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We conducted a joint theoretical and experimental study to investigate the collisional dissipation of molecular alignment. By comparing experimental measurements to the quantum simulations, the nonsecular effect in the collision dissipation of molecular alignment was unveiled from the gas-density-dependent decay rates of the molecular alignment revival signals. Different from the conventional perspective that the nonsecular collisional effect rapidly fades within the initial few picoseconds following laser excitation, our simulations of the time-dependent decoherence process demonstrated that this effect can last for tens of picoseconds in the low-pressure regime. This extended timescale allows for the distinct identification of the nonsecular effect from molecular alignment signals. Our findings present the pioneering evidence that nonsecular molecular collisional dissipation can endure over an extended temporal span, challenging established concepts and strengthening our understanding of molecular dynamics within dissipative environments.

Real-time visualization of molecular transformations is a captivating yet challenging frontier of ultrafast optical science and physical chemistry. While ultrafast x-ray and electron diffraction methods can achieve the needed subangstrom spatial resolution, their temporal resolution is still limited to hundreds of femtoseconds, much longer than the few femtoseconds required to probe real-time molecular dynamics. Here, we show that high-order harmonics generated by intense femtosecond lasers can be used to image molecules with few-ten-attosecond temporal resolution and few-picometer spatial resolution. This is achieved by exploiting the sensitive dependence of molecular recombination dipole moment to the geometry of the molecule at the time of harmonic emission. In a proof-of-principle experiment, we have applied this high-harmonic structure imaging (HHSI) method to monitor the structural rearrangement in NH_{3}, ND_{3}, and N_{2} from one to a few femtoseconds after the molecule is ionized by an intense laser. Our findings establish HHSI as an effective approach to resolve molecular dynamics with unprecedented spatiotemporal resolution, which can be extended to trace photochemical reactions in the future.

If the time evolution of a quantum state leads back to the initial state, a geometric phase is accumulated that is known as the Berry phase for adiabatic evolution or as the Aharonov-Anandan (AA) phase for nonadiabatic evolution. We evaluate these geometric phases using Floquet theory for systems in time-dependent external fields with a focus on paths leading through a degeneracy of the eigenenergies. Contrary to expectations, the low-frequency limits of the two phases do not always coincide. This happens as the degeneracy leads to a slow convergence of the quantum states to adiabaticity, resulting in a nonzero finite or divergent contribution to the AA phase. Steering the system adiabatically through a degeneracy provides control over the geometric phase as it can cause a π shift of the Berry phase. On the other hand, we revisit an example of degeneracy crossing proposed by AA. We find that, at suitable driving frequencies, both geometric-phase definitions give the same result and the dynamical phase is zero due to the symmetry of time evolution about the point of degeneracy, providing an advantageous setup for manipulation of quantum states.

We experimentally explore the fingerprint of the microscopic electron dynamics in second-order harmonic generation (SHG). It is shown that the interbond electron hopping induces a novel source of nonlinear polarization and plays an important role even when the driving laser intensity is 2 orders of magnitude lower than the characteristic atomic field. Our model predicts anomalous anisotropic structures of the SHG yield contributed by the interbond electron hopping, which is identified in our experiments with ZnO crystals. Moreover, a generalized second-order susceptibility with an explicit form is proposed, which provides a unified description in both the weak and strong field regimes. Our work reveals the nonlinear responses of materials at the electron scale and extends the nonlinear optics to a previously unexplored regime, where the nonlinearity related to the interbond electron hopping becomes dominant. It paves the way for realizing controllable nonlinearity on an ultrafast time scale.

