Search

The orientation and ellipticity of terahertz (THz) polarization generated by a two-color strong field not only casts light on underlying mechanisms of laser–matter interaction, but also plays an important role for various applications. We develop the Coulomb-corrected classical trajectory Monte Carlo (CTMC) method to well reproduce the joint measurements, that the THz polarization generated by the linearly polarized 800 nm and circularly polarized 400 nm fields is independent on two-color phase delay. The trajectory analysis shows that the Coulomb potential twists the THz polarization by deflecting the orientation of asymptotic momentum of electron trajectories. Further, the CTMC calculations predict that, the two-color mid-infrared field can effectively accelerate the electron rapidly away from the parent core to relieve the disturbance of Coulomb potential, and simultaneously create large transverse acceleration of trajectories, leading to the circularly polarized THz radiation.

The two-color strong-field mixing in gas medium is a widely used approach to generate bright broadband terahertz (THz) radiation. Here, we present a new, to the best of our knowledge, and counterintuitive method to promote THz performance in the two-color scheme. Beyond our knowledge that the maximum THz generation occurs with two-color foci overlapped, we found that, when the foci of two-color beams are noticeably separated along the propagation axis resulting in cascading plasmas, the THz conversion efficiency is surged by one order of magnitude and the bandwidth is stretched by more than two times, achieving 10−3 conversion efficiency and >100 THz bandwidth under the condition of 800/400 nm, ∼35 fs driving lasers. With the help of the pulse propagation equation and photocurrent model, the observations can be partially understood by the compromise between THz generation and absorption due to the spatial redistribution of laser energy in cascading plasmas. The present method can be extended to a mid-infrared driving laser, and new records of THz peak power and conversion efficiency are expected.

Focusing two-color laser fields in gas-phase medium produces ultrashort ultra-broadband low-order harmonics spanning from terahertz to extreme ultraviolet regime. The low-order harmonic generation can be explained by both macroscopic photocurrent model and microscopic strong field approximation theory. Here, we analytically build a bridge between the macroscopic and microscopic theories by means of the trajectory method, which manifests correspondences between macroscopic and microscopic theories. And we demonstrate the trajectory analysis to explain phase-dependent terahertz and third-harmonic generations, and contribute the phase-dependent yields and spectral shapes to the coherent superposition of electron trajectories released at distinct ionization instants, reflecting electron interfering with itself in radiation process. The trajectory method readily connects the low-order harmonics characteristics and behaviors of electron wavepacket, which has potential for reconstructing ultrafast electron dynamics by means of low-harmonics observations.

We perform high-resolution measurements of momentum distribution on ${\mathrm{Rb}}^{n+}$ recoil ions up to charge state $n=4$, where laser-cooled rubidium atoms are ionized by femtosecond elliptically polarized lasers with the pulse duration of 35 fs and the intensity of $3.3\ifmmode\times\else\texttimes\fi{}{10}^{15}\phantom{\rule{0.16em}{0ex}}\mathrm{W}/\mathrm{c}{\mathrm{m}}^{2}$ in the over-barrier ionization (OBI) regime. The momentum distributions of the recoil ions are found to exhibit multiband structures as the ellipticity varies from the linear to circular polarizations. The origin of these band structures can be explained quantitatively by the simple man model based on the OBI mechanism and dedicated classical trajectory Monte Carlo simulations with Heisenberg potential. Specifically, with back analysis of the classical trajectories, we reveal the ionization time and the OBI geometry of the sequentially released electrons, disentangling the mechanisms behind the tilted angle of the band structures. These results indicate that the classical treatment can describe the strong-field multiple ionization processes of alkali atoms.

