Abstract

Novel feature of high order harmonic generation process for molecules is presented for several molecules at their equilibrium geometries. The high order harmonic spectra reveal additional sidebands for each odd harmonic, which are a consequence of the resonant coupling of two valence orbitals, a mechanism analogous to Mollow triplets known from quantum optics. Strong modification of the high order harmonic generation process is illustrated with time frequency analysis in which there appear additional minima dependent on the Rabi frequency for the corresponding transition. The orbital coupling further leads to the modification of the electron dynamics which is presented using total electron density difference maps.

© 2016 Optical Society of America

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References

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2015 (1)

D. Popmintchev, C. Hernandez-Garcia, F. Dollar, C. Mancuso, J. Perez-Hernndez, M. C. Chen, A. Hankla, X. Gao, B. Shim, A. Gaeta, M. Tarazkar, D. Romanov, R. Levis, J. Gaffney, M. Foord, S. Libby, A. Jaron-Becker, A. Becker, L. Plaja, M. Murnane, H. Kapteyn, and T. Popmintchev, “Efficient soft X-ray high harmonic generation in multiply- ionized plasmas: the ultraviolet surprise,” Science 3501225–123131 (2015).
[Crossref]

2014 (3)

M.-C. Chen, C. Mancuso, C. Hernandez-Garcia, F. Dollar, B. Galloway, D. Popmintchev, P.-C. Huang, B. Walker, L. Plaja, A. A. Jaron-Becker, A. Becker, M. M. Murnane, H. C. Kapteyn, and T. Popmintchev, “Generation of bright isolated attosecond soft X-ray pulses driven by multicycle midinfrared lasers,” Proc. Nat. Acad. Sciences U.S.A. 111, E2361–E2367 (2014).
[Crossref]

D. Baykusheva, P. M. Kraus, S. B. Zhang, N. Rohringer, and H. J. Wörner, “The sensitivities of high-harmonic generation and strong-field ionization to coupled electronic and nuclear dynamics,” Faraday Discuss. 171, 113–132 (2014).
[Crossref] [PubMed]

Y. Xia and A. Jaron-Becker, “Multielectron contributions in elliptically polarized high-order harmonic emission from nitrogen molecule,” Opt. Lett. 39, 1461–1464 (2014).
[Crossref] [PubMed]

2013 (1)

I. Lopez-Quintas, M. Oujja, M. Sanz, M. Martin, R. A. Ganeev, and M. Castillejo, “Low-order harmonic generation in nanosecond laser ablation plasmas of carbon containing materials,” Appl. Surf. Sci. 27833–37 (2013).
[Crossref]

2012 (3)

T. Popmintchev, M.-C. Chen, D. Popmintchev, P. Arpin, S. Brown, S. Alisauskas, G. Andriukaitis, T. Balciunas, O.D. Mücke, A. Pugzlys, A. Baltuska, B. Shim, S. E. Schrauth, A. Gaeta, C. Hernandez-Garcia, L. Plaja, A. Becker, A. Jaron-Becker, M. M. Murnane, and H. C. Kapteyn, “Bright Coherent Ultrahigh Harmonics in the keV X-ray Regime from Mid-Infrared Femtosecond Lasers,” Science 91, 1287–1291 (2012).
[Crossref]

D. Dundas, “Multielectron effects in high harmonic generation in N2 and benzene: Simulation using a non-adiabatic quantum molecular dynamics approach for laser-molecule interactions,” J. Chem. Phys. 136, 194303 (2012).
[Crossref]

E. Luppi and M. Head-Gordon, “Computation of high-harmonic generation spectra of H2 And N2 in intense laser pulses using quantum chemistry methods and time-dependent density functional theory,” Mol. Phys. 110909–923 (2012).
[Crossref]

2011 (2)

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

H. J. Wörner, J. B. Bertrand, B. Fabre, J. Hiquet, H. Ruf, A. A. Dubrouil, S. Patchkovskii, M. Spanner, Y. Mairesse, V. Blanchet, E. Mvel, 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]

2010 (8)

A. Etches and L. B. Madsen, “Extending the strong-eld approximation of high-order harmonic generation to polar molecules: gating mechanisms and extension of the harmonic cutoff,” J. Phys. B 43155602 (2010).
[Crossref]

E. PenkaFowe and Andre D. Bandrauk, “Nonlinear time-dependent density-functional-theory study of ionization and harmonic generation in CO2 by ultrashort intense laser pulses: orientational effects,” Phys. Rev. A 81, 023411 (2010).
[Crossref]

D. B. Milosevic, “Resonant high-order harmonic generation from plasma ablation: Laser intensity dependence of the harmonic intensity and phase,” Phys. Rev. A 81, 023802 (2010).
[Crossref]

V. Strelkov, “Role of Autoionizing State in Resonant High-Order Harmonic Generation and Attosecond Pulse Production,” Phys. Rev. Lett. 104, 123901 (2010).
[Crossref] [PubMed]

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

Y. Mairesse, J. Higuet, N. Dudovich, D. Shafir, B. Fabre, E. Mevel, E. Constant, S. Patchkovskii, Z. Walters, M.Yu. Ivanov, and O. Smirnova, “High harmonic spectroscopy of multichannel dynamics in strong-field ionization,” Phys. Rev. Lett. 104, 213601 (2010).
[Crossref] [PubMed]

