. Phys. Lett. 9, 13 (1966).
  6. D. M. Bagnall, Y. F. Chen, Z. Zhu, T. Yao, S. Koyama, M. Y. Shen, and T. Goto, Optically pumped lasing of ZnO at room temperature, Appl. Phys. Lett. 70, 2230 (1997).
  7. P. Yu, Z. K. Tang, G. K. L. Wong, M. Kawasaki, A. Ohtomo, H. Koinuma, and Y. Segawa, Room-temperature gain spectra and lasing in microcrystalline ZnO thin films, J. Cryst. Growth. 184–185, 601 (1998).
  8. T. Makino, Y. Segawa, M. Kawasaki, and H. Koinuma, Optical properties of excitons in ZnO-based quantum well heterostructures, Semicond. Sci. Technol. 20, S78 (2005).
  9. M. Huang, S. Mao, H. Feick, H. Yan, Y. Wu, H. Kind, E. Weber, R. Russo, and P. Yang, Room-temperature ultraviolet nanowire nanolasers, Science 292, 1897 (2001).
  10. L. Mädler, W. J. Stark, and S. E. Pratsinis, Rapid synthesis of stable ZnO quantum dots, J. Appl. Phys. 92, 6537 (2002).
  11. Ü. Özgür, Y. I. Alivov, C. Liu, A. Teke, M. A. Reshchikov, S. Dogan, V. Avrutin, S.-J. Cho, and H. Morkoc, A comprehensive review of ZnO materials and devices, J. Appl. Phys. 98, 041301 (2005).
  12. R.-M. Ma and R. F. Oulton, Applications of nanolasers, Nat. Nanotech. 14, 12 (2019).
  13. D. H. Jones and H. R. Reiss, Intense-field effects in solids, Phys. Rev. B 16, 2466 (1977).
  14. S. J. Hua and W. D. Zhang, Multiphoton absorption and dispersive nonlinear refraction of ZnO in VIS-NIR bands, Opt. Laser. Technol. 145, 107478 (2022).
  15. S. K. Das, M. Biswas, D. Byrne, M. Bock, E. McGlynn, M. Breusing, and R. Grunwald, Multiphoton-absorption induced ultraviolet luminescence of ZnO nanorods using low-energy femtosecond pulses, J. Appl. Phys. 108, 043107 (2010).
  16. R. Hollinger, P. Malevich, V. Shumakova, S. Alisauskas, M. Zapf, R. Röder, A. Pugžlys, A. Baltuška, C. Ronning, C. Spielmann, and D. Kartashov, Strong light-field driven nanolasers, Nano Lett. 19, 3563 (2019).
  17. S. Ghimire, A. D. DiChiara, E. Sistrunk, U. B. Szafruga, P. Agostini, L. F. DiMauro, and D. A. Reis, Redshift in the optical absorption of ZnO single crystals in the presence of an intense midinfrared laser field, Phys. Rev. Lett. 107, 167407 (2011).
  18. R. Boge, C. Cirelli, A. S. Landsman, S. Heuser, A. Ludwig, J. Maurer, M. Weger, L. Gallmann, and U. Keller, Probing nonadiabatic effects in strong-field tunnel ionization, Phys. Rev. Lett. 111, 103003 (2013).
  19. See Supplemental Material at http://link.aps.org/supplemental/10.1103/p3r8-6grq for further details on the calculation of dipole matrix elements; the impact of dephasing time on the SBE solution; the influence of band-gap errors on the SBE and Keldysh model; and the intensity-dependent optical parameters in TDDFT.
  20. L. V. Keldysh, Ionization in the field of a strong electromagnetic wave, Zh. Eksp. Teor. Fiz. 47, 1945 (1964).
  21. S. V. Popruzhenko, Keldysh theory of strong field ionization: History, applications, difficulties and perspectives, J. Phys. B: At., Mol. Opt. Phys. 47, 204001 (2014).
  22. L. A. Siiman, J. Lumeau, and L. B. Glebov, Nonlinear photoionization and laser-induced damage in silicate glasses by infrared ultrashort laser pulses, Appl. Phys. B 96, 127 (2009).
  23. T. J.-Y. Derrien, N. Tancogne-Dejean, V. P. Zhukov, H. Appel, A. Rubio, and N. M. Bulgakova, Photoionization and transient Wannier-Stark ladder in silicon: First-principles simulations versus Keldysh theory, Phys. Rev. B 104, L241201 (2021).
