Probing Molecular Electronic Structure Using High Harmonic Generation TomographyChelsey Crosse
The structure of valence electronic orbitals of a molecule determines the majority of chemical properties. Generation of high-order harmonic frequencies from atomic sources has been directly related to the electronic structure of the atom, (1) and extended as far as tomographic reconstruction of linearly symmetric polyatomic molecular systems with some success. (2,3,4)
However, because of the increased resolution of these reconstructions, discrimination of fine details of the orbital reconstructions reveals some inconsistencies in the orbital shapes when compared with past models & theoretical calculations. (2) There are several proposed corrections to the Strong Field Approximation (SFA) that currently underlies tomographic reconstruction as well as all other experiments that use high harmonic generation (HHG) to probe molecular systems. (5,6,7)
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1. Lewenstein et al. Phys Rev A 49 (3) 1994.
2. Salieres, Maquet, Haessler, Caillat, Taieb. Rep. Prog. Phys. 75 (2012) 062401.
3. Li, Liu, Yang, Song, Zhao, Lu, Li, Xu. Opt. Ex. 21 (6) 2013. 7599.
4. Torres et al. Phys Rev. Lett. 98 (2007) 203007.
5. Diveki et. al. J. Chem Phys. 414 (2013) 121.
6. Yip, Palacios, Rescigno, McCurdy, Martin. J. Chem Phys 414 (2013) 112.
7. Spanner, Patchkovskii. J. Chem. Phys. 414 (2013) 10.
Probing Molecular Electronic Structure Using High Harmonic Generation TomographyChelsey Crosse
The structure of valence electronic orbitals of a molecule determines the majority of chemical properties. Generation of high-order harmonic frequencies from atomic sources has been directly related to the electronic structure of the atom, (1) and extended as far as tomographic reconstruction of linearly symmetric polyatomic molecular systems with some success. (2,3,4)
However, because of the increased resolution of these reconstructions, discrimination of fine details of the orbital reconstructions reveals some inconsistencies in the orbital shapes when compared with past models & theoretical calculations. (2) There are several proposed corrections to the Strong Field Approximation (SFA) that currently underlies tomographic reconstruction as well as all other experiments that use high harmonic generation (HHG) to probe molecular systems. (5,6,7)
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1. Lewenstein et al. Phys Rev A 49 (3) 1994.
2. Salieres, Maquet, Haessler, Caillat, Taieb. Rep. Prog. Phys. 75 (2012) 062401.
3. Li, Liu, Yang, Song, Zhao, Lu, Li, Xu. Opt. Ex. 21 (6) 2013. 7599.
4. Torres et al. Phys Rev. Lett. 98 (2007) 203007.
5. Diveki et. al. J. Chem Phys. 414 (2013) 121.
6. Yip, Palacios, Rescigno, McCurdy, Martin. J. Chem Phys 414 (2013) 112.
7. Spanner, Patchkovskii. J. Chem. Phys. 414 (2013) 10.