Strong-field Control and Spectroscopy of Attosecond Electron-hole Dynamics in Molecules

Overview

Journal Proc Natl Acad Sci U S A

Specialty Science

Date 2009 Oct 7

PMID 19805337

Citations 7

Authors

Olga Smirnova

Serguei Patchkovskii

Yann Mairesse

Nirit Dudovich

Misha Yu Ivanov

Affiliations

Soon will be listed here.

Abstract

Molecular structures, dynamics and chemical properties are determined by shared electrons in valence shells. We show how one can selectively remove a valence electron from either Pi vs. Sigma or bonding vs. nonbonding orbital by applying an intense infrared laser field to an ensemble of aligned molecules. In molecules, such ionization often induces multielectron dynamics on the attosecond time scale. Ionizing laser field also allows one to record and reconstruct these dynamics with attosecond temporal and sub-Angstrom spatial resolution. Reconstruction relies on monitoring and controlling high-frequency emission produced when the liberated electron recombines with the valence shell hole created by ionization.

Citing Articles

Tracking Charge Migration with Frequency-Matched Strobo-Spectroscopy.

Hamer K, Folorunso A, Lopata K, Schafer K, Gaarde M, Mauger F J Phys Chem A. 2024; 128(1):20-27.

PMID: 38165105 PMC: 10788909. DOI: 10.1021/acs.jpca.3c04234.

Filming movies of attosecond charge migration in single molecules with high harmonic spectroscopy.

He L, Sun S, Lan P, He Y, Wang B, Wang P Nat Commun. 2022; 13(1):4595.

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Ionization of HCCI Neutral and Cations by Strong Laser Fields Simulated With Time Dependent Configuration Interaction.

Schlegel H, Hoerner P, Li W Front Chem. 2022; 10:866137.

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Extracting sub-cycle electronic and nuclear dynamics from high harmonic spectra.

Austin D, Johnson A, McGrath F, Wood D, Miseikis L, Siegel T Sci Rep. 2021; 11(1):2485.

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High-harmonic spectroscopy of transient two-center interference calculated with time-dependent density-functional theory.

Mauger F, Abanador P, Scarborough T, Gorman T, Agostini P, DiMauro L Struct Dyn. 2019; 6(4):044101.

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References

Levis R, Menkir G, Rabitz H . Selective bond dissociation and rearrangement with optimally tailored, strong-field laser pulses. Science. 2001; 292(5517):709-13. DOI: 10.1126/science.1059133. View

Corkum . Plasma perspective on strong field multiphoton ionization. Phys Rev Lett. 1993; 71(13):1994-1997. DOI: 10.1103/PhysRevLett.71.1994. View

Uiberacker M, Uphues T, Schultze M, Verhoef A, Yakovlev V, Kling M . Attosecond real-time observation of electron tunnelling in atoms. Nature. 2007; 446(7136):627-32. DOI: 10.1038/nature05648. View

Tate J, Auguste T, Muller H, Salieres P, Agostini P, DiMauro L . Scaling of wave-packet dynamics in an intense midinfrared field. Phys Rev Lett. 2007; 98(1):013901. DOI: 10.1103/PhysRevLett.98.013901. View

Salieres P, Carre B, Le Deroff L, Grasbon F, Paulus G, Walther H . Feynman's path-integral approach for intense-laser-atom interactions. Science. 2001; 292(5518):902-5. DOI: 10.1126/science.108836. View

Drescher M, Hentschel M, Kienberger R, Uiberacker M, Yakovlev V, Scrinzi A . Time-resolved atomic inner-shell spectroscopy. Nature. 2002; 419(6909):803-7. DOI: 10.1038/nature01143. View

Pavicic D, Lee K, Rayner D, Corkum P, Villeneuve D . Direct measurement of the angular dependence of ionization for N2, O2, and CO2 in intense laser fields. Phys Rev Lett. 2007; 98(24):243001. DOI: 10.1103/PhysRevLett.98.243001. View

Branderhorst M, Londero P, Wasylczyk P, Brif C, Kosut R, Rabitz H . Coherent control of decoherence. Science. 2008; 320(5876):638-43. DOI: 10.1126/science.1154576. View

Zewail A . 4D ultrafast electron diffraction, crystallography, and microscopy. Annu Rev Phys Chem. 2006; 57:65-103. DOI: 10.1146/annurev.physchem.57.032905.104748. View

10.

LEZIUS , Blanchet V , Rayner , VILLENEUVE , Stolow , IVANOV . Nonadiabatic Multielectron Dynamics in Strong Field Molecular Ionization. Phys Rev Lett. 2001; 86(1):51-54. DOI: 10.1103/PhysRevLett.86.51. View

11.

Remacle F, Levine R . An electronic time scale in chemistry. Proc Natl Acad Sci U S A. 2006; 103(18):6793-8. PMC: 1458974. DOI: 10.1073/pnas.0601855103. View

12.

Shapiro M . EPR breakup of polyatomic molecules. J Phys Chem A. 2006; 110(27):8580-4. DOI: 10.1021/jp0568071. View

13.

Rabitz H . Chemistry. Shaped laser pulses as reagents. Science. 2003; 299(5606):525-7. DOI: 10.1126/science.1080683. View

14.

Shapiro E, Walmsley I, Ivanov M . Suppression of decoherence in a wave packet via nonlinear resonance. Phys Rev Lett. 2007; 98(5):050501. DOI: 10.1103/PhysRevLett.98.050501. View

15.

Assion , BAUMERT , Bergt , Brixner , Kiefer , Seyfried V . Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses . Science. 1998; 282(5390):919-22. DOI: 10.1126/science.282.5390.919. View

16.

Baker S, Robinson J, Haworth C, Teng H, Smith R, Chirila C . Probing proton dynamics in molecules on an attosecond time scale. Science. 2006; 312(5772):424-7. DOI: 10.1126/science.1123904. View

17.

Schoffler M, Titze J, Petridis N, Jahnke T, Cole K, Schmidt L . Ultrafast probing of core hole localization in N2. Science. 2008; 320(5878):920-3. DOI: 10.1126/science.1154989. View

18.

Becker , Faisal . Suppressed molecular ionization for a class of diatomics in intense femtosecond laser fields. Phys Rev Lett. 2000; 85(11):2280-3. DOI: 10.1103/PhysRevLett.85.2280. View

19.

Cavalieri A, Muller N, Uphues T, Yakovlev V, Baltuska A, Horvath B . Attosecond spectroscopy in condensed matter. Nature. 2007; 449(7165):1029-32. DOI: 10.1038/nature06229. View

20.

Sussman B, Townsend D, Ivanov M, Stolow A . Dynamic stark control of photochemical processes. Science. 2006; 314(5797):278-81. DOI: 10.1126/science.1132289. View