Abstract

In this review, we briefly summarize more than a decade of experimental and theoretical investigations regarding the nonadiabatic electron response to intense femtosecond duration laser fields in a variety of molecular systems. Historically, experimental signatures of nonadiabaticity have emerged readily in large, conjugated, or multi-electron systems, disrupting fragmentation behavior and modulating observed rates of ionization. As model theoretical studies performed in H2+ and other diatomic species show, departure from traditional quasi-static or cycle-averaged descriptions of laser-induced ionization is often necessary to accommodate the rich and frequently counterintuitive electron dynamics that characterize the nonadiabatic response. Nonadiabatic effects such as transient electron localization or the observation of multiple ionization bursts per driving field cycle possess the capacity to modulate the signal of many strong-field physical effects, such as high-order harmonic generation, photoelectron momentum distributions, and molecular fragmentation products. As the advancement of experimental technologies expands the pursuit of laser-driven physics further into the mid-infrared wavelength regime, we suggest that these nonadiabatic effects will become increasingly pronounced and relevant to the imaging and control of a wide array of molecular species.

© 2016 Optical Society of America

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2016 (1)

M. R. Miller, A. Jaroń-Becker, and A. Becker, “High harmonic spectroscopy of laser-driven nonadiabatic electron dynamics in the hydrogen molecular ion,” Phys. Rev. A 93, 013406 (2016).
[Crossref]

2015 (2)

H. Xu, F. He, D. Kielpinski, R. T. Sang, and I. V. Litvinyuk, “Experimental observation of the elusive double-peak structure in R-dependent strong-field ionization rate of H2+,” Sci. Rep. 5, 13527 (2015).
[Crossref]

P.-L. He, N. Takemoto, and F. He, “Photoelectron momentum distributions of atomic and molecular systems in strong circularly or elliptically polarized laser fields,” Phys. Rev. A 91, 063413 (2015).
[Crossref]

2014 (2)

X.-B. Bian and A. D. Bandrauk, “Probing nuclear motion by frequency modulation of molecular high-order harmonic generation,” Phys. Rev. Lett. 113, 193901 (2014).
[Crossref]

C. Huang, P. Lan, Y. Zhou, Q. Zhang, K. Liu, and P. Lu, “Tunneling site of electrons in strong-field-enhanced ionization of molecules,” Phys. Rev. A 90, 043420 (2014).
[Crossref]

2013 (1)

A. Stolow, “The three pillars of photo-initiated quantum molecular dynamics,” Faraday Discuss. 163, 9–32 (2013).
[Crossref]

2012 (3)

Z. Diveki, A. Camper, S. Haessler, T. Auguste, T. Ruchon, B. Carre, P. Salieres, R. Guichard, J. Caillat, A. Maquet, and R. Taieb, “Spectrally resolved multi-channel contributions to the harmonic emission in N2,” New J. Phys. 14, 023062 (2012).
[Crossref]

H. Vincenti and F. Quéré, “Attosecond lighthouses: how to use spatiotemporally coupled light fields to generate isolated attosecond pulses,” Phys. Rev. Lett. 108, 113904 (2012).
[Crossref]

J. A. Wheeler, A. Borot, S. Monchocé, H. Vincenti, A. Ricci, A. Malvache, R. Lopez-Martens, and F. Quéré, “Attosecond lighthouses from plasma mirrors,” Nat. Photonics 6, 829–833 (2012).
[Crossref]

2011 (7)

H. J. Wörner, J. B. Bertrand, B. Fabre, J. Higuet, H. Ruf, A. Dubrouil, S. Patchkovskii, M. Spanner, Y. Mairesse, V. Blanchet, E. Mevel, E. Constant, P. B. Corkum, and D. M. Villeneuve, “Conical intersection dynamics in NO2 probed by homodyne high-harmonic spectroscopy,” Science 334, 208–212 (2011).
[Crossref]

C. Vozzi, M. Negro, F. Calegari, G. Sansone, M. Nisoli, S. De Silvestri, and S. Stagira, “Generalized molecular orbital tomography,” Nat. Phys. 7, 822–826 (2011).
[Crossref]

M. Odenweller, N. Takemoto, A. Vredenborg, K. Cole, K. Pahl, J. Titze, L. P. Schmidt, T. Jahnke, R. Dörner, and A. Becker, “Strong field emission from fixed in space H2+,” Phys. Rev. Lett. 107, 143004 (2011).
[Crossref]

N. Takemoto and A. Becker, “Time-resolved view on charge-resonance-enhanced ionization,” Phys. Rev. A 84, 023401 (2011).
[Crossref]

N. Takemoto and A. Becker, “Visualization and interpretation of attosecond electron dynamics in laser-driven hydrogen molecular ion using Bohmian trajectories,” J. Chem. Phys. 134, 074309 (2011).
[Crossref]

I. Bocharova, R. Karimi, E. F. Penka, J.-P. Brichta, P. Lassonde, X. Fu, J.-C. Kieffer, A. D. Bandrauk, I. Litvinyuk, J. Sanderson, and F. Legare, “Charge resonance enhanced ionization of CO2 probed by laser Coulomb explosion imaging,” Phys. Rev. Lett. 107, 063201 (2011).
[Crossref]

M. Spanner, J. Mikosch, A. Gijsberten, A. E. Boguslavskiy, and A. Stolow, “Multielectron effects and nonadiabatic electronic dynamics in above threshold ionization and high-harmonic generation,” New J. Phys. 13, 093010 (2011).
[Crossref]