The gas-phase medium ionized by two-color femtosecond field produces supercontinuum radiation ranging from the terahertz to midinfrared band. Under the strong-field approximation, the electron trajectory backanalysis is exploited to interpret the spectral profile of terahertz radiation. Meanwhile, the electron trajectory method can correlate terahertz spectral profiles and photoelectron momentum distributions (PEMDs). The coherent superposition of electron trajectories released from the consecutive cycles is found to induce the high-frequency cutoff and sharpen the spectral bandwidth of supercontinuum radiation, tightly coinciding with the intercycle interference fringes in PEMDs. The trajectory analysis exhibits that single electron interference plays an important role in the terahertz generation process. Our method provides an intuitive interpretation in terms of electron trajectory perspective and sheds light on the microscopic mechanisms of terahertz generation.

High-order harmonic generation by a femtosecond laser pulse in the presence of a moderately strong terahertz (THz) field is studied under the strong field approximation. We demonstrate a simple proportionality of near-cutoff even-order harmonic (NCEH) amplitude to the THz electric field. The formation of the THz-induced NCEHs is analytically shown for both continuous-wave and Gaussian pulses. The perturbation analysis with regard to the frequency ratio of the THz field to the femtosecond pulse shows the THz-induced NCEHs originate from its first-order correction of the action in the presence of the THz vector potential, and the available parametric conditions for the phenomenon are also clarified. As the complete characterization of the time-domain waveform of the broadband THz field is essential for a wide variety of applications, the paper provides an alternative time-resolved field-detection technique, allowing for a robust broadband characterization of pulses in THz spectral range.

Employing recently developed magneto-optical trap recoil ion momentum spectroscopy (MOTRIMS) combined with cold atoms, strong laser pulse, and ultrafast technologies, we study momentum distributions of the multiply ionized cold rubidium (Rb) induced by the elliptically polarized laser pulses (35 fs, 1.3 × 1015 W/cm2). The complete vector momenta of Rb n+ ions up to charge state n = 4 are recorded with extremely high resolution (0.12 a.u. for Rb+). Variations of characteristic multi-bands are displayed in momentum distributions because the ellipticity varies from the linear to circular polarization, are interpreted qualitatively with the classical over-barrier ionization model. Present momentum spectroscopy of cold heavy alkali atoms presents novel strong-field phenomena beyond the noble gases.

The low-order harmonic generation induced by a strong laser field produces a bright, ultrashort, supercontinuum radiation ranging from the terahertz to ultraviolet band. By controlling the phase-delay and ellipticity of the bi-chromatic laser fields, the third harmonic generation is experimentally and theoretically investigated for elucidating the mechanism of the low-order harmonics. The third harmonic generation is found to be strongly suppressed in the counter-rotating bi-chromatic laser field due to the selection rule for harmonic emissions. The continuum-continuum transition in the strong field approximation is extended to explain the third harmonic generation as a function of the phase delay and ellipticity of the bi-chromatic laser fields. Compared with the semi-classical photocurrent model, the continuum-continuum transition on the basis of quantum-mechanical treatment achieves better agreement with the experimental observations. Our work indicates that the overlapping in continuum states via different quantum paths of a single electron plays a role in low-order harmonics generation under elliptical bi-chromatic laser fields.

The transient transmittance spectra of laser dye IR144 in methanol were investigated experimentally in the moderately strong pump-probe field. Observed emission spectra in the red edge of the incident-field bandwidth, created by resonant impulsive stimulated Raman scattering (RISRS), display significant nonlinear intensity dependence as the pulse intensity increases. Dynamic perspectives of RISRS spectra can be understood well in a wavepacket picture. The excitation of high vibrational levels in the ground electronic state leading to the redshift of emissions presents high dependence of the pump-pulse intensity and ultrafast dynamical features, mapping the spatial overlap and separation of ground and excited wave functions and resolving the ultrafast vibrational relaxation in the femtosecond regime.

