High-Order Harmonic Generation and Molecular Orbital Tomography: Characteristics of Molecular Recollision Electronic Wave Packets

Control of recollision wave packets for molecular orbital tomography using short laser pulses

The tomographic imaging of arbitrary molecular orbitals via high-order harmonic generation requires that electrons recollide from one direction only. Within a semi-classical model, we show that extremely short phase-stabilized laser pulses offer control over the momentum distribution of the returning electrons. By adjusting the carrier-envelope phase, recollisions can be forced to occur from mainly one side, while retaining a broad energy spectrum. The signatures of the semi-classical distributions are observed in harmonic spectra obtained by numerical solution of the time-dependent Schrödinge…

Coherent Control and Entanglement in the Attosecond Electron Recollision Dissociation of D2+

We examine the attosecond electron recollision dissociation of D2+ recently demonstrated experimentally [H. Niikura et al., Nature (London) 421, 826 (2003)] from a coherent control perspective. In this process, a strong laser field incident on D2 ionizes an electron, accelerates the electron in the laser field to eV energies, and then drives the electron to recollide with the parent ion, causing D2+ dissociation. A number of results are demonstrated. First, a full dimensional Strong Field Approximation (SFA) model is constructed and shown to be in agreement with the original experiment. This i…

Imperfect Recollisions in High-Harmonic Generation in Solids

We theoretically investigate high-harmonic generation in hexagonal boron nitride with linearly polarized laser pulses. We show that imperfect recollisions between electron-hole pairs in the crystal give rise to an electron-hole-pair polarization energy that leads to a double-peak structure in the subcycle emission profiles. An extended recollision model (ERM) is developed that allows for such imperfect recollisions, as well as effects related to Berry connections, Berry curvatures, and transition-dipole phases. The ERM illuminates the distinct spectrotemporal characteristics of harmonics emitt…

Influence of large permanent dipoles on molecular orbital tomography

The influence of large permanent dipoles on molecular orbital tomography via high-order harmonic generation (HHG) is investigated in this work. It is found that, owing to the modification of the angle-dependent ionization rate resulting from the Stark shift, the one-side-recollision condition for the tomographic imaging can not be satisfied even with the few-cycle driving pulses. To overcome this problem, we employ a tailored driving pulse by adding a weak low-frequency pulse to the few-cycle laser pulse to control the HHG process and the recollision of the continuum electrons are effectively …

Expanded view of electron-hole recollisions in solid-state high-order harmonic generation: Full-Brillouin-zone tunneling and imperfect recollisions

We theoretically investigate electron-hole recollisions in high-harmonic generation (HHG) in band-gap solids irradiated by linearly and elliptically polarized drivers. We find that in many cases the emitted harmonics do not originate in electron-hole pairs created at the minimum band gap, where the tunneling probability is maximized, but rather in pairs created across an extended region of the Brillouin zone (BZ). In these situations, the analogy to gas-phase HHG in terms of the short- and long-trajectory categorizations is inadequate. Our analysis methodology comprises three complementary lev…

亚势垒再碰撞与强场电离中隧穿时间延迟的三类

Sub-barrier recollisions and the three classes of tunneling time delays in strong-field ionization

本文研究亚势垒再碰撞对强场电离隧穿时间延迟的影响，发现干涉减小出口延迟但保持正值，并提出描述隧穿波包起始的新时间特性。