2010 (4)

S. M. Smith, D. A. Romanov, X. Li, J. A. Sonk, H. B. Schlegel, and R. J. Levis, “Numerical bound state electron dynamics of carbon dioxide in the strong-field regime,” J. Phys. Chem. A 114, 2576–2587 (2010).
[Crossref]

N. Takemoto and A. Becker, “Multiple ionization bursts in laser-driven hydrogen molecular ion,” Phys. Rev. Lett. 105, 203004 (2010).
[Crossref]

H. J. Wörner, J. B. Bertrand, P. Hockett, P. B. Corkum, and D. M. Villeneuve, “Controlling the interference of multiple molecular orbitals in high-harmonic generation,” Phys. Rev. Lett. 104, 233904 (2010).
[Crossref]

H. J. Wörner, J. P. Bertand, D. V. Kartashov, P. B. Corkum, and D. M. Villeneuve, “Following a chemical reaction using high-harmonic interferometry,” Nature 466, 604–607 (2010).
[Crossref]

2009 (1)

O. Smirnova, Y. Mairesse, S. Patchkovskii, N. Dudovich, D. Villeneuve, P. Corkum, and M. Y. Ivanov, “High harmonic interferometry of multi-electron dynamics in molecules,” Nature 460, 972–977 (2009).
[Crossref]

2008 (7)

W. Boutu, S. Haessler, H. Merdij, P. Breger, G. Waters, M. Stankiewicz, L. J. Frasinski, R. Taieb, J. Caillat, A. Maquet, P. Manchicourt, B. Carre, and P. Salieres, “Coherent control of attosecond emission from aligned molecules,” Nat. Phys. 4, 545–549 (2008).
[Crossref]

X. Zhou, R. Lock, W. Li, N. Wagner, M. M. Murnane, and H. C. Kapteyn, “Molecular recollision interferometry in high harmonic generation,” Phys. Rev. Lett. 100, 073902 (2008).
[Crossref]

W. Li, X. Zhou, R. Lock, S. Patchkovskii, A. Stolow, H. C. Kapteyn, and M. M. Murnane, “Time-resolved dynamics in N2O4 probed using high harmonic generation,” Science 322, 1207–1211 (2008).
[Crossref]

S. Baker, J. S. Robinson, M. Lein, C. C. Chirila, R. Torres, H. C. Bandulet, D. Comtois, J. C. Kieffer, D. M. Villeneuve, J. W. G. Tisch, and J. P. Marangos, “Dynamic two-center interference in high-order harmonic generation from molecules with attosecond nuclear motion,” Phys. Rev. Lett. 101, 053901 (2008).
[Crossref]

F. He, A. Becker, and U. Thumm, “Strong-field modulated diffraction effects in the correlated electron-nuclear motion in dissociating H2+,” Phys. Rev. Lett. 101, 213002 (2008).
[Crossref]

P. Eckle, M. Smolarski, P. Schlup, J. Biegert, A. Staudte, M. Schöffler, J. G. Muller, R. Dörner, and U. Keller, “Attosecond angular streaking,” Nat. Phys. 4, 565–570 (2008).
[Crossref]

S. Gräfe, V. Engel, and M. Y. Ivanov, “Attosecond photoelectron spectroscopy of electron tunneling in an dissociating hydrogen molecular ion,” Phys. Rev. Lett. 101, 103001 (2008).
[Crossref]

2007 (3)

M. F. Ciappina, A. Becker, and A. Jaron-Becker, “Multislit interference patterns in high-order harmonic generation in C60,” Phys. Rev. A 76, 063406 (2007).
[Crossref]

S. M. Smith, X. Li, A. N. Markevitch, D. Romanov, R. J. Levis, and H. B. Schlegel, “Numerical simulation of nonadiabatic electron excitation in the strong field regime. 3. Polyacene neutrals and cations,” J. Phys. Chem. A 111, 6920–6932 (2007).
[Crossref]

H. B. Schlegel, S. M. Smith, and X. Li, “Electronic optical response of molecules in intense fields: comparison of TD-HF, TD-CIS, and TD-CIS(D) approaches,” J. Chem. Phys 126, 244110 (2007).
[Crossref]

2006 (3)

A. Jaroń-Becker, A. Becker, and F. H. M. Faisal, “Saturated ionization of fullerenes in intense laser fields,” Phys. Rev. Lett. 96, 143006 (2006).
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S. Baker, J. S. Robinson, C. A. Haworth, H. Teng, R. A. Smith, C. C. Chirila, M. Lein, J. W. G. Tisch, and J. P. Marangos, “Probing proton dynamics in molecules on an attosecond time scale,” Science 312, 424–427 (2006).
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N. L. Wagner, A. Wüst, I. P. Christov, T. Popmintchev, X. Zhou, M. M. Murnane, and H. C. Kapteyn, “Monitoring molecular dynamics using coherent electrons from high harmonic generation,” Proc. Natl. Acad. Sci. U.S.A. 103, 13279–13285 (2006).
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2005 (6)

