Igor Litvinyuk

Field-Free Orientation of CO Molecules by Femtosecond Two-Color Laser Fields

We report the first experimental observation of nonadiabatic field-free orientation of a heteronuclear diatomic molecule (CO) induced by an intense two-color (800 and 400 nm) femtosecond laser field. We monitor orientation by measuring fragment ion angular distributions after Coulomb explosion with an 800 nm pulse. The orientation of the molecules is controlled by the relative phase of the two-color field. The results are compared to quantum mechanical rigid rotor calculations. The demonstrated method can be applied to study molecular frame dynamics under field-free conditions in conjunction with a variety of spectroscopy methods, such as high-harmonic generation, electron diffraction, and molecular frame photoelectron emission.

Two-pulse alignment of molecules

Field-free alignment of gas-phase molecules can be achieved by creating rotational wavepackets with a short laser pulse. We demonstrate that the degree of alignment can be improved by illuminating the molecules with a second laser pulse at a specific time during the evolution of the original rotational wavepacket.

IR-assisted ionization of helium by attosecond extreme ultraviolet radiation

Attosecond science has opened up the possibility of manipulating electrons on their fundamental timescales. Here, we use both theory and experi- ment to investigate ionization dynamics in helium on the attosecond timescale by simultaneously irradiating the atom with a soft x-ray attosecond pulse train (APT) and an ultrafast laser pulse. Because the APT has resolution in both energy and time, we observe processes that could not be observed without resolu- tion in both domains simultaneously. We show that resonant absorption is impor- tant in the excitation of helium and that small changes in energies of harmonics that comprise the APT can result in large changes in the ionization process. With the help of theory, ionization pathways for the infrared-assisted excitation and ionization of helium by extreme ultraviolet (XUV) attosecond pulses have been identified and simple model interpretations have been developed that should be of general applicability to more complex systems (Zewail A 2000 J. Phys. Chem. A 104 5660-94).

Momentum-imaging investigations of the dissociation of D2+ and the isomerization of acetylene to vinylidene by intense short laser pulses

We present momentum images of the ionic products from the ionization of D2 and C2H2 by short laser pulses. For D2, we use a pump–probe approach to investigate the dependence of the enhanced ionization on the internuclear distance. Evidence for two (not well separated) regions of enhancement is found near internuclear distances of 6 and 10 au. In the case of acetylene, we report clear evidence for the production of both acetylene and vinylidene dications with kinetic energy releases similar to those reported earlier by core electron removal. We also find very different angular distributions for the fragments in the two channels, consistent with a finite time for the isomerization.

Wavelength dependence of momentum-space images of low-energy electrons generated by short intense laser pulses at high intensities

We have measured momentum-space images of low-energy electrons generated by the interaction of short intense laser pulses with argon atoms at high intensities. We have done this over a wavelength range from 400 to 800 nm. The spectra show considerable structure in both the energy and angular distributions of the electrons. Some, but not all, energy features can be identified as multi-photon resonances. The angular structure shows a regularity which transcends the resonant structure and may be due instead to diffraction. The complexity of the results defies easy model-dependent interpretations and invites full solutions to Schrodingers equation for these systems.

Experimental observation of the elusive double-peak structure in R-dependent strong-field ionization rate of H2(+).

When a diatomic molecule is ionized by an intense laser field, the ionization rate depends very strongly on the inter-nuclear separation. That dependence exhibits a pronounced maximum at the inter-nuclear separation known as the “critical distance”. This phenomenon was first demonstrated theoretically in H2+ and became known as “charge-resonance enhanced ionization” (CREI, in reference to a proposed physical mechanism) or simply “enhanced ionization”(EI). All theoretical models of this phenomenon predict a double-peak structure in the R-dependent ionization rate of H2+. However, such double-peak structure has never been observed experimentally. It was even suggested that it is impossible to observe due to fast motion of the nuclear wavepackets. Here we report a few-cycle pump-probe experiment which clearly resolves that elusive double-peak structure. In the experiment, an expanding H2+ ion produced by an intense pump pulse is probed by a much weaker probe pulse. The predicted double-peak structure is clearly seen in delay-dependent kinetic energy spectra of protons when pump and probe pulses are polarized parallel to each other. No structure is seen when the probe is polarized perpendicular to the pump.

