Spin polarized electrons produced by strong field ionization

We show that ionization of noble gas atoms by strong infrared circularly polarized laser field under standard exerimental conditions can yield electrons with up to 100% spin polarization in energy resolved measurements. Spin polarization arises due to the interplay of the electron-core entanglement and the sensitivity of ionization in circularly polarized fields to the sense of electron rotation in the initial state.Comment: 10 pages, 2 figure

Hole dynamics and spin currents after ionization in strong circularly polarized laser fields

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 time. Analysing the relationship between the relative phases in different ionization channels we show that in the case of short-range electron-core interaction the hole is always initially aligned along the instantaneous direction of the laser field, signifying zero delays in ionization. Finally, we show that strong-field ionization in circular fields creates spin currents (i.e. different flow of spin-up and spin-down density in space) in the ions. This phenomenon is intimately related to the production of spin-polarized electrons in strong laser fields [Barth I and Smirnova O 2013 Phys. Rev. A 88 013401]. We demonstrate that rich spin dynamics of electrons and holes produced during strong field ionization can occur in typical experimental conditions and does not require relativistic intensities or strong magnetic fields

Nonadiabatic tunneling in circularly polarized laser fields: Derivation of formulas

We provide detailed analysis of strong field ionization of degenerate valence p orbitals by circularly polarized fields. Our analytical approach is conceptually equivalent to the Perelomov, Popov, and Terent'ev (PPT) theory and is virtually exact for short range potentials. After benchmarking our results against the PPT theory for s orbitals, we obtain the results for p orbitals. We also show that, as long as the dipole approximation is valid, both the PPT method and our results are gauge invariant, in contrast with widely used strong field approximation (SFA). Our main result, which has already been briefly outlined in [I. Barth and O. Smirnova, Phys. Rev. A 84, 063415 (2011)], is that strong field ionization preferentially removes electrons counter-rotating to the circularly polarized laser field. The result is illustrated using the example of Kr atom. Strong, up to one order of magnitude, sensitivity of strong field ionization to the sense of electron rotation in the initial state is one of the key signatures of non-adiabatic regime of strong field ionization.Comment: 42 pages, 3 figure

Non-adiabatic Coulomb effects in strong field ionisation in circularly polarised laser fields

We develop the recently proposed analytical R-matrix (ARM) method to encompass strong field ionisation by circularly polarised fields, for atoms with arbitrary binding potentials. Through ARM, the effect of the potential can now be included consistently both during and after ionisation, providing a complete picture for the effects of the long-range potential. We find that the Coulomb effects modify the ionisation dynamics in several ways, including modification of (i) the ionisation (exit) times, (ii) the initial conditions for the electron continuum dynamics, (iii) the "tunnelling angle", at which the electron "enters" the barrier, and (iv) the electron drift momentum. We derive analytical expressions for the Coulomb-corrected ionisation times, initial velocities, momentum shifts and ionisation rates in circularly polarised fields, for arbitrary angular momentum of the initial state. We also analyse how the non-adiabatic Coulomb effects modify (i) the calibration of the attoclock in the angular streaking method, and (ii) the ratio of ionisation rates from $p^{-}$ and $p^{+}$ orbitals.Comment: 46 pages, 5 figures, Appendix A-

Multidimensional high harmonic spectroscopy: A semi-classical perspective on measuring multielectron rearrangement upon ionization

High harmonic spectroscopy has the potential to combine attosecond temporal with sub-Angstrom spatial resolution of the early nuclear and multielectron dynamics in molecules. It involves strong field ionization of the molecule by the IR laser field followed by time-delayed recombination of the removed electron with the molecular ion. The time-delay is controlled on the attosecond time scale by the oscillation of the IR field and is mapped into the harmonic number, providing a movie of molecular dynamics between ionization and recombination. One of the challenges in the analysis of high harmonic signal stems from the fact that the complex dynamics of both ionization and recombination with their multiple observables are entangled in the harmonic signal. Disentangling this information requires multidimensional approach, capable of mapping ionization and recombination dynamics into different independent parameters. We suggest multidimensional high harmonic spectroscopy as a tool for characterizing of ionization and recombination processes separately allowing for simultaneous detection of both the ionization delays and sub-cycle ionization rates. Our method extends the capability of the two dimensional (2D) set-up suggested recently by Shafir et al on reconstructing ionization delays, while keeping the reconstruction procedure as simple as in the original proposal. The scheme is based on the optimization of the high harmonic signal in orthogonally polarized strong fundamental and relatively weak multicolour control fields.Comment: 11 pages, 3 figure

Propensity rules in photoelectron circular dichroism in chiral molecules II: General picture

