Native Frames: Disentangling Sequential from Concerted Three-Body Fragmentation.

A key question concerning the three-body fragmentation of polyatomic molecules is the distinction of sequential and concerted mechanisms, i.e., the stepwise or simultaneous cleavage of bonds. Using laser-driven fragmentation of OCS into O^{+}+C^{+}+S^{+} and employing coincidence momentum imaging, we demonstrate a novel method that enables the clear separation of sequential and concerted breakup. The separation is accomplished by analyzing the three-body fragmentation in the native frame associated with each step and taking advantage of the rotation of the intermediate molecular fragment, CO^{2+} or CS^{2+}, before its unimolecular dissociation. This native-frame method works for any projectile (electrons, ions, or photons), provides details on each step of the sequential breakup, and enables the retrieval of the relevant spectra for sequential and concerted breakup separately. Specifically, this allows the determination of the branching ratio of all these processes in OCS^{3+} breakup. Moreover, we find that the first step of sequential breakup is tightly aligned along the laser polarization and identify the likely electronic states of the intermediate dication that undergo unimolecular dissociation in the second step. Finally, the separated concerted breakup spectra show clearly that the central carbon atom is preferentially ejected perpendicular to the laser field.

Carrier-envelope phase control over pathway interference in strong-field dissociation of H2+.

The dissociation of an H2+ molecular-ion beam by linearly polarized, carrier-envelope-phase-tagged 5 fs pulses at 4×10(14) W/cm2 with a central wavelength of 730 nm was studied using a coincidence 3D momentum imaging technique. Carrier-envelope-phase-dependent asymmetries in the emission direction of H+ fragments relative to the laser polarization were observed. These asymmetries are caused by interference of odd and even photon number pathways, where net zero-photon and one-photon interference predominantly contributes at H+ + H kinetic energy releases of 0.2-0.45 eV, and net two-photon and one-photon interference contributes at 1.65-1.9 eV. These measurements of the benchmark H2+ molecule offer the distinct advantage that they can be quantitatively compared with ab initio theory to confirm our understanding of strong-field coherent control via the carrier-envelope phase.

Coherent control at its most fundamental: carrier-envelope-phase-dependent electron localization in photodissociation of a H2(+) molecular ion beam target.

Measurements and calculations of the absolute carrier-envelope-phase (CEP) effects in the photodissociation of the simplest molecule, H2(+), with a 4.5-fs Ti:sapphire laser pulse at intensities up to (4±2)×10(14) W/cm2 are presented. Localization of the electron with respect to the two nuclei (during the dissociation process) is controlled via the CEP of the ultrashort laser pulses. In contrast to previous CEP-dependent experiments with neutral molecules, the dissociation of the molecular ions is not preceded by a photoionization process, which strongly influences the CEP dependence. Kinematically complete data are obtained by time- and position-resolved coincidence detection. The phase dependence is determined by a single-shot phase measurement correlated to the detection of the dissociation fragments. The experimental results show quantitative agreement with ab initio 3D time-dependent Schrödinger equation calculations that include nuclear vibration and rotation.

Multiphoton above threshold effects in strong-field fragmentation.

We present a study of multiphoton dissociative ionization from molecules. By solving the time-dependent Schrödinger equation for H(2)(+) and projecting the solution onto double continuum scattering states, we observe the correlated electron-nuclear ionization dynamics in detail. We show-for the first time-how multiphoton structure prevails as long as one accounts for the energies of all the fragments. Our current work provides a new avenue to analyze strong-field fragmentation that leads to a deeper understanding of the correlated molecular dynamics.

Enhancing the intense field control of molecular fragmentation.

We describe a pump-probe scheme with which the spatial asymmetry of dissociating molecular fragments-as controlled by the carrier-envelope phase of an intense few-cycle laser pulse-can be enhanced by an order of magnitude or more. We illustrate the scheme using extensive, full-dimensional calculations for dissociation of H(2)(+) and include the averaging necessary for comparison with experiment.

New class of three-body states.

We calculate the three-body spectrum for identical bosons interacting via attractive 1/r(2) potentials. We find an infinite number of three-body states even when the pair interactions are too weak to support any two-body states. These new states thus share this surprising scenario with the Efimov effect, but are not themselves Efimov states. Our effect occurs for both identical bosons and identical fermions, and it persists in the presence of two-body bound states.

Origin of the three-body parameter universality in Efimov physics.

In recent years extensive theoretical and experimental studies of universal few-body physics have advanced our understanding of universal Efimov physics. Whereas theory had been the driving force behind our understanding of Efimov physics for decades, recent experiments have contributed an unexpected discovery. Specifically, measurements have found that the so-called three-body parameter determining several properties of the system is universal, even though fundamental assumptions in the theory of the Efimov effect suggest that it should be a variable property that depends on the precise details of the short-range two- and three-body interactions. The present Letter resolves this apparent contradiction by elucidating previously unanticipated implications of the two-body interactions. Our study shows that the three-body parameter universality emerges because a universal effective barrier in the three-body potentials prevents the three particles from simultaneously getting close together. Our results also show limitations on this universality, as it is more likely to occur for neutral atoms but less likely to extend to light nuclei.

