Intense Mid-infrared Laser Fields Research Articles

Shift of the photoelectron momentum against the radiation pressure force in linearly polarized intense midinfrared laser fields

The propagation direction momentum component of direct photoelectrons emitted by ionization of an atomic target in an intense, linearly polarized, midinfrared laser field is analyzed. Within the dipole approximation, the average value of this component is zero. However, when nondipole corrections are included, it becomes nonzero. Applying the saddle-point approximation to compute the integral over the ionization times in the expression for the nondipole strong-field approximation differential ionization rate, we surprisingly find a negative momentum shift, corresponding to a shift against the radiation pressure force. Our analysis shows that there is a positive contribution originating from individual ionization pathways within one optical cycle. The interference of contributions from ionization pathways arising within the same optical cycle of the field (intracycle interference) causes an oscillatory behavior, which, crossing to negative values, induces the shift against the radiation pressure force.

Strong-field approximation with leading-order nondipole corrections

Employing the nondipole Volkov states, i.e., the solutions of the time-dependent Schr\"odinger equation for an electron in a laser field whose spatial dependence is accounted for by including the first-order term in a $1/c$ expansion of the vector potential, we present an analytic approach based on the strong-field approximation that is able to describe ionization and detachment in intense midinfrared laser fields. Our approach includes both the direct transition amplitude and the improved strong-field approximation transition amplitude, accounting for the field-induced rescattering of the liberated electron on its parent core. We apply the theory to strong-field detachment from the ${F}^{\ensuremath{-}}$ ion. Comparing the results to those obtained invoking the dipole approximation, we identify and analyze the effects caused by including the nondipole corrections for the cases of circular and linear polarization. We demonstrate that the introduced nondipole corrections induce asymmetries in photoelectron momentum distributions along the propagation direction. For the case of linear polarization, we report a shift of the low-energy region of the momentum distribution against the propagation direction, a feature previously studied on neutral targets and related to Coulomb focusing effects.

Strong-field physics in three-dimensional topological insulators

We investigate theoretically the strong-field regime of light-matter interactions in the topological-insulator class of quantum materials. In particular, we focus on the process of non-perturbative high-order harmonic generation from the paradigmatic three-dimensional topological insulator bismuth selenide (Bi$_2$Se$_3$) subjected to intense mid-infrared laser fields. We analyze the contributions from the spin-orbit-coupled bulk states and the topological surface bands separately and reveal a major difference in how their harmonic yields depend on the ellipticity of the laser field. Bulk harmonics show a monotonous decrease in their yield as the ellipticity increases, in a manner reminiscent of high harmonic generation in gaseous media. However, the surface contribution exhibits a highly non-trivial dependence, culminating with a maximum for circularly polarized fields. We attribute the observed anomalous behaviour to: (i) the enhanced amplitude and the circular pattern of the interband dipole and the Berry connections in the vicinity of the Dirac point; and (ii) the influence of the higher-order, "hexagonal warping" terms in the Hamiltonian, which are responsible for the hexagonal deformation of the energy surface at higher momenta. The latter are associated directly with spin-orbit-coupling parameters. Our results thus establish the sensitivity of strong-field driven high harmonic emission to the topology of the band structure as well as to the manifestations of spin-orbit interaction.

Application of the time-dependent surface flux method to the time-dependent multiconfiguration self-consistent-field method

