Tomographic imaging of molecular orbitals

Itatani, Jiro; Lévesque, Julie; Zeidler, D.; Niikura, Hiromichi; Pépin, H.; Kieffer, Jean‐Claude; Corkum, P. B.; Villeneuve, D. M.

doi:10.1038/nature03183

Cited by 2,156 publications

(1,831 citation statements)

References 35 publications

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“…Since the returning electron wave diffracts in the electrostatic molecular potential before it recombines, the high-harmonic spectrum reveals structural signatures such as twocenter interference [12] and features of electronic structure. [13][14][15][16] In addition, a high-harmonic spectrum also encodes dynamical information. Under precisely controlled experimental conditions, each photon energy in the spectrum is emitted by a unique electron trajectory, i.e.…”

Section: Introductionmentioning

confidence: 99%

High-Harmonic Spectroscopy: From Femtosecond to Attosecond Molecular Dynamics

Wörner

2011

Chimia

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The principles of high-harmonic spectroscopy (HHS) are illustrated using two recent examples from the literature. The method can be applied as a probe to measure the evolution of the electronic structure of a molecule during a chemical reaction on the femtosecond time scale. Alternatively, it can be used as a comprehensive method unifying pump and probe steps into a single laser cycle to measure electronic dynamics on the at to second time scale.

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Section: Introductionmentioning

confidence: 99%

High-Harmonic Spectroscopy: From Femtosecond to Attosecond Molecular Dynamics

Wörner

2011

Chimia

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“…To analyse this possibility at the microscopic level, we consider semi-classical electron trajectory calculations in the crystal. In the gas phase, such analysis has proved useful in capturing basic recollision dynamics, including the anisotropy in molecular HHG 13 . We extend that analysis to the solid state by including the effects from the periodic potential that produce the non-parabolic energy dispersion and folding of the band structure.…”

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confidence: 99%

“…For a complete electronic structure, it is desirable to exploit the microscopic process to measure the periodic potential in three dimensions (real space). This is analogous to tomographic imaging of a molecule, where the three-dimensional spatial information (that is, orbital wavefunction) of the target molecule is extracted [13][14][15] . Those measurement techniques are based critically on the dependence of HHG efficiency on molecular alignment with respect to the laser field 16 .…”

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confidence: 99%

Anisotropic high-harmonic generation in bulk crystals

2016

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The microscopic valence electron density determines the optical, electronic, structural and thermal properties of materials. However, current techniques for measuring this electron charge density are limited: for example, scanning tunnelling microscopy is confined to investigations at the surface, and electron di raction requires very thin samples to avoid multiple scattering 1 . Therefore, an optical method is desirable for measuring the valence charge density of bulk materials. Since the discovery of high-harmonic generation (HHG) in solids 2 , there has been growing interest in using HHG to probe the electronic structure of solids 3-11 . Here, using single-crystal MgO, we demonstrate that high-harmonic generation in solids is sensitive to interatomic bonding. We find that harmonic e ciency is enhanced (diminished) for semi-classical electron trajectories that connect (avoid) neighbouring atomic sites in the crystal. These results indicate the possibility of using materials' own electrons for retrieving the interatomic potential and thus the valence electron density, and perhaps even wavefunctions, in an all-optical setting.High-harmonic generation (HHG) in bulk crystal is attributed to the sub-cycle electronic motion driven by an intense laser field [2][3][4][5][6][7][8][9][10][11] . There has been a growing interest in utilizing HHG to probe the electronic structure of solids 8,9,11 . Vampa et al. reconstructed the momentum-dependent bandgap of ZnO along the -M direction using HHG from a two-colour driving field 11 . Luu et al. retrieved the energy dispersion of the lowest conduction band of SiO 2 assuming that the harmonics are produced by the intraband currents 8 . The dependence of solid-state HHG on the coupling of multiple electronic bands has also been identified with the production of even harmonics in GaSe 9 and the emergence of a second plateau in rare-gas solids 12 . These findings show the possibility of using solidstate HHG to probe the electronic band structures in solids, but the analyses are so far limited to one dimension. For a complete electronic structure, it is desirable to exploit the microscopic process to measure the periodic potential in three dimensions (real space). This is analogous to tomographic imaging of a molecule, where the three-dimensional spatial information (that is, orbital wavefunction) of the target molecule is extracted [13][14][15] . Those measurement techniques are based critically on the dependence of HHG efficiency on molecular alignment with respect to the laser field 16 .In this letter, we demonstrate the strong sensitivity of HHG to the atomic-scale structure in the cubic wide-bandgap crystal MgO. First, using a linearly polarized field, we measure a highly anisotropic angular distribution in high-harmonic signal-despite the isotropic linear and weakly anisotropic nonlinear optical properties of the cubic crystal in the perturbative regime 17 . Second, we observe a strong ellipticity dependence of the HHG yield similar to the gas-phase HHG 18 for small elliptic...

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“…6 As can be seen in equation 3, this deviation becomes pronounced when the potential experienced by the electron is comparable to the scattering energy. In this case, the measured d k will depart from the Fourier transform of xψ g ( x).…”

Section: Scattering States and Ramifications For Molecular Tomographymentioning

confidence: 93%

Limits of the Plane Wave Approximation in the Measurement of Molecular Properties

2008

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Rescattering electrons offer great potential as probes of molecular properties on ultrafast timescales. The most famous example is molecular tomography, in which high harmonic spectra of oriented molecules are mapped to "tomographic images" of the relevant molecular orbitals.The accuracy of such reconstructions may be greatly affected by the distortion of scattering wavefunctions from their asymptotic forms due to interactions with the parent ion. We investigate the validity of the commonly used plane wave approximation in molecular tomography, showing how such distortions affect the resulting orbital reconstructions.

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Tomographic imaging of molecular orbitals

Cited by 2,156 publications

References 35 publications

High-Harmonic Spectroscopy: From Femtosecond to Attosecond Molecular Dynamics

High-Harmonic Spectroscopy: From Femtosecond to Attosecond Molecular Dynamics

Anisotropic high-harmonic generation in bulk crystals

Limits of the Plane Wave Approximation in the Measurement of Molecular Properties

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