Tomographic reconstruction of molecular orbitals with twofold mirror antisymmetry: Overcoming the nodal plane problem

Abstract

We propose a new method to overcome the nodal plane problem for the tomographic reconstruction of molecular orbitals with twofold mirror antisymmetry in the length form based on high-order harmonic generation. It is shown that, by carrying out the reconstruction procedure in the rotating laboratory frame using the component of the dipole moment parallel to the electron recollision direction, the nodal plane problem is avoided and the target orbital is successfully reconstructed. Moreover, it is found that, the proposed method can completely avoid the additional artificial lobes found in the results from the traditional method in the velocity form and therefore provides a more reliable reproduction of the target orbital.

Quantum path interference in the wavelength-dependent below-threshold harmonic generation

“…Nowadays, HHG has been the most effective approach to produce attosecond extreme ultraviolet pulses [2][3][4][5][6][7][8][9][10], which can serve as an important tool for probing the ultrafast electronic dynamics inside atoms or molecules [11][12][13][14][15][16], and inaugurating a new domain for time-resolved metrology on the attosecond time scale [17]. During the laser-molecular interaction, the generated harmonics also provide an effective way for the tomographic imaging of molecular orbital [18][19][20][21][22][23]. Due to its potential applications, the HHG has attracted much attention in the past several decades.…”

Wavelength dependence of high-order-harmonic yield in inhomogeneous fields

“…Currently, high-order harmonic generation (HHG) has been considered to be the most promising method to produce attosecond extreme ultraviolet pulses [1][2][3][4], which provides an important tool for probing the ultrafast electronic dynamics in atoms [5][6][7], attosecond time-resolved spectroscopy [8], and tomographic imaging of molecular orbitals [9][10][11][12][13], etc. The HHG process can be well depicted in terms of the semiclassical three-step model [14]: ionization, acceleration, and recombination of the electrons in the intense laser field.…”

Ultrafast oscillating-magnetic-field generation based on electronic-current dynamics

“…Recently, based on the HHG, the attosecond laser pulse has been available [12][13][14][15][16], which has drawn considerable attention for its possibility for imaging and detection of the electronic structures and ultrafast dynamics in atoms, molecules, or condensed matter with a combination of Å-scale spatial resolution and attosecond temporal resolution [17][18][19][20]. For example, the attosecond pulses have been used to resolve the time when an electron exits a tunneling barrier [21], observe the valence electron motion in real time [22], and control the simple chemical reaction in a molecule [23].…”