A.-T. Le, R. R. Lucchese, and C. D. Lin, “Polarization and ellipticity of high-order harmonics from aligned molecules generated by linearly polarized intense laser pulses,” Phys. Rev. A 82, 023814 (2010).
[Crossref]

S.-K. Son, D. A. Telnow, and S. I. Chu, “Probing the origin of elliptical high-order harmonic generation from aligned molecules in linearly polarized laser fields,” Phys. Rev. A 82, 043829 (2010).
[Crossref]

2009 (3)

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

C. Figueira de Morisson Faria, “One and two-center processes in high-order harmonic generation in diatomic molecules: Influence of the internuclear separation,” Laser Phys. 19, 797–804 (2009).
[Crossref]

D. B. Milosevic, E. Hasovic, S. Odzak, M. Busuladzic, A. Gazibegovic-Busuladzic, and W. Becker, “New results in above-threshold ionization and high-order harmonic generation of atomic and molecular systems,” Laser Phys. 19, 185–190 (2009).
[Crossref]

2008 (4)

M. F. Ciappina, A. Becker, and A. Jaron-Becker, “High-order harmonic generation in fullerenes with icosahedral symmetry,” Phys. Rev. A 78, 063405 (2008).
[Crossref]

X. B. 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] [PubMed]

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

2007 (2)

M. Lein, “Molecular imaging using recolliding electrons,” J. Phys. B: At. Mol. Opt. Phys. 40, R135–R173 (2007).
[Crossref]

D. B. Milosevic, “High-energy stimulated emission from plasma ablation pumped by resonant high-order harmonic generation,” J. Phys. B 40, 3367–3376 (2007).
[Crossref]

2006 (1)

2005 (2)

2001 (2)

M. Hentschel, R. Kienberger, Ch. Spielmann, G. A. Reider, N. Milosevic, T. Brabec, P. Corkum, U. Heinzmann, M. Drescher, and F. Krausz, “Attosecond metrology,” Nature 414, 509–513 (2001).
[Crossref] [PubMed]

P. M. Paul, E. S. Toma, P. Breger, G. Mullot, F. Auge, Ph. Balcou, H. G. Muller, and P. Agostini, “Observation of a Train of Attosecond Pulses from High Harmonic Generation,” Science 292, 1689–1692 (2001).
[Crossref] [PubMed]

1997 (1)

I. P. Christov, M. M. Murnane, and H. C. Kapteyn, “High-Harmonic Generation of Attosecond Pulses in the ’Single-Cycle’ Regime,” Phys. Rev. Lett. 78, 1251–1254 (1997).
[Crossref]

1996 (2)

J. B. Watson, A. Sanpera, X. Chen, and K. Burnett, “Harmonic generation from a coherent superposition of states,” Phys. Rev. A 53, R1962–R1965 (1996).
[Crossref] [PubMed]

A. Sanpera, J. B. Watson, M. Lewenstein, and K. Burnett, “Harmonic-generation control,” Phys. Rev. A 54, 4320–4326 (1996).
[Crossref] [PubMed]

1995 (1)

T. Zuo and A. D. Bandrauk, “Charge-resonance-enhanced ionization of diatomic molecular ions by intense lasers,” Phys. Rev. A 52, R2511–R2514 (1995).
[Crossref] [PubMed]

1994 (1)

R. van Leeuwen and E. J. Baerends, “Exchange-correlation potential with correct asymptotic behavior,” Phys. Rev. A 49, 2421–2431 (1994).
[Crossref] [PubMed]

1993 (2)

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] [PubMed]

P. B. Corkum, “Plasma perspective on strong field multiphoton ionization,” Phys. Rev. Lett. 71, 1994–1998 (1993).
[Crossref] [PubMed]

1988 (1)

M. Ferray, A. L’Huillier, X.F. Li, L.A. Lompre, G. Mainfray, and C. Manus, “Multiple-harmonic conversion of 1064 nm radiation in rare gases,” J. Phys. B: At. Mol. Opt. Phys. 21, L31–L35 (1988).
[Crossref]

1987 (1)

1969 (1)

B. R. Mollow, “Power Spectrum of Light Scattered by Two-Level Systems,” Phys. Rev. 188, 1969–1975 (1969).
[Crossref]

Agostini, P.

P. M. Paul, E. S. Toma, P. Breger, G. Mullot, F. Auge, Ph. Balcou, H. G. Muller, and P. Agostini, “Observation of a Train of Attosecond Pulses from High Harmonic Generation,” Science 292, 1689–1692 (2001).
[Crossref] [PubMed]

Alisauskas, S.

T. Popmintchev, M.-C. Chen, D. Popmintchev, P. Arpin, S. Brown, S. Alisauskas, G. Andriukaitis, T. Balciunas, O.D. Mücke, A. Pugzlys, A. Baltuska, B. Shim, S. E. Schrauth, A. Gaeta, C. Hernandez-Garcia, L. Plaja, A. Becker, A. Jaron-Becker, M. M. Murnane, and H. C. Kapteyn, “Bright Coherent Ultrahigh Harmonics in the keV X-ray Regime from Mid-Infrared Femtosecond Lasers,” Science 91, 1287–1291 (2012).
[Crossref]

Andriukaitis, G.

