arXiv subjects

Pengfei Lan

Publications and source records attributed to Pengfei Lan.

52 records · Page 3Linked to original sources

arXiv2016

The selection rules of high harmonic generation: the symmetries of molecules and laser fields

The selection rules of high harmonic generation (HHG) are investigated using three-dimensional time-dependent density functional theory (TDDFT). From the harmonic spectra obtained with various real molecules and different forms of laser fields, several factors that contribute to selection rules are revealed. Extending the targets to stereoscopic molecules, it is shown that the allowed harmonics are dependent on the symmetries of the projections of molecules. For laser fields, the symmetries contributing to the selection rules are discussed according to Lissajous figures and their dynamical directivities. All the phenomena are explained by the symmetry of the full time-dependent Hamiltonian under a combined transformation. We present a systematic study on the selection rules and propose an intuitive method for the judgment of allowed harmonic orders, which can be extended to more complex molecules and various forms of laser pulses.

physics.atom-ph↗

arXiv2016

Frequency shift in high order harmonic generation from isotopic molecules

We report the first experimental observation of frequency shift in high order harmonic generation (HHG) from isotopic molecules H2 and D2 . It is found that harmonics generated from the isotopic molecules exhibit obvious spectral red shift with respect to those from Ar atom. The red shift is further demonstrated to arise from the laser-driven nuclear motion in isotopic molecules. By utilizing the red shift observed in experiment, we successfully retrieve the nuclear vibrations in H2 and D2, which agree well with the theoretical calculations from the time-dependent Schrodinger equation (TDSE) with Non-Born-Oppenheimer approximation. Moreover, we demonstrate that the frequency shift can be manipulated by changing the laser chirp.

physics.atom-ph↗

arXiv2015

Selective enhancement of resonant multiphoton ionization with strong laser fields

High-resolution photoelectron momentum distributions of Xe atoms ionized by 800-nm linearly polarized laser fields have been traced at intensities from 1.1*1013 to 3.5*1013W/cm2 using velocity-map imaging techniques. At certain laser intensities, the momentum spectrum exhibits a distinct double-ring structure for low-order above-threshold ionization, which appears to be absent at lower or higher laser intensities. By investigating the intensity-resolved photoelectron energy spectrum, we find that this double-ring structure originates from resonant multiphoton ionization involving multiple Rydberg states of atoms. Varying the laser intensity, we can selectively enhance the resonant multiphoton ionization through certain atomic Rydberg states. The photoelectron angular distributions of multiphoton resonance are also investigated for the low-order above-threshold ionization.

physics.atom-ph↗

arXiv2015

Spectrally resolved spatiotemporal features of quantum paths in high-order harmonic generation

We experimentally disentangle the contributions of different quantum paths in high-order harmonic generation (HHG) from the spectrally and spatially resolved harmonic spectra. By adjusting the laser intensity and focusing position, we simultaneously observe the spectrum splitting, frequency shift and intensity-dependent modulation of harmonic yields both for the short and long paths. Based on the simulations, we discriminate the physical mechanisms of the intensity-dependent modulation of HHG due to the quantum path interference and macroscopic interference effects. Moreover, it is shown that the atomic dipole phases of different quantum paths are encoded in the frequency shift. In turn, it enables us to retrieve the atomic dipole phases and the temporal chirps of different quantum paths from the measured harmonic spectra. This result gives an informative mapping of spatiotemporal and spectral features of quantum paths in HHG.

physics.atom-ph↗

arXiv2014

Enhanced dissociation of H2+ into highly excited states via laser-induced sequential resonant excitation

We study the dissociation of H$_2$$^+$ in uv laser pulses by solving the non-Born-Oppenheimer time-dependent Schrödinger equation as a function of the photon energy $ω$ of the pulse. Significant enhancements of the dissociation into highly excited electronic states are observed at critical $ω$. This is found to be attributed to a sequential resonant excitation mechanism where the population is firstly transferred to the first excited state by absorbing one photon and sequentially to higher states by absorbing another one or more photons at the same internuclear distance. We have substantiated the underlying dynamics by separately calculating the nuclear kinetic energy spectra for individual dissociation pathways through different electronic states.

physics.atm-clus↗

arXiv2014

Revealing Correlated Electron-Nuclear Dynamics in Molecules with Energy-Resolved Population Image

We explore a new fashion, named energy-resolved population image (EPI), to represent on an equal footing the temporary electronic transition and nuclear motion during laser-molecular interaction. By using the EPI we have intuitively demonstrated the population transfer in vibrational H$_2^+$ exposed to extreme ultraviolet pulses, revealing the energy sharing rule for the correlated electron and nuclei. We further show that the EPI can be extended to uncover the origins of the distinct energy sharing mechanisms in multi-photon and tunneling regimes. The present study has clarified a long-standing issue about the dissociative ionization of H$_2^+$ and paves the way to identify instantaneous molecular dynamics in strong fields.

physics.atm-clus↗

arXiv2014

Molecular orbital tomography beyond the plane wave approximation

The use of plane wave approximation in molecular orbital tomography via high-order harmonic generation has been questioned since it was proposed, owing to the fact that it ignores the essential property of the continuum wave function. To address this problem, we develop a theory to retrieve the valence molecular orbital directly utilizing molecular continuum wave function which takes into account the influence of the parent ion field on the continuum electrons. By transforming this wave function into momentum space, we show that the mapping from the relevant molecular orbital to the high-order harmonic spectra is still invertible. As an example, the highest orbital of $\mathrm{N_2}$ is successfully reconstructed and it shows good agreement with the \emph{ab initio} orbital. Our work clarifies the long-standing controversy and strengthens the theoretical basis of molecular orbital tomography.