Laser-induced tunneling ionization is one of the fundamental light-matter interaction processes. An accurate description of the tunnel-ionized electron wave packet is central to understanding and controlling subsequent electron dynamics. Because of the anisotropic molecular structure, tunneling ionization of molecules involves considerable challenges in accurately describing the tunneling electron wave packet. Up to now, some basic properties of the tunneling electron from molecules still remain unexplored. Here, we demonstrate that the tunneling electron from a molecule is not always emitted from the geometric center of the molecule along the tunnel direction. Rather, the photoemission position depends on the molecular orientation. Using a photoelectron holographic technique, we determine the photoemission position for a nitrogen molecule relative to the molecular geometric center to be 95±21  pm when the molecular axis is oriented along the tunnel direction. Our Letter poses, and answers experimentally, a fundamental question as to where the molecular photoionization actually begins, which has significant implications for time-resolved probing of valence electron dynamics in molecules.

High harmonic generation (HHG) is usually described by the laser-induced recollision of particlelike electrons, which lies at the heart of attosecond physics and also inspires numerous attosecond spectroscopic methods. Here, we demonstrate that the wavelike behavior of electrons plays an important role in solid HHG. By taking an analogy to the Huygens-Fresnel principle, an electron wave perspective on solid HHG is proposed by using the wavelet stationary-phase method. From this perspective, we have explained the deviation between the cutoff law predicted by the particlelike recollision model and the numerical simulation of semiconductor Bloch equations. Moreover, the emission times of HHG can be well predicted with our method involving the wave property of electrons. However, in contrast, the prediction with the particlelike recollision model shows obvious deviations compared to the semiconductor Bloch equations simulation. The wavelike properties of the electron motion can also be revealed by the HHG in a two-color field.

Previously, the strong field processes in solids have always been explained by the single-active-electron (SAE) model with a frozen core excluding the fluctuation of background electrons. In this work, we demonstrate the strong field induced dynamic core polarization effect and propose a model for revealing its role in high harmonic generation (HHG) from solids. We show that the polarized core induces an additional polarization current beyond the SAE model based on the frozen cores. It gives a new mechanism for HHG and leads to new anisotropic structures, which are experimentally observed with MgO. Our experiments indicate that the influences of dynamic core polarization on HHG are obvious for both linearly and elliptically polarized laser fields. Our work establishes the bridge between the HHG and the dynamic changes of the effective many-electron interaction in solids, which paves the way to probe the ultrafast electron dynamics.

While recent experiments provided compelling evidence for an intricate dependence of attosecond photoemission-time delays on the solid's electronic band structure, the extent to which electronic transport and dispersion in solids can be imaged in time-resolved photoelectron (PE) spectra remains poorly understood. Emphasizing the distinction between photoemission time delays measured with two-photon, two-color interferometric spectroscopy, and transport times, we demonstrate how the effect of energy dispersion in the solid on photoemission delays can, in principle, be observed in interferometric photoemission. We reveal analytically a scaling relation between the PE transport time in the solid and the observable photoemission delay and confirm this relation in numerical simulations for a model system. We trace photoemission delays to the phase difference the PE accumulates inside the solid and, in particular, predict negative photoemission delays. Based on these findings, we suggest a novel time-domain interferometric solid-state energy-momentum-dispersion imaging method.

Exceptional points (EPs) are branch point singularities of self-intersecting Riemann sheets, and they can be observed in a non-Hermitian system with complex eigenvalues. It has been revealed recently that dynamically encircling EPs by adiabatically changing the parameters of a system composed of lossy optical waveguides could lead to asymmetric (input-output) mode transfer. However, the length of the waveguides had to be considerable to ensure adiabatic evolution. Here we demonstrate that the parameters can change adiabatically along a smaller encircling loop by utilizing moving EPs, leading to significant shortening of the structures compared to fixed EPs. Meanwhile, the mode transmittance is remarkably improved and the transfer efficiency persists at ∼90%. Moving EPs are very promising for applications such as highly integrated broadband optical switches and convertors operating at telecommunication wavelengths.

We propose an all-optical method to directly reconstruct the band structure of semiconductors. Our scheme is based on the temporal Young's interferometer realized by high harmonic generation with a few-cycle laser pulse. As a time-energy domain interferometer, temporal interference encodes the band structure into the fringe in the energy domain. The relation between the band structure and the emitted harmonic frequencies is established. This enables us to retrieve the band structure from the spectrum of high harmonic generation with a single-shot measurement. Our scheme paves the way to study matters under ambient conditions and to track the ultrafast modification of band structures.