  24. M. Lindberg and S. W. Koch, Effective Bloch equations for semiconductors, Phys. Rev. B 38, 3342 (1988).
  25. Y. Lun and B. G. Mette, Introduction to theory of high-harmonic generation in solids: Tutorial, J. Opt. Soc. Am. B 39, 535 (2022).
  26. I. Floss, C. Lemell, G. Wachter, V. Smejkal, S. A. Sato, X.-M. Tong, K. Yabana, and J. Burgdörfer, Ab initio multiscale simulation of high-order harmonic generation in solids, Phys. Rev. A 97, 011401(R) (2018).
  27. 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).
  28. 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).
  29. T. T. Luu and H. J. Wörner, High-order harmonic generation in solids: A unifying approach, Phys. Rev. B 94, 115164 (2016).
  30. M. Kira and S. W. Koch, Many-body correlations and excitonic effects in semiconductor spectroscopy, Prog. Quantum Electron. 30, 155 (2006).
  31. H. Akima, A new method of interpolation and smooth curve fitting based on local procedures, J. ACM 17, 589 (1970).
  32. J. Peinado, J. Ibáñez, E. Arias, and V. Hernández, Adams–Bashforth and Adams–Moulton methods for solving differential Riccati equations, Comput. Math. Appl. 60, 3032 (2010).
  33. E. Runge and E. K. U. Gross, Density-functional theory for time-dependent systems, Phys. Rev. Lett. 52, 997 (1984).
  34. T. Otobe, M. Yamagiwa, J.-I. Iwata, K. Yabana, T. Nakatsukasa, and G. F. Bertsch, First-principles electron dynamics simulation for optical breakdown of dielectrics under an intense laser field, Phys. Rev. B 77, 165104 (2008).
  35. K. Yabana, T. Sugiyama, Y. Shinohara, T. Otobe, and G. F. Bertsch, Time-dependent density functional theory for strong electromagnetic fields in crystalline solids, Phys. Rev. B 85, 045134 (2012).
  36. N. Tancogne-Dejean, M. A. Sentef, and A. Rubio, Ultrafast transient absorption spectroscopy of the charge-transfer insulator NiO: Beyond the dynamical Franz-Keldysh effect, Phys. Rev. B 102, 115106 (2020).
  37. K. Yabana, T. Nakatsukasa, J.-I. Iwata, and G. F. Bertsch, Real-time, real-space implementation of the linear response time-dependent density-functional theory, Phys. Status Solidi B 243, 1121 (2006).
  38. G. Le Breton, A. Rubio, and N. Tancogne-Dejean, High-harmonic generation from few-layer hexagonal boron nitride: Evolution from monolayer to bulk response, Phys. Rev. B 98, 165308 (2018).
  39. D. R. Hamann, Optimized norm-conserving Vanderbilt pseudopotentials, Phys. Rev. B 88, 085117 (2013).
  40. J. P. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77, 3865 (1996).
  41. N. Tancogne-Dejean, M. J. T. Oliveira, and A. Rubio, Self-consistent DFT+U method for real-space time-dependent density functional theory calculations, Phys. Rev. B 96, 245133 (2017).
  42. L. A. Agapito, S. Curtarolo, and M. Buongiorno Nardelli, Reformulation of DFT+U as a pseudohybrid Hubbard density functional for accelerated materials discovery, Phys. Rev. X 5, 011006 (2015).
  43. M. Schultze, K. Ramasesha, C. Pemmaraju, S. Sato, D. Whitmore, A. Gandman, J. S. Prell, L. J. Borja, D. Prendergast, K. Yabana, D. M. Neumark, and S. R. Leone, Attosecond band-gap dynamics in silicon, Science 346, 1348 (2014).
  44. C. Ullrich, Time-Dependent Density-Functional Theory: Concepts and Applications (Oxford University Press, Oxford, 2012).
  45. A. Castro, H. Appel, M. Oliveira, C. A. Rozzi, X. Andrade, F. Lorenzen, M. A. L. Marques, E. K. U. Gross, and A. Rubio, Octopus: A tool for the application of time-dependent density functional theory, Phys. Status Solidi B 243, 2465 (2006).
