arXiv subjects

C. D. Lin

Publications and source records attributed to C. D. Lin.

At least 37 records · Page 2Linked to original sources

arXiv2011

Intensity dependence of multiple orbital contributions and shape resonance in high-order harmonic generation of aligned N$_{2}$ molecules}

We report measurements and theoretical simulations of high-order harmonic generation (HHG) in aligned N$_2$ molecules using a 1200-nm intense laser field when the generating pulse is perpendicular to the aligning one. With increasing laser intensity, the minimum in the HHG spectra first shifts its position and then disappears. Theoretical simulations including the macroscopic propagation effects in the medium reproduce these observations and the disappearance of the minimum is attributed to the additional contribution of HHG from inner orbitals. We also predict that the well-known shape resonance in the photoionization spectra of N$_2$ should exist in the HHG spectra. It is most clearly seen when the generating laser is parallel to the aligning one, and disappears gradually as the angle between the two lasers increases. No clear evidence of this shape resonance has been reported so far when using lasers with different wavelengths. Further experimentation is needed to draw conclusions.

physics.optics↗

arXiv2011

Generation of broad XUV continuous high harmonic spectra and isolated attosecond pulses with intense mid-infrared lasers

We present experimental results showing the appearance of a near-continuum in the high-order harmonic generation (HHG) spectra of atomic and molecular species as the driving laser intensity of an infrared pulse increases. Detailed macroscopic simulations reveal that these near-continuum spectra are capable of producing IAPs in the far field if a proper spatial filter is applied. Further, our simulations show that the near-continuum spectra and the IAPs are a product of strong temporal and spatial reshaping (blue shift and defocusing) of the driving field. This offers a possibility of producing IAPs with a broad range of photon energy, including plateau harmonics, by mid-IR laser pulses even without carrier-envelope phase stabilization.

physics.atom-ph↗

arXiv2011

Influence of gas pressure on high-order harmonic generation of Ar and Ne

We study the effect of gas pressure on the generation of high-order harmonics where harmonics due to individual atoms are calculated using the recently developed quantitative rescattering theory, and the propagation of the laser and harmonics in the medium is calculated by solving the Maxwell's wave equation. We illustrate that the simulated spectra are very sensitive to the laser focusing conditions at high laser intensity and high pressure since the fundamental laser field is severely reshaped during the propagation. By comparing the simulated results with several experiments we show that the pressure dependence can be qualitatively explained. The lack of quantitative agreement is tentatively attributed to the failure of the complete knowledge of the experimental conditions.

physics.atom-ph↗

arXiv2011

Generation of isolated attosecond pulses in the far field by spatial filtering with an intense few-cycle mid-infrared laser

We report theoretical calculations of high-order harmonic generation (HHG) of Xe with the inclusion of multi-electron effects and macroscopic propagation of the fundamental and harmonic fields in an ionizing medium. By using the time-frequency analysis we show that the reshaping of the fundamental laser field is responsible for the continuum structure in the HHG spectra. We further suggest a method for obtaining an isolated attosecond pulse (IAP) by using a filter centered on axis to select the harmonics in the far field with different divergence. We also discuss the carrier-envelope-phase dependence of an IAP and the possibility to optimize the yield of the IAP. With the intense few-cycle mid-infrared lasers, this offers a possible method for generating isolated attosecond pulses.

physics.atom-ph↗

arXiv2011

Analysis of effects of macroscopic propagation and multiple molecular orbitals on the minimum in high-order harmonic generation of aligned CO$_{2}$

We report theoretical calculations on the effect of the multiple orbital contribution in high-order harmonic generation (HHG) from aligned CO$_2$ with inclusion of macroscopic propagation of harmonic fields in the medium. Our results show very good agreements with recent experiments for the dynamics of the minimum in HHG spectra as laser intensity or alignment angle changes. Calculations are carried out to check how the position of the minimum in HHG spectra depends on the degrees of molecular alignment, laser focusing conditions, and the effects of alignment-dependent ionization rates of the different molecular orbitals. These analyses help to explain why the minima observed in different experiments may vary.

physics.atom-ph↗

arXiv2011

Calibration of distorted wave Born approximation for electron impact excitation of Ne and Ar at incident energies below 100 eV

We calibrate the distorted wave Born approximation (DWBA) for electron impact excitation processes empirically. Differential cross sections (DCS) for the excitation of the $2p^53s$, $2p^53p$,$2p^54s$, and $2p^54p$ configurations of Ne and the $3p^54s$ and $3p^54p$ configurations of Ar by electron impact are calculated using DWBA for incident energies between 20 and 100 eV. The calculated results are compared with the absolute experimental measurements and other theoretical results. We found that the structure of the DCS can be well reproduced by the DWBA model while the magnitude is overestimated for most cases considered here. The differences in magnitude between DWBA and experiment are used to test the calibration of DWBA such that the DWBA can be used to describe laser-induced electron impact excitation processes. These processes are involved in the non-sequential double ionization of atoms in strong laser fields.