Strong-field non-sequential double ionization: wavelength dependence of ion momentum distributions for neon and argon

Strong-field double ionization of atoms in a non-sequential regime produces longitudinal ion momentum distributions with a characteristic double-peak structure. At 800 nm laser wavelength in Ne2+ the structure is very pronounced with a well-resolved dip at zero momentum, while for Ar2+ the dip is very shallow, possibly indicating different mechanisms in the two atoms. We investigated the source of this difference by measuring longitudinal momentum distributions of Ne2+ and Ar2+ ions at different laser wavelengths (485, 800, 1313 and 2000 nm) and intensities. The shapes of the experimental momentum distributions for the two atoms exhibit strong dependence on laser wavelength: for both the dip becomes more pronounced at longer wavelengths. At 1300 nm the longitudinal momentum spectrum for Ar2+ is similar to that of Ne2+ at 800 nm. On the other hand, the Ne2+ spectrum measured at 485 nm has the same shape as that of Ar2+ at 800 nm. This observation indicates that the difference between Ne and Ar observed at 800 nm should not be attributed solely to differences in relative electron impact ionization and excitation cross-sections of the two atoms. It is, to a larger extent, due to the interplay between the ponderomotive energy of electron and the ionization potentials of the target atom.

Coherent control of D2/H2 dissociative ionization by a mid-infrared two-color laser field

Steering the electrons during an ultrafast photo-induced process in a molecule influences the chemical behavior of the system, opening the door to the control of photochemical reactions and photobiological processes. Electrons can be efficiently localized using a strong laser field with a well-designed temporal shape of the electric component. Consequently, many experiments have been performed with laser sources in the near-infrared region (800 nm) in the interest of studying and enhancing the electron localization. However, due to its limited accessibility, the mid-infrared (MIR) range has barely been investigated, although it allows to efficiently control small molecules and even more complex systems. To push further the manipulation of basic chemical mechanisms, we used a MIR two-color (1800 and 900 nm) laser field to ionize H2 and D2 molecules and to steer the remaining electron during the photo-induced dissociation. The study of this prototype reaction led to the simultaneous control of four fragmentation channels. The results are well reproduced by a theoretical model solving the time-dependent Schrodinger equation for the molecular ion, identifying the involved dissociation mechanisms. By varying the relative phase between the two colors, asymmetries (i.e., electron localization selectivity) of up to 65% were obtained, corresponding to enhanced or equivalent levels of control compared to previous experiments. Experimentally easier to implement, the use of a two-color laser field leads to a better electron localization than carrier-envelope phase stabilized pulses and applying the technique in the MIR range reveals more dissociation channels than at 800 nm.

Benchmarking strong-field ionization with atomic hydrogen

As the simplest atomic system, the hydrogen atom plays a key benchmarking role in laser and quantum physics. Atomic hydrogen is a widely used atomic test system for theoretical calculations of strong-field ionization, since approximate theories can be directly compared to numerical solutions of the time-dependent Schrodinger equation. However, relatively little experimental data is available for comparison to these calculations, since atomic hydrogen sources are difficult to construct and use. We review the existing experimental results on strong-field ionization of atomic hydrogen in multi-cycle and few-cycle laser pulses. Quantitative agreement has been achieved between experiment and theoretical predictions at the 10% uncertainty level, and has been used to develop an intensity calibration method with 1% uncertainty. Such quantitative agreement can be used to certify experimental techniques as being free from systematic errors, guaranteeing the accuracy of data obtained on species other than H. We review the experimental and theoretical techniques that enable these results.

Wavelength-dependent study of strong-field Coulomb explosion of hydrogen

We present the first systematic wavelength-dependent study of laser Coulomb explosion of deuterium molecules at various peak intensities and polarizations. We measured the kinetic energy spectra of D+ for laser wavelengths in the range 480–2000 nm. In addition to the well-known enhanced ionization channel present for all wavelengths, we observe a new high-energy band at short wavelengths. This new band exhibits wavelength dependence, with fragment energy decreasing with increasing wavelengths until it merges with the enhanced ionization band for 800 nm and longer. We attribute the emergence of this band to a new pathway that involves resonant three-photon coupling to the first excited electronic state of the molecular ion during the Coulomb explosion process. This pathway should be accounted for in controlling molecular dynamics of hydrogen by intense laser pulses.