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. To expose the physical mechanism responsible for asymmetric electron ejection, we first establish a rigorous relation between the responses of unaligned and partially or perfectly aligned molecules. Next, we identify a propensity field, which is responsible for the chiral response in the electric-dipole approximation, i.e. a chiral response without magnetic interactions. We find that this propensity field, up to notations, is equivalent to the Berry curvature in a two-band solid. The propensity field directly encodes optical propensity rules, extending our conclusions regarding the role of propensity rules in defining the sign of forward-backward asymmetry from the specific case of chiral hydrogen to generic chiral systems. Optical propensity rules underlie the chiral response in photoelectron circular dichroism. The enantiosensitive flux of the propensity field through the sphere in momentum space determines the forward-backward asymmetry in unaligned molecules and suggests a geometrical origin of the chiral response. This flux has opposite sign for opposite enantiomers and vanishes for achiral molecules.Comment: Added Fig. 4, Added Table 1, shortened section

Opportunities for chiral discrimination using high harmonic generation in tailored laser fields

Chiral discrimination with high harmonic generation (cHHG method) has been introduced in the recent work by R. Cireasa et al ( Nat. Phys. 11, 654 - 658, 2015). In its original implementation, the cHHG method works by detecting high harmonic emission from randomly oriented ensemble of chiral molecules driven by elliptically polarized field, as a function of ellipticity. Here we discuss future perspectives in the development of this novel method, the ways of increasing chiral dichroism using tailored laser pulses, new detection schemes involving high harmonic phase measurements, and concentration-independent approaches. Using the example of the epoxypropane molecule C$_3$H$_6$O (also known as 1,2-propylene oxide), we show theoretically that application of two-color counter-rotating elliptically polarized laser fields yields an order of magnitude enhancement of chiral dichroism compared to single color elliptical fields. We also describe how one can introduce a new functionality to cHHG: concentration-independent measurement of the enatiomeric excess in a mixture of randomly oriented left-handed and right-handed molecules. Finally, for arbitrary configurations of laser fields, we connect the observables of the cHHG method to the amplitude and phase of chiral response, providing a basis for reconstructing wide range of chiral dynamics from cHHG measurements, with femtosecond to sub-femtosecond temporal resolution

Opportunities for detecting ring currents using the attoclock set-up

Strong field ionization by circularly polarized laser fields from initial states with internal orbital momentum has interesting propensity rule: electrons counter-rotating with respect to the laser field can be liberated more easily than co-rotating electrons [Barth and Smirnova PRA 84, 063415, 2011}]. Here we show that application of few-cycle IR pulses allows one to use this propensity rule to detect ring currents associated with such quantum states, by observing angular shifts of the ejected electrons. Such shifts present the main observable of the attoclock method. We use time-dependent Analytical $R$-Matrix (A$R$M) theory to show that the attoclock measured angular shifts of an electron originating from two counter-rotating orbitals ($p^{+}$ and $p^{-}$) are noticeably different. Our work opens new opportunities for detecting ring currents excited in atoms and molecules, using the attoclock set-up

Time-resolving electron-core dynamics during strong field ionization in circularly polarized fields

Electron-core interactions play a key role in strong-field ionization and the formation of photoelectron spectra. We analyse the temporal dynamics of strong field ionization associated with these interactions using the time-dependent analytical R-matrix (ARM) method, developed in our previous work [J. Kaushal and O. Smirnova, Phys. Rev. A 88, 013421 (2013)]. The approach is fully quantum but includes the concept of trajectories. However, the trajectories are not classical in the sense that they have both real and imaginary components all the way to the detector. We show that the imaginary parts of these trajectories, which are usually ignored, have a clear physical meaning and are crucial for the correct description of electron-core interactions after ionization. In particular, they give rise to electron deceleration, as well as dynamics associated with electron recapture and release. Our approach is analytical and time-dependent, and allows one to gain access to the electron energy distribution and ionization yield as a function of time. Thus we can also rigorously answer the question: when is ionization completed?Comment: 19 pages, 9 figure

General theory of photoexcitation induced photoelectron circular dichroism

The photoionization of chiral molecules prepared in a coherent superposition of excited states can give access to the underlying chiral coherent dynamics in a procedure known as photoexcitation induced photoelectron circular dichroism (PXECD). This exclusive dependence on coherence can also be seen in a different part of the angular spectrum, where it is not contingent on the chirality of the molecule, thus allowing extension of PXECD's sensitivity to tracking coherence to non-chiral molecules. Here we present a general theory of PXECD based on angular momentum algebra and derive explicit expressions for all pertinent asymmetry parameters which arise for arbitrary polarisation of pump and probe pulses. The theory is developed in a way that clearly and simply separates chiral and non-chiral contributions to the photoelectron angular distribution, and also demonstrates how PXECD and PECD-type contributions, which may be distinguished by whether pump or ionizing probe enables chiral response, are mixed when arbitrary polarization is used