We revisit the mechanism of high-harmonic generation (HHG) from solids by comparing HHG in laser fields with different ellipticities but a constant maximum amplitude. It is shown that the cutoff of HHG is strongly extended in a circularly polarized field. Moreover, the harmonic yield with large ellipticity is comparable to or even higher than that in the linearly polarized field. To understand the underlying physics, we develop a reciprocal-space-trajectory method, which explains HHG in solids by a trajectory ensemble from different ionization times and different initial states in the reciprocal space. We show that the cutoff extension is related to an additional preacceleration step prior to ionization, which has been overlooked in solids. By analyzing the trajectories and the time-frequency spectrogram, we show that the HHG in solids cannot be interpreted in terms of the classical recollision picture alone. Instead, the radiation should be described by the electron-hole interband polarization, which leads to the unusual ellipticity dependence. We propose a new four-step model to understand the mechanism of HHG in solids.

Laser-induced electron tunneling underlies numerous emerging spectroscopic techniques to probe attosecond electron dynamics in atoms and molecules. The improvement of those techniques requires an accurate knowledge of the exit momentum for the tunneling wave packet. Here we demonstrate a photoelectron interferometric scheme to probe the electron momentum longitudinal to the tunnel direction at the tunnel exit by measuring the photoelectron holographic pattern in an orthogonally polarized two-color laser pulse. In this scheme, we use a perturbative 400-nm laser field to modulate the photoelectron holographic fringes generated by a strong 800-nm pulse. The fringe shift offers direct experimental access to the intermediate canonical momentum of the rescattering electron, allowing us to reconstruct the momentum offset at the tunnel exit with high accuracy. Our result unambiguously proves the existence of nonzero initial longitudinal momentum at the tunnel exit and provides fundamental insights into the nonquasistatic nature of the strong-field tunneling.

The nonadiabaticity of quantum tunneling through an evolving barrier is relevant to resolving laser-driven dynamics of atoms and molecules at an attosecond timescale. Here, we propose and demonstrate a novel scheme to detect the nonadiabatic behavior of tunnel ionization studied in an attoclock configuration, without counting on the laser intensity calibration or the modeling of the Coulomb effect. In our scheme, the degree of nonadiabaticity for tunneling scenarios in elliptically polarized laser fields can be steered continuously simply with the pulse ellipticity, while the critical instantaneous vector potentials remain identical. We observe the characteristic feature of the measured photoelectron momentum distributions, which matches the distinctive prediction of nonadiabatic theories. In particular, our experiments demonstrate that the nonadiabatic initial transverse momentum at the tunnel exit is approximately proportional to the instantaneous effective Keldysh parameters in the tunneling regime, as predicted theoretically by Ohmi, Tolstikhin, and Morishita [Phys. Rev. A 92, 043402 (2015)PLRAAN1050-294710.1103/PhysRevA.92.043402]. Our study clarifies a long-standing controversy over the validation of the adiabatic approximation and will substantially advance studies of laser-induced ultrafast dynamics in experiments.

Laser-induced electron tunneling ionization from atoms and molecules plays as the trigger for a broad class of interesting strong-field phenomena in attosecond community. Understanding the time of electron tunneling ionization is vital to achieving the ultimate accuracy in attosecond metrology. We propose a novel attosecond photoelectron interferometer, which is based on the interference of the direct and near-forward rescattering electron wave packets, to determine the time information characterizing the tunneling process. Adding a weak perturbation in orthogonal to the strong fundamental field, the phases of the direct and the near-forward rescattering electron wave packets are modified, leading to the shift of the interferogram in the photoelectron momentum distributions. By analyzing the response of the interferogram to the perturbation, the real part of the ionization time, which denotes the instant when the electron exits the potential barrier, and the associated rescattering time are precisely retrieved. Moreover, the imaginary part of the ionization time, which has been interpreted as a quantity related to electron motion under the potential barrier, is also unambiguously determined.