T. Kanai, S. Minemoto, and H. Sakai, “Quantum interference during high-order harmonic generation from aligned molecules,” Nature 435, 470–474 (2005).
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C. Vozzi, F. Calegari, E. Benedetti, J. P. Caumes, G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel, N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, “Controlling two-center interference in molecular high harmonic generation,” Phys. Rev. Lett. 95, 153902 (2005).
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G. L. Yudin, S. Chelkowski, J. Itatani, A. D. Bandrauk, and P. B. Corkum, “Attosecond photoionization of coherently coupled electronic states,” Phys. Rev. A 72, 051401(R) (2005).
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X. Li, S. M. Smith, A. N. Markevitch, D. A. Romanov, R. J. Levis, and H. B. Schlegel, “A time-dependent Hartree-Fock approach for studying the electronic optical response of molecules in intense fields,” Phys. Chem. Chem. Phys. 7, 233–239 (2005).
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S. M. Smith, X. Li, A. N. Markevitch, D. A. Romanov, R. J. Levis, and H. B. Schlegel, “A numerical simulation of nonadiabatic electron excitation in the strong field regime: linear polyenes,” J. Phys. Chem. A 109, 5176–5185 (2005).
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S. M. Smith, X. Li, A. N. Markevitch, D. A. Romanov, R. J. Levis, and H. B. Schlegel, “Numerical simulation of nonadiabatic electron excitation in the strong field regime. 2. Linear polyene cations,” J. Phys. Chem. A 109, 10527–10534 (2005).
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2004 (2)

A. N. Markevitch, D. A. Romanov, S. M. Smith, H. B. Schlegel, M. Y. Ivanov, and R. J. Levis, “Sequential nonadiabatic excitation of large molecules and ions driven by strong laser fields,” Phys. Rev. A 69, 013401 (2004).
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J. Itatani, J. Levesque, D. Zeidler, H. Niikura, H. Pepin, J. C. Kieffer, P. B. Corkum, and D. M. Villeneuve, “Tomographic imaging of molecular orbitals,” Nature 432, 867–871 (2004).
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2003 (1)

A. N. Markevitch, S. M. Smith, D. A. Romanov, H. B. Schlegel, M. Y. Ivanov, and R. J. Levis, “Nonadiabatic dynamics of polyatomic molecules and ions in strong laser fields,” Phys. Rev. A 68, 011402(R) (2003).
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2002 (3)

M. Lezius, V. Blanchet, M. Y. Ivanov, and A. Stolow, “Polyatomic molecules in strong laser fields: nonadiabatic multielectron dynamics,” J. Chem. Phys. 117, 1575–1588 (2002).
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M. Lein, N. Hay, R. Velotta, J. P. Marangos, and P. L. Knight, “Interference effects in high-order harmonic generation with molecules,” Phys. Rev. A 66, 023805 (2002).
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M. Lein, N. Hay, R. Velotta, J. P. Marangos, and P. L. Knight, “Role of the intramolecular phase in high-harmonic generation,” Phys. Rev. Lett. 88, 183903 (2002).
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2001 (2)

A. Santana, J. M. Gomez Llorente, and V. Delgado, “Semiclassical dressed states of two-level quantum systems driven by non-resonant and/or strong laser fields,” J. Phys. B 34, 2371–2382 (2001).

M. Lezius, V. Blanchet, D. M. Rayner, D. M. Villeneuve, A. Stolow, and M. Y. Ivanov, “Nonadiabatic multielectron dynamics in strong field molecular ionization,” Phys. Rev. Lett. 86, 51–54 (2001).
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2000 (1)

J. Muth-Böhm, A. Becker, and F. H. M. Faisal, “Suppressed molecular ionization for a class of diatomics in intense femtosecond laser fields,” Phys. Rev. Lett. 85, 2280–2283 (2000).
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1999 (1)

I. Kawata, H. Kono, and Y. Fujimura, “Adiabatic and diabatic responses of H2+ to an intense femtosecond laser pulse: dynamics of the electronic and nuclear wave packet,” J. Chem. Phys. 110, 11152–11165 (1999).
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1997 (1)

A. Talebpour, C.-Y. Chien, Y. Liang, S. Larochelle, and S. L. Chin, “Non-sequential ionization of Xe and Kr in an intense femtosecond Ti:sapphire laser pulse,” J. Phys. B 30, 1721–1730 (1997).

1996 (1)

S. Chelkowski, A. Conjusteau, T. Zuo, and A. Bandrauk, “Dissociative ionization of H2+ in an intense laser field: charge-resonance-enhanced ionization, Coulomb explosion, and harmonic generation at 600  nm,” Phys. Rev. A 54, 3235–3244 (1996).
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1995 (2)

T. Zuo and A. D. Bandrauk, “Charge-resonance-enhanced ionization of diatomic molecular ion by intense laser fields,” Phys. Rev. A 52, R2511–R2514 (1995).
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T. Seideman, M. Y. Ivanov, and P. B. Corkum, “Role of electron localization in intense-field molecular ionization,” Phys. Rev. Lett. 75, 2819–2822 (1995).
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1994 (2)

B. Walker, B. Sheehy, L. F. Di Mauro, P. Agostini, K. J. Schafer, and K. C. Kulander, “Precision measurement of strong field double ionization of helium,” Phys. Rev. Lett. 73, 1227–1230 (1994).
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T. Zuo, S. Chelkowski, and A. D. Bandrauk, “Photon-emission spectra of the H2+ molecular ion in an intense laser field,” Phys. Rev. A 49, 3943–3953 (1994).
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1993 (3)

