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Peixiang Lu

Publications and source records attributed to Peixiang Lu.

At least 91 records · Page 5Linked to original sources

Interference of high-order harmonics generated from molecules at different alignment angles

We theoretically investigate the interference effect of high-order harmonics generated from molecules at different alignment angles. It is shown that the interference of the harmonic emissions from molecules aligned at different angles can significantly modulate the spectra and result in the anomalous harmonic cutoffs observed in a recent experiment [ Nature Phys. 7, 822 (2011) ]. The shift of the spectral minimum position with decreasing the degree of alignment is also explained by the interference effect of the harmonic emissions.

physics.optics↗

Imprints of the molecular-orbital geometry on the high-harmonic ellipticity

The influence of the orbital symmetry on the ellipticity of the high-order harmonics is investigated. It is found that the ellipticity maps have distinct shapes for the molecular orbital with different symmetry. Our analysis shows that the feature of the harmonic ellipticity map is essentially determined by the nodal structure of the nonsymmetric orbital. The results indicate that the molecular-orbital geometry is imprinted on the ellipticity of the high-order harmonics, which invites the use of ellipticity measurements as a probe of the orbital structure for polar molecules.

physics.optics↗

Tomographic imaging of asymmetric molecular orbitals with a two-color multicycle laser field

We theoretically demonstrate a scheme for tomographic reconstruction of asymmetric molecular orbitals based on high-order harmonic generation with a two-color multicycle laser field. It is shown that by adjusting the relative phase of the two fields, the returning electrons can be forced to recollide from one direction for all the orientations of molecules. Thus the reconstruction of the asymmetric orbitals can be carried out with multicycle laser field. This releases the stringent requirement of a single-cycle pulse with a stabilized and controllable carrier-envelop phase for the tomographic imaging of asymmetric molecular orbitals.

physics.atom-ph↗

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

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.

physics.chem-ph↗

Laterally emitted surface second harmonic generation in a single ZnTe nanowire

We report a direct observation on the unique laterally emitted surface second harmonic generation (SHG) in a single ZnTe nanowire. The highly directional surface SHG signal that polarizes along the direction vertical to the nanowire growth axis, is significantly larger than the bulk SHG contribution, indicating a high efficiency of surface SHG. Two strong SHG peaks are observed on both sides of the nanowire surfaces in the far-field scanning images, which is further supported by FDTD simulations, demonstrating that the unique laterally emitted signal is ascribed to surface SHG in the ZnTe nanowire. The surface SHG in a single ZnTe nanowire with unique lateral emission and high conversion efficiency shows great potential applications in short-wavelength nanolasers, nonlinear microscopy and polarization dependent photonic integrating.

physics.optics↗

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 restricted to only one side of the core. Then we carried out the orbital reconstruction in both the length and velocity forms. The results show that, the orbital structure can only be successfully reproduced by using the dipole matrix elements projected perpendicular to the permanent dipole in both forms.

physics.atom-ph↗

Role of the Coulomb potential on the ellipticity in atomic high-order harmonics generation

The role of the Coulomb potential on the generation of elliptically polarized high-order harmonics from atoms driven by elliptically polarized laser is investigated analytically. It is found that the Coulomb effect makes a contribution to the harmonic ellipticity for low harmonic orders and short quantum path. By using the strong-field eikonal-Volkov approximation, we analyze the influence of the Coulomb potential on the dynamics of the continuum state and find that the obtained harmonic ellipticity in our simulation originates from the break of symmetry of the continuum state.

physics.atom-ph↗

Anomalous isotopic effect on electron-directed reactivity by a 3-μm midinfrared pulse

We have theoretically studied the effect of nuclear mass on electron localization in dissociating H_2^+ and its isotopes subjected to a few-cycle 3-μm laser pulse. Compared to the isotopic trend in the near-infrared regime, our results reveal an inverse isotopic effect in which the degree of electron-directed reactivity is even higher for heavier isotopes. With the semi-classical analysis, we find, for the first time, the pronounced electron localization is established by the interferences through different channels of one- and, more importantly, higher-order photon coupling. Interestingly, due to the enhanced high-order above-threshold dissociation of heavier isotopes, the interference maxima gradually become in phase with growing mass and ultimately lead to the anomalous isotopic behavior of the electron localization. This indicates that the multi-photon coupling channels will play an important role in controlling the dissociation of larger molecules with midinfrared pulses.

physics.atm-clus↗

Classical simulations including electron correlations for sequential double ionization

With a classical ensemble model that including electron correlations during the whole ionization process, we investigated strong-field sequential double ionization of Ar by elliptically polarized pulses at the quantitative level. The experimentally observed intensity-dependent three-band or four-band structures in the ion momentum distributions are well reproduced with this classical model. More importantly, the experimentally measured ionization time of the second electrons [A. N. Pfeiffer et al., Nature Phys. 7, 428 (2011)], which can not be predicted by the standard independent-electron model, is quantitatively reproduced by this fully classical correlated model. The success of our work encourages classical description and interpretation of the complex multi-electron effects in strong field ionization where nonperturbative quantum approaches are currently not feasible.