physics.atom-ph↗

arXiv2014

Probing rotational wave-packet dynamics with the structural minimum in high-order harmonic spectra

We investigate the alignment-dependent high-order harmonic spectrum generated from nonadiabatically aligned molecules around the first half rotational revival. It is found that the evolution of the molecular alignment is encoded in the structural minima. To reveal the relation between the molecular alignment and the structural minimum in the high-order harmonic spectrum, we perform an analysis based on the two-center interference model. Our analysis shows that the structural minimum position depends linearly on the inverse of the alignment parameter $<\cos^2θ>$. This linear relation indicates the possibility of probing the rotational wave-packet dynamics by measuring the spectral minima.

physics.atom-ph↗

arXiv2014

Revealing the role of electron correlation in sequential double ionization

The experimental observations of sequential double ionization (SDI) of Ar [A. N. Pfeiffer {\it et al.}, Nature Phys. {\bf 7}, 428 (2011)], such as the four-peak momentum distribution and the ionization time of the first and second electrons, are investigated and reproduced with a quantum model by including and excluding the $e$-$e$ correlation effect. Based on the comparison of experiment and simulation, the role of $e$-$e$ correlation in SDI is discussed. It is shown that the inclusion of $e$-$e$ correlation is necessary to reproduce the momentum distribution of electrons.

physics.atom-ph↗

arXiv2014

Revisiting the tunnelling site of electrons in strong field enhanced ionization of molecules

We investigated electron emissions in strong field enhanced ionization of asymmetric diatomic molecules by quantum calculations. It is demonstrated that the widely-used intuitive physical pic- ture, i.e., electron wave packet direct ionization from the up-field site (DIU), is incomplete. Besides DIU, we find another two new ionization channels, the field-induced excitation with subsequent ionization from the down-field site (ESID), and the up-field site (ESIU). The contributions from these channels depend on the molecular asymmetry and internuclear distance. Our work provides a more comprehensive physical picture for the long-standing issue about enhanced ionization of diatomic molecules.

physics.atom-ph↗

arXiv2013

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↗

arXiv2012

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↗

arXiv2011

Sub-cycle waveform synthesis for effective control of electron localization

We have proposed and demonstrated an effective scheme to steer both the electronic and molecular motions of hydrogen molecule and its isotopes. Our scheme lies in the idea of sub-cycle waveform shaping (SWS) with synthesizing coherent IR pulses of different wavelengths. The quantum model simulation indicates a remarkable enhancement of the electron localization asymmetry compared with the few-cycle pulse. 68% and 89% electrons of the dissociating fragmentation can be localized to one nucleus for H_2^+ and H_2, respectively.

physics.atom-ph↗

arXiv2008

Isolated sub-100-attosecond pulse generation via controlling electron dynamics

A new method to coherently control the electron dynamics is proposed using a few-cycle laser pulse in combination with a controlling field. It is shown that this method not only broadens the attosecond pulse bandwidth, but also reduces the chirp, then an isolated 80-as pulse is straightforwardly obtained and even shorter pulse is achievable by increasing the intensity of the controlling field. Such ultrashort pulses allow one to investigate ultrafast electronic processes which have never be achieved before. In addition, the few-cycle synthesized pulse is expected to manipulate a wide range of laser-atom interactions.

physics.atom-ph↗

arXiv2008

Carrier-envelope phase measurement from half-cycle high harmonics

We present a method to distinguish the high harmonics generated in individual half-cycle of the driving laser pulse by mixing a weak ultraviolet pulse, enabling one to observe the cutoff of each half-cycle harmonic. We show that the detail information of the driving laser pulse, including the laser intensity, pulse duration and carrier-envelope phase, can be {\it in situ} retrieved from the harmonic spectrogram. In addition, our results show that this method also distinguishes the half-cycle high harmonics for a pulse longer than 10 fs, suggesting a potential to extend the CEP measurement to the multi-cycle regime.

physics.atom-ph↗

arXiv2007

Efficient generation of an isolated single-cycle attosecond pulse

A new method for efficiently generating an isolated single-cycle attosecond pulse is proposed. It is shown that the ultraviolet (UV) attosecond pulse can be utilized as a robust tool to control the dynamics of electron wave packets (EWPs). By adding a UV attosecond pulse to an infrared (IR) few-cycle pulse at a proper time, only one return of the EWP to the parent ion is selected to effectively contribute to the harmonics, then an isolated two-cycle 130-as pulse with a bandwidth of 45 eV is obtained. After complementing the chirp, an isolated single-cycle attosecond pulse with a duration less than 100 as seems achievable. In addition, the contribution of the quantum trajectories can be selected by adjusting the delay between the IR and UV fields. Using this method, the harmonic and attosecond pulse yields are efficiently enhanced in contrast to the scheme [G. Sansone {\it et al.}, Science {\bf314}, 443 (2006)] using a few-cycle IR pulse in combination with the polarization gating technique.

physics.atom-ph↗