T. Zuo, S. Chelkowski, and A. D. Bandrauk, “Harmonic generation by the H2+ molecular ion in intense laser fields,” Phys. Rev. A 48, 3837–3844 (1993).
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P. B. Corkum, “Plasma perspective on strong field multiphoton ionization,” Phys. Rev. Lett. 71, 1994–1997 (1993).
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K. J. Schafer, B. Yang, L. F. DiMauro, and K. C. Kulander, “Above threshold ionization beyond the high harmonic cutoff,” Phys. Rev. Lett. 70, 1599–1602 (1993).
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1989 (1)

X. F. Li, A. L’Huillier, M. Ferray, L. A. Lompre, and G. Mainfray, “Multiple-harmonic generation in rare gases at high laser intensity,” Phys. Rev. A 39, 5751–5754 (1989).
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1987 (1)

1986 (1)

M. V. Ammosov, N. B. Delone, and V. P. Krainov, “Tunnel ionization of complex atoms and of atomic ions in an alternatic electromagnetic field,” Sov. Phys. JETP 64, 1191–1194 (1986).

1980 (1)

H. R. Reiss, “Effect of an intense electromagnetic field on a weakly bound system,” Phys. Rev. A 22, 1786–1813 (1980).
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1979 (1)

P. Agostini, F. Fabre, G. Mainfray, G. Petite, and N. K. Rahman, “Free-free transitions following six-photon ionization of xenon atoms,” Phys. Rev. Lett. 42, 1127–1130 (1979).
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1973 (1)

F. H. M. Faisal, “Multiple absorption of laser photons by atoms,” J. Phys. B 6, L89–L92 (1973).

1969 (1)

B. R. Mollow, “Power spectrum of light scattered by two-level systems,” Phys. Rev. 188, 1969–1975 (1969).
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1966 (2)

A. M. Perelomov, S. V. Popov, and M. V. Terent’ev, “Ionization of atoms in an alternating electric field,” Sov. Phys. JETP 23, 924–934 (1966).

H. D. Cohen and U. Fano, “Interference in the photo-ionization of molecules,” Phys. Rev. 150, 30–33 (1966).
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1965 (1)

L. V. Keldysh, “Ionization in the field of a strong electromagnetic wave,” Sov. Phys. JETP 20, 1307–1314 (1965).

1939 (1)

R. S. Mulliken, “Intensities of electronic transitions in molecular spectra II. Charge-transfer spectra,” J. Chem. Phys. 7, 20–34 (1939).
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1802 (1)

T. Young, “The Bakerian lecture: on the theory of light and colours,” Philos. Trans. R. Soc. 92, 12–48 (1802).
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Agostini, P.

B. Walker, B. Sheehy, L. F. Di Mauro, P. Agostini, K. J. Schafer, and K. C. Kulander, “Precision measurement of strong field double ionization of helium,” Phys. Rev. Lett. 73, 1227–1230 (1994).
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P. Agostini, F. Fabre, G. Mainfray, G. Petite, and N. K. Rahman, “Free-free transitions following six-photon ionization of xenon atoms,” Phys. Rev. Lett. 42, 1127–1130 (1979).
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Altucci, C.

C. Vozzi, F. Calegari, E. Benedetti, J. P. Caumes, G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel, N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, “Controlling two-center interference in molecular high harmonic generation,” Phys. Rev. Lett. 95, 153902 (2005).
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Ammosov, M. V.

M. V. Ammosov, N. B. Delone, and V. P. Krainov, “Tunnel ionization of complex atoms and of atomic ions in an alternatic electromagnetic field,” Sov. Phys. JETP 64, 1191–1194 (1986).

Auguste, T.

Z. Diveki, A. Camper, S. Haessler, T. Auguste, T. Ruchon, B. Carre, P. Salieres, R. Guichard, J. Caillat, A. Maquet, and R. Taieb, “Spectrally resolved multi-channel contributions to the harmonic emission in N2,” New J. Phys. 14, 023062 (2012).
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Baker, S.

S. Baker, J. S. Robinson, M. Lein, C. C. Chirila, R. Torres, H. C. Bandulet, D. Comtois, J. C. Kieffer, D. M. Villeneuve, J. W. G. Tisch, and J. P. Marangos, “Dynamic two-center interference in high-order harmonic generation from molecules with attosecond nuclear motion,” Phys. Rev. Lett. 101, 053901 (2008).
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S. Baker, J. S. Robinson, C. A. Haworth, H. Teng, R. A. Smith, C. C. Chirila, M. Lein, J. W. G. Tisch, and J. P. Marangos, “Probing proton dynamics in molecules on an attosecond time scale,” Science 312, 424–427 (2006).
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Bandrauk, A.

S. Chelkowski, A. Conjusteau, T. Zuo, and A. Bandrauk, “Dissociative ionization of H2+ in an intense laser field: charge-resonance-enhanced ionization, Coulomb explosion, and harmonic generation at 600  nm,” Phys. Rev. A 54, 3235–3244 (1996).
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Bandrauk, A. D.