We present a numerical implementation of the time-dependent surface flux (tSURFF) method [New J. Phys. 14, 013021 (2012)], an efficient computational scheme to extract photoelectron energy spectra, to the time-dependent multiconfiguration self-consistent-field (TD-MCSCF) method. Extending the original tSURFF method developed for single particle systems, we formulate the equations of motion for the spectral amplitude of orbital functions constutiting the TD-MCSCF wave function, from which the angle-resolved photoelectron energy spectrum, and more generally, photoelectron reduced density matrices (RDMs) are readiliy obtained. The tSURFF method applied to the TD-MCSCF wave function, in combination with an efficient absorbing boundary offered by the infinite-range exterior complex scaling, enables accurate {\it ab initio} computations of photoelectron energy spectra from multielectron systems subject to an intense and ultrashort laser pulse with a computational cost significantly reduced compared to that required in projecting the total wave function onto scattering states. We apply the present implementation to the photoionization of Ne exposed to an attosecond extreme-ultraviolet (XUV) pulse and above-threshold ionization of Ar irradiated by an intense mid-infrared laser field, demonstrating both accuracy and efficiency of the present method.

High harmonic interferometry of the Lorentz force in strong mid-infrared laser fields

The interaction of intense mid-infrared laser fields with atoms and molecules leads to a range of new opportunities, from the production of bright, coherent radiation in the soft x-ray range, to imaging molecular structures and dynamics with attosecond temporal and sub-angstrom spatial resolution. However, all these effects, which rely on laser-driven recollision of an electron removed by the strong laser field and its parent ion, suffer from the rapidly increasing role of the magnetic field component of the driving pulse: the associated Lorentz force pushes the electrons off course in their excursion and suppresses all recollision-based processes, including high harmonic generation as well as elastic and inelastic scattering. Here we show how the use of two non-collinear beams with opposite circular polarizations produces a forwards ellipticity which can be used to monitor, control, and cancel the effect of the Lorentz force. This arrangement can thus be used to re-enable recollision-based phenomena in regimes beyond the long-wavelength breakdown of the dipole approximation, and it can be used to observe this breakdown in high harmonic generation using currently available light sources.

Generation of Raman lasers from nitrogen molecular ions driven by ultraintense laser fields

Atmospheric lasing has aroused much interest in the past few years. The ‘air–laser’ opens promising potential for remote chemical sensing of trace gases with high sensitivity and specificity. At present, several approaches have been successfully implemented for generating highly coherent laser beams in atmospheric condition, including both amplified-spontaneous emission, and narrow-bandwidth stimulated emission in the forward direction in the presence of self-generated or externally injected seed pulses. Here, we report on generation of multiple-wavelength Raman lasers from nitrogen molecular ions (), driven by intense mid-infrared laser fields. Intuitively, the approach appears problematic for the small nonlinear susceptibility of ions, whereas the efficiency of Raman laser can be significantly promoted in near-resonant condition. More surprisingly, a Raman laser consisting of a supercontinuum spanning from ∼310 to ∼392 nm has been observed resulting from a series near-resonant nonlinear processes including four-wave mixing, stimulated Raman scattering and cross phase modulation. To date, extreme nonlinear optics in molecular ions remains largely unexplored, which provides an alternative means for air–laser-based remote sensing applications.

Nonadiabatic ponderomotive effects in photoemission from nanotips in intense midinfrared laser fields

Transient near fields around metallic nanotips drive many applications, including the generation of ultrafast electron pulses and their use in electron microscopy. We have investigated the electron emission from a gold nanotip driven by midinfrared few-cycle laser pulses. We identify a low-energy peak in the kinetic energy spectrum and study its shift to higher energies with increasing laser intensities from 1.7 to $8.9\ifmmode\times\else\texttimes\fi{}{10}^{11}\phantom{\rule{0.28em}{0ex}}\mathrm{W}/{\mathrm{cm}}^{2}$. The experimental observation of the upshift of the low-energy peak is compared to a simple model and numerical simulations, which show that the decay of the near field on a nanometer scale results in nonadiabatic transfer of the ponderomotive potential to the kinetic energy of emitted electrons and in turn to a shift of the peak. We derive an analytic expression for the nonadiabatic ponderomotive shift, which, after the previously found quenching of the quiver motion, completes the understanding of the role of inhomogeneous fields in strong-field photoemission from nanostructures.

