We perform ab initio calculations for the hydrogen atom initially in one of the six circular bound states with the principal quantum numbers n = 2, 3 and 4, irradiated by a short circularly polarized laser pulse of 400 nm. The field propagates in the direction parallel to the z-component of the angular momentum of the atom. We investigate probabilities for the atom to ionize or to get on some bound (excited) state or to remain in the initial state after the end of the laser pulse. In most cases, we find pronounced differences in ionization probabilities for atoms in states having different signs of magnetic quantum number. Usually electrons corotating (with respect to the laser field) ionize faster than their counter-rotating equivalents. We have found important difference in the behavior of the excitation (as a function of the peak laser intensity) for initial states with n = 2 and other n (3 or 4). For higher n the excitation is always weaker than the ionization and starts for higher intensities. For n = 2 the strong excitation appears before strong ionization due to large probability of one-photon absorption combined with population of many bound states having principal quantum numbers n from 3 up to several dozen. Quite accurate analysis of the excitation process is presented.
We theoretically study frustrated double ionization (FDI) of atoms subjected to intense circularly polarized laser pulses using a three-dimensional classical model. We find a novel "knee" structure of FDI probability as a function of intensity, which is similar to the intensity dependence of nonsequential double ionization probability. The observation of FDI is more favourable when using targets with low ionization potentials and short driving laser wavelengths. This is attributed to the crucial role of recollision therein, which can be experimentally inferred from the photoelectron momentum d…
Two-, three-, and four-photon ionization of Mg in the circularly and linearly polarized laser fields: Comparative study using the Hartree-Fock and model potentials
The full three-dimensional photoelectron momentum distributions of argon are measured in intense near-circularly polarized laser fields. We observed that the transverse momentum distribution of ejected electrons by 410-nm near-circularly polarized field is unexpectedly narrowed with increasing laser intensity, which is contrary to the conventional rules predicted by adiabatic theory. By analyzing the momentum-resolved angular momentum distribution measured experimentally and the corresponding trajectories of ejected electrons semiclassically, the narrowing can be attributed to a temporary trap…
Hole dynamics and spin currents after ionization in strong circularly polarized laser fields
本文应用含时解析R矩阵理论，给出了强圆极化场电离下氪原子中空穴运动的一个实验结果。我们发现丰富的洞动态，从旋转到摆动运动。空穴的运动取决于光电子的最终能量和自旋，并且可以通过激光频率和强度来控制。重要的是，空穴旋转是一种纯粹的非绝热效应，在准静态（绝热）隧穿理论的框架中完全缺失。我们探讨了利用空穴旋转作为测量电离时间的时钟的可能性。通过分析不同电离通道中相对相位的关系，我们发现在短程电子-芯相互作用的情况下，空穴总是沿着激光场的瞬时方向初始排列，这意味着电离的零延迟。最后，我们表明，强场电离在圆形领域创建自旋电流（即不同的流动的自旋和自旋密度在空间）的离子。这种现象与强激光场中自旋极化电子的产生密切相关[Barth I and Smirnova O 2013 Phys. Rev. A 88 013401]。我们证明了在强场电离过程中产生的电子和空穴的丰富的自旋动力学可以发生在典型的实验条件下，不需要相对论强度或强磁场。
We study the double ionization of atoms subjected to circularly polarized (CP) laser pulses. We analyze two fundamental ionization processes: the sequential (SDI) and non-sequential (NSDI) double ionization in the light of the rotating frame (RF) which naturally embeds nonadiabatic effects in CP pulses. We use and compare two adiabatic approximations: The adiabatic approximation in the laboratory frame (LF) and the adiabatic approximation in the RF. The adiabatic approximation in the RF encapsulates the energy variations of the electrons on subcycle timescales happening in the LF and this, by …
We discuss the mechanism by which the inclusion of multielectron polarization improves the solution of the time-dependent Schrödinger equation (TDSE) for the oriented CO molecule in a strong external laser pulse within the single-active-electron (SAE) approximation. A challenging problem of using the SAE approximation is that the active electron, instead of undergoing ionization, may be driven by the external field to lower-lying orbitals. For the oriented CO molecule, dipole coupling to the lower-lying bound states of the potential depends on the orientation angle, thereby affecting the orien…