X.-B. Bian and A. D. Bandrauk, “Probing nuclear motion by frequency modulation of molecular high-order harmonic generation,” Phys. Rev. Lett. 113, 193901 (2014).
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I. Bocharova, R. Karimi, E. F. Penka, J.-P. Brichta, P. Lassonde, X. Fu, J.-C. Kieffer, A. D. Bandrauk, I. Litvinyuk, J. Sanderson, and F. Legare, “Charge resonance enhanced ionization of CO2 probed by laser Coulomb explosion imaging,” Phys. Rev. Lett. 107, 063201 (2011).
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G. L. Yudin, S. Chelkowski, J. Itatani, A. D. Bandrauk, and P. B. Corkum, “Attosecond photoionization of coherently coupled electronic states,” Phys. Rev. A 72, 051401(R) (2005).
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T. Zuo and A. D. Bandrauk, “Charge-resonance-enhanced ionization of diatomic molecular ion by intense laser fields,” Phys. Rev. A 52, R2511–R2514 (1995).
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T. Zuo, S. Chelkowski, and A. D. Bandrauk, “Photon-emission spectra of the H2+ molecular ion in an intense laser field,” Phys. Rev. A 49, 3943–3953 (1994).
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T. Zuo, S. Chelkowski, and A. D. Bandrauk, “Harmonic generation by the H2+ molecular ion in intense laser fields,” Phys. Rev. A 48, 3837–3844 (1993).
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Bandulet, H. C.

S. Baker, J. S. Robinson, M. Lein, C. C. Chirila, R. Torres, H. C. Bandulet, D. Comtois, J. C. Kieffer, D. M. Villeneuve, J. W. G. Tisch, and J. P. Marangos, “Dynamic two-center interference in high-order harmonic generation from molecules with attosecond nuclear motion,” Phys. Rev. Lett. 101, 053901 (2008).
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Becker, A.

M. R. Miller, A. Jaroń-Becker, and A. Becker, “High harmonic spectroscopy of laser-driven nonadiabatic electron dynamics in the hydrogen molecular ion,” Phys. Rev. A 93, 013406 (2016).
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N. Takemoto and A. Becker, “Time-resolved view on charge-resonance-enhanced ionization,” Phys. Rev. A 84, 023401 (2011).
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N. Takemoto and A. Becker, “Visualization and interpretation of attosecond electron dynamics in laser-driven hydrogen molecular ion using Bohmian trajectories,” J. Chem. Phys. 134, 074309 (2011).
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M. Odenweller, N. Takemoto, A. Vredenborg, K. Cole, K. Pahl, J. Titze, L. P. Schmidt, T. Jahnke, R. Dörner, and A. Becker, “Strong field emission from fixed in space H2+,” Phys. Rev. Lett. 107, 143004 (2011).
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N. Takemoto and A. Becker, “Multiple ionization bursts in laser-driven hydrogen molecular ion,” Phys. Rev. Lett. 105, 203004 (2010).
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F. He, A. Becker, and U. Thumm, “Strong-field modulated diffraction effects in the correlated electron-nuclear motion in dissociating H2+,” Phys. Rev. Lett. 101, 213002 (2008).
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M. F. Ciappina, A. Becker, and A. Jaron-Becker, “Multislit interference patterns in high-order harmonic generation in C60,” Phys. Rev. A 76, 063406 (2007).
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A. Jaroń-Becker, A. Becker, and F. H. M. Faisal, “Saturated ionization of fullerenes in intense laser fields,” Phys. Rev. Lett. 96, 143006 (2006).
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J. Muth-Böhm, A. Becker, and F. H. M. Faisal, “Suppressed molecular ionization for a class of diatomics in intense femtosecond laser fields,” Phys. Rev. Lett. 85, 2280–2283 (2000).
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C. Vozzi, F. Calegari, E. Benedetti, J. P. Caumes, G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel, N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, “Controlling two-center interference in molecular high harmonic generation,” Phys. Rev. Lett. 95, 153902 (2005).
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H. J. Wörner, J. P. Bertand, D. V. Kartashov, P. B. Corkum, and D. M. Villeneuve, “Following a chemical reaction using high-harmonic interferometry,” Nature 466, 604–607 (2010).
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H. J. Wörner, J. B. Bertrand, B. Fabre, J. Higuet, H. Ruf, A. Dubrouil, S. Patchkovskii, M. Spanner, Y. Mairesse, V. Blanchet, E. Mevel, E. Constant, P. B. Corkum, and D. M. Villeneuve, “Conical intersection dynamics in NO2 probed by homodyne high-harmonic spectroscopy,” Science 334, 208–212 (2011).
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H. J. Wörner, J. B. Bertrand, P. Hockett, P. B. Corkum, and D. M. Villeneuve, “Controlling the interference of multiple molecular orbitals in high-harmonic generation,” Phys. Rev. Lett. 104, 233904 (2010).
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Bian, X.-B.

X.-B. Bian and A. D. Bandrauk, “Probing nuclear motion by frequency modulation of molecular high-order harmonic generation,” Phys. Rev. Lett. 113, 193901 (2014).
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P. Eckle, M. Smolarski, P. Schlup, J. Biegert, A. Staudte, M. Schöffler, J. G. Muller, R. Dörner, and U. Keller, “Attosecond angular streaking,” Nat. Phys. 4, 565–570 (2008).
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H. J. Wörner, J. B. Bertrand, B. Fabre, J. Higuet, H. Ruf, A. Dubrouil, S. Patchkovskii, M. Spanner, Y. Mairesse, V. Blanchet, E. Mevel, E. Constant, P. B. Corkum, and D. M. Villeneuve, “Conical intersection dynamics in NO2 probed by homodyne high-harmonic spectroscopy,” Science 334, 208–212 (2011).
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M. Lezius, V. Blanchet, M. Y. Ivanov, and A. Stolow, “Polyatomic molecules in strong laser fields: nonadiabatic multielectron dynamics,” J. Chem. Phys. 117, 1575–1588 (2002).
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M. Lezius, V. Blanchet, D. M. Rayner, D. M. Villeneuve, A. Stolow, and M. Y. Ivanov, “Nonadiabatic multielectron dynamics in strong field molecular ionization,” Phys. Rev. Lett. 86, 51–54 (2001).
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Bocharova, I.