We present an approach, a Terahertz streaking-assisted photoelectron spectrum (THz SAPS), to achieve direct observations of ultrafast coherence dynamics with timescales beyond the pulse duration. Using a 24 fs probe pulse, the THz SAPS enables us to well visualize Rabi oscillations of 11.76 fs and quantum beats of 2.62 fs between the 5S 1/2 and 5P 3/2 in rubidium atoms. The numerical results show that the THz SAPS can simultaneously achieve high resolution in both frequency and time domains without the limitation of Heisenberg uncertainty of the probe pulse. The long probe pulse promises sufficiently high frequency resolution in photoelectron spectroscopy allowing to observe Autler–Townes splittings, whereas the streaking THz field enhances temporal resolution for not only Rabi oscillations but also quantum beats between the ground and excited states. The THz SAPS demonstrates a potential applicability for observation and manipulation of ultrafast coherence processes in frequency and time domains.

The origin of terahertz (THz) generation in a gas-phase medium is still in controversy, although the THz sources have been applied across many disciplines. Herein, the THz generation in a dual-color field is investigated experimentally by precisely controlling the relative phase and polarization of dual-color lasers, where the accompanying third-harmonic generation is employed for in situ determination of the relative phase up to sub-wavelength accuracy. Joint studies with the strong approximation (SFA) theory reveal that the continuum-continuum (CC) transition within an escaped electron wave packet in the single atom gives birth to THz emission, without the necessity of considering the plasma effect. Meanwhile, we develop the analytic form from SFA-based CC description, which is able to reproduce and decompose the classical photocurrent model from the viewpoint of microscopic quantum theory, establishing the quantum-classical correspondence and bringing a novel insight into the mechanism of THz generation. Present studies leave open the possibility for probing the ultrafast dynamics of continuum electrons and a new dimension for the study of THz-related science and methodology.

Terahertz (THz) wave generation (TWG) in a dual-color laser is investigated with joint measurements between THz and third-harmonic generation, where the relative phase delay of dual-color fields is determined in situ in sub-wavelength accuracy, allowing for the clarification of the TWG mechanism in a direct comparison with various theoretical predictions. The delay- and polarization-dependent experiment validates that the continuum–continuum transition within the escaped electron wavepacket in the single atom gives birth to THz emission, while the bound energetic level does not contribute to TWG. TWG from atoms and molecules would provide an all-optical, vacuum-free, and ultrafast tool to record the spatiotemporal evolution of tunneling electron wavepackets.

The characterization of an unknown quantum system requires the Hamiltonian identification. The full access to the system, however, is usually restricted, hindering the direct retrieval of the relevant parameters, and a reliable indirect estimation is usually required. In this work, based on the reformulated form of the original algorithm of Burgarth et al. [Phys. Rev. A 79 020305 (2009)], the robustness of the estimation scheme against numerous sources of errors during the actual measurement is analyzed. The scheme is numerically studied for sites with a chain structure, exploring its applicability against observational errors including the limited signal-noise ratio and the finite spectral width. The spectral distribution of the end site is shown to determine the applicability of the method, and reducing the influence from truncated spectral components is critical to realize the robust reconstruction of the coupling strengths.

We propose a scheme that is able to generate the microwave controlled optical double optome-chanical induced transparency (OMIT) in a hybrid piezo-optomechanical cavity system, which a piezoelectric optomechanical crystal AlN-nanobeam resonator is placed in a superconducting microwave cavity, and the AlN-nanobeam resonator can be simultaneously driven by both the optical field via the radiation pressure and the microwave field via the piezoelectric interaction. We show that in the presence of a strong pumped optical field applied to the optomechanical crystal cavity through the optical waveguide and an intensely stimulated microwave field applied to the superconducting microwave cavity, a double-OMIT window can be observed in the weak output probe field. The mechanism is that a N-type four-level system can be formed by the system, when two driving fields and a probe field are applied to the corresponding levels, under the effect of quantum interference between different energy level pathways, the third-order nonlinear absorption is enhanced by the constructive quantum interference while the linear absorption is inhibited by the destruc- tive quantum interference, as a result, the double-OMIT window is generated. Our scheme can be applied to realize high-speed optical switches, high-resolution spectroscopy, coherent population trapping or quantum information processing in the solid state quantum systems., 7 pages, 8 figures

