Christian Per Juul Martiny

Photoelectron angular distributions from strong-field ionization of oriented molecules

An experimental study shows how a polar molecule can be oriented in three dimensions by using a combination of laser and electrostatic fields. The approach should help to obtain molecular-frame information about strong-field ionization processes in molecules for which the orientation cannot be determined after ionization.

Symmetry of Carrier-Envelope Phase Difference Effects in Strong-Field, Few-Cycle Ionization of Atoms and Molecules

In few-cycle pulses, the exact value of the carrier-envelope phase difference (CEPD) has a pronounced influence on the ionization dynamics of atoms and molecules. We show that, for atoms in circularly polarized light, a change in the CEPD is mapped uniquely to an overall rotation of the system, and results for arbitrary CEPD are obtained by rotation of the results from a single calculation with fixed CEPD. For molecules, this is true only for linear molecules aligned parallel with the propagation direction of the field. The effects of CEPD are classified as geometric or nongeometric. The observations are exemplified by strong-field calculations on hydrogen.

Ionization of one- and three-dimensionally-oriented asymmetric-top molecules by intense circularly polarized femtosecond laser pulses

We present a combined experimental and theoretical study on strong-field ionization of a three-dimensionally-oriented asymmetric top molecule, benzonitrile (C{sub 7}H{sub 5}N), by circularly polarized, nonresonant femtosecond laser pulses. Prior to the interaction with the strong field, the molecules are quantum-state selected using a deflector and three-dimensionally (3D) aligned and oriented adiabatically using an elliptically polarized laser pulse in combination with a static electric field. A characteristic splitting in the molecular frame photoelectron momentum distribution reveals the position of the nodal planes of the molecular orbitals from which ionization occurs. The experimental results are supported by a theoretical tunneling model that includes and quantifies the splitting in the momentum distribution. The focus of the present article is to understand strong-field ionization from 3D-oriented asymmetric top molecules, in particular the suppression of electron emission in nodal planes of molecular orbitals. In the preceding article [Dimitrovski et al., Phys. Rev. A 83, 023405 (2011)] the focus is to understand the strong-field ionization of one-dimensionally-oriented polar molecules, in particular asymmetries in the emission direction of the photoelectrons.

Counterintuitive angular shifts in the photoelectron momentum distribution for atoms in strong few-cycle circularly polarized laser pulses

We solve the three-dimensional time-dependent Schrodinger equation for a three-cycle circularly polarized laser pulse interacting with an atom. The photoelectron momentum distributions show counterintuitive shifts, similar to those observed in a recent experiment (Eckle et al 2008 Science 322 1525). The physical origin of the shifts is examined by a detailed investigation of the wave packet after the pulse. We show that the shifts arise as a consequence of an intimate interplay between the external field and the binding potential, and that the shifts occur also at lower intensities than used in the experiment, corresponding to the multiphoton regime. In contrast to the recent experiment we do not invoke the concept of a tunnelling time in our explanation of the shifts.

Strong-field ionization of polar molecules: Stark-shift-corrected strong-field approximation

We extend the molecular strong-field approximation for ionization, in the tunneling limit, to include systematically the linear and quadratic static Stark shifts of the ionizing molecular orbital. This approach, simple to implement, is capable of describing the essential physics of the process of strong-field ionization of oriented polar molecules by circularly polarized laser pulses. The modification of the molecular orbitals in strong fields is also discussed and in cases of extreme polarization of inner electrons a simple model is devised. We find very good agreement between the results from our model and those obtained in the recent experiment on ionizaton of oriented carbonyl sulphide and benzonitrile molecules [L. Holmegaard et al., Nature Phys. 6, 428 (2010)].