physics.atom-ph↗

arXiv2010

Medium propagation effects in high harmonic generation of Ar and N$_{2}$

We report theoretical calculations of high harmonic generation (HHG) by intense infrared lasers in atomic and molecular targets taking into account the macroscopic propagation of both fundamental and harmonic fields. On the examples of Ar and N$_2$, we demonstrate that these {\it ab initio} calculations are capable of accurately reproducing available experimental results with isotropic and aligned target media. We further present detailed analysis of HHG intensity and phase, under various experimental conditions, in particular, as the wavelength of the driving laser changes. Most importantly, our results strongly support the factorization of HHG at the macroscopic level into a product of a returning electron wave packet and the photorecombination transition dipole, under typical experimental conditions. This implies that the single-atom/molecule structure information can be retrieved from experimentally measured HHG spectra.

physics.atom-ph↗

arXiv2010

Separation of Target Structure and Medium Propagation Effects in High-Harmonic Generation

We calculate high-harmonic generation (HHG) by intense infrared lasers in atoms and molecules with the inclusion of macroscopic propagation of the harmonics in the gas medium. We show that the observed experimental spectra can be accurately reproduced theoretically despite that HHG spectra are sensitive to the experimental conditions. We further demonstrate that the simulated (or experimental) HHG spectra can be factored out as a product of a \macroscopic wave packet" and the photo-recombination transition dipole moment where the former depends on the laser properties and the experimental conditions, while the latter is the property of the target only. The factorization makes it possible to extract target structure from experimental HHG spectra, and for ultrafast dynamic imaging of transient molecules.

physics.atom-ph↗

arXiv2010

Polarization and ellipticity of high-order harmonics from aligned molecules generated by linearly polarized intense laser pulses

We present theoretical calculations for polarization and ellipticity of high-order harmonics from aligned N$_2$, CO$_2$, and O$_2$ molecules generated by linearly polarized lasers. Within the rescattering model, the two polarization amplitudes of the harmonics are determined by the photo-recombination amplitudes for photons emitted parallel and perpendicular to the direction of the {\em same} returning electron wave packet. Our results show clear species-dependent polarization states, in excellent agreement with experiments. We further note that the measured polarization ellipse of the harmonic furnishes the needed parameters for a "complete" experiment in molecules.

physics.atom-ph↗

arXiv2010

New determination of structure parameters in strong field tunneling ionization theory of molecules

In the strong field molecular tunneling ionization theory of Tong et al. [Phys. Rev. A 66, 033402 (2002)], the ionization rate depends on the asymptotic wavefunction of the molecular orbital from which the electron is removed. The orbital wavefunctions obtained from standard quantum chemistry packages in general are not good enough in the asymptotic region. Here we construct a one-electron model potential for several linear molecules using density functional theory (DFT). We show that the asymptotic wavefunction can be improved with an iteration method and after one iteration accurate asymptotic wavefunctions and structure parameters are determined. With the new parameters we examine the alignment-dependent tunneling ionization probabilities for several molecules and compare with other calculations and with recent measurements, including ionization from inner molecular orbitals.

physics.atom-ph↗

arXiv2009

Uncovering multiple orbitals influence in high harmonic generation from aligned N$_2$

Recent measurements on high-order harmonic generation (HHG) from N$_2$ aligned perpendicular to the driving laser polarization [B. K. McFarland {\it el al}, Science {\bf 322}, 1232 (2008)] have shown a maximum at the rotational half-revival. This has been interpreted as the signature of the HHG contribution from the molecular orbital just below the highest occupied molecular orbital (HOMO). By using the recently developed quantitative rescattering theory combined with accurate photoionization transition dipoles, we show that the maximum at the rotational half-revival is indeed associated with the HOMO-1 contribution. Our results also show that the HOMO-1 contribution becomes increasingly more important near the HHG cutoff and therefore depends on the laser intensity.

physics.atom-ph↗

arXiv2009

A robust all-non-optical method for the characterization of single-shot few-cycle laser pulses

An all non-optical method for accurately determining the pulse parameters of individual few-cycle laser shots is presented. By analyzing the "left" and "right" asymmetry of high-energy photoelectrons along the polarization axis using the recently developed quantitative rescattering theory, we show that the carrier-envelope phase, the pulse duration and the peak intensity of each single-shot pulse can be readily retrieved. Unlike optical measurements, this method provides the laser intensity in the interaction region directly.

physics.atom-ph↗

arXiv2009

Quantitative Rescattering Theory for high-order harmonic generation from molecules