I. Bocharova, R. Karimi, E. F. Penka, J.-P. Brichta, P. Lassonde, X. Fu, J.-C. Kieffer, A. D. Bandrauk, I. Litvinyuk, J. Sanderson, and F. Legare, “Charge resonance enhanced ionization of CO2 probed by laser Coulomb explosion imaging,” Phys. Rev. Lett. 107, 063201 (2011).
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M. Spanner, J. Mikosch, A. Gijsberten, A. E. Boguslavskiy, and A. Stolow, “Multielectron effects and nonadiabatic electronic dynamics in above threshold ionization and high-harmonic generation,” New J. Phys. 13, 093010 (2011).
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J. A. Wheeler, A. Borot, S. Monchocé, H. Vincenti, A. Ricci, A. Malvache, R. Lopez-Martens, and F. Quéré, “Attosecond lighthouses from plasma mirrors,” Nat. Photonics 6, 829–833 (2012).
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W. Boutu, S. Haessler, H. Merdij, P. Breger, G. Waters, M. Stankiewicz, L. J. Frasinski, R. Taieb, J. Caillat, A. Maquet, P. Manchicourt, B. Carre, and P. Salieres, “Coherent control of attosecond emission from aligned molecules,” Nat. Phys. 4, 545–549 (2008).
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W. Boutu, S. Haessler, H. Merdij, P. Breger, G. Waters, M. Stankiewicz, L. J. Frasinski, R. Taieb, J. Caillat, A. Maquet, P. Manchicourt, B. Carre, and P. Salieres, “Coherent control of attosecond emission from aligned molecules,” Nat. Phys. 4, 545–549 (2008).
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Brichta, J.-P.

I. Bocharova, R. Karimi, E. F. Penka, J.-P. Brichta, P. Lassonde, X. Fu, J.-C. Kieffer, A. D. Bandrauk, I. Litvinyuk, J. Sanderson, and F. Legare, “Charge resonance enhanced ionization of CO2 probed by laser Coulomb explosion imaging,” Phys. Rev. Lett. 107, 063201 (2011).
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Caillat, J.

Z. Diveki, A. Camper, S. Haessler, T. Auguste, T. Ruchon, B. Carre, P. Salieres, R. Guichard, J. Caillat, A. Maquet, and R. Taieb, “Spectrally resolved multi-channel contributions to the harmonic emission in N2,” New J. Phys. 14, 023062 (2012).
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C. Vozzi, F. Calegari, E. Benedetti, J. P. Caumes, G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel, N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, “Controlling two-center interference in molecular high harmonic generation,” Phys. Rev. Lett. 95, 153902 (2005).
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Z. Diveki, A. Camper, S. Haessler, T. Auguste, T. Ruchon, B. Carre, P. Salieres, R. Guichard, J. Caillat, A. Maquet, and R. Taieb, “Spectrally resolved multi-channel contributions to the harmonic emission in N2,” New J. Phys. 14, 023062 (2012).
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Z. Diveki, A. Camper, S. Haessler, T. Auguste, T. Ruchon, B. Carre, P. Salieres, R. Guichard, J. Caillat, A. Maquet, and R. Taieb, “Spectrally resolved multi-channel contributions to the harmonic emission in N2,” New J. Phys. 14, 023062 (2012).
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W. Boutu, S. Haessler, H. Merdij, P. Breger, G. Waters, M. Stankiewicz, L. J. Frasinski, R. Taieb, J. Caillat, A. Maquet, P. Manchicourt, B. Carre, and P. Salieres, “Coherent control of attosecond emission from aligned molecules,” Nat. Phys. 4, 545–549 (2008).
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C. Vozzi, F. Calegari, E. Benedetti, J. P. Caumes, G. Sansone, S. Stagira, M. Nisoli, R. Torres, E. Heesel, N. Kajumba, J. P. Marangos, C. Altucci, and R. Velotta, “Controlling two-center interference in molecular high harmonic generation,” Phys. Rev. Lett. 95, 153902 (2005).
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Chelkowski, S.

G. L. Yudin, S. Chelkowski, J. Itatani, A. D. Bandrauk, and P. B. Corkum, “Attosecond photoionization of coherently coupled electronic states,” Phys. Rev. A 72, 051401(R) (2005).
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S. Chelkowski, A. Conjusteau, T. Zuo, and A. Bandrauk, “Dissociative ionization of H2+ in an intense laser field: charge-resonance-enhanced ionization, Coulomb explosion, and harmonic generation at 600  nm,” Phys. Rev. A 54, 3235–3244 (1996).
[Crossref]

T. Zuo, S. Chelkowski, and A. D. Bandrauk, “Photon-emission spectra of the H2+ molecular ion in an intense laser field,” Phys. Rev. A 49, 3943–3953 (1994).
[Crossref]

T. Zuo, S. Chelkowski, and A. D. Bandrauk, “Harmonic generation by the H2+ molecular ion in intense laser fields,” Phys. Rev. A 48, 3837–3844 (1993).
[Crossref]

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A. Talebpour, C.-Y. Chien, Y. Liang, S. Larochelle, and S. L. Chin, “Non-sequential ionization of Xe and Kr in an intense femtosecond Ti:sapphire laser pulse,” J. Phys. B 30, 1721–1730 (1997).

