我们展示了氩二聚体在共旋转双色（CoRTC）激光场中强场电离的实验数据。我们在光电子动量分布中观察到亚周期干涉图样，并利用电子的全息角条纹法（HASE）推断出 Wigner 时间延迟。我们发现，Wigner 时间延迟随电子发射方向相对于分子轴的变化而改变超过 400 阿秒。测得的时间延迟被发现与二聚体阳离子的宇称无关，并且与我们基于对齐的原子 p 轨道电离的理论模型吻合良好。
英文摘要：
We present experimental data on the strong-field ionization of the argon dimer in a co-rotating two-color (CoRTC) laser field. We observe a sub-cycle interference pattern in the photoelectron momentum distribution and infer the Wigner time delay using holographic angular streaking of electrons (HASE). We find that the Wigner time delay varies by more than 400 attoseconds as a function of the electron emission direction with respect to the molecular axis. The measured time delay is found to be independent of the parity of the dimer-cation and is in good agreement with our theoretical model based on the ionization of an aligned atomic p-orbital.
More than 100 years after its discovery and its explanation in the energy domain, the duration of the photoelectric effect is still heavily studied. The emission time of a photoelectron can be quantified by the Wigner time delay. Experiments addressing this time delay for single-photon ionization became feasible during the last 10 years. A missing piece, which has not been studied, so far, is the Wigner time delay for strong-field ionization of molecules. Here we show experimental data on the Wigner time delay for tunnel ionization of $H_{2}$ molecules and demonstrate its dependence on the emi…
The Salecker-Wigner-Peres quantum-clock approach is applied in order to determine the tunneling time of an electron in strong-field tunnel ionization via a time-dependent electric field. Our results show that the ionization of the electron takes a nonvanishing period of time. This tunneling time is of the order of the Keldysh time but strictly larger than the Keldysh time. Comparing the quantum-clock tunneling time to the mean tunneling time as obtained by the virtual-detector approach, one finds that these two complementary methods give very similar results. Due to the asymmetric distribution…
We study single-photon ionization of aligned H$_2^+$ in a high-frequency low-intensity laser field. We focus on the case where the laser frequency is not far larger than the ionization potential of the target. The calculated photoelectron momentum distribution through numerical solution of time-dependent Schrödinger equation shows clear interference patterns. By developing a theory model applicable for high-frequency laser field, we show that the interference patterns can not be explained by the interference of the electronic wave with the observed momentum between these two atomic centers of …
A new pathway of strong laser field induced ionization of an atom is identified which is based on recollisions under the tunneling barrier. With an amended strong field approximation, the interference of the direct and the under-the-barrier recolliding quantum orbits are shown to induce a measurable shift of the peak of the photoelectron momentum distribution. The scaling of the momentum shift is derived relating the momentum shift to the tunneling delay time according to the Wigner concept. This allows to extend the Wigner concept for the quasistatic tunneling time delay into the nonadiabatic…
We revisit strong-field ionization of aligned O$_2$, CO$_2$, and CS$_2$ molecules in light of recent advances in the field of strong-field physics, in particular the inclusion of multielectron polarization in the numerical solution of the time-dependent Schr{ö}dinger equation (TDSE) within the singe-active-electron approximation. Upon inclusion of multielectron polarization and the associated induced dipole potential in the TDSE model, we obtain angular distributions of total ionization yields which are in better agreement with the available experimental results for CO$_2$ and CS$_2$. For the …
We present measurements of single-photon ionization time delays between valence electrons of argon and neon using a coincidence detection technique that allows for the simultaneous measurement of both species under identical conditions. Taking into account the chirp of the ionizing single attosecond pulse (attochirp) ensures that the clock of our measurement technique is started at the same time for both types of electrons, revealing with high accuracy and resolution energy-dependent time delays of a few tens of attoseconds. By comparing our results with theoretical predictions, we confirm tha…
We propose a method to study the tunneling process by analyzing the time-dependent ionization yield in circularly polarized laser. A numerical calculation shows that for an atom exposed to a long laser pulse, if its initial electronic state wave function is non-spherical symmetric, the delayed phase shift of the ionization rate vs. the laser cycle period in real time in the region close to the peak intensity of the laser pulse can be used to probe the tunneling time. In this region, an obvious delay phase shift is observed, showing the tunneling time is in order of tens of attoseconds. Further…
We show that time ordering underlying time-dependent quantum dynamics is a physical observable accessible by attosecond streaking. We demonstrate the extraction of time ordering for the prototypical case of time-resolved two-photon double ionization (TPDI) of helium by an attosecond XUV pulse. The Eisenbud-Wigner-Smith time delay for the emission of a two-electron wavepacket and the time interval between subsequent emission events can be unambiguously determined by attosecond streaking. The delay between the two emission events sensitively depends on the energy, pulse duration, and angular dis…
For a circularly polarized single-color field at a central frequency of $2ω$ the final electron momentum distribution upon strong field ionization does not carry any information about the phase of the initial momentum distribution. Adding a weak, co-rotating, circularly polarized field at a central frequency of $ω$ gives rise to a sub-cycle interference pattern (holographic angular streaking of electrons (HASE)). This interference pattern allows for the retrieval of the derivative of the phase of the initial momentum distribution after tunneling $ϕ^{\prime}_{\mathrm{off}}(p_i)$. A trajectory-b…
We describe numerically the ionization process induced by linearly and circularly polarized XUV attosecond laser pulses on an aligned atomic target, specifically, the excited state Ne$^*(1s^22s^22p^5[{}^2\text{P}^\text{o}_{1/2}]3s[^1\text{P}^o])$. We compute the excited atomic state by applying the time-dependent restricted-active-space self-consistent field (TD-RASSCF) method to fully account for the electronic correlation. We find that correlation-assisted ionization channels can dominate over channels accessible without correlation. We also observe that the rotation of the photoelectron mom…
We analyze tunnel ionization of a single atom based on the Wigner function over the classical phase space which inspires improved classical electron trajectories: these start with exit momenta based on the quantum momentum function and correspond very well to the subsequent quantum evolution. We derive an approximate analytic formula to reconstruct the tunnel exit time and exit momentum from electron momentum data that can be measured e.g. with a usual time-of-flight electron detector.