The Quantitative Rescattering Theory (QRS) for high-order harmonic generation (HHG) by intense laser pulses is presented. According to the QRS, HHG spectra can be expressed as a product of a returning electron wave packet and the photo-recombination differential cross section of the {\em laser-free} continuum electron back to the initial bound state. We show that the shape of the returning electron wave packet is determined mostly by the laser only. The returning electron wave packets can be obtained from the strong-field approximation or from the solution of the time-dependent Schrödinger equation (TDSE) for a reference atom. The validity of the QRS is carefully examined by checking against accurate results for both harmonic magnitude and phase from the solution of the TDSE for atomic targets within the single active electron approximation. Combining with accurate transition dipoles obtained from state-of-the-art molecular photoionization calculations, we further show that available experimental measurements for HHG from partially aligned molecules can be explained by the QRS. Our results show that quantitative description of the HHG from aligned molecules has become possible. Since infrared lasers of pulse durations of a few femtoseconds are easily available in the laboratory, they may be used for dynamic imaging of a transient molecule with femtosecond temporal resolutions.

physics.atom-ph↗

arXiv2009

Probing molecular frame photoionization via laser generated high-order harmonics from aligned molecules

Present photoionization experiments cannot measure molecular frame photoelectron angular distributions (MFPAD) from the outermost valence electrons of molecules. We show that details of the MFPAD can be retrieved with high-order harmonics generated by infrared lasers from aligned molecules. Using accurately calculated photoionization transition dipole moments for fixed-in-space molecules, we show that the dependence of the magnitude and phase of the high-order harmonics on the alignment angle of the molecules observed in recent experiments can be quantitatively reproduced. This result provides the needed theoretical basis for ultrafast dynamic chemical imaging using infrared laser pulses.

physics.atom-ph↗

arXiv2008

Quantitative rescattering theory for laser-induced high-energy plateau photoelectron spectra

A comprehensive quantitative rescattering (QRS) theory for describing the production of high-energy photoelectrons generated by intense laser pulses is presented. According to the QRS, the momentum distributions of these electrons can be expressed as the product of a returning electron wave packet with the elastic differential cross sections (DCS) between free electrons with the target ion. We show that the returning electron wave packets are determined mostly by the lasers only, and can be obtained from the strong field approximation. The validity of the QRS model is carefully examined by checking against accurate results from the solution of the time-dependent Schrödinger equation for atomic targets within the single active electron approximation. We further show that experimental photoelectron spectra for a wide range of laser intensity and wavelength can be explained by the QRS theory, and that the DCS between electrons and target ions can be extracted from experimental photoelectron spectra. By generalizing the QRS theory to molecular targets, we discuss how few-cycle infrared lasers offer a promising tool for dynamic chemical imaging with temporal resolution of a few femtoseconds.

physics.atom-ph↗

arXiv2008

Origin of Plateau and Species dependence of Laser-Induced High-Energy Photoelectron Spectra

We analyzed the energy and momentum distributions of laser-induced high-energy photoelectrons of alkali and rare gas atoms. For the plateau electrons with energies above $4U_p$, ($U_p$ is the ponderomotive energy), in the tunneling ionization regime, we showed that they originate from the backscattering of laser-induced returning electrons. Using the differential elastic scattering cross sections between the target ion with \emph{free} electrons, we explain experimental observations of whether the plateau electron spectra is flat or steeply descending, and their dependence on species and laser intensity. This quantitative rescattering theory can be used to obtain energy and momentum distributions of plateau electrons without the need of solving the time-dependent Schrödinger equation, but with similar accuracy.

physics.atom-ph↗

arXiv2008

Retrieval of interatomic separations of molecules from laser-induced high-order harmonic spectra

We illustrate an iterative method for retrieving the internuclear separations of N$_2$, O$_2$ and CO$_2$ molecules using the high-order harmonics generated from these molecules by intense infrared laser pulses. We show that accurate results can be retrieved with a small set of harmonics and with one or few alignment angles of the molecules. For linear molecules the internuclear separations can also be retrieved from harmonics generated using isotropically distributed molecules. By extracting the transition dipole moment from the high-order harmonic spectra, we further demonstrated that it is preferable to retrieve the interatomic separation iteratively by fitting the extracted dipole moment. Our results show that time-resolved chemical imaging of molecules using infrared laser pulses with femtosecond temporal resolutions is possible.

physics.atom-ph↗

arXiv2008

Theory of high-order harmonic generation from molecules by intense laser pulses

We show that high-order harmonics generated from molecules by intense laser pulses can be expressed as the product of a returning electron wave packet and the photo-recombination cross section (PRCS) where the electron wave packet can be obtained from simple strong-field approximation (SFA) or from a companion atomic target. Using these wave packets but replacing the PRCS obtained from SFA or from the atomic target by the accurate PRCS from molecules, the resulting HHG spectra are shown to agree well with the benchmark results from direct numerical solution of the time-dependent Schrödinger equation, for the case of H$_2^+$ in laser fields. The result illustrates that these powerful theoretical tools can be used for obtaining high-order harmonic spectra from molecules. More importantly, the results imply that the PRCS extracted from laser-induced HHG spectra can be used for time-resolved dynamic chemical imaging of transient molecules with temporal resolutions down to a few femtoseconds.

physics.atom-ph↗