TOMOGRAPHY OF PARTIALLY ALIGNED N2 MOLECULES FROM HIGH-ORDER HARMONIC GENERATION
Main Article Content
Abstract
Using the molecular tomography method, we reconstruct the highest-occupied molecular orbital (HOMO) from the high-order harmonic generation (HHG) emitted from N2 molecules when considering the alignment effect. We utilize two different approaches to describe the alignment distribution – (i) exactly by numerically solving the time-dependent Schrӧdinger equation and (ii) by an approximately analytical function. The results show that when lowering the degree of alignment, the accuracy of the reconstructed molecular HOMO decreases. When the alignment degree is less than 0.5, the HOMO cannot be reconstructed exactly. Also, the two different approaches of the alignment distribution offer the same results.
Keywords
high-order harmonic generation, N2 molecules, partially alignment, tomography
Article Details
References
Baker, S., Robinson, J. S., Haworth, C. A., Teng, H., Smith, R. A., Chirilǎ, C. C.,… Marangos, J. P. (2006). Probing proton dynamics in molecules on an attosecond time scale. Science, 312(5772), 424-427.
Chen, Y. J., Fu, L. B., & Liu, J. (2013). Asymmetric Molecular Imaging through Decoding Odd-Even High-Order Harmonics. Physical Review Letters, 111(7), 073902.
Cho, V. A., & Bernstein, R. B. (1991). Tight focusing of beams of polar polyatomic molecules via the electrostatic hexapole lens. Journal of Physical Chemistry, 95(21), 8129-8136.
De, S., Znakovskaya, I., Ray, D., Anis, F., Johnson, N. G., Bocharova, I. A.,… & Kling, M. F. (2009). Field-Free Orientation of CO Molecules by Femtosecond Two-Color Laser Fields. Physical Review Letters, 103(15), 153002.
Friedrich, B., & Herschbach, D. R. (1991). On the possibility of orienting rotationally cooled polar molecules in an electric field. Zeitschrift Für Physik D Atoms, Molecules and Clusters, 18(2), 153-161.
Frisch, Æ., Plata, R. E., & Singleton, D. A. (2009). Gaussian 09W Reference. J. Am. Chem. Soc., 137, 3811-3826.
Haessler, S., Caillat, J., Boutu, W., Ruchon, T., Diveki, Z., Breger, P., …& Ruchon, T. (2015). Attosecond imaging of molecular electronic wave-packets. Nature Physics, 200-206.
Itatani, J., Levesque, J., Zeidler, D., Niikura, H., Pépin, H., Kieffer, J. C.,… & Villeneuve, D. M. (2004). Tomographic imaging of molecular orbitals. Nature, 432(7019), 867-871.
Jin, C., Bertrand, J. B., Lucchese, R. R., Wörner, H. J., Corkum, P. B., Villeneuve, D. M.,… & Lin, C. D. (2012). Intensity dependence of multiple orbital contributions and shape resonance in high-order harmonic generation of aligned N2 molecules. Physical Review A, 85(1), 013405.
Kak, A. C., & Slaney, M. (2001). Principles of Computerized Tomographic Imaging. Society for Industrial and Applied Mathemathics, New York.
Kraus, P. M., Baykusheva, D., & Wörner, H. J. (2014). Two-pulse field-free orientation reveals anisotropy of molecular shape resonance. Physical Review Letters, 113(2), 023001.
Le, V.-H., Le, A.-T., Xie, R.-H., & Lin, C. D. (2007). Theoretical analysis of dynamic chemical imaging with lasers using high-order harmonic generation. Physical Review A, 76(1), 013414.
Lein, M., De Nalda, R., Heesel, E., Hay, N., Springate, E., Velotta, R.,… & Marangos, J. P. (2005). Signatures of molecular structure in the strong-field response of aligned molecules. Journal of Modern Optics, 52(2-3), 465-478.
Lewenstein, M., Balcou, P., Ivanov, M. Y., & Huillier, A. L. (1994). Theory of high-harmonic generation by low-frequency laser fields. Physical Review A, 49(3), 2117-2132.
Lin, C. D., Le, A. T., Jin, C., & Wei, H. (2018). Attosecond and Strong-Field Physics: Principles and Applications. In Cambridge University Press.
Maiman, T. H. (1960). Stimulated Optical Radiation in Ruby. Nature, 187(4736), 493-494.
Pullman, D. P., Friedrich, B., & Herschbach, D. R. (1990). Facile alignment of molecular rotation in supersonic beams. The Journal of Chemical Physics, 93(5), 3224-3236.
Qin, M., & Zhu, X. (2017). Molecular orbital imaging for partially aligned molecules. Optics and Laser Technology, 87, 79–86.
Qin, M., Zhu, X., Zhang, Q., & Lu, P. (2012). Tomographic imaging of asymmetric molecular orbitals with a two-color multicycle laser field. Optics Letters, 37(24), 5208.
Seideman, T. (1995a). On the selection of magnetic states in angle-resolved photodissociation. The Journal of Chemical Physics, 102(16), 6487-6498.
Seideman, T. (1995b). On the selection of magnetic states in angle‐resolved photodissociation. The Journal of Chemical Physics, 102(16), 6487-6498.
Stapelfeldt, H., & Seideman, T. (2003). Colloquium: Aligning molecules with strong laser pulses. Rewiews of Modern Physics, 75, 543-557.
Xie, X., Yu, S., Li, W., Wang, S., & Chen, Y. (2018). Routes of odd-even harmonic emission from oriented polar molecules. Optics Express, 26(14), 18578.
Yu, S. J., Li, W. Y., Li, Y. P., & Chen, Y. J. (2017). Probing degrees of orientation of top molecules with odd-even high-order harmonics. Physical Review A, 96(1), 013432.
Yuan, H., He, L., Wang, F., Wang, B., Zhu, X., Lan, P., & Lu, P. (2018). Tomography of asymmetric molecular orbitals with a one-color inhomogeneous field. Optics Letters, 43(4), 931.
Zhai, C., He, L., Lan, P., Zhu, X., Li, Y., Wang, F.,…& Lu, P. (2016). Coulomb-corrected molecular orbital tomography of nitrogen. Scientific Reports, 6, 23236.
Zhai, C., Zhang, X., Zhu, X., He, L., Zhang, Y., Wang, B.,… & Lu, P. (2018). Single-shot molecular orbital tomography with orthogonal two-color fields. Optics Express, 26(3), 314573.
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(5), 053833.
Zhou, X., Tong, X. M., Zhao, Z. X., & Lin, C. D. (2005). Alignment dependence of high-order harmonic generation from N2 and O2 molecules in intense laser fields. Physical Review A - Atomic, Molecular, and Optical Physics, 72(3), 033412.