Zengxiu Zhao

High harmonic generation and molecular orbital tomography in multielectron systems.

High harmonic radiation is produced when atoms or molecules are ionized by an intense femtosecond laser pulse. The radiated spectrum has been shown experimentally to contain information on the electronic structure of the molecule, which can be interpreted as an image of a single molecular orbital. Previous theory for high harmonic generation has been limited to the single-active-electron approximation. Utilizing semisudden approximation, the authors develop a theory of the recombination step in high harmonic generation and tomographic reconstruction in multielectron systems, taking into account electron spin statistics and electron-electron correlations within the parent molecule and the ion. They show that the resulting corrections significantly modify the theoretical predictions, and bring them in a better agreement with experiment. They further show that exchange contributions to harmonic radiation can be used to extract additional information on the electronic wave function.

Synchronizing terahertz wave generation with attosecond bursts.

We perform a joint measurement of terahertz waves and high-harmonics generated from argon atoms driven by a fundamental laser pulse and its second harmonic. By correlating their dependence on the phase delay between the two pulses, we determine the generation of THz waves in tens of attoseconds precision. Compared with simulations and models, we find that the laser-assisted soft collision of the electron wave packet with the atomic core plays a key role. It is demonstrated that the rescattering process, being indispensable in high-harmonic generation processes, dominates THz wave generation as well in a more elaborate way. The new finding might be helpful for the full characterization of the rescattering dynamics.

Dynamic ionic clusters with flowing electron bubbles from warm to hot dense iron along the Hugoniot curve.

Complex structures of warm and hot dense matter are essential to understanding the behavior of materials in high energy density processes and provide new features of matter constitutions. Here, around a new unified first-principles determined Hugoniot curve of iron from the normal condensed condition up to 1 Gbar, the novel structures characterized by the ionic clusters with electron bubbles are found using quantum Langevin molecular dynamics. Subsistence of complex clusters can persist in the time scale of 50 fs dynamically with quantum flowing bubbles, which are produced by the interplay of Fermi electron degeneracy, the ionic coupling, and the dynamical nature. With the inclusion of those complicated features in quantum Langevin molecular dynamics, the present equation of states could serve as a first-principles based database in a wide range of temperatures and densities.

Dynamic core polarization in strong-field ionization of CO molecules.

The orientation-dependent strong-field ionization of CO molecules is investigated using the fully propagated three-dimensional time-dependent Hartree-Fock theory. The full ionization results are in good agreement with recent experiments. The comparisons between the full method and the single active orbital method show that although the core electrons are generally more tightly bound and contribute little to the total ionization yields, their dynamics cannot be ignored, which effectively modifies the behavior of electrons in the highest occupied molecular orbital. By incorporating it into the single active orbital method, we identify that the dynamic core polarization plays an important role in the strong-field tunneling ionization of CO molecules, which is helpful for the future development of the tunneling ionization theory of molecules beyond the single active electron approximation.

Theoretical study of terahertz generation from atoms and aligned molecules driven by two-color laser fields

We study the generation of terahertz (THz) radiation from atoms and molecules driven by an ultrashort fundamental laser and its second harmonic field by solving time-dependent Schrödinger equation. The simulations show that the initial wave-packet and its subsequent acceleration in the laser field, and rescattering with long-range Coulomb potential play key roles on THz generation. We also present the dependence of the optimal phase delay and yield of terahertz radiation on the laser intensity, wavelength, duration, the ratio of two-color laser components, and against the molecular alignment.

Polarization-sensitive air-biased-coherent-detection for terahertz wave

Employing an orientation-modulated bias field, a polarization-sensitive scheme for terahertz air-biased-coherent-detection (THz-ABCD) is presented to directly measure the amplitude and polarization angle of THz field in the time domain. It can provide all characteristics of arbitrarily polarized THz wave with one single-scan measurement. Measuring convenience, broad bandwidth, and high angular resolution have been achieved. Polarization-sensitive THz time-domain spectroscopy can surely be developed based on this technology. Many other applications in the THz spectral region are also believed.

