- Open Access
Photoelectron Holography of a Heteronuclear Molecule
Phys. Rev. Lett. 136, 153202 – Published 15 April, 2026
DOI: https://doi.org/10.1103/z4xn-m554
Abstract
We present strong-field photoelectron holography measurements of hydrogen chloride (HCl) that resolve subcycle dynamics in two ionization channels associated with the HOMO and HOMO-1 orbitals. The holograms in the photoelectron momentum distributions show different cutoffs and interference fringes tied to orbital-specific ionization potentials. Furthermore, molecular-frame photoelectron holograms from oriented HCl exhibit pronounced asymmetries that arise from the interplay of the molecular dipole and the ionic Coulomb field. These findings establish strong-field photoelectron holography as a sensitive probe of subcycle electron wave packet dynamics in polar molecules.
Physics Subject Headings (PhySH)
Article Text
Supplemental Material
References (45)
- M. Spanner, O. Smirnova, P. B. Corkum, and M. Y. Ivanov, Reading diffraction images in strong field ionization of diatomic molecules, J. Phys. B 37, L243 (2004).
- Y. Huismans et al., Time-resolved holography with photoelectrons, Science 331, 61 (2011).
- X.-B. Bian, Y. Huismans, O. Smirnova, K.-J. Yuan, M. J. J. Vrakking, and A. D. Bandrauk, Subcycle interference dynamics of time-resolved photoelectron holography with midinfrared laser pulses, Phys. Rev. A 84, 043420 (2011).
- D. D. Hickstein, P. Ranitovic, S. Witte, X.-M. Tong, Y. Huismans, P. Arpin, X. Zhou, K. E. Keister, C. W. Hogle, B. Zhang, C. Ding, P. Johnsson, N. Toshima, M. J. J. Vrakking, M. M. Murnane, and H. C. Kapteyn, Direct visualization of laser-driven electron multiple scattering and tunneling distance in strong-field ionization, Phys. Rev. Lett. 109, 073004 (2012).
- M. Haertelt, X.-B. Bian, M. Spanner, A. Staudte, and P. B. Corkum, Probing molecular dynamics by laser-induced backscattering holography, Phys. Rev. Lett. 116, 133001 (2016).
- S. G. Walt, N. Bhargava Ram, M. Atala, N. I. Shvetsov-Shilovski, A. von Conta, D. Baykusheva, M. Lein, and H. J. Wörner, Dynamics of valence-shell electrons and nuclei probed by strong-field holography and rescattering, Nat. Commun. 8, 15651 (2017).
- G. Porat, G. Alon, S. Rozen, O. Pedatzur, M. Krüger, D. Azoury, A. Natan, G. Orenstein, B. D. Bruner, M. J. J. Vrakking, and N. Dudovich, Attosecond time-resolved photoelectron holography, Nat. Commun. 9, 2805 (2018).
- D. Gabor, A new microscopic principle, Nature (London) 161, 777 (1948).
- M. Meckel, D. Comtois, D. Zeidler, A. Staudte, D. Pavičić, H. C. Bandulet, H. Pépin, J. C. Kieffer, R. Dörner, D. M. Villeneuve, and P. B. Corkum, Laser-induced electron tunneling and diffraction, Science 320, 1478 (2008).
- D. Comtois, H.-C. Bandulet, M. Spanner, D. Pavičić, M. Meckel, D. Zeidler, H. Pépin, R. Dörner, J.-C. Kieffer, D. Villeneuve, P. Corkum, and A. Staudte, Laser-induced orbital projection and diffraction of with velocity map imaging, J. Mod. Opt. 60, 1395 (2013).
- Y. Huismans, A. Rouzée, A. Gijsbertsen, P. S. W. M. Logman, F. Lépine, C. Cauchy, S. Zamith, A. S. Stodolna, J. H. Jungmann, J. M. Bakker, G. Berden, B. Redlich, A. F. G. van der Meer, K. J. Schafer, and M. J. J. Vrakking, Photoelectron angular distributions from the ionization of xenon Rydberg states by midinfrared radiation, Phys. Rev. A 87, 033413 (2013).
- M. Meckel, A. Staudte, S. Patchkovskii, D. M. Villeneuve, P. B. Corkum, R. Dörner, and M. Spanner, Signatures of the continuum electron phase in molecular strong-field photoelectron holography, Nat. Phys. 10, 594 (2014).
