Coulomb potential determining terahertz polarization in a two-color laser field.

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.

Trajectory analysis for low-order harmonic generation in two-color strong laser fields.

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.

Intensity-surged and bandwidth-extended terahertz radiation in two-foci cascading plasmas.

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.

Third-order harmonic generation in a bi-chromatic elliptical laser field.

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.

Experimental evidence for terahertz emission of continuum electrons in the dual-color laser field.

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.

Ultrafast Mapping of Coherent Dynamics and Density Matrix Reconstruction in a Terahertz-Assisted Laser Field.

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 photoexcited multilevel open quantum system, the method shows potential applications for subfemtosecond time-resolved measurements of coherent dynamics with free electron lasers and tabletop laser fields.

Information processing in parallel through directionally resolved molecular polarization components in coherent multidimensional spectroscopy.

We propose that information processing can be implemented by measuring the directional components of the macroscopic polarization of an ensemble of molecules subject to a sequence of laser pulses. We describe the logic operation theoretically and demonstrate it by simulations. The measurement of integrated stimulated emission in different phase matching spatial directions provides a logic decomposition of a function that is the discrete analog of an integral transform. The logic operation is reversible and all the possible outputs are computed in parallel for all sets of possible multivalued inputs. The number of logic variables of the function is the number of laser pulses used in sequence. The logic function that is computed depends on the chosen chromophoric molecular complex and on its interactions with the solvent and on the two time intervals between the three pulses and the pulse strengths and polarizations. The outputs are the homodyne detected values of the polarization components that are measured in the allowed phase matching macroscopic directions, kl, kl=∑iliki where ki is the propagation direction of the ith pulse and {li} is a set of integers that encodes the multivalued inputs. Parallelism is inherently implemented because all the partial polarizations that define the outputs are processed simultaneously. The outputs, which are read directly on the macroscopic level, can be multivalued because the high dynamical range of partial polarization measurements by nonlinear coherent spectroscopy allows for fine binning of the signals. The outputs are uniquely related to the inputs so that the logic is reversible.

Low-energy structures in strong field ionization revealed by quantum orbits.

Experiments on atoms in intense laser pulses and the corresponding exact ab initio solutions of the time-dependent Schrödinger 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 semiclassical 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 semiclassical regime, in particular, the recently discovered "low-energy structure" [C. I. Blaga, Nature Phys. 5, 335 (2009) and W. Quan, Phys. Rev. Lett. 103, 093001 (2009).

Steering dissociation of Br2 molecules with two femtosecond pulses via wave packet interference.

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.