We demonstrate an angular high-harmonic spectroscopy method to probe the spinning dynamics of a molecular rotation wave packet in real time. With the excitation of two time-delayed, polarization-skewed pump pulses, the molecular ensemble is impulsively kicked to rotate unidirectionally, which is subsequently irradiated by another delayed probe pulse for high-order harmonic generation (HHG). The spatiotemporal evolution of the molecular rotation wave packet is visualized from the time-dependent angular distributions of the HHG yields and frequency shift measured at various polarization directions and time delays of the probe pulse. The observed frequency shift in HHG is demonstrated to arise from the nonadiabatic effect induced by molecular spinning. Different from the previous spectroscopic and Coulomb explosion imaging techniques, the angular high-harmonic spectroscopy method can reveal additionally the electronic structure and multiple orbitals of the sampled molecule. All the experimental findings are well reproduced by numerical simulations. Further extension of this method would provide a powerful tool for probing complex polyatomic molecules with HHG spectroscopy.

A photon channel perspective on high harmonic generation (HHG) is proposed by quantizing both the driving laser and high harmonics. It is shown that the HHG yield can be expressed as a sum of the contribution of all the photon channels. From this perspective, the contribution of a specific photon channel follows a simple scaling law and the competition between the channels is well interpreted. Our prediction is shown to be in good agreement with the simulations by solving the time-dependent Schrödinger equation. It also can explain well the experimental results of the HHG in the noncollinear two-color field and bicicular laser field.

By using optical phase modulators in a fiber-optical circuit, we theoretically and experimentally demonstrate large control over the spectrum of an impinging signal, which may evolve analogously to discrete diffraction in spatial waveguide arrays. The modulation phase acts as a photonic gauge potential in the frequency dimension, realizing efficient control of the central frequency and bandwidth of frequency combs. We experimentally achieve a 50 GHz frequency shift and threefold bandwidth expansion of an impinging comb, as well as the frequency analogue of various refraction phenomena, including negative refraction and perfect focusing in the frequency domain, both for discrete and continuous incident spectra. Our study paves a promising way towards versatile frequency management for optical communications and signal processing using time modulation schemes.

Watching the valence electron move in molecules on its intrinsic timescale has been one of the central goals of attosecond science and it requires measurements with subatomic spatial and attosecond temporal resolutions. The time-resolved photoelectron holography in strong-field tunneling ionization holds the promise to access this realm. However, it remains to be a challenging task hitherto. Here we reveal how the information of valence electron motion is encoded in the hologram of the photoelectron momentum distribution (PEMD) and develop a novel approach of retrieval. As a demonstration, applying it to the PEMDs obtained by solving the time-dependent Schrödinger equation for the prototypical molecule H_{2}^{+}, the attosecond charge migration is directly visualized with picometer spatial and attosecond temporal resolutions. Our method represents a general approach for monitoring attosecond charge migration in more complex polyatomic and biological molecules, which is one of the central tasks in the newly emerging attosecond chemistry.

We report attosecond-scale probing of the laser-induced dynamics in molecules. We apply the method of high-harmonic spectroscopy, where laser-driven recolliding electrons on various trajectories record the motion of their parent ion. Based on the transient phase-matching mechanism of high-order harmonic generation, short and long trajectories contributing to the same harmonic order are distinguishable in both the spatial and frequency domains, giving rise to a one-to-one map between time and photon energy for each trajectory. The short and long trajectories in H_{2} and D_{2} are used simultaneously to retrieve the nuclear dynamics on the attosecond and ångström scale. Compared to using only short trajectories, this extends the temporal range of the measurement to one optical cycle. The experiment is also applied to methane and ammonia molecules.

Double ionization of neon with orthogonally polarized two-color (OTC) laser fields is investigated using coincidence momentum imaging. We show that the two-electron emission dynamics in nonsequential double ionization can be controlled by tuning the subcycle shape of the electric field of the OTC pulses. We demonstrate experimentally switching from correlated to anticorrelated two-electron emission, and control over the directionality of the two-electron emission. Simulations based on a semiclassical trajectory model qualitatively explain the experimental results by a subcycle dependence of the electron recollision time on the OTC field shape.

