MANIFESTATION OF DYNAMIC CORE-ELECTRON POLARIZATION IN HIGH-ORDER HARMONIC GENERATION SPECTRA
Main Article Content
Abstract
We have recently demonstrated that incorporating Dynamic Core-electron Polarization (DCeP) into simulation aligns the high-order harmonic generation (HHG) of CO molecules with experimental data. However, the previous study was limited to the case where the laser is irradiated parallel to the molecule, corresponding to an orientation angle of 0°. In this paper, we extend the investigation of DCeP’s role in odd-even HHG to include various molecular orientations beyond 0°. Additionally, we examine the DCeP effect on attosecond bursts, focusing on harmonic generation in the time domain. To calculate HHG, we numerically solve the time-dependent Schrödinger equation under Single Active-Electron approximation (SAE), incorporating DCeP potential. The results demonstrate the substantial role of DCeP on the even-odd HHG ratio (the ratio of even-order harmonic intensity to the average of two adjacent odd orders) across different molecular orientations. A detailed analysis at an orientation angle of 70° indicates that, in the frequency domain, DCeP increases the even-to-odd ratio compared to the case without DCeP. In the time domain, DCeP remarkably changes the intensity ratio between consecutive attosecond bursts.
Keywords
alignment, dynamic core-electron polarization, even-to-odd ratio, high-order harmonic generation
Article Details
References
Baker, S., Robinson, J. S., Haworth, C. A., Teng, H., Smith, R. A., Chirilă, C. C., Lein, M., Tisch, J. W. G., & Marangos, J. P. (2006). Probing proton dynamics in molecules on an attosecond time scale. Science, 312, 424. https://doi.org/10.1126/science.1123904
Chen, Y. J., Fu, L., & Liu, J. (2013). Asymmetric Molecular Imaging through Decoding Odd-Even High-Order Harmonics. Physical Review Letters, 111, 073902. https://doi.org/10.1103/PhysRevLett.111.073902
Frumker, E., Hebeisen, C. T., Kajumba, N., Bertrand, J. B., Wörner, H. J., Spanner, M., Villeneuve, D. M., Naumov, A., & Corkum, P. B. (2012a). Oriented Rotational Wave-Packet Dynamics Studies via high harmonic Generation. Physical Review Letters, 109, 113901. https://doi.org/10.1103/PhysRevLett.109.113901
Frumker, E., Kajumba, N., Bertrand, J. B., Wörner, H. J., Hebeisen, C. T., Hockett, P., Spanner, M., Patchkovskii, S., Paulus, G. G., Villeneuve, D. M., Naumov, A., & Corkum, P. B. (2012b). Probing Polar Molecules with High Harmonic Spectroscopy. Physical Review Letters, 109, 233904. https://doi.org/10.1103/PhysRevLett.109.233904
Gordon, A., Kärtner, F. X., Rohringer, N., & Santra, R. (2006). Role of many-electron dynamics in high harmonic generation. Physical Review Letters, 96, 223902. https://doi.org/10.1103/PhysRevLett.96.223902
Hoang, V. H., Zhao, S. F., Le, V. H., & Le, A. T. (2017). Influence of permanent dipole and dynamic core-electron polarization on tunneling ionization of polar molecules. Physical Review, 95, 023407. https://doi.org/10.1103/PhysRevA.95.023407
Itatani, J., Lévesque, J., Zeidler, D., Niikura, H., Pépin, H., Kieffer, J., Corkum, P. B., & Villeneuve, D. M. (2004). Tomographic imaging of molecular orbitals. Nature, 432, 867. https://doi.org/10.1038/nature03183
Ivanov, M., & Corkum, P. B. (1993). Generation of high-order harmonics from inertially confined molecular ions. Physical Review A, 48, 580. https://doi.org/10.1103/PhysRevA.48.580