T. Popmintchev, M.-C. Chen, D. Popmintchev, P. Arpin, S. Brown, S. Alisauskas, G. Andriukaitis, T. Balciunas, O.D. Mücke, A. Pugzlys, A. Baltuska, B. Shim, S. E. Schrauth, A. Gaeta, C. Hernandez-Garcia, L. Plaja, A. Becker, A. Jaron-Becker, M. M. Murnane, and H. C. Kapteyn, “Bright Coherent Ultrahigh Harmonics in the keV X-ray Regime from Mid-Infrared Femtosecond Lasers,” Science 91, 1287–1291 (2012).
[Crossref]

Arpin, P.

T. Popmintchev, M.-C. Chen, D. Popmintchev, P. Arpin, S. Brown, S. Alisauskas, G. Andriukaitis, T. Balciunas, O.D. Mücke, A. Pugzlys, A. Baltuska, B. Shim, S. E. Schrauth, A. Gaeta, C. Hernandez-Garcia, L. Plaja, A. Becker, A. Jaron-Becker, M. M. Murnane, and H. C. Kapteyn, “Bright Coherent Ultrahigh Harmonics in the keV X-ray Regime from Mid-Infrared Femtosecond Lasers,” Science 91, 1287–1291 (2012).
[Crossref]

Auge, F.

P. M. Paul, E. S. Toma, P. Breger, G. Mullot, F. Auge, Ph. Balcou, H. G. Muller, and P. Agostini, “Observation of a Train of Attosecond Pulses from High Harmonic Generation,” Science 292, 1689–1692 (2001).
[Crossref] [PubMed]

Baba, M.

Baerends, E. J.

R. van Leeuwen and E. J. Baerends, “Exchange-correlation potential with correct asymptotic behavior,” Phys. Rev. A 49, 2421–2431 (1994).
[Crossref] [PubMed]

Balciunas, T.

T. Popmintchev, M.-C. Chen, D. Popmintchev, P. Arpin, S. Brown, S. Alisauskas, G. Andriukaitis, T. Balciunas, O.D. Mücke, A. Pugzlys, A. Baltuska, B. Shim, S. E. Schrauth, A. Gaeta, C. Hernandez-Garcia, L. Plaja, A. Becker, A. Jaron-Becker, M. M. Murnane, and H. C. Kapteyn, “Bright Coherent Ultrahigh Harmonics in the keV X-ray Regime from Mid-Infrared Femtosecond Lasers,” Science 91, 1287–1291 (2012).
[Crossref]

Balcou, Ph.

P. M. Paul, E. S. Toma, P. Breger, G. Mullot, F. Auge, Ph. Balcou, H. G. Muller, and P. Agostini, “Observation of a Train of Attosecond Pulses from High Harmonic Generation,” Science 292, 1689–1692 (2001).
[Crossref] [PubMed]

Baltuska, A.

T. Popmintchev, M.-C. Chen, D. Popmintchev, P. Arpin, S. Brown, S. Alisauskas, G. Andriukaitis, T. Balciunas, O.D. Mücke, A. Pugzlys, A. Baltuska, B. Shim, S. E. Schrauth, A. Gaeta, C. Hernandez-Garcia, L. Plaja, A. Becker, A. Jaron-Becker, M. M. Murnane, and H. C. Kapteyn, “Bright Coherent Ultrahigh Harmonics in the keV X-ray Regime from Mid-Infrared Femtosecond Lasers,” Science 91, 1287–1291 (2012).
[Crossref]

Bandrauk, A. D.

T. Zuo and A. D. Bandrauk, “Charge-resonance-enhanced ionization of diatomic molecular ions by intense lasers,” Phys. Rev. A 52, R2511–R2514 (1995).
[Crossref] [PubMed]