中红外波段超快强激光场驱动的原子单电离

中红外波段超快强激光场驱动的原子单电离

Nonperturbative generation of above-threshold harmonics from pre-excited argon atoms in intense mid-infrared laser fields

We experimentally investigate the generation of above-threshold harmonics completely from argon atoms on an excited state using mid-infrared femtosecond laser pulses. The highly nonlinear dependences of the observed signal on the pulse energy and polarization of the probe laser pulses indicate its nonperturbative characteristic.

Exploration of the electron multiple recollision dynamics in intense laser fields with Bohmian trajectories

Electron multiple recollision dynamics under intense midinfrared laser fields is studied by means of the de Broglie--Bohm framework of Bohmian mechanics. Bohmian trajectories contain all the information embedded in the time-dependent wave function. This makes the method suitable to investigate the coherent dynamic processes for which the phase information is crucial. In this study, the appearance of the subpeaks in the high-harmonic-generation time-frequency profiles and the asymmetric fine structures in the above-threshold ionization spectrum are analyzed by the comprehensive and intuitive picture provided by Bohmian mechanics. The time evolution of the individual electron trajectories is closely studied to address some of the major structural features of the photoelectron angular distributions.

Generation of the ultrabroad bandwidth with keV by three-color low intense mid-infrared inhomogeneous pulse

We numerically investigate the high-order harmonic generation and the isolated attosecond pulse generation from the coherent superposition initial state of He+ ion by using the three-color low intense mid-infrared laser field. It is found that by properly controlling the delay times and the carrier envelope phases of the three-color mid-infrared pulse, the harmonic cutoff has been extended, and the harmonic modulations can be controlled. Further, with the introduction of the inhomogeneous parameter of the three-color field, the harmonic cutoff can be further enhanced. As a result, a supercontinuum with the bandwidth of 1773eV can be obtained. Moreover, we found the harmonic yield is almost 4–6 orders of magnitude higher than that generated from the single initial state case. Classical and the quantum time–frequency analyses have been shown to explain the harmonic emission process. Finally, by properly superposing the harmonics, a series of wavelength-tunable sub-32as X-ray pulses can be obtained, which are almost 4–6 orders of magnitude improvement in comparison with the single ground initial state case.

The influences of multiphoton excitation on near-threshold Harmonic emission in atoms

When an atom or a molecule interacts with an intense laser field, a coherent high-order harmonic emission is observed at a frequency that is an integer multiple magnitude of the initial frequency of the incident laser field. The harmonic emission has the characteristic of high emission efficiency at relatively high orders, and it also has a wide expansion in the frequency domain. Thus, the high-order harmonic generation can be utilized to generate coherent EUV or soft X-ray light sources as well as ultrashort at to second laser pulses. It is promising that the attosecond laser pulse will be an important tool for detecting and controlling the electron dynamics in atom and molecule systems. The mechanisms of high-order harmonics especially the high energy part of the harmonic spectrum can be explained by the well-known three-step model. The three-step model assumes that the electron in the bound state firstly are ionized by the potential barrier formed by the laser electric field and the atomic potential, then the ionized electrons oscillate in the laser field, and finally the electron with high kinetic energy gained in the laser field has the possibility to return back to the parent ion and recombines with the ground state of the system with a high energy photon emitted. As for harmonics with low orders, especially those with single photon energy near the ionization threshold, the Coulomb potential of the atom has significant influences on them. However,the effect of the Coulomb potential of the atom are not included in the three-step model, so the mechanism of near-threshold harmonics (NTH) cannot be clearly interpreted with the three-step model alone. In this circumstance, the study of the mechanism of near-threshold harmonic emission attracted people's attention in general. One important application of NTH is that it can be utilized to generate optical comb with EUV frequencies. Theoretically, Xiong et al. studied the mechanism of below-threshold harmonic (BTH) emission and found that the mechanism of this part of harmonics include the effect of the quantum-path interference and the Coulomb potential. He et al. analyzed the emission of BTH in various laser intensity regions and found that the harmonic spectrum exhibits a periodic structure as a function of the harmonic frequency when the incident laser intensity is about 1013 W/cm2. Utilizing the quantum-path and time-frequency analyses of the harmonic emission, He et al. indicated that this periodic structure can be attributed to the interference effect between two specific quantum paths. Li et al. adopted the synchrosqueezing scheme to study the near-and below-threshold harmonic emission of Cs atoms in an intense mid-infrared laser field and they showed that the multiphoton and the multiple rescattering trajectories have an effect on the NTH and BTH generation processes. Shafir et al. found that the ionic potential plays an critical role in NTH emission. Under the interaction between the atom and the intense laser field, electron in the ground state not only can be ionized but also be pumped into excited state, and these excitation processes also affect the harmonic emission. We studied the harmonic emission process near the ionization threshold by solving the time-dependent Schrdinger equation of an atom interacting with a strong laser field. Utilizing the obtained wavefunction, we systematically studied the high-order harmonic emission with the variation of the incident laser intensity. Meanwhile, through solving the TDSE with the momentum-space method, the excited-state population is precisely calculated and achieved. We show that the ninth harmonic exhibits a periodic oscillation structure with the intensity of the incident laser field increasing, and we reveals that there is a synchronous variation between the harmonic intensity and the relatively high bound state population.Within a certain range of laser intensity, the increase of the total population of the excited states corresponds to the low efficiency of harmonic emission, and this competition relationship is quite clear. Therefore, when the wavelength of the driving laser pulse is fixed, we can optimize the driving laser intensity to achieve the near-threshold harmonic emission with high efficiency.

