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.

The dissociation of an H + 2 molecular-ion beam by linearly polarized, carrier-envelope-phase-tagged 5 fs pulses at 4×10 14 W/cm 2 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 1-photon interference predominantly contributes at H + +H kinetic energy releases of 0.2 -0.45 eV, and net-2-photon and 1-photon interference contributes at 1.65 -1.9 eV. These measurements of the benchmark H + 2 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. PACS numbers: XXXOne ultimate goal of ultrafast, strong-field laser science is to coherently control chemical reactions [1][2][3]. A prerequisite to achieving this goal is to understand the control mechanisms and reaction pathways. To this end, tailoring the electric field waveform of few-cycle laser pulses to control reactions and uncover the underlying physics has become a powerful tool [4][5][6]. It has been applied to the dissociative ionization of H 2 and its isotopologues [7][8][9][10][11][12] and has recently been extended to more complex diatomic molecules, such as CO [13][14][15], and to small polyatomic molecules [16,17].Conceptually, one of the most basic features of a fewcycle laser pulse to control is the carrier-envelope phase (CEP). When the laser's electric field is written as E(t) = E 0 (t) cos(ωt + φ), E 0 (t) is an envelope function, ω is the carrier angular frequency, and φ is the CEP. In fact, all of the few-cycle waveform experiments cited above used the CEP as the control parameter.For example, Kling et al. used 5 fs, 1.2×10 14 W/cm 2 pulses with stabilized CEP to dissociatively ionize D 2 and found asymmetries in the emission direction of D + ions for kinetic energy releases (KER) above 6 eV [7,8]. The diminished dissociation signal in a circularly polarized laser field indicated that recollision played a role. Recollision entails a tunnel-ionized electron undergoing a collision with its parent ion after acceleration by the oscillating laser field [18,19]. The energy exchange between the laser-driven electron and the parent ion can promote the D + 2 to the 2pσ u excited state. Coupling of the 2pσ u and 1sσ g states [20] on the trailing edge of the laser pulse during the dissociation of D + 2 was suggested as the explanation for the CEP-dependent asymmetry [7,8].Another example comes from Kremer et al. who exposed an H 2 target to 6 fs, 4.4×10 14 W/cm 2 CEPstabilized laser pulses and observed asymmetries for KER values between 0.4 and 3 eV [9] -energies they attributed to bond softening (BS) [21] and not electron recollision, which has higher KER. They proposed that the initial ionization of H 2 generates a coherent wav...

In a recent Letter, Manschwetus et al. [Phys. Rev. Lett. 102, 113002 (2009)] reported evidence of electron recapture during strong-field fragmentation of H 2 -explained using a frustrated tunneling ionization model. Unusually, the signature of this process was detection of excited H * atoms. We report here an extensive study of this process in D 2 . Our measurements encompass a study of the pulse duration, intensity, ellipticity, and angular distribution dependence of D * formation. While we find that the mechanism suggested by Manschwetus et al. is consistent with our experimental data, our theoretical work shows that electron recollision excitation cannot be completely ruled out as an alternative mechanism for D * production.

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We study few-cycle, strong-field dissociation of aligned H + 2 by solving the time-dependent Schrödinger equation including rotation. We examine the dependence of the final angular distribution, the kinetic energy release spectrum, and the total dissociation yield on the initial nuclear angular distribution. In particular, we look at the dependence on the relative angle θ 0 between the laser polarization and the symmetry axis of a well-aligned initial distribution, as well as the dependence on the delay between the "pump" pulse that prepares the alignment and the few-cycle probe pulse. Surprisingly, we find the dissociation probability for θ 0 = 90• can be appreciable even though the transitions involved are purely parallel. We therefore address the limits of the commonly held "ball-and-stick" picture for molecules in intense fields as well as the validity of the axial recoil approximation.