We investigate dissociative single and double ionization of HeH+ induced by intense femtosecond laser pulses. By employing a semi-classical model with nuclear trajectories moving on field-dressed surfaces and ionization events treated as stochastical jumps, we identify a strong-field mechanism wherein the molecules dynamically align along the laser polarization axis and stretch towards a critical internuclear distance before getting dissociative ionized. As the tunnel-ionization rate is greater for larger internuclear distance and for aligned samples, ionization is enhanced. The strong dynamic…
Phase retrieval from angular streaking of XUV atomic ionization
Research School of Physics, The Australian National University（澳大利亚国立大学物理研究生院）；General, Theoretical and Computer Physics, Saratov State University（萨马拉国立大学一般、理论与计算物理）；Center for Relativistic Laser Science, Institute for Basic Science (IBS)（基础科学研究院相对论激光科学中心）；Stanford PULSE Institute, SLAC National Accelerator Laboratory（斯坦福PULSE研究所，SLAC国家加速器实验室）
We numerically study models of $\mathrm{H}_2$ and $\mathrm{LiH}$ molecules, aligned collinearly with the linear polarization of the external field, to elucidate the possible role of correlation in the enhanced-ionization phenomena. Correlation is considered at different levels of approximation with the time-dependent generalized-active-space configuration-interaction method. The results of our studies show that enhanced ionization occurs in multielectron molecules, that correlation is important and they also demonstrate significant deviations between the results of the single-active-electron a…
The alignment- and internuclear-distance dependent ionization of H$_2$ exposed to intense, ultrashort laser fields is studied by solving the time-dependent two-electron Schrödinger equation. In the regime of perturbative few-photon ionization, a strong dependence of the ionization yield on the internuclear distance is found. While this finding confirms a previously reported breakdown of the fixed-nuclei approximation for parallel alignment, a simpler explanation is provided and it is demonstrated that this breakdown is not due to vibrational dynamics during the laser pulse. The persistence of …
We study ionization of aligned H$_2^+$ in strong elliptically-polarized laser fields numerically and analytically. The calculated offset angle in photoelectron momentum distribution is several degrees larger for the molecule than a model atom with similar ionization potential at diverse laser parameters. Using a strong-field model that considers the properties of multi-center and single-center Coulomb potentials, we are able to quantitatively reproduce this angle difference between the molecule and the atom. Further analyses based on this model show that the response time of electron to light …
In the semiclassical picture of photoionization process in intense laser fields, the ionization rate solely depends on the amplitude of the electric field and the final photoelectron momentum corresponds to the instant of ionization of the photoelectron, however, this picture has never been checked rigorously. Recently an attosecond angular streaking technique based on this semiclassical perspective has been widely applied to temporal measurement of the atomic and molecular dynamics in intense laser fields. We use a Wigner-distribution-like function to calculate the time-emission angle distrib…
The use of semiclassical models based on the Strong Field Approximation (SFA) is ubiquitous in strong field multi-photon ionization and underlies many key developments in attosecond science, including the description of High Harmonic Generation (HHG). However, such models are notably lacking in streaking experiments, which use an attosecond pulse to initiate single-photon ionization and a lower frequency infrared pulse to provide timing information. Here, we introduce a classical Wigner propagation (CWP) method, which analogously to semiclassical models in strong field ionization, treats the i…
We use a Wigner distribution-like function based on the strong field approximation theory to obtain the time-energy distributions and the ionization time distributions of electrons ionized by an XUV pulse alone and in the presence of an infrared (IR) pulse. In the case of a single XUV pulse, although the overall shape of the ionization time distribution resembles the XUV-envelope, its detail shows dependence on the emission direction of the electron and the carrier-envelope phase of the pulse, which mainly results from the low-energy interference structure. It is further found that the electro…
On the measurability of Wigner time delays at shape resonances in photodetachment of polyatomic anions
University of Central Florida（中佛罗里达大学）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；University of California, Davis（加州大学戴维斯分校）；Charles University（查理大学）；Cal Poly Maritime Academy（加州海事学院）；California Polytechnic State University（加州州立理工大学）
We apply the time-dependent analytical R-matrix theory to develop a movie of hole motion in a Kr atom upon ionization by strong circularly polarized field. We find rich hole dynamics, ranging from rotation to swinging motion. The motion of the hole depends on the final energy and the spin of the photoelectron and can be controlled by the laser frequency and intensity. Crucially, hole rotation is a purely non-adiabatic effect, completely missing in the framework of quasistatic (adiabatic) tunneling theories. We explore the possibility to use hole rotation as a clock for measuring ionization tim…
