Molecular alignment-assisted spectral broadening and shifting in the near-infrared with a recycled depleted pump from an optical parametric amplifier.

We demonstrate how the depleted pump of an optical parametric amplifier can be recycled for impulsive alignment of a molecular gas inside a hollow-core fiber and use such alignment for the broadening and frequency shift of the signal pulse at a center wavelength of ∼1300 nm. Our results combine non-adiabatic molecular alignment, self-phase modulation, and Raman non-linearities. We demonstrate spectral shifts of up to 204 nm and a spectral broadening of more than one octave.

Enhanced cutoff energies for direct and rescattered strong-field photoelectron emission of plasmonic nanoparticles.

The efficient generation, accurate detection, and detailed physical tracking of energetic electrons are of applied interest for high harmonics generation, electron-impact spectroscopy, and femtosecond time-resolved scanning tunneling microscopy. We here investigate the generation of photoelectrons (PEs) by exposing plasmonic nanostructures to intense laser pulses in the infrared (IR) spectral regime and analyze the sensitivity of PE spectra to competing elementary interactions for direct and rescattered photoemission pathways. Specifically, we measured and numerically simulated emitted PE momentum distributions from prototypical spherical gold nanoparticles (NPs) with diameters between 5 and 70 nm generated by short laser pulses with peak intensities of 8.

A plano-convex thick-lens velocity map imaging apparatus for direct, high resolution 3D momentum measurements of photoelectrons with ion time-of-flight coincidence.

Since their inception, velocity map imaging (VMI) techniques have received continued interest in their expansion from 2D to 3D momentum measurements through either reconstructive or direct methods. Recently, much work has been devoted to the latter of these by relating electron time-of-flight (TOF) to the third momentum component. The challenge is having a timing resolution sufficient to resolve the structure in the narrow (<10 ns) electron TOF spread.

Increased phase precision of spatial light modulators using irrational slopes: application to attosecond metrology.

The ability