We show that the combination of two achiral components - atomic or molecular target plus a circularly polarized photon - can yield chirally structured photoelectron angular distributions. For photoionization of CO, the angular distribution of carbon K-shell photoelectrons is chiral when the molecular axis is neither perpendicular nor (anti-)parallel to the light propagation axis. In photo-double-ionization of He, the distribution of one electron is chiral, if the other electron is oriented like the molecular axis in the former case and if the electrons are distinguishable by their energy. In b…
We report on the appearance of a structure at low energies in the photo-electron momentum distribution of the hydrogen atom exposed to two-color counter-rotating bi-circular laser fields. These structures, which arise due to AC-Stark shifted resonances, break the three-fold symmetry, typical for the $ω-2ω$ bi-circular fields. We discuss the physical origin of this structure in terms of partial-wave interference between direct ionization channels and a resonant pathway, that passes through the AC-Stark shifted state and show how the underlying Rydberg state population depend on the field streng…
We investigate electron correlation effects in internuclear-distance-dependent enhanced ionization of $\mathrm{H}_2$, $\mathrm{LiH}$, and $\mathrm{HF}$ molecules by intense near-infrared laser pulses using a 3D description of the systems with the time-dependent generalized-active-space configuration-interaction method. This method systematically incorporates electron-electron correlation of the quantum many-electron system under consideration. Our correlated description of diatomic molecules shows that enhanced ionization occurs at certain critical internuclear separations and electron correla…
Nonadiabatic tunneling in circularly polarized laser fields. III. Comparison with experiment
我们比较了Herath等人[T.赫拉特湖Yan，S. K.李和W。Li，Phys. Rev. Lett. 109，043004（2012）]在圆偏振激光场中的强场非绝热隧穿与我们的理论的原始预测[I. Barth和O. Smirnova，Phys. Rev A 84，063415（2011）]刺激这些实验。我们表明，理论和实验是在非常好的协议。我们还解释了为什么Herath等人[T.赫拉特湖Yan，S. K.李和W。Li，Phys. Rev. Lett. 109，043004（2012）]提出了与我们的理论的定量差异。我们确认，这些看似不一致的删除与我们的理论模型的准确应用。我们提出了一个实验，独特的确定电离价轨道p+或p-的偏好。
Chiral molecules ionized by circularly polarized fields produce a photoelectron current orthogonal to the polarization plane. This current has opposite directions for opposite enantiomers and provides an extremely sensitive probe of molecular handedness. Recently, such photoelectron currents have been measured in the strong-field ionization regime, where they may serve as an ultrafast probe of molecular chirality. Here we provide a mechanism for the emergence of such strong-field photoelectron currents in terms of two propensity rules that link the properties of the initial electronic chiral s…
The total ionization rate of biharmonic ($ω+ 3ω$) ionization is studied within the independent particle approximation and the third order perturbation theory. Particular attention is paid to how the polarization of the biharmonic light field affects the total rate. The ratios of the biharmonic ionization rates for linearly and circularly polarized beams as well as for corotating and counterrotating elliptically polarized beams are analyzed, and how they depend on the beam parameters, such as photon frequency or phase between $ω$ and $3ω$ light beams. We show that the interference of the biharm…
Recent experiments [D. Pengel, S. Kerbstadt, L. Englert, T. Bayer, and M. Wollenhaupt, \href{https://journals.aps.org/pra/abstract/10.1103/PhysRevA.96.043426}{{\PRA} {\bf 96} 043426 (2017)}] have measured the photoelectron momentum distribution for three-photon ionization of potassium by counter-rotating circularly polarized 790-nm laser pulses. The distribution displays spiral vortices, arising from the interference of ionizing wavepackets with different magnetic quantum numbers. The high level of multidimensional detail observed in the distribution makes this an ideal case in which to demons…
We report on three-dimensional (3D) electron momentum distributions from single ionization of helium by a laser pulse consisting of two counterrotating circularly polarized fields (390 nm and 780 nm). A pronounced 3D low energy structure and sub-cycle interferences are observed experimentally and reproduced numerically using a trajectory based semi-classical simulation. The orientation of the low energy structure in the polarization plane is verified by numerical simulations solving the time dependent Schrödinger equation.