- M. Li, X. Sun, X. Xie, Y. Shao, Y. Deng, C. Wu, Q. Gong, and Y. Liu, Revealing backward rescattering photoelectron interference of molecules in strong infrared laser fields, Sci. Rep. 5, 8519 (2015).
- X.-B. Bian and A. D. Bandrauk, Orientation-dependent forward-backward photoelectron holography from asymmetric molecules, Phys. Rev. A 89, 033423 (2014).
- S. Wang, J. Y. Che, C. Chen, G. G. Xin, and Y. J. Chen, Tracing the origins of an asymmetric momentum distribution for polar molecules in strong linearly polarized laser fields, Phys. Rev. A 102, 053103 (2020).
- D. Habibović, A. Gazibegović-Busuladžić, M. Busuladžić, and D. B. Milošević, Strong-field ionization of heteronuclear diatomic molecules using an orthogonally polarized two-color laser field, Phys. Rev. A 103, 053101 (2021).
- H. Akagi, T. Otobe, A. Staudte, A. Shiner, F. Turner, R. Dörner, D. M. Villeneuve, and P. B. Corkum, Laser tunnel ionization from multiple orbitals in HCl, Science 325, 1364 (2009).
- B. Friedrich and D. Herschbach, Enhanced orientation of polar molecules by combined electrostatic and nonresonant induced dipole forces, J. Chem. Phys. 111, 6157 (1999).
- M. Härtelt and B. Friedrich, Directional states of symmetric-top molecules produced by combined static and radiative electric fields, J. Chem. Phys. 128, 224313 (2008).
- L. Holmegaard, J. H. Nielsen, I. Nevo, H. Stapelfeldt, F. Filsinger, J. Küpper, and G. Meijer, Laser-induced alignment and orientation of quantum-state-selected large molecules, Phys. Rev. Lett. 102, 023001 (2009).
- O. Ghafur, A. Rouzée, A. Gijsbertsen, W. K. Siu, S. Stolte, and M. J. J. Vrakking, Impulsive orientation and alignment of quantum-state-selected NO molecules, Nat. Phys. 5, 289 (2009).
- S. De, I. Znakovskaya, D. Ray, F. Anis, N. G. Johnson, I. A. Bocharova, M. Magrakvelidze, B. D. Esry, C. L. Cocke, I. V. Litvinyuk, and M. F. Kling, Field-free orientation of CO molecules by femtosecond two-color laser fields, Phys. Rev. Lett. 103, 153002 (2009).
- P. H. Bucksbaum, A. Zavriyev, H. G. Muller, and D. W. Schumacher, Softening of the molecular bond in intense laser fields, Phys. Rev. Lett. 64, 1883 (1990).
- J. Ullrich, R. Moshammer, A. Dorn, R. Dörner, L. P. H. Schmidt, and H. Schmidt-Böcking, Recoil-ion and electron momentum spectroscopy: Reaction-microscopes, Rep. Prog. Phys. 66, 1463 (2003).
- See Supplemental Material at http://link.aps.org/supplemental/10.1103/z4xn-m554 for detailed experimental methods, additional data, and theoretical derivations, which includes Refs. [2,5,17,23,24,26–43].
- X.-Y. Lai, C. Poli, H. Schomerus, and C. F. d. M. Faria, Influence of the Coulomb potential on above-threshold ionization: A quantum-orbit analysis beyond the strong-field approximation, Phys. Rev. A 92, 043407 (2015).
- C. F. de M. Faria and A. S. Maxwell, It is all about phases: Ultrafast holographic photoelectron imaging, Rep. Prog. Phys. 83, 034401 (2020).
- X. Lai, R. Sun, S. Yu, Y. Wang, W. Quan, A. Staudte, and X. Liu, Reconstructing molecular orbitals with laser-induced electron tunneling spectroscopy, Ultrafast Sci. 4, 0038 (2024).
- A. Maxwell, A. Al-Jawahiry, T. Das, and C. F. d. M. Faria, Coulomb-corrected quantum interference in above-threshold ionization: Working towards multitrajectory electron holography, Phys. Rev. A 96, 023420 (2017).
- T. Khurelbaatar, J. Heo, S. Yu, X. Lai, X. Liu, and D. E. Kim, Strong-field photoelectron holography in the subcycle limit, Light 13, 108 (2024).