Dynamical origin of near- and below-threshold harmonic generation of Cs in an intense mid-infrared laser field.

Near- and below-threshold harmonic generation provides a potential approach to generate vacuum-ultraviolet frequency comb. However, the dynamical origin of in these lower harmonics is less understood and largely unexplored. Here we perform an ab initio quantum study of the near- and below-threshold harmonic generation of caesium (Cs) atoms in an intense 3,600-nm mid-infrared laser field. Combining with a synchrosqueezing transform of the quantum time-frequency spectrum and an extended semiclassical analysis, the roles of multiphoton and multiple rescattering trajectories on the near- and below-threshold harmonic generation processes are clarified. We find that the multiphoton-dominated trajectories only involve the electrons scattered off the higher part of the combined atom-field potential followed by the absorption of many photons in near- and below-threshold regime. Furthermore, only the near-resonant below-threshold harmonic is exclusive to exhibit phase locked features. Our results shed light on the dynamic origin of the near- and below-threshold harmonic generation.

Bond-Selective Dissociation of Polyatomic Cations in Mid-Infrared Strong Fields

Strong field-induced dissociation by intense mid-infrared pulses was investigated in bromofluoroform monocation (CF3Br(+)) and iodobenzene dication (C6H5I(2+)) using ab initio molecular dynamics calculations. In both systems, bond -selective dissociation was achieved using appropriate laser polarizations and wavelengths. For CF3Br(+), energetically disfavored fluorine elimination was strongly enhanced at wavelengths of 7 to 8 μm with polarization along a C-F bond. This is the result of two effects: the deposition of high enough kinetic energy into the molecule by the laser field and the near-resonant excitation of the C-F stretching mode. At shorter and off-resonant wavelengths, bromine elimination becomes significant due to rapid intramolecular vibrational energy redistribution (IVR). For C6H5I(2+), the branching ratios for the dissociation of the ortho-, meta-, and para-hydrogens can be controlled simply by changing the laser polarization. These results show the general applicability of bond selective dissociation of cations by intense mid-infrared laser fields.