  46. N. Tancogne-Dejean, M. J. T. Oliveira, X. Andrade, H. Appel, C. H. Borca, G. Le Breton, F. Buchholz, A. Castro, S. Corni, A. A. Correa, U. De Giovannini, A. Delgado, F. G. Eich, J. Flick, G. Gil, A. Gomez, N. Helbig, H. Hübener, R. Jestädt, J. Jornet-Somoza, et al., Octopus, a computational framework for exploring light-driven phenomena and quantum dynamics in extended and finite systems, J. Chem. Phys. 152, 124119 (2020).
  47. H. Karzel, W. Potzel, M. Köfferlein, W. Schiessl, M. Steiner, U. Hiller, G. M. Kalvius, D. W. Mitchell, T. P. Das, P. Blaha, K. Schwarz, and M. P. Pasternak, Lattice dynamics and hyperfine interactions in ZnO and ZnSe at high external pressures, Phys. Rev. B 53, 11425 (1996).
  48. H. J. Monkhorst and J. D. Pack, Special points for Brillouin-zone integrations, Phys. Rev. B 13, 5188 (1976).
  49. A. Gómez Pueyo, M. A. L. Marques, A. Rubio, and A. Castro, Propagators for the time-dependent Kohn–Sham equations: Multistep, Runge–Kutta, exponential Runge–Kutta, and commutator free Magnus methods, J. Chem. Theory Comput. 14, 3040 (2018).
  50. G. F. Bertsch, J. Giansiracusa, and K. Yabana, Application of time-dependent density-functional theory to electron—ion coupling in ethylene, Isr. J. Chem. 42, 151 (2002).
  51. V. Turkowski and C. A. Ullrich, Time-dependent density-functional theory for ultrafast interband excitations, Phys. Rev. B 77, 075204 (2008).
  52. V. Turkowski, A. Leonardo, and C. A. Ullrich, Time-dependent density-functional approach for exciton binding energies, Phys. Rev. B 79, 233201 (2009).
  53. M. A. M. Versteegh, T. Kuis, H. T. C. Stoof, and J. I. Dijkhuis, Ultrafast screening and carrier dynamics in ZnO: Theory and experiment, Phys. Rev. B 84, 035207 (2011).
  54. M. Wu, S. Ghimire, D. A. Reis, K. J. Schafer, and M. B. Gaarde, High-harmonic generation from Bloch electrons in solids, Phys. Rev. A 91, 043839 (2015).
  55. J. D. Jackson, Classical Electrodynamics (Wiley, Hoboken, NJ, 2021).
  56. A. Yamada and K. Yabana, Energy transfer from intense laser pulse to dielectrics in time-dependent density functional theory, Eur. Phys. J. D 73, 87 (2019).
  57. R. Hollinger, D. Gupta, M. Zapf, M. Karst, R. Röder, I. Uschmann, U. Reislöhner, D. Kartashov, C. Ronning, and C. Spielmann, Polarization dependent multiphoton absorption in ZnO thin films, J. Phys. D: Appl. Phys. 53, 055102 (2020).
  58. W. Franz, Einfluß eines elektrischen feldes auf eine optische absorptionskante, Z. Naturforsch. A 13, 484 (1958).
  59. L. Keldysh, in Selected Papers of Leonid V Keldysh (World Scientific, Singapore, 2024).
  60. A. P. Jauho and K. Johnsen, Dynamical Franz-Keldysh effect, Phys. Rev. Lett. 76, 4576 (1996).
  61. K. B. Nordstrom, K. Johnsen, S. J. Allen, A.-P. Jauho, B. Birnir, J. Kono, T. Noda, H. Akiyama, and H. Sakaki, Excitonic dynamical Franz-Keldysh effect, Phys. Rev. Lett. 81, 457 (1998).
  62. T. Meier, H. Kolbe, A. Thränhardt, G. Weiser, P. Thomas, and S. Koch, Coherent dynamics of photoexcited semiconductor superlattices in homogeneous electric fields, Phys. E (Amsterdam) 7, 267 (2000).
  63. T. Meier, G. von Plessen, P. Thomas, and S. W. Koch, Coherent effects induced by static and time-dependent electric fields in semiconductors, Phys. Rev. B 51, 14490 (1995).
  64. H. Haug and S. Koch, Quantum Theory of the Optical and Electronic Properties of Semiconductors, G - Reference,Information and Interdisciplinary Subjects Series (World Scientific, Singapore, 2009).

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Phys. Rev. B 113, 085208– Published 25 February, 2026
  • Received 21 March 2025
  • Revised 20 October 2025
  • Accepted 20 January 2026
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

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