Implementing parallel and multivalued logic operations at the molecular scale has the potential to improve the miniaturization and efficiency of a new generation of nanoscale computing devices. Two-dimensional photon-echo spectroscopy is capable of resolving dynamical pathways on electronic and vibrational molecular states. We experimentally demonstrate the implementation of molecular decision trees, logic operations where all possible values of inputs are processed in parallel and the outputs are read simultaneously, by probing the laser-induced dynamics of populations and coherences in a rhodamine dye mounted on a short DNA duplex. The inputs are provided by the bilinear interactions between the molecule and the laser pulses, and the output values are read from the two-dimensional molecular response at specific frequencies. Our results highlights how ultrafast dynamics between multiple molecular states induced by light−matter interactions can be used as an advantage for performing complex logic operations in parallel, operations that are faster than electrical switching.

Non-linear optical spectroscopies probe the dynamics of optically active molecular systems interacting with a sequence of laser pulses. By encoding logical inputs into the allowed optical transitions, quantum dynamics of populations and coherences implement logic processing in parallel and a macroscopically readable output is obtained from the spectroscopic response. The resulting hardware-based logic improves the potentialities of molecular sized devices for computing applications. We introduce the basic concepts of this molecular computing scheme and discuss its strengths and drawbacks with respect to several performance indicators.

The origin of THz generation in dual-color laser fields is investigated by joint measurement of THz and third-harmonic generation, showing the single-atom-ionization determined THz wave is modulated by photocurrent behavior.

In a typical two-dimensional electronic spectroscopy (2DES) experiment, the timing errors of the coherence and emission time when determining the absolute time zeros usually introduce extraneous spectral phase slopes and distort the 2D spectrum. In this work, a phase-correction method that merely relies on the data post-processing algorithm is proposed. The method allows reconstructing the spectrum by simply subtracting the artificial linear spectral-phase slopes from the phase component of the 2D spectrum along both coherence and emission frequency axes. The new method has the advantages of ease of implementation and no need for the supplementary experiments and iterative fitting algorithm as commonly-used phasing methods, which may improve the phasing issue in 2DES and serve as a cross-check of now available phasing methods.

Terahertz-streaking photoionization can be exploited to resolve ultrafast quantum beating and reconstruct the ultrafast evolution of density matrix. Here, we propose an experimental strategy to implement the method merely with the tabletop femtosecond system and magneto-optical trap reaction microscopy. The probe pulse consists of an ultraviolet pulse with pulse duration of about 30 fs and a strong terahertz pulse with strength of about 2.6 fs in rubidium-atom superposition. The population and coherence terms of the density matrix can be projected into different positions of the photoelectron momentum distribution. The reconstruction algorithm was designed to acquire the ultrafast evolution of density matrix from the time-dependent photoelectron spectrum. The experimental conception can demonstrate the newly proposed transient spectral method only with the commercial femtosecond laser system and magneto-optical trap reaction microscopy, thus preventing the complex laser system, such as extreme ultraviolet free electron lasers and attosecond higher harmonics, allowing a new metrology to explore the coherence dynamics of quantum systems.

Bichromatic circularly polarized fields provide a useful tool to probe the ionization dynamics. In this work, we compare the photoelectron momentum distribution in few-cycle bichromatic field of different helicities. The spectral features are analyzed with semiclassical trajectories derived from the strong field approximation. In particular, the interference fringes in momentum distribution are investigated by tracking the ionization time and tunneling exits of released photoelectrons. Different types of trajectories that contribute to the interference fringes are elucidated.