Joint Measurements of Terahertz Wave Generation and High-Harmonic Generation from Aligned Nitrogen Molecules Reveal Angle-Resolved Molecular Structures.

We report the synchronized measurements of terahertz wave generation and high-harmonic generation from aligned nitrogen molecules in dual-color laser fields. Both yields are found to be alignment dependent, showing the importance of molecular structures in the generation processes. By calibrating the angular ionization rates with the terahertz yields, we present a new way of retrieving the angular differential photoionization cross section (PICS) from the harmonic signals which avoids specific model calculations or separate measurements of the alignment-dependent ionization rates. The measured PICS is found to be consistent with theoretical predications, although some discrepancies exist. This all-optical method provides a new alternative for investigating molecular structures.

Nuclear quantum dynamics in dense hydrogen

Nuclear dynamics in dense hydrogen, which is determined by the key physics of large-angle scattering or many-body collisions between particles, is crucial for the dynamics of planets evolution and hydrodynamical processes in inertial confinement confusion. Here, using improved ab initio path-integral molecular dynamics simulations, we investigated the nuclear quantum dynamics regarding transport behaviors of dense hydrogen up to the temperatures of 1 eV. With the inclusion of nuclear quantum effects (NQEs), the ionic diffusions are largely higher than the classical treatment by the magnitude from 20% to 146% as the temperature is decreased from 1 eV to 0.3 eV at 10 g/cm3, meanwhile, electrical and thermal conductivities are significantly lowered. In particular, the ionic diffusion is found much larger than that without NQEs even when both the ionic distributions are the same at 1 eV. The significant quantum delocalization of ions introduces remarkably different scattering cross section between protons compared with classical particle treatments, which explains the large difference of transport properties induced by NQEs. The Stokes-Einstein relation, Wiedemann-Franz law, and isotope effects are re-examined, showing different behaviors in nuclear quantum dynamics.Nuclear quantum effects (NQEs) on the structures and transport properties of dense liquid hydrogen at densities of 10-100 g/cm3 and temperatures of 0.1-1 eV are fully assessed using \textit{ab initio} path-integral molecular dynamics simulations. With the inclusion of NQEs, ionic diffusions are strongly enhanced by the magnitude from 100% to 15% with increasing temperature, while electrical conductivities are significantly suppressed. The analyses of ionic structures and zero-point energy show also the importance of NQEs in these regime. The significant quantum delocalization of ions introduces expressively different scattering cross section between protons compared with classical particle treatments, which can explain the large alterability of transport behaviors. Furthermore, the energy, pressure, and isotope effects are also greatly influenced by NQEs. The complex behaviors show that NQEs can not be neglected for dense hydrogen even in the warm dense regime.

Attosecond synchronization of terahertz wave and high-harmonics

Argon atom ionizing in the ultrafast two-colour field has been used to investigate the physical mechanism of terahertz (THz) generation. We measured simultaneously pulse energies of THz and high-harmonics as the phase delay between the fundamental and its second harmonic was varied. The optimal phase delay of THz generation is determined according to the inherent attochirp of the emitted high-harmonics. The dynamic analysis of the tunnelling electron wave packet driven by the Coulomb–laser coupling shows that laser-assisted soft collisions of the electron wave packet with the atomic core play a key role. It is demonstrated that the rescattering process, being indispensable in high-harmonic generation processes, dominates THz wave generation as well in a more elaborate way.

Dynamic orbitals in high-order harmonic generation from CO molecules

We identify that both the dynamic core polarization and dynamic orbital deformation are important in the orientation-dependent high-order harmonic generation of CO molecules subjected to intense few cycle laser fields. These polarization dynamics allow for the observation of strong orientation effects and dynamic minimum in the harmonic spectra. The generated attosecond pulses can be greatly affected by these multielectron effects. This work sheds light on future development of dynamic orbital imaging on attosecond time scale.