Kraus, P. M., Baykusheva, D., & Wörner, H. J. (2014). Two-Pulse Field-Free orientation reveals anisotropy of molecular shape resonance. Physical Review Letters, 113, 023001. https://doi.org/10.1103/PhysRevLett.113.023001
Kraus, P. M., Rupenyan, A., & Wörner, H. J. (2012). High-Harmonic spectroscopy of oriented OCS molecules: emission of even and odd harmonics. Physical Review Letters, 109, 233903. https://doi.org/10.1103/PhysRevLett.109.233903
Le, C. T., Hoang, V. H., Tran, L. P., & Le, V. H. (2018). Effect of the dynamic core-electron polarization of CO molecules on high-order harmonic generation. Physical Review, 97, 043405. https://doi.org/10.1103/PhysRevA.97.043405
Lewenstein, M., Balcou, P., Ivanov, M., L’Huillier, A., & Corkum, P. B. (1994). Theory of high-harmonic generation by low-frequency laser fields. Physical Review A, 49, 2117. https://doi.org/10.1103/PhysRevA.49.2117
McFarland, B. K., Farrell, J., Bucksbaum, P. H., & Gühr, M. (2008). High Harmonic Generation from Multiple Orbitals in N2. Science, 322, 1232. https://doi.org/10.1126/science.1162780
Nguyen, H. T., Nguyen, K. H., Phan, N. L., Le, C. T., Vu, D., Tran, L. P., & Le, V. H. (2022). Imprints of multielectron polarization effects in odd-even harmonic generation from CO molecules. Physical Review, 105, 023106. https://doi.org/10.1103/PhysRevA.105.023106
Nguyen, K. H., Phan, N. L., Le, C. T., Vu, D., & Le, V. H. (2022). Parameter-free retrieval of subcycle asymmetry of polar molecules by high-order harmonic spectroscopy. Physical Review, 106, 063108. https://doi.org/10.1103/PhysRevA.106.063108
Niikura, H., Dudovich, N., Villeneuve, D. M., & Corkum, P. B. (2010). Mapping molecular orbital symmetry on High-Order Harmonic Generation spectrum using Two-Color laser fields. Physical Review Letters, 105, 053003. https://doi.org/10.1103/PhysRevLett.105.053003
Phan, N. L., Le, C. T., Hoang, V. H., & Le, V. H. (2019). Odd–even harmonic generation from oriented CO molecules in linearly polarized laser fields and the influence of the dynamic core-electron polarization. Physical Chemistry Chemical Physics, 21, 24177. https://doi.org/10.1039/C9CP04064A
Trieu, D. A., Phan, N. L., Truong, Q. H., Nguyen, H. T., Le, C. T., Vu, D., & Le, V. H. (2023). Universality in odd-even harmonic generation and application in terahertz waveform sampling. Physical Review, 108, 023109. https://doi.org/10.1103/PhysRevA.108.023109
Vozzi, C., Negro, M., Calegari, F., Sansone, G., Nisoli, M., De Silvestri, S., & Stagira, S. (2011). Generalized molecular orbital tomography. Nature Physics, 7, 822. https://doi.org/10.1038/nphys2029
Yu, S., Zhang, B., Li, Y., Yang, S., & Chen, Y. (2014). Ellipticity of odd-even harmonics from oriented asymmetric molecules in strong linearly polarized laser fields. Physical Review A, 90, 053844. https://doi.org/10.1103/PhysRevA.90.053844
Yun, H., Lee, K., Sung, J. H., Kim, K. T., Kim, H. T., & Nam, C. H. (2015). Resolving multiple molecular orbitals using Two-Dimensional High-Harmonic spectroscopy. Physical Review Letters, 114, 153901. https://doi.org/10.1103/PhysRevLett.114.153901
Zhang, B., Yu, S., Chen, Y., Jiang, X., & Sun, X. (2015). Time-resolved dynamics of odd and even harmonic emission from oriented asymmetric molecules. Physical Review A, 92, 053833. https://doi.org/10.1103/PhysRevA.92.053833
Zhang, B., Yuan, J., & Zhao, Z. (2013). Dynamic core polarization in strong-field ionization of CO molecules. Physical Review Letters, 111, 163001. https://doi.org/10.1103/PhysRevLett.111.163001