Efimov physics in heteronuclear four-body systems.

We study three- and four-body Efimov physics in a heteronuclear atomic system with three identical heavy bosonic atoms and one light atom. We show that exchange of the light atom between the heavy atoms leads to both three- and four-body features in the low-energy inelastic rate constants that trace to the Efimov effect. Further, the effective interaction generated by this exchange can provide an additional mechanism for control in ultracold experiments. Finally, we find that there is no true four-body Efimov effect-that is, no infinite number of four-body states in the absence of two- and three-body bound states-resolving a decades-long controversy.

Colliding Bose-Einstein condensates to observe Efimov physics.

We explore the manifestation of Efimov physics through the collision energy dependence of the three-body scattering observables and propose that it can be measured by observing atom loss in collisions of Bose-Einstein condensates. Our study shows that log-periodic Efimov features in the scattering observables extend beyond the usual threshold regime to nonzero collision energies and result from two interfering pathways. Further, these oscillations have a one-to-one connection with the scattering length oscillations at zero energy and thus to Efimov states themselves.

Magnetically controlled exchange process in an ultracold atom-dimer mixture.

We report on the observation of an elementary exchange process in an optically trapped ultracold sample of atoms and Feshbach molecules. We can magnetically control the energetic nature of the process and tune it from endoergic to exoergic, enabling the observation of a pronounced threshold behavior. In contrast to relaxation to more deeply bound molecular states, the exchange process does not lead to trap loss. We find excellent agreement between our experimental observations and calculations based on the solutions of three-body Schrödinger equation in the adiabatic hyperspherical representation. The high efficiency of the exchange process is explained by the halo character of both the initial and final molecular states.

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.

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.

Ultracold three-body collisions near overlapping Feshbach resonances.

We present a comprehensive collection of ultracold three-body collisions properties near overlapping Feshbach resonances. Our results incorporate variations of all scattering lengths and demonstrate novel collisional behavior, such as atom-molecule interference effects. Taking advantage of the unique ways in which these collisions reflect Efimov physics, new pathways to control atomic and molecular losses open up. Further, we show that overlapping resonances can greatly improve the chances of observing multiple Efimov features in an ultracold quantum gas for nearly any system.

Efimov trimer formation via ultracold four-body recombination.

We discuss the collisional formation of Efimov trimers via ultracold four-body recombination. In particular, we consider the reaction A+A+A+B-->A_{3}+B with A and B ultracold atoms. We obtain expressions for the four-body recombination rate up to an overall constant and show that it reflects the three-body Efimov physics either as a function of collision energy or as a function of the two-body s-wave scattering length between A atoms. In addition, we briefly discuss issues important for experimentally observing this interesting and unexplored process.

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.

Suppression of molecular decay in ultracold gases without Fermi statistics.

We study inelastic processes for ultracold three-body systems in which only one interaction is resonant. We show that at ultracold temperatures three-body recombination in such systems leads mainly to the formation of weakly bound molecules. In addition, and perhaps more importantly, we have found that the decay rates for weakly bound molecules due to collisions with other atoms can be suppressed not only without fermionic statistics but also when bosonic statistics applies. These results indicate that recombination in three-component atomic gases can be used as an efficient mechanism for molecular formation, allowing the achievement of high molecular densities.

General theory of carrier-envelope phase effects.

We present a general framework for understanding carrier-envelope phase (CEP) effects in a quantum system interacting with an intense, short laser pulse. We establish a simple connection between the CEP and the wave function that can be exploited to obtain the full CEP dependence of an observable given the wave function at a single CEP. Within this framework, all CEP effects are interpreted as interference between different photon amplitudes which, in turn, can be used to put limits on the pulse lengths and intensities required to see significant CEP effects.

Above threshold Coulomb explosion of molecules in intense laser pulses.

We have measured and explained a new mechanism of molecular ionization near the appearance intensity that produces a sequence of peaks in the nuclear kinetic energy spectrum separated by the photon energy. Our interpretation is based on an internally consistent model for the nuclear motion during an intense laser pulse. Within this model, the same concepts and language can be used for both dissociation and ionization, leading to a more unified understanding of the dynamics.

Dissociation and ionization of H+2 by ultrashort intense laser pulses probed by coincidence 3D momentum imaging.

Laser-induced dissociation and ionization of H(+)(2) were simultaneously measured using coincidence 3D momentum imaging, allowing direct separation of the two processes, even where the fragment kinetic energy is the same for both processes. The results for 45 and 135 fs 790 nm pulses with an intensity of approximately 2.5 x 10(14) W/cm(2) differ from each other much more than one would expect from previous measurements with longer pulses. Ionization was negligible for the longer pulse and was strongly aligned along the laser polarization for the shorter pulse, but showed no structure in its kinetic energy distribution. In addition, the ionization to dissociation ratio was found to be much smaller than theoretically predicted for H(+)(2).