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Y. Mairesse, J. Higuet, N. Dudovich, D. Shafir, B. Fabre, E. Mevel, E. Constant, S. Patchkovskii, Z. Walters, M.Yu. Ivanov, and O. Smirnova, “High harmonic spectroscopy of multichannel dynamics in strong-field ionization,” Phys. Rev. Lett. 104, 213601 (2010).
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W. Boutu, S. Haessler, H. Merdji, P. Breger, G. Waters, M. Stankiewicz, L. J. Frasinski, R. Taieb, J. Caillat, A. Maquet, P. Monchicourt, B. Carre, and P. Salieres, “Coherent control of attosecond emission from aligned molecules,” Nat. Phys. 4, 545–549 (2008).
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D. Popmintchev, C. Hernandez-Garcia, F. Dollar, C. Mancuso, J. Perez-Hernndez, M. C. Chen, A. Hankla, X. Gao, B. Shim, A. Gaeta, M. Tarazkar, D. Romanov, R. Levis, J. Gaffney, M. Foord, S. Libby, A. Jaron-Becker, A. Becker, L. Plaja, M. Murnane, H. Kapteyn, and T. Popmintchev, “Efficient soft X-ray high harmonic generation in multiply- ionized plasmas: the ultraviolet surprise,” Science 3501225–123131 (2015).
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T. Popmintchev, M.-C. Chen, D. Popmintchev, P. Arpin, S. Brown, S. Alisauskas, G. Andriukaitis, T. Balciunas, O.D. Mücke, A. Pugzlys, A. Baltuska, B. Shim, S. E. Schrauth, A. Gaeta, C. Hernandez-Garcia, L. Plaja, A. Becker, A. Jaron-Becker, M. M. Murnane, and H. C. Kapteyn, “Bright Coherent Ultrahigh Harmonics in the keV X-ray Regime from Mid-Infrared Femtosecond Lasers,” Science 91, 1287–1291 (2012).
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D. Popmintchev, C. Hernandez-Garcia, F. Dollar, C. Mancuso, J. Perez-Hernndez, M. C. Chen, A. Hankla, X. Gao, B. Shim, A. Gaeta, M. Tarazkar, D. Romanov, R. Levis, J. Gaffney, M. Foord, S. Libby, A. Jaron-Becker, A. Becker, L. Plaja, M. Murnane, H. Kapteyn, and T. Popmintchev, “Efficient soft X-ray high harmonic generation in multiply- ionized plasmas: the ultraviolet surprise,” Science 3501225–123131 (2015).
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M.-C. Chen, C. Mancuso, C. Hernandez-Garcia, F. Dollar, B. Galloway, D. Popmintchev, P.-C. Huang, B. Walker, L. Plaja, A. A. Jaron-Becker, A. Becker, M. M. Murnane, H. C. Kapteyn, and T. Popmintchev, “Generation of bright isolated attosecond soft X-ray pulses driven by multicycle midinfrared lasers,” Proc. Nat. Acad. Sciences U.S.A. 111, E2361–E2367 (2014).
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Ganeev, R. A.

I. Lopez-Quintas, M. Oujja, M. Sanz, M. Martin, R. A. Ganeev, and M. Castillejo, “Low-order harmonic generation in nanosecond laser ablation plasmas of carbon containing materials,” Appl. Surf. Sci. 27833–37 (2013).
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D. Popmintchev, C. Hernandez-Garcia, F. Dollar, C. Mancuso, J. Perez-Hernndez, M. C. Chen, A. Hankla, X. Gao, B. Shim, A. Gaeta, M. Tarazkar, D. Romanov, R. Levis, J. Gaffney, M. Foord, S. Libby, A. Jaron-Becker, A. Becker, L. Plaja, M. Murnane, H. Kapteyn, and T. Popmintchev, “Efficient soft X-ray high harmonic generation in multiply- ionized plasmas: the ultraviolet surprise,” Science 3501225–123131 (2015).
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W. Boutu, S. Haessler, H. Merdji, P. Breger, G. Waters, M. Stankiewicz, L. J. Frasinski, R. Taieb, J. Caillat, A. Maquet, P. Monchicourt, B. Carre, and P. Salieres, “Coherent control of attosecond emission from aligned molecules,” Nat. Phys. 4, 545–549 (2008).
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D. Popmintchev, C. Hernandez-Garcia, F. Dollar, C. Mancuso, J. Perez-Hernndez, M. C. Chen, A. Hankla, X. Gao, B. Shim, A. Gaeta, M. Tarazkar, D. Romanov, R. Levis, J. Gaffney, M. Foord, S. Libby, A. Jaron-Becker, A. Becker, L. Plaja, M. Murnane, H. Kapteyn, and T. Popmintchev, “Efficient soft X-ray high harmonic generation in multiply- ionized plasmas: the ultraviolet surprise,” Science 3501225–123131 (2015).
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D. B. Milosevic, E. Hasovic, S. Odzak, M. Busuladzic, A. Gazibegovic-Busuladzic, and W. Becker, “New results in above-threshold ionization and high-order harmonic generation of atomic and molecular systems,” Laser Phys. 19, 185–190 (2009).
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M. Hentschel, R. Kienberger, Ch. Spielmann, G. A. Reider, N. Milosevic, T. Brabec, P. Corkum, U. Heinzmann, M. Drescher, and F. Krausz, “Attosecond metrology,” Nature 414, 509–513 (2001).
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D. Popmintchev, C. Hernandez-Garcia, F. Dollar, C. Mancuso, J. Perez-Hernndez, M. C. Chen, A. Hankla, X. Gao, B. Shim, A. Gaeta, M. Tarazkar, D. Romanov, R. Levis, J. Gaffney, M. Foord, S. Libby, A. Jaron-Becker, A. Becker, L. Plaja, M. Murnane, H. Kapteyn, and T. Popmintchev, “Efficient soft X-ray high harmonic generation in multiply- ionized plasmas: the ultraviolet surprise,” Science 3501225–123131 (2015).
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M.-C. Chen, C. Mancuso, C. Hernandez-Garcia, F. Dollar, B. Galloway, D. Popmintchev, P.-C. Huang, B. Walker, L. Plaja, A. A. Jaron-Becker, A. Becker, M. M. Murnane, H. C. Kapteyn, and T. Popmintchev, “Generation of bright isolated attosecond soft X-ray pulses driven by multicycle midinfrared lasers,” Proc. Nat. Acad. Sciences U.S.A. 111, E2361–E2367 (2014).
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T. Popmintchev, M.-C. Chen, D. Popmintchev, P. Arpin, S. Brown, S. Alisauskas, G. Andriukaitis, T. Balciunas, O.D. Mücke, A. Pugzlys, A. Baltuska, B. Shim, S. E. Schrauth, A. Gaeta, C. Hernandez-Garcia, L. Plaja, A. Becker, A. Jaron-Becker, M. M. Murnane, and H. C. Kapteyn, “Bright Coherent Ultrahigh Harmonics in the keV X-ray Regime from Mid-Infrared Femtosecond Lasers,” Science 91, 1287–1291 (2012).
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Y. Mairesse, J. Higuet, N. Dudovich, D. Shafir, B. Fabre, E. Mevel, E. Constant, S. Patchkovskii, Z. Walters, M.Yu. Ivanov, and O. Smirnova, “High harmonic spectroscopy of multichannel dynamics in strong-field ionization,” Phys. Rev. Lett. 104, 213601 (2010).
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M.-C. Chen, C. Mancuso, C. Hernandez-Garcia, F. Dollar, B. Galloway, D. Popmintchev, P.-C. Huang, B. Walker, L. Plaja, A. A. Jaron-Becker, A. Becker, M. M. Murnane, H. C. Kapteyn, and T. Popmintchev, “Generation of bright isolated attosecond soft X-ray pulses driven by multicycle midinfrared lasers,” Proc. Nat. Acad. Sciences U.S.A. 111, E2361–E2367 (2014).
[Crossref]