Time-delays in the photoionization of molecules are investigated. As compared to atomic ionization, the time-delays expected from molecular ionization present a much richer phenomenon, with a strong spatial dependence due to the anisotropic nature of the molecular scattering potential. We investigate this from a scattering theory perspective, and make use of molecular photoionization calculations to examine this effect in representative homonuclear and hetronuclear diatomic molecules, nitrogen and carbon monoxide. We present energy and angle-resolved maps of the Wigner delay time for single-ph…
The realization of electron vortex beams in the past decade has led to numerous proposed applications in fields from electron microscopy to control and manipulation of individual molecules. Yet despite the many unique characteristics and promising advantages of electron vortex beams, such as transverse momentum and quantized orbital angular momentum, there remains a limited understanding of their fundamental interactions with matter at the atomic scale. Collisions between electron vortex projectiles and atomic targets can provide some insight into these interactions and we present here fully d…
Several recent attoclock experiments have investigated the fundamental question of a quantum mechanically induced time delay in tunneling ionization via extremely precise photoelectron momentum spectroscopy. The interpretations of those attoclock experimental results were controversially discussed, because the entanglement of the laser and Coulomb field did not allow for theoretical treatments without undisputed approximations. The method of semiclassical propagation matched with the tunneled wavefunction, the quasistatic Wigner theory, the analytical R-matrix theory, the backpropagation metho…
We study the generation of terahertz radiation from atoms and molecules driven by an ultrashort fundamental laser and its second harmonic field by solving time-dependent Schrödinger equation (TDSE). The comparisons between one-, two-, and three- dimensional TDSE numerical simulations show that initial ionized wave-packet and its subsequent acceleration in the laser field and rescattering with long-range Coulomb potential play key roles. We also present the dependence of the optimum phase delay and yield of terahertz radiation on the laser intensity, wavelength, duration, and the ratio of two-c…
Tunneling of a particle through a potential barrier remains one of the most remarkable quantum phenomena. Owing to advances in laser technology, electric fields comparable to those electrons experience in atoms are readily generated and open opportunities to dynamically investigate the process of electron tunneling through the potential barrier formed by the superposition of both laser and atomic fields. Attosecond-time and angstrom-space resolution of the strong laser-field technique allow to address fundamental questions related to tunneling, which are still open and debated: Which time is s…
Characterizing time delays in molecular photoionization as a function of the ejected electron emission direction relative to the orientation of the molecule and the light polarization axis pro-vides unprecedented insights into the attosecond dynamics induced by extreme ultraviolet or X-ray one-photon absorption, including the role of electronic correlation and continuum resonant states. Here, we report completely resolved experimental and computational angular depend-ence of single-photon ionization delays in NO molecules across a shape resonance, relying on synchrotron radiation and time inde…
Photoelectron circular dichroism results from one-photon ionization of chiral molecules by circularly polarized light and manifests itself in forward-backward asymmetry of electron emission in the direction orthogonal to the light polarization plane. What is the physical mechanism underlying asymmetric electron ejection? How "which way" information builds up in a chiral molecule and maps into forward-backward asymmetry? We introduce instances of bound chiral wave functions resulting from stationary superpositions of states in a hydrogen atom and use them to show that the chiral response in one…
We study ionization dynamics of aligned diatomic molecules N$_2$ in strong elliptical laser fields experimentally and theoretically. The alignment dependence of photoelectron momentum distributions (PMDs) of N$_2$ measured in experiments is highlighted with comparing to Ar measured synchronously. Our results show that the PMDs of N$_2$ depend strongly on the alignment of the molecule, relative to the main axis of the laser ellipse. In particular, the most-probable electron-emission angle which is often used in attosecond measurement, differs remarkably when changing the molecular alignment. We…
We employ the recently developed multi-photon R-matrix method for molecular above-threshold photoionization to obtain second-order ionization amplitudes that govern the interference in RABITT experiments. This allows us to extract RABITT time delays that are in better agreement with non-perturbative time-dependent simulations of this process than the typically used combination of first-order (Wigner) delays and asymptotic corrections. We calculate molecular-frame as well as orientation-averaged RABITT delays for H$_2$, N$_2$, CO$_2$, H$_2$O and N$_2$O and analyze the origin of various structur…