In this study, a new magneto-optical trap (MOT) recoil ion momentum spectrometer is built for investigating the interactions between cold rubidium (Rb) atoms and strong laser fields. This compact device can provide cold Rb in three different modes: 2D MOT mode, in which the beam generated by a two-dimensional MOT is pushed directly to the interaction regime; molasses mode, in which cooling lasers are applied at the interaction regime; and 3D MOT mode, in which a quadrupole magnetic field is applied to form a three-dimensional MOT. The typical densities of the three target modes are estimated to be 107, 108, and 109 atoms/cm3, respectively. Switching between the target modes is expected to provide a broad range of laser intensities with reasonable count rates while avoiding space charge effects. A single photoionization experiment serves as a benchmark test of the recoil ion momentum resolution. The best resolution is estimated as an unprecedented 0.12 a.u. in the time-of-flight direction, demonstrating significant potential for strong field ionization dynamics using this technique.

The study of quantum evolution on graphs for diversified topologies is beneficial to modeling various realistic systems. A systematic method, the dimerized decomposition, is proposed to analyze the dynamics on an arbitrary network. By introducing global “flows” among interlinked dimerized subsystems, each of which locally consists of an input and an output port, the method provides an intuitive picture that the local properties of the subsystem are separated from the global structure of the network. The pictorial interpretation of quantum evolution as multiple flows through the graph allows for the analysis of the complex network dynamics supplementary to the conventional spectral method. Using the decomposition, the relation between spectral coefficients of adjacent sites with regard to individual dimer is obtained.

A time-resolved spectroscopic protocol exploiting terahertz-assisted photoionization is proposed to reconstruct transient density matrix. Population and coherence elements are effectively mapped onto spectrally separated peaks in photoionization spectra. The beatings of coherence dynamics can be temporally resolved beyond the pulse duration, and the relative phase between involved states is directly readable from the oscillatory spectral distribution. As demonstrated by a photo-excited multilevel open quantum system, the method shows potential applications for sub-femtosecond time-resolved measurements of coherent dynamics with free electron lasers and tabletop laser fields.

The population transfer via continuum for the Li2 molecule is theoretically investigated using time-dependent quantum wave packet method. With proper laser pulses, a high efficient population transfer can be achieved, and the selective ro-vibrational population transfer via continuum can be realized. The population transfer process is qualitatively interpreted employing the concept of light-induced potential. The effect of molecular rotation on the population transfer and the angular distribution of population is described in detail.

A new method determining the precise phase of pulse sequences in two-dimensional electronic spectroscopy (2DES) is proposed merely using the already built-in spectral interferometry. The approach is easily implemented without the supplementary instrumental construction, only at the expense of a few additional scanning and data-fitting processes. This method is executed with the sample in place, effectively avoiding the phase ambiguities of the beam propagation in samples, thus calibrating the absolute phase at the exact interaction region. The new proposed method is expected to improve the phasing procedure in 2DES in a more convenient way.

We present a passively phase-stabilized two-dimensional electronic spectroscopy (2DES) with a compact size, and the ease of implementation and maintenance. Our design relies on a mask beam-splitter with four holes to form non-collinear box geometry, and a homebuilt stacked retroreflector, which introduces the phase-locked pulse sequence, remedying the instability of commonly used translation stages. The minimized size of the setup suppresses the influences of optical path-length fluctuations during measurements, improving the phase stability and precise timing of pulse sequences. In our 2DES, only few conventional optical components are used, which make this sophisticated instrumentation convenient to establish and particularly easy to conduct alignment. In data analysis, the self-referencing spectral interferometry (SRSI) method is first introduced to extract the complex-valued signal from spectral interferometry in 2DES. The alternative algorithm achieves the improvement of the signal-to-noise ratio (SNR) and considerable reduction of data acquisition time. The new setup is suitable over a tunable range of spectroscopic wavelength, from ultraviolet (UV) to the near-infrared (NIR) regime, and for ultra-broadband bandwidth, few-cycle laser pulses.