T. Popmintchev, M.-C. Chen, D. Popmintchev, P. Arpin, S. Brown, S. Alisauskas, G. Andriukaitis, T. Balciunas, O.D. Mücke, A. Pugzlys, A. Baltuska, B. Shim, S. E. Schrauth, A. Gaeta, C. Hernandez-Garcia, L. Plaja, A. Becker, A. Jaron-Becker, M. M. Murnane, and H. C. Kapteyn, “Bright Coherent Ultrahigh Harmonics in the keV X-ray Regime from Mid-Infrared Femtosecond Lasers,” Science 91, 1287–1291 (2012).
[Crossref]

Popmintchev, D.

D. Popmintchev, C. Hernandez-Garcia, F. Dollar, C. Mancuso, J. Perez-Hernndez, M. C. Chen, A. Hankla, X. Gao, B. Shim, A. Gaeta, M. Tarazkar, D. Romanov, R. Levis, J. Gaffney, M. Foord, S. Libby, A. Jaron-Becker, A. Becker, L. Plaja, M. Murnane, H. Kapteyn, and T. Popmintchev, “Efficient soft X-ray high harmonic generation in multiply- ionized plasmas: the ultraviolet surprise,” Science 3501225–123131 (2015).
[Crossref]

M.-C. Chen, C. Mancuso, C. Hernandez-Garcia, F. Dollar, B. Galloway, D. Popmintchev, P.-C. Huang, B. Walker, L. Plaja, A. A. Jaron-Becker, A. Becker, M. M. Murnane, H. C. Kapteyn, and T. Popmintchev, “Generation of bright isolated attosecond soft X-ray pulses driven by multicycle midinfrared lasers,” Proc. Nat. Acad. Sciences U.S.A. 111, E2361–E2367 (2014).
[Crossref]

T. Popmintchev, M.-C. Chen, D. Popmintchev, P. Arpin, S. Brown, S. Alisauskas, G. Andriukaitis, T. Balciunas, O.D. Mücke, A. Pugzlys, A. Baltuska, B. Shim, S. E. Schrauth, A. Gaeta, C. Hernandez-Garcia, L. Plaja, A. Becker, A. Jaron-Becker, M. M. Murnane, and H. C. Kapteyn, “Bright Coherent Ultrahigh Harmonics in the keV X-ray Regime from Mid-Infrared Femtosecond Lasers,” Science 91, 1287–1291 (2012).
[Crossref]

Popmintchev, T.

D. Popmintchev, C. Hernandez-Garcia, F. Dollar, C. Mancuso, J. Perez-Hernndez, M. C. Chen, A. Hankla, X. Gao, B. Shim, A. Gaeta, M. Tarazkar, D. Romanov, R. Levis, J. Gaffney, M. Foord, S. Libby, A. Jaron-Becker, A. Becker, L. Plaja, M. Murnane, H. Kapteyn, and T. Popmintchev, “Efficient soft X-ray high harmonic generation in multiply- ionized plasmas: the ultraviolet surprise,” Science 3501225–123131 (2015).
[Crossref]

M.-C. Chen, C. Mancuso, C. Hernandez-Garcia, F. Dollar, B. Galloway, D. Popmintchev, P.-C. Huang, B. Walker, L. Plaja, A. A. Jaron-Becker, A. Becker, M. M. Murnane, H. C. Kapteyn, and T. Popmintchev, “Generation of bright isolated attosecond soft X-ray pulses driven by multicycle midinfrared lasers,” Proc. Nat. Acad. Sciences U.S.A. 111, E2361–E2367 (2014).
[Crossref]

T. Popmintchev, M.-C. Chen, D. Popmintchev, P. Arpin, S. Brown, S. Alisauskas, G. Andriukaitis, T. Balciunas, O.D. Mücke, A. Pugzlys, A. Baltuska, B. Shim, S. E. Schrauth, A. Gaeta, C. Hernandez-Garcia, L. Plaja, A. Becker, A. Jaron-Becker, M. M. Murnane, and H. C. Kapteyn, “Bright Coherent Ultrahigh Harmonics in the keV X-ray Regime from Mid-Infrared Femtosecond Lasers,” Science 91, 1287–1291 (2012).
[Crossref]

Pugzlys, A.