Chin, S. L.

A. Talebpour, C.-Y. Chien, Y. Liang, S. Larochelle, and S. L. Chin, “Non-sequential ionization of Xe and Kr in an intense femtosecond Ti:sapphire laser pulse,” J. Phys. B 30, 1721–1730 (1997).

Chirila, C. C.

S. Baker, J. S. Robinson, M. Lein, C. C. Chirila, R. Torres, H. C. Bandulet, D. Comtois, J. C. Kieffer, D. M. Villeneuve, J. W. G. Tisch, and J. P. Marangos, “Dynamic two-center interference in high-order harmonic generation from molecules with attosecond nuclear motion,” Phys. Rev. Lett. 101, 053901 (2008).
[Crossref]

S. Baker, J. S. Robinson, C. A. Haworth, H. Teng, R. A. Smith, C. C. Chirila, M. Lein, J. W. G. Tisch, and J. P. Marangos, “Probing proton dynamics in molecules on an attosecond time scale,” Science 312, 424–427 (2006).
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N. L. Wagner, A. Wüst, I. P. Christov, T. Popmintchev, X. Zhou, M. M. Murnane, and H. C. Kapteyn, “Monitoring molecular dynamics using coherent electrons from high harmonic generation,” Proc. Natl. Acad. Sci. U.S.A. 103, 13279–13285 (2006).
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Ciappina, M. F.

M. F. Ciappina, A. Becker, and A. Jaron-Becker, “Multislit interference patterns in high-order harmonic generation in C60,” Phys. Rev. A 76, 063406 (2007).
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Cohen, H. D.

H. D. Cohen and U. Fano, “Interference in the photo-ionization of molecules,” Phys. Rev. 150, 30–33 (1966).
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M. Odenweller, N. Takemoto, A. Vredenborg, K. Cole, K. Pahl, J. Titze, L. P. Schmidt, T. Jahnke, R. Dörner, and A. Becker, “Strong field emission from fixed in space H2+,” Phys. Rev. Lett. 107, 143004 (2011).
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Comtois, D.

S. Baker, J. S. Robinson, M. Lein, C. C. Chirila, R. Torres, H. C. Bandulet, D. Comtois, J. C. Kieffer, D. M. Villeneuve, J. W. G. Tisch, and J. P. Marangos, “Dynamic two-center interference in high-order harmonic generation from molecules with attosecond nuclear motion,” Phys. Rev. Lett. 101, 053901 (2008).
[Crossref]

Conjusteau, A.

S. Chelkowski, A. Conjusteau, T. Zuo, and A. Bandrauk, “Dissociative ionization of H2+ in an intense laser field: charge-resonance-enhanced ionization, Coulomb explosion, and harmonic generation at 600  nm,” Phys. Rev. A 54, 3235–3244 (1996).
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Figures (10)

Fig. 1.
Fig. 1.

Ionization and fragmentation patterns represented by the mass spectra of hexatriene, decatetraene, and β -carotene for the interaction with laser pulses at 800 and 1450 nm. Figure reprinted with permission from Lezius et al., Phys. Rev. Lett., 86, 51 (2001) [16]. Copyright 2001 by the American Physical Society. http://journals.aps.org/prl/abstract/10.1103/PhysRevLett.86.51

Fig. 2.
Fig. 2.

Results of time-dependent Hartree–Fock simulations for the interaction of the anthracene 1 + cation with strong electric fields of different intensities. The instantaneous dipole response in each case shows a nonadiabatic behavior, and the frequency composition of the residual dipole moment is determined by the field strength used. The total pulsewidth of the laser field is 7    fs . Reprinted with permission from Smith et al., J. Phys. Chem. A, 111, 6920 (2007) [24]. Copyright 2007 by the American Physical Society.

Fig. 3.
Fig. 3.

High harmonic spectra showing fractional harmonics for (a)  NO 2 at 400 nm, 10 14    W cm 2 , and 40 fs pulse length; (b)  CO 2 + at 350 nm, 10 14    W cm 2 , and 34 fs; and (c)  C 2 H 4 + at 400 nm, 10 14    W cm 2 , and 18 fs [28].

Fig. 4.
Fig. 4.

Charge-resonance-enhanced ionization in H 2 + is attributable to the energy level structure of the two lowest states of H 2 + , which are pictured at a peak field strength of 10 14    W cm 2 when (a)  R 0 = 6.0 , (b)  R 0 = 10.0 , and (c)  R 0 = 14.0    a.u. along the laser polarization axis z . In (d), theoretical predictions for the ionization rate for a 10 14    W cm 2 , 1064 nm laser source spanning an interval of internuclear distances. Figures adapted with permission from Zuo and Bandrauk, Phys. Rev. A, 52, R2511 (1995) [14]. Copyright 1995 by the American Physical Society.

Fig. 5.
Fig. 5.

