Ultrafast temporal evolution of interatomic Coulombic decay in NeKr dimers.

We investigate interatomic Coulombic decay in NeKr dimers after neon inner-valence photoionization [Ne+(2s-1)] using a synchrotron light source. We measure with high energy resolution the two singly charged ions of the Coulomb-exploding dimer dication and the photoelectron in coincidence. By carefully tracing the post-collision interaction between the photoelectron and the emitted ICD electron we are able to probe the temporal evolution of the state as it decays. Although the ionizing light pulses are 80 picoseconds long, we determine the lifetime of the intermediate dimer cation state and visualize the contraction of the nuclear structure on the femtosecond time scale.

Incorporating real time velocity map image reconstruction into closed-loop coherent control.

We report techniques developed to utilize three-dimensional momentum information as feedback in adaptive femtosecond control of molecular dynamics. Velocity map imaging is used to obtain the three-dimensional momentum map of the dissociating ions following interaction with a shaped intense ultrafast laser pulse. In order to recover robust feedback information, however, the two-dimensional momentum projection from the detector must be inverted to reconstruct the full three-dimensional momentum of the photofragments. These methods are typically slow or require manual inputs and are therefore accomplished offline after the images have been obtained. Using an algorithm based upon an "onion-peeling" (also known as "back projection") method, we are able to invert 1040 × 1054 pixel images in under 1 s. This rapid inversion allows the full photofragment momentum to be used as feedback in a closed-loop adaptive control scheme, in which a genetic algorithm tailors an ultrafast laser pulse to optimize a specific outcome. Examples of three-dimensional velocity map image based control applied to strong-field dissociation of CO and O2 are presented.

Adaptive strong-field control of chemical dynamics guided by three-dimensional momentum imaging.

Shaping ultrafast laser pulses using adaptive feedback can manipulate dynamics in molecular systems, but extracting information from the optimized pulse remains difficult. Experimental time constraints often limit feedback to a single observable, complicating efforts to decipher the underlying mechanisms and parameterize the search process. Here we show, using two strong-field examples, that by rapidly inverting velocity map images of ions to recover the three-dimensional photofragment momentum distribution and incorporating that feedback into the control loop, the specificity of the control objective is markedly increased. First, the complex angular distribution of fragment ions from the nω+C2D4→C2D3++D interaction is manipulated. Second, isomerization of acetylene (nω+C2H2→C2H2(2+)→CH2++C+) is controlled via a barrier-suppression mechanism, a result that is validated by model calculations. Collectively, these experiments comprise a significant advance towards the fundamental goal of actively guiding population to a specified quantum state of a molecule.

Benchmark measurements of H(3)(+) nonlinear dynamics in intense ultrashort laser pulses.

The H(3)(+) ion is the simplest polyatomic molecule and is destined to play a central role in understanding such molecules in intense ultrashort laser pulses. We present the first measurements of the intense field dissociation and ionization of D(3)(+) using coincidence three-dimensional momentum imaging. Our results show features that are a consequence of this molecule's unique equilateral triangular geometry, providing a fundamentally new system for theoretical development.

Suppressed dissociation of H(2)(+) vibrational states by reduced dipole coupling.

The suppression of H(2)(+) strong-field dissociation has intrigued experimentalists and theorists since the early days of laser-molecular science. We unravel a vibrational suppression effect due to weak dipole-matrix element coupling strengths of certain vibrational states, dependent on the laser frequency-a form of Cooper minima. This effect is demonstrated by our full-dimensional calculations on H(2)(+) dissociation and persists for a broad range of laser conditions including both weak and strong-field dissociation. Using a crossed-beams coincidence, three-dimensional momentum-imaging technique, the vibrational suppression effect is clearly observed for H(2)(+) and HD(+) at 790 and 395 nm, in good agreement with our theory.

Enhancing high-order above-threshold dissociation of H2+ beams with few-cycle laser pulses.

High-order (three-photon or more) above-threshold dissociation (ATD) of H(2)(+) has generally not been observed using 800 nm light. We demonstrate a strong enhancement of its probability using intense 7 fs laser pulses interacting with beams of H(2)(+), HD(+), and D(2)(+) ions. The mechanism invokes a dynamic control of the dissociation pathway. These measurements are supported by theory that additionally reveals, for the first time, an unexpectedly large contribution to ATD from highly excited electronic states.

Determining the absolute efficiency of a delay line microchannel-plate detector using molecular dissociation.

We present a method to measure the absolute detection efficiency of a delay-line microchannel-plate detector using the breakup of diatomic molecular ions. This method provides the absolute total detection efficiency, as well as the individual efficiency for each signal of the detector. The method is based on the fact that molecular breakup always yields two hits on the detector, but due to finite detection efficiency some of these events are recorded as single particles while others are detected in pairs. We demonstrate the method by evaluating the detection efficiency for both timing and position signals of a delay-line detector using laser-induced dissociation of molecular ions. In addition, the detection efficiency as a function of position has been determined by dividing the detector into sectors.