T. Popmintchev, M.-C. Chen, D. Popmintchev, P. Arpin, S. Brown, S. Alisauskas, G. Andriukaitis, T. Balciunas, O.D. Mücke, A. Pugzlys, A. Baltuska, B. Shim, S. E. Schrauth, A. Gaeta, C. Hernandez-Garcia, L. Plaja, A. Becker, A. Jaron-Becker, M. M. Murnane, and H. C. Kapteyn, “Bright Coherent Ultrahigh Harmonics in the keV X-ray Regime from Mid-Infrared Femtosecond Lasers,” Science 91, 1287–1291 (2012).
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Reider, G. A.

M. Hentschel, R. Kienberger, Ch. Spielmann, G. A. Reider, N. Milosevic, T. Brabec, P. Corkum, U. Heinzmann, M. Drescher, and F. Krausz, “Attosecond metrology,” Nature 414, 509–513 (2001).
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Rhodes, C. K.

Rohringer, N.

D. Baykusheva, P. M. Kraus, S. B. Zhang, N. Rohringer, and H. J. Wörner, “The sensitivities of high-harmonic generation and strong-field ionization to coupled electronic and nuclear dynamics,” Faraday Discuss. 171, 113–132 (2014).
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D. Popmintchev, C. Hernandez-Garcia, F. Dollar, C. Mancuso, J. Perez-Hernndez, M. C. Chen, A. Hankla, X. Gao, B. Shim, A. Gaeta, M. Tarazkar, D. Romanov, R. Levis, J. Gaffney, M. Foord, S. Libby, A. Jaron-Becker, A. Becker, L. Plaja, M. Murnane, H. Kapteyn, and T. Popmintchev, “Efficient soft X-ray high harmonic generation in multiply- ionized plasmas: the ultraviolet surprise,” Science 3501225–123131 (2015).
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H. J. Wörner, J. B. Bertrand, B. Fabre, J. Hiquet, H. Ruf, A. A. Dubrouil, S. Patchkovskii, M. Spanner, Y. Mairesse, V. Blanchet, E. Mvel, 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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Salieres, P.

W. Boutu, S. Haessler, H. Merdji, P. Breger, G. Waters, M. Stankiewicz, L. J. Frasinski, R. Taieb, J. Caillat, A. Maquet, P. Monchicourt, B. Carre, and P. Salieres, “Coherent control of attosecond emission from aligned molecules,” Nat. Phys. 4, 545–549 (2008).
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J. B. Watson, A. Sanpera, X. Chen, and K. Burnett, “Harmonic generation from a coherent superposition of states,” Phys. Rev. A 53, R1962–R1965 (1996).
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A. Sanpera, J. B. Watson, M. Lewenstein, and K. Burnett, “Harmonic-generation control,” Phys. Rev. A 54, 4320–4326 (1996).
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I. Lopez-Quintas, M. Oujja, M. Sanz, M. Martin, R. A. Ganeev, and M. Castillejo, “Low-order harmonic generation in nanosecond laser ablation plasmas of carbon containing materials,” Appl. Surf. Sci. 27833–37 (2013).
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T. Popmintchev, M.-C. Chen, D. Popmintchev, P. Arpin, S. Brown, S. Alisauskas, G. Andriukaitis, T. Balciunas, O.D. Mücke, A. Pugzlys, A. Baltuska, B. Shim, S. E. Schrauth, A. Gaeta, C. Hernandez-Garcia, L. Plaja, A. Becker, A. Jaron-Becker, M. M. Murnane, and H. C. Kapteyn, “Bright Coherent Ultrahigh Harmonics in the keV X-ray Regime from Mid-Infrared Femtosecond Lasers,” Science 91, 1287–1291 (2012).
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Y. Mairesse, J. Higuet, N. Dudovich, D. Shafir, B. Fabre, E. Mevel, E. Constant, S. Patchkovskii, Z. Walters, M.Yu. Ivanov, and O. Smirnova, “High harmonic spectroscopy of multichannel dynamics in strong-field ionization,” Phys. Rev. Lett. 104, 213601 (2010).
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D. Popmintchev, C. Hernandez-Garcia, F. Dollar, C. Mancuso, J. Perez-Hernndez, M. C. Chen, A. Hankla, X. Gao, B. Shim, A. Gaeta, M. Tarazkar, D. Romanov, R. Levis, J. Gaffney, M. Foord, S. Libby, A. Jaron-Becker, A. Becker, L. Plaja, M. Murnane, H. Kapteyn, and T. Popmintchev, “Efficient soft X-ray high harmonic generation in multiply- ionized plasmas: the ultraviolet surprise,” Science 3501225–123131 (2015).
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T. Popmintchev, M.-C. Chen, D. Popmintchev, P. Arpin, S. Brown, S. Alisauskas, G. Andriukaitis, T. Balciunas, O.D. Mücke, A. Pugzlys, A. Baltuska, B. Shim, S. E. Schrauth, A. Gaeta, C. Hernandez-Garcia, L. Plaja, A. Becker, A. Jaron-Becker, M. M. Murnane, and H. C. Kapteyn, “Bright Coherent Ultrahigh Harmonics in the keV X-ray Regime from Mid-Infrared Femtosecond Lasers,” Science 91, 1287–1291 (2012).
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Smirnova, O.