Theoretical predictions of the ionization rate of (a) hydrogen and (b)  H 2 + with R 0 = 7.0 are pictured when driven by 800 nm light with peak intensity 6 × 10 13    W cm 2 . In hydrogen, ionization is observed to peak when the electric field (red dashed line) is strongest. In contrast, H 2 + evidences discrete bursts of ionization with strong suppression during the electric field maxima. Figure adapted with permission from Takemoto and Becker, Phys. Rev. Lett., 105, 203004 (2010) [39]. Copyright 2010 by the American Physical Society.

Fig. 6.
Fig. 6.

Wigner distribution of the electron wavefunction of H 2 + shows the transfer of electron population between nuclear wells, and is depicted for six instances of time spanning a quarter cycle of the driving field, beginning with E ( t ) = 0 in panel (a) and concluding with E ( t ) = E max in panel (f). The respective snapshots are taken at times (in field cycles) (a)  t = 0.500 , (b)  t = 0.450 , (c)  t = 0.400 , (d)  t = 0.351 , (e)  t = 0.301 , and (f)  t = 0.251 . Red sections in the distribution indicate areas where the electron is likely to be found. Figure reprinted with permission from Takemoto and Becker, Phys. Rev. A, 84, 023401 (2011) [40]. Copyright 2011 by the American Physical Society. http://journals.aps.org/pra/abstract/10.1103/PhysRevA.84.023401

Fig. 7.
Fig. 7.

Bohmian trajectories visualize the behavior of the electron when driven by an intense laser field. In (a), quantum trajectories near protons located at z = ± 3.5    a.u. are plotted over the central field cycle, demonstrating bursts of ionization at time points A–D. Absorbing departing electron trajectories at 7 a.u. isolates intramolecular dynamics from rescattering trajectories, clarifying the transient localization of the electron. The laser field driving this behavior is reproduced in (c). Reprinted with permission from Takemoto and Becker, J. Chem. Phys., 134, 074309 (2011) [41]. Copyright 2011, AIP Publishing LLC.

Fig. 8.
Fig. 8.

Rotation of the PMD due to nonadiabatic dynamics that shift the timing of ionization. In (a), the experimental PMD from H 2 + is shown integrated over the internuclear coordinate and p z directions. In (b), experimental results (blue circles) and TDSE predictions (red squares) for the angular displacement of the PMD are shown in comparison with the quasi-static ionization prediction (dashed line). The results of further theoretical studies in (c) indicate that the angular displacement of the PMD of H 2 + (solid black line) is sensitive to the wavelength of the driving field used due to transient electron localization, in contrast to adiabatically responsive atomic hydrogen (red dashed line). Panels (a) and (b) reprinted with permission from Odenweller et al., Phys. Rev. Lett., 107, 143004 (2011) [49]. Copyright 2011 by the American Physical Society. http://journals.aps.org/prl/abstract/10.1103/PhysRevLett.107.143004. Panel (c) reprinted with permission from He et al., Phys. Rev. A, 91, 063413 (2015) [50]. Copyright 2015 by the American Physical Society. http://journals.aps.org/pra/abstract/10.1103/PhysRevA.91.063413

Fig. 9.
Fig. 9.

Subsequent to UV-laser-induced population of the dissociating 2 p σ u state, H 2 + is driven with an IR laser source with a profile as shown in (a). The electron density occupying the positive (red dashed line) and negative (black solid line) spatial regions is shown during and following interaction with a laser field of intensity (b)  3 × 10 12    W cm 2 , (c)  2 × 10 13    W cm 2 , and (d)  10 14    W cm 2 . Comparison of results following field interaction (e.g., at 10 fs) shows that the dissociation product distribution is highly influenced by the laser intensity selected due to the participation of transient electron localization. Figure reprinted with permission from He et al., Phys. Rev. Lett., 101, 213002 (2008) [42]. Copyright 2008 by the American Physical Society. http://journals.aps.org/prl/abstract/10.1103/PhysRevLett.101.213002

Fig. 10.
Fig. 10.

Theoretical calculations of the HHG spectrum emitted by fixed nuclei H 2 + at R 0 = 7.0 driven by a 1400 nm, 20-cycle full width source with intensity 6 × 10 13    W cm 2 are shown in (a). The position of the minimum is marked by the dashed line; the overall modulation of the high-energy plateau is demonstrated by lines superimposed above the spectrum. In (b), the temporal origin of the minimum is investigated through a time-frequency analysis (TFA) of emission during recombination throughout a center cycle of the driving field. A minimum is found in the TFA at the same energetic location as the full HHG spectrum. (c) A classical analysis maps emission at recombination to approximate the moment of ionization of the electron wavepacket, enabling reconstruction of the electron density (d) during ionization corresponding to times of recombination in the TFA. The minimum feature is seen to coincide with maximal localization upon the downhill well. Panels (a) and (b) adapted with permission from Miller et al., Phys. Rev. A, 93, 013406 (2016) [71]. Copyright 2016 by the American Physical Society.

Equations (5)

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W ( z , p z ; t ) = 1 π ρ d ρ d R d y Ψ * ( R , z + y , ρ ; t ) × Ψ ( R , z y , ρ ; t ) exp ( 2 i p z y ) .
d z j d t = v ( z j ( t ) , t ) = S ( z j , t ) z .
Ψ ( z , t ) = C ( z , t ) exp ( i S ( z , t ) ) ,
A ( t loc ) = m π + ξ 2 d g u , with    m = 0 , ± 1 , ± 2 , .
C ( t 0 , ω ) = 1 2 π 0 T d a z ( t ) W ( ω ( t t 0 ) 2 π ) d t ,

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