physics.atom-ph↗

Broadband large-ellipticity harmonic generation with polar molecule

We investigate the polarization properties of high harmonic generation from polar molecules with a linearly polarized field. It is found that elliptically polarized harmonics are observed in a wide spectral range from the plateau to the cutoff. Further analyses show that the nonsymmetric structure of the highest occupied molecular orbital is the origin of ellipticity of the harmonics. The results provide a method for generation of large-ellipticity XUV pulses, which will benefit the application of HHG as a tool of detection in materials and biology science.

physics.optics↗

Wavelength dependence of electron localization in the laser-driven dissociation of H$_2^+$

We theoretically investigate the laser wavelength dependence of asymmetric dissociation of H$_2^+$. It is found that the electron localization in molecular dissociation is significantly manipulated by varying the wavelength of the driving field. Through creating a strong nuclear vibration in the laser-molecular interaction, our simulations demonstrate that the few-cycle mid-infrared pulse can effectively localize the electron at one of the dissociating nuclei with weak ionization. Moreover, we show that the observed phase-shift of the dissociation asymmetry is attributed to the different population transfers by the remaining fields after the internuclear distances reach the one-photon coupling point.

physics.atm-clus↗

Phase dependence of electron localization in HeH$^{2+}$ dissociation with an intense few-cycle laser pulse

The electron localization in the dissociation of the asymmetric charged molecular ion HeH$^{2+}$ exposed to an intense few-cycle laser pulse is studied by solving numerically the 3D time-dependent Schrödinger equation. By varying the carrier-envelope phase (CEP) and the intensity of the pulse, the upward shift of the localization probability and the suppression of the dissociation channel He$^{2+}$+H are observed . Our analysis shows that the phenomenon is attributed to the asymmetric structure of the molecule as well as the recollision-assistant field-induced ionization of the electron wave packets localized on H$^+$ in the trailing of the pulse.

physics.atom-ph↗

Laser-polarization-dependent photoelectron angular distributions from polar molecules

Photoelectron angular distributions (PADs) of oriented polar molecules in response to different polarized lasers are systematically investigated. It is found that the PADs of polar CO molecules show three distinct styles excited by linearly, elliptically and circularly polarized lasers respectively. In the case of elliptical polarization, a deep suppression is observed along the major axis and the distribution concentrates approximately along the minor axis. Additionally, it is also found that the concentrated distributions rotate clockwise as the ellipticity increases. Our investigation presents a method to manipulate the motion and angular distribution of photoelectrons by varying the polarization of the exciting pulses, and also implies the possibility to control the processes in laser-molecule interactions in future work.

physics.chem-ph↗

Efficient generation of isolated attosecond pulses with high beam-quality by two-color Bessel-Gauss beams

The generation of isolated attosecond pulses with high efficiency and high beam quality is essential for attosec- ond spectroscopy. We numerically investigate the supercontinuum generation in a neutral rare-gas medium driven by a two-color Bessel-Gauss beam. The results show that an efficient smooth supercontinuum in the plateau is obtained after propagation, and the spatial profile of the generated attosecond pulse is Gaussian-like with the divergence angle of 0.1 degree in the far field. This bright source with high beam quality is beneficial for detecting and controlling the microscopic processes on attosecond time scale.

physics.optics↗

Asymmetric electron energy sharing in strong-field double ionization of helium

With the classical three-dimensional ensemble model, we have investigated the microscopic recollision dynamics in nonsequential double ionization of helium by 800 nm laser pulses at 2.0 PW/cm^2. We demonstrate that the asymmetric energy sharing between the two electrons at recollision plays a decisive role in forming the experimentally observed V-shaped structure in the correlated longitudinal electron momentum spectrum at the high laser intensity [Phys. Rev. Lett. 99, 263003 (2007)]. This asymmetric energy sharing recollision leaves footprints on the transverse electron momentum spectra, which provide a new insight into the attosecond three-body interactions.

physics.atom-ph↗

The Role of Nuclear Coulomb Attraction in Nonsequential Double Ionization of Argon Atom

The role of nucleus in strong-field nonsequential double ionization of Ar atoms is investigated using three-dimensional classical ensembles. By adjusting the nuclear Coulomb potential, we can excellently reproduce the experimental correlated electron and ion momentum spectra with laser intensities above the recollision threshold [Phys. Rev. Lett. 93, 263001 (2004)] and below the recollision threshold [Phys. Rev. Lett. 101, 053001 (2008)] quantitatively. Analysis reveals the detailed electronic dynamics when the nuclear Coulomb attraction plays a key role in the recollision process of nonsequential double ionization of Ar atoms. Comparison between our results for Ar and those for He shows that atom species have a strong influence on nonsequential double ionization.

physics.atom-ph↗

Energy Correlation in Above-Threshold Nonsequential Double Ionization at 800 nm

We have investigated the energy correlation of the two electrons from nonsequential double ionization of helium atom in 800 nm laser fields at intensities below the recollision threshold by quantum calculations. The circular arcs structure of the correlated electron momentum spectra reveals a resonant double ionization process in which the two electrons transit from doubly excited states into continuum states by simultaneously absorbing and sharing excess energy in integer units of the photon energy. Coulomb repulsion between the two electrons in continuum states is responsible for the dominant back-to-back electron emission and two intensity-independent cutoffs in the two-electron energy spectra.

physics.optics↗