Y. Mairesse, J. Higuet, N. Dudovich, D. Shafir, B. Fabre, E. Mevel, E. Constant, S. Patchkovskii, Z. Walters, M.Yu. Ivanov, and O. Smirnova, “High harmonic spectroscopy of multichannel dynamics in strong-field ionization,” Phys. Rev. Lett. 104, 213601 (2010).
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O. Smirnova, Y. Mairesse, S. Patchkovskii, N. Dudovich, D. Villeneuve, P. Corkum, and M. Yu. Ivanov, “High harmonic interferometry of multi-electron dynamics in molecules,” Nature 460, 972–977 (2009).
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S.-K. Son, D. A. Telnow, and S. I. Chu, “Probing the origin of elliptical high-order harmonic generation from aligned molecules in linearly polarized laser fields,” Phys. Rev. A 82, 043829 (2010).
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H. J. Wörner, J. B. Bertrand, B. Fabre, J. Hiquet, H. Ruf, A. A. Dubrouil, S. Patchkovskii, M. Spanner, Y. Mairesse, V. Blanchet, E. Mvel, 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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D. Popmintchev, C. Hernandez-Garcia, F. Dollar, C. Mancuso, J. Perez-Hernndez, M. C. Chen, A. Hankla, X. Gao, B. Shim, A. Gaeta, M. Tarazkar, D. Romanov, R. Levis, J. Gaffney, M. Foord, S. Libby, A. Jaron-Becker, A. Becker, L. Plaja, M. Murnane, H. Kapteyn, and T. Popmintchev, “Efficient soft X-ray high harmonic generation in multiply- ionized plasmas: the ultraviolet surprise,” Science 3501225–123131 (2015).
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S.-K. Son, D. A. Telnow, and S. I. Chu, “Probing the origin of elliptical high-order harmonic generation from aligned molecules in linearly polarized laser fields,” Phys. Rev. A 82, 043829 (2010).
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P. M. Paul, E. S. Toma, P. Breger, G. Mullot, F. Auge, Ph. Balcou, H. G. Muller, and P. Agostini, “Observation of a Train of Attosecond Pulses from High Harmonic Generation,” Science 292, 1689–1692 (2001).
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O. Smirnova, Y. Mairesse, S. Patchkovskii, N. Dudovich, D. Villeneuve, P. Corkum, and M. Yu. Ivanov, “High harmonic interferometry of multi-electron dynamics in molecules,” Nature 460, 972–977 (2009).
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H. J. Wörner, J. B. Bertrand, B. Fabre, J. Hiquet, H. Ruf, A. A. Dubrouil, S. Patchkovskii, M. Spanner, Y. Mairesse, V. Blanchet, E. Mvel, 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, 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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C. Vozzi, C. Negro, F. Calegari, G. Sansone, M. Nisoli, S. DeSilvestri, and S. Stagira, “Generalized molecular orbital tomography,” Nat. Phys. 7, 822–826 (2011).
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X. B. 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).
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M.-C. Chen, C. Mancuso, C. Hernandez-Garcia, F. Dollar, B. Galloway, D. Popmintchev, P.-C. Huang, B. Walker, L. Plaja, A. A. Jaron-Becker, A. Becker, M. M. Murnane, H. C. Kapteyn, and T. Popmintchev, “Generation of bright isolated attosecond soft X-ray pulses driven by multicycle midinfrared lasers,” Proc. Nat. Acad. Sciences U.S.A. 111, E2361–E2367 (2014).
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Y. Mairesse, J. Higuet, N. Dudovich, D. Shafir, B. Fabre, E. Mevel, E. Constant, S. Patchkovskii, Z. Walters, M.Yu. Ivanov, and O. Smirnova, “High harmonic spectroscopy of multichannel dynamics in strong-field ionization,” Phys. Rev. Lett. 104, 213601 (2010).
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W. Boutu, S. Haessler, H. Merdji, P. Breger, G. Waters, M. Stankiewicz, L. J. Frasinski, R. Taieb, J. Caillat, A. Maquet, P. Monchicourt, B. Carre, and P. Salieres, “Coherent control of attosecond emission from aligned molecules,” Nat. Phys. 4, 545–549 (2008).
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D. Baykusheva, P. M. Kraus, S. B. Zhang, N. Rohringer, and H. J. Wörner, “The sensitivities of high-harmonic generation and strong-field ionization to coupled electronic and nuclear dynamics,” Faraday Discuss. 171, 113–132 (2014).
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H. J. Wörner, J. B. Bertrand, B. Fabre, J. Hiquet, H. Ruf, A. A. Dubrouil, S. Patchkovskii, M. Spanner, Y. Mairesse, V. Blanchet, E. Mvel, 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, 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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Zhang, S. B.