With a classical ensemble model that includes electron correlations during the whole ionization process, we investigate strong-field sequential double ionization of Ar by elliptically polarized pulses at the quantitative level. The experimentally observed intensity-dependent three-band or four-band structures in the ion momentum distributions are well reproduced with this classical model. More importantly, the experimentally measured ionization time of the second electrons by A. N. Pfeiffer et al. [Nature Phys. 7, 428 (2011)], which cannot be predicted by the standard independent-electron model, is quantitatively reproduced by this fully classical correlated model. The success of our work encourages classical descriptions and interpretations of the complex multielectron effects in strong-field ionization where nonperturbative quantum approaches are currently not feasible.

The phase fluctuations of arbitrarily nonlinearity- and dispersion-managed solitons propagating in a noisy fiber channel are studied both analytically and numerically. We begin by discussing the stability problem of such linearly chirped solitons with a full linear stability analysis. It is shown that these sophisticated solitons possess an enhanced stability against perturbations and therefore hold promise for applications in optical telecommunications. We then make an approach to the phase statistics of these solitons, which stems from an inevitable random walk in phase evolutions due to amplified spontaneous emission noise. By using the variational approach together with impulse-response (Green) functions, an elegant closed-form expression for the phase variance is derived based on an unconstrained self-similar soliton ansatz in which the effect of chirp fluctuations has been critically taken into account as well as the dispersive and nonlinear effects. An inspection of the intriguing subtleties of the interplay among these effects reveals that the chirp fluctuations effect does play an important role in the control of nonlinear phase noise via fiber dispersion, independently of whether the input solitons are initially chirped or not. Our analytical result also offers many possibilities of optimally manipulating nonlinear phase noise with engineered fiber parameters that may lead to the steady pulse propagation, broadening, or compression under favorable parametric conditions. Last, we demonstrate our result by several convincible examples and show an excellent agreement between analytical predictions and numerical simulations.

Nonlinear Thomson backscattering of an intense circularly polarized laser by a counterpropagating energetic electron is investigated. The results show that in the scattering of a non-tightly-focused laser pulse with an intensity around 10(19) W/cm2 and a pulse duration of full width at half maximum by a counterpropagating electron with an initial energy of 10 MeV, a crescent-shaped pulse with a pulse duration of 469 s and the photon energy ranging from 230 eV to 2.5 keV is generated in the backward direction. It is shown that the radiated pulse shape and monochromaticity can be modified by changing the laser beam waist, while in the case of a tightly focused laser field, a single peak pulse with a shorter duration and better monochromaticity can be obtained. With increase of the electron initial energy, the peak power of the radiated pulse increases and the pulse duration decreases. An isolated powerful zeptosecond pulse with a peak power of about and photon energy up to several MeV can be obtained with a electron.

Three novel types of self-similar solutions, termed parabolic, Hermite-Gaussian, and hybrid pulses, of the generalized nonlinear Schrödinger equation with varying dispersion, nonlinearity, and gain or absorption are obtained. The properties of the self-similar evolutions in various nonlinear media are confirmed by numerical simulations. Despite the diversity of their formations, these self-similar pulses exhibit many universal features which can facilitate significantly the achievement of well-defined linearly chirped output pulses from an optical fiber, an amplifier, or an absorption medium, under certain parametric conditions. The other intrinsic characteristics of each type of self-similar pulses are also discussed.

Ponderomotive force driven acceleration of an electron at the focus of a high-intensity short-pulse laser is considered. Accounting for the asymmetry of acceleration and deceleration due to the evolution of the Gaussian laser beam waist, the energized electron is extracted from the laser pulse by the longitudinal ponderomotive force. It is shown that an electron's energy gain in the range of MeV can be realized for laser intensities above 10(19) W microm(2)/cm(2). Final energy gain as a function of the scattering angle and the electron's initial position has also been discussed.