International audience; Midinfrared strong-field laser ionization offers the promise of measuring holograms of atoms and molecules, which contain both spatial and temporal information of the ion and the photoelectron with subfemtosecond temporal and angstrom spatial resolution. We report on the scaling of photoelectron holographic interference patterns with the laser pulse duration, wavelength, and intensity. High-resolution holograms for the ionization of metastable xenon atoms by 7-16 m light from the FELICE free electron laser are presented and compared to semiclassical calculations that provide analytical insight.

The velocity map recorded in above-threshold ionization of xenon at 800 nm exhibits a distinct carpetlike pattern of maxima and minima for emission in the direction approximately perpendicular to the laser polarization. The pattern is well reproduced by a numerical solution of the time-dependent Schr\"odinger equation. In terms of the simple-man model and the strong-field approximation, it is explained by the constructive and destructive interference of the contribution of the long and the short orbit. Strictly perpendicular emission is caused by ionization at the two peaks of the laser field per cycle, which results in a $2\ensuremath{\hbar}\ensuremath{\omega}$ separation of the above-threshold ionization rings.

We use a quantum trajectory-based semi-classical method to account for Coulomb interaction between the photoelectron and the parent ion in the classically forbidden, sub-barrier region during strong-field tunneling ionization processes. We show that---besides the well-known modification of the tunneling ionization probability---there is also an influence on the interference pattern in the photoelectron spectra. In the long-wavelength limit, the shift of the intra-cycle interference fringes caused by sub-barrier Coulomb effects in the laser polarization direction can be derived analytically. We compare our results with \emph{ab initio} solutions of the time-dependent Schr\"odinger equation and find good agreement in the long-wavelength regime, whereas the standard strong field approximation fails. We show that the nodal structure along low-order above-threshold ionization rings is also affected by sub-barrier Coulomb effects., Comment: 10 pages, 4 figures, RevTeX

The strong field approximation (SFA) is one of the most successful theoretical approaches to tackle the problem of atomic or molecular ionization in intense laser fields. In the semi-classical limit, the SFA possesses an appealing interpretation in terms of interfering quantum trajectories, which mathematically originate from the saddle point approximation to the SFA transition matrix element. The trajectories not only allow to interpret particular features in photoelectron spectra in an intuitive way in terms of possible electron pathways typical for a quantum mechanical “multi-slit experiment” but also serve as a starting point for adopting Coulomb corrections.

Experiments on atoms in intense laser pulses and the corresponding exact ab initio solutions of the time-dependent Schr\"odinger equation (TDSE) yield photoelectron spectra with low-energy features that are not reproduced by the otherwise successful work horse of strong field laser physics: the "strong field approximation" (SFA). In the semi-classical limit, the SFA possesses an appealing interpretation in terms of interfering quantum trajectories. It is shown that a conceptually simple extension towards the inclusion of Coulomb effects yields very good agreement with exact TDSE results. Moreover, the Coulomb quantum orbits allow for a physically intuitive interpretation and detailed analysis of all low-energy features in the semi-classical regime, in particular the recently discovered "low-energy structure" [C.I. Blaga et al., Nature Physics 5, 335 (2009) and W. Quan et al., Phys. Rev. Lett. 103, 093001 (2009)]., Comment: 4 pages, 3 figures, REVTeX

The dissociation dynamics of Br2 molecules induced by two femtosecond pump pulses are studied based on the calculation of time-dependent quantum wave packet. Perpendicular transition from X 1Sigma g+ to A 3Pi 1u+ and 1Pi 1u+ and parallel transition from X 1Sigma g+ to B 3Pi 0u+, involving two product channels Br (2P3/2)+Br (2P3/2) and Br (2P3/2)+Br* (2P1/2), respectively, are taken into account. Two pump pulses create dissociating wave packets interfering with each other. By varying laser parameters, the interference of dissociating wave packets can be controlled, and the dissociation probabilities of Br2 molecules on the three excited states can be changed to different degrees. The branching ratio of Br*/(Br+Br*) is calculated as a function of pulse delay time and phase difference.