D. Baykusheva, P. M. Kraus, S. B. Zhang, N. Rohringer, and H. J. Wörner, “The sensitivities of high-harmonic generation and strong-field ionization to coupled electronic and nuclear dynamics,” Faraday Discuss. 171, 113–132 (2014).
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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).
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X. B. 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).
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Appl. Surf. Sci. (1)

I. Lopez-Quintas, M. Oujja, M. Sanz, M. Martin, R. A. Ganeev, and M. Castillejo, “Low-order harmonic generation in nanosecond laser ablation plasmas of carbon containing materials,” Appl. Surf. Sci. 27833–37 (2013).
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Faraday Discuss. (1)

D. Baykusheva, P. M. Kraus, S. B. Zhang, N. Rohringer, and H. J. Wörner, “The sensitivities of high-harmonic generation and strong-field ionization to coupled electronic and nuclear dynamics,” Faraday Discuss. 171, 113–132 (2014).
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C. Vozzi, C. Negro, F. Calegari, G. Sansone, M. Nisoli, S. DeSilvestri, and S. Stagira, “Generalized molecular orbital tomography,” Nat. Phys. 7, 822–826 (2011).
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Nature (3)

O. Smirnova, Y. Mairesse, S. Patchkovskii, N. Dudovich, D. Villeneuve, P. Corkum, and M. Yu. Ivanov, “High harmonic interferometry of multi-electron dynamics in molecules,” Nature 460, 972–977 (2009).
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H. J. Wörner, J. B. Bertrand, D. V. Kartashov, P. B. Corkum, and D. M. Villeneuve, “Following a chemical reaction using high-harmonic interferometry,” Nature 466, 604–607 (2010).
[Crossref] [PubMed]

M. Hentschel, R. Kienberger, Ch. Spielmann, G. A. Reider, N. Milosevic, T. Brabec, P. Corkum, U. Heinzmann, M. Drescher, and F. Krausz, “Attosecond metrology,” Nature 414, 509–513 (2001).
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Phys. Rev. A (10)

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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T. Zuo and A. D. Bandrauk, “Charge-resonance-enhanced ionization of diatomic molecular ions by intense lasers,” Phys. Rev. A 52, R2511–R2514 (1995).
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D. B. Milosevic, “Resonant high-order harmonic generation from plasma ablation: Laser intensity dependence of the harmonic intensity and phase,” Phys. Rev. A 81, 023802 (2010).
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J. B. Watson, A. Sanpera, X. Chen, and K. Burnett, “Harmonic generation from a coherent superposition of states,” Phys. Rev. A 53, R1962–R1965 (1996).
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Figures (6)

Fig. 1
Fig. 1

High harmonic spectra of N 2 +, aligned parallel (a) and perpendicular (b) to the polarization axis of a 15 fs laser pulse at 400 nm and 2 × 1014 W/cm2. The insets show an enlarged view of part of the spectrum, which clearly exhibit the first and second order Mollow sidebands displaced by the Rabi frequency Ωr and 2Ωr from the odd harmonics for the aligned molecules (panel a).

Fig. 2
Fig. 2

Shift of the first (red solid line with circles) and second-order (red dashed line with circles) Mollow sidebands for the 9th harmonic in N 2 +, aligned parallel to the polarization direction, as function of the electric field strength. Also shown is the Rabi frequency (green solid line with stars) and twice the Rabi frequency (green dashed line with stars) for the transition between HOMO-2 (σu) and HOMO (σg). Other laser parameters are the same as in Fig. 1.

Fig. 3
Fig. 3

High harmonic spectrum of N 2 + aligned perpendicular to the polarization axis of a 60 fs laser pulse at 800 nm and 2 × 1014 W/cm2. The inset provides an enlarged view of part of the spectrum.

Fig. 4
Fig. 4

Difference between the full time-dependent electron density of N 2 +, aligned along the polarization axis, and the initial electron density as a function of time and the position along the molecular axis. The densities are integrated over the spatial dimensions transversal to the molecular axis. Laser parameters as in Fig. 1.

Fig. 5
Fig. 5

Wavelet analysis of high harmonic generation in N 2 + aligned along (a) and perpendicular to (b) the polarization direction. Laser parameters are the same as in Fig. 1.

Fig. 6
Fig. 6

High harmonic spectra showing fractional harmonics for (a) NO2 at 400 nm, 1014 W/cm2, and 40 fs pulse length, (b) CO 2 + at 350 nm, 1014 W/cm2 and 34 fs, and (c) C 2 H 4 + at 400 nm, 1014 W/cm2 and 18 fs.

Equations (3)

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i t ϕ k ( r , t ) = 2 ϕ k ( r , t ) + ( V K S [ ρ ( r , t ) ] + U ( r , t ) ) ϕ ( r , t )
ρ ( r , t ) = k ϕ k * ( r , t ) ϕ k ( r , t )
d ( ω , t ) = d ( τ ) exp ( ( τ t ) 2 / 2 σ 2 ) exp ( i ω τ ) d τ .

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