Citation: ALEXANDROV, A.S., 1994. From electron to small polaron: an exact cluster solution. Physical Review B, 49 (14),

Abstract:The first time-resolved x-ray/optical pump-probe experiments at the SLAC Linac Coherent Light Source (LCLS) used a combination of feedback methods and post-analysis binning techniques to synchronize an ultrafast optical laser to the linac-based x-ray laser. Transient molecular nitrogen alignment revival features were resolved in time-dependent x-rayinduced fragmentation spectra. These alignment features were used to find the temporal overlap of the pump and probe pulses. The strong-field dissociation of x-ray generated quasi-bound molecular dications was used to establish the residual timing jitter. This analysis shows that the relative arrival time of the Ti:Sapphire laser and the x-ray pulses had a distribution with a standard deviation of approximately 120 fs. The largest contribution to the jitter noise spectrum was the locking of the laser oscillator to the reference RF of the accelerator, which suggests that simple technical improvements could reduce the jitter to better than 50 fs. ©2010 Optical Society of America

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-color (800 and 400 nm) short (45 fs) linearly polarized pulses are used to ionize and dissociate D2 into a neutral deuterium atom and a deuteron. The yields and energies of the ions are measured left and right along the polarization vector. As the relative phase of the two colors is varied, strong yield asymmetries are found in the ion-energy regions traditionally identified as bond softening, above-threshold dissociation and rescattering. The asymmetries in these regions are quite different. A model based on the dynamic coupling by the laser field of the gerade and ungerade states in the molecular ion accounts for many of the observed features.

Two-color (800-and 400-nm) short (45-fs) linearly polarized pulses are used to ionize and dissociate CO and NO. The emission of C q + , N q + , and O + fragments indicates that the higher ionization rate occurs when the peak electric field points from C to O in CO and from N to O in NO. This preferred direction is in agreement with that predicted by Stark-corrected strong-field-approximation calculations.

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Abstract:We study the evolution of nuclear wave packets launched in molecular nitrogen, oxygen and carbon monoxide by intense 8fs infrared pulses.We use velocity map imaging to measure the momentum of the ion fragments when these wave packets are interrogated by a second such pulse after a variable time delay. Both quasi-bound and dissociative wave packets are observed. For the former, measurements of bound-state oscillations are used to identify the participating states and in some cases extract properties of the relevant potential energy surfaces. Vibrational structure is resolved in both energy and oscillation-frequency for the cations of oxygen and carbon monoxide, displaying the same quantum wave packet motion in both energy and time domains. In addition, vibrational structure is seen in the dication of carbon 2 monoxide in a situation where the energy resolution by itself is inadequate to resolve the structure.

We demonstrate an experimental control of electron localization in deuterium molecular ions created and dissociated by the combined action of an attosecond pulse train and a many-cycle infrared (IR) pulse. The attosecond pulse train is synthesized using both even and odd high order harmonics of the driving IR frequency so that it can strobe the IR field once per IR cycle. An asymmetric ejection of the deuterium ions oscillates with the full IR period when the APT-IR time-delay is scanned. The observed control is due to the creation of a coherent superposition of 1s sigma{g} and 2p sigma{u} states via interference between one-photon and two-photon dissociation channels.