- C. T. L. Smeenk, L. Arissian, A. V. Sokolov, M. Spanner, K. F. Lee, A. Staudte, D. M. Villeneuve, and P. B. Corkum, Alignment dependent enhancement of the photoelectron cutoff for multiphoton ionization of molecules, Phys. Rev. Lett. 112, 253001 (2014).
- R. Moshammer, M. Unverzagt, W. Schmitt, J. Ullrich, and H. Schmidt-Böcking, A recoil-ion electron momentum analyzer: A high-resolution microscope for the investigation of the dynamics of atomic, molecular and nuclear reactions, Nucl. Instrum. Methods Phys. Res., Sect. B 108, 425 (1996).
- R. Dörner, V. Mergel, O. Jagutzki, L. Spielberger, J. Ullrich, R. Moshammer, and H. Schmidt-Böcking, Cold target recoil ion momentum spectroscopy: A ‘momentum microscope’ to view atomic collision dynamics, Phys. Rep. 330, 95 (2000).
- T. Jahnke, T. Weber, T. Osipov, A. Landers, O. Jagutzki, L. P. H. Schmidt, C. Cocke, M. Prior, H. Schmidt-Böcking, and R. Dörner, Multicoincidence studies of photo and auger electrons from fixed-in-space molecules using the COLTRIMS technique, J. Electron Spectrosc. Relat. Phenom. 141, 229 (2004).
- M. J. Frisch, G. W. Trucks, H. B. Schlegel, G. E. Scuseria, M. A. Robb, J. R. Cheeseman, G. Scalmani, V. Barone, B. Mennucci, G. A. Petersson et al., Gaussian 09, revision d.01 (Gaussian, Inc., Wallingford, CT, 2013).
- T. M. Yan, S. V. Popruzhenko, M. J. J. Vrakking, and D. Bauer, Low-energy structures in strong field ionization revealed by quantum orbits, Phys. Rev. Lett. 105, 253002 (2010).
- A. S. Maxwell and C. F. de M. Faria, Quantum-orbit analysis of the effect of the Coulomb potential on the dynamics of atomic ionization by strong linearly polarized laser pulses, J. Phys. B 51, 124001 (2018).
- E. Hasović, M. Busuladžić, W. Becker, and D. B. Milošević, Dressed-bound-state molecular strong-field approximation: Application to above-threshold ionization of heteronuclear diatomic molecules, Phys. Rev. A 84, 063418 (2011).
- M. Kübel, M. Spanner, Z. Dube, A. Y. Naumov, S. Chelkowski, A. Bandrauk, M. Vrakking, P. Corkum, D. Villeneuve, and A. Staudte, Probing multiphoton light-induced molecular potentials, Nat. Commun. 11, 2596 (2020).
- A. Rudenko, K. Zrost, T. Ergler, A. B. Voitkiv, B. Najjari, V. L. B. de Jesus, B. Feuerstein, C. D. Schröter, R. Moshammer, and J. Ullrich, Coulomb singularity in the transverse momentum distribution for strong-field single ionization, J. Phys. B 38, L191 (2005).
- D. Comtois, D. Zeidler, H. Pépin, J. C. Kieffer, D. M. Villeneuve, and P. B. Corkum, Observation of Coulomb focusing in tunnelling ionization of noble gases, J. Phys. B 38, 1923 (2005).
- J. Chen and C. H. Nam, Ion momentum distributions for he single and double ionization in strong laser fields, Phys. Rev. A 66, 053415 (2002).
- R. Moshammer, J. Ullrich, B. Feuerstein, D. Fischer, A. Dorn, Crespo D. Schröter, J. R. C. Lopez-Urrutia, C. Hoehr, H. Rottke, C. Trump, M. Wittmann, G. Korn, and W. Sandner, Rescattering of ultralow-energy electrons for single ionization of Ne in the tunneling regime, Phys. Rev. Lett. 91, 113002 (2003).
- W. Quan, Z. Lin, M. Wu, H. Kang, H. Liu, X. Liu, J. Chen, J. Liu, X. T. He, S. G. Chen, H. Xiong, L. Guo, H. Xu, Y. Fu, Y. Cheng, and Z. Z. Xu, Classical aspects in above-threshold ionization with a midinfrared strong laser field, Phys. Rev. Lett. 103, 093001 (2009).
- T. Wang, Z. Dube, Y. Mi, G. Vampa, D. M. Villeneuve, P. B. Corkum, X. Liu, and A. Staudte, Disentangling interferences in the photoelectron momentum distribution from strong-field ionization, Phys. Rev. A 106, 013106 (2022).