Enhanced multiple-scattering and intra-half-cycle interferences in the photoelectron angular distributions of atoms ionized in midinfrared laser fields

We investigate the physical mechanisms responsible for fine structure in the photoelectron angular distributions from atoms subject to intense midinfrared laser fields by solving the time-dependent Schr\"odinger equation in the integral form. By restricting the ionization to a half cycle of the laser field and then propagating the liberated electron wave packet during the laser pulse, we show conclusively that low-energy-momenta structure in the photoelectron angular distribution originates from multiple scatterings of the tunnel-ionized electron with the ion. We also show that two conditions must be satisfied simultaneously in order to observe prominent low-energy features. First, multiple scattering of the tunnel-ionized electron wave packet is necessary. Second, tunnel ionization must dominate over multiphoton ionization. While the first condition is generally satisfied for all laser wavelengths, the second condition is satisfied only for longer laser wavelengths.

Spectral Minimum and Giant Enhancement in Photoelectron Spectra from Xenon Atoms Driven by Intense Midinfrared Laser Fields

Our theoretical study shows that the spectral minimum and the giant enhancement structures observed in the high harmonic spectra also exist in the photoelectron spectra from driven Xe atoms. They are attributed to the inherent property of the radial part of the wave function of the Xe 5p subshell in momentum space. The spectral minimum is caused by the nodal point in the modulus of the radial wave function in momentum space, and the giant enhancement reflects the increase in magnitude of the modulus of the wave function. To observe these structures, midinfrared lasers of about 0.2 PW/cm(2) intensity are preferred. Employing circularly polarized laser light is suggested for exhibiting these structures in photoelectron spectra.

Inelastic Scattering of Broadband Electron Wave Packets Driven by an Intense Midinfrared Laser Field

Intense, 100 fs laser pulses at 3.2 and 3.6 μm are used to generate, by multiphoton ionization, broadband wave packets with up to 400 eV of kinetic energy and charge states up to Xe(+6). The multiple ionization pathways are well described by a white electron wave packet and field-free inelastic cross sections, averaged over the intensity-dependent energy distribution for (e, ne) electron impact ionization. The analysis also suggests a contribution from a 4d core excitation, or giant resonance, in xenon.

Redshift in the Optical Absorption of ZnO Single Crystals in the Presence of an Intense Midinfrared Laser Field

We report time-resolved electroabsorption of a weak probe in a 500 μm thick zinc-oxide crystal in the presence of a strong midinfrared pump in the tunneling limit. We observe a substantial redshift in the absorption edge that scales with the cube root of intensity up to 1 TW/cm(2) (0.38 eV cm(2/3) TW(-1/3)) after which it increases more slowly to 0.4 eV at a maximum applied intensity of 5 TW/cm(2). The maximum shift corresponds to more than 10% of the band gap. The change in scaling occurs in a regime of nonperturbative high-order harmonic generation where electrons undergo periodic Bragg scattering from the Brillouin zone boundaries. It also coincides with the limit where the electric field becomes comparable to the ratio of the band gap to the lattice spacing.

Phonon scattering of hot electrons in intense mid‐infrared laser fields

AbstractWe calculated intravalley and intervalley phonon scattering rates of accelerated electrons under intense midinfrared laser fields. We extended the Keldysh theory, which assumes oscillatory motion of Bloch electrons driven by intense laser fields, to phonon scattering of electrons in semiconductors. We find that phonon emission is possible even if the initial electron energy is less than the phonon energy due to multi‐photon absorption processes. We also find that the scattering rates increase with electric field strength and wavelength. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)

Two-Electron Dissociative Ionization of H2 and D2 in Infrared Laser Fields.

We present a quantitative physical model of above-threshold dissociation of homonuclear molecular ions in intense midinfrared laser fields. This allows us to describe self-consistently all three processes that occur during dissociative ionization of ${\mathrm{H}}_{2}$ and ${\mathrm{D}}_{2}$ (ionization of the neutral molecule, dissociation of the molecular ion, and its secondary ionization) using a semiclassical approach. The kinetic energy spectrum of the dissociating fragments is obtained and analyzed.