Phase-of-the-phase spectroscopy using two-color colinearly polarized laser pulses has been introduced and experimentally applied to strong-field tunneling ionization in S. Skruszewicz et al., Phys. Rev. Lett. 115, 043001 (2015) and recently to multiphoton ionization in M. A. Almajid et al., J. Phys. B: At. Mol. Opt. Phys. 50, 194001 (2017). The idea behind phase-of-the-phase spectroscopy is to study in a systematic way the change in the photoelectron yield as a function of the relative phase between the strong fundamental field component (of carrier frequency $ω$) and a weak, second color comp…
The spin polarization of electrons from multiphoton ionization of Xe by 395 nm circularly polarized laser pulses at $6\cdot10^{13}$ W/cm$^2$ has been measured. At this photon energy of 3.14 eV the above threshold ionization peaks connected to Xe$^+$ ions in the ground state ($J=3/2$, ionization potential $I_p=12.1$ eV) and the first exicted state ($J=1/2$, $I_p=13.4$ eV) are clearly separated in the electron energy distribution. These two combs of ATI peaks show opposite spin polarizations. The magnitude of the spin polarization is a factor of two higher for the $J=1/2$ than for the $J=3/2$ fi…
A way to considerably enhance terahertz radiation, emitted in the interaction of intense mid-infrared laser pulses with atomic gases, in both the total energy and the electric-field amplitude is suggested. The scheme is based on the application of a two-color field consisting of a strong circularly polarized mid-infrared pulse with wavelengths of $1.6÷4\,μ{\rm m}$ and its linearly or circularly polarized second harmonic of lower intensity. By combining the strong-field approximation for the ionization of a single atom with particle-in-cell simulations of the collective dynamics of the generate…
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 investigate the resonance-enhanced few-photon ionization of atomic lithium by linearly polarized light whose frequency is tuned near the 2s-2p transition. Considering the direction of light polarization orthogonal to the quantization axis, the process can be viewed as an atomic "double-slit experiment" where the 2p states with magnetic quantum numbers m_l=+-1 act as the slits. In our experiment, we can virtually close one of the two slits by preparing lithium in one of the two circularly polarized 2p states before subjecting it to the ionizing radiation. This allows us to extract the interf…
Strong-field ionization of atoms by circularly polarized femtosecond laser pulses produces a donut-shaped electron momentum distribution. Within the dipole approximation this distribution is symmetric with respect to the polarization plane. The magnetic component of the light field is known to shift this distribution forward. Here, we show that this magnetic non-dipole effect is not the only non-dipole effect in strong-field ionization. We find that an electric non-dipole effect arises that is due to the position dependence of the electric field and which can be understood in analogy to the Do…
Chirality causes symmetry breaks in a large variety of natural phenomena ranging from particle physics to biochemistry. We investigate one of the simplest conceivable chiral systems, a laser-excited, oriented, effective one-electron Li target. Prepared in a polarized p state with |m|=1 in an optical trap, the atoms are exposed to co- and counter-rotating circularly polarized femtosecond laser pulses. For a field frequency near the excitation energy of the oriented initial state, a strong circular dichroism is observed and the photoelectron energies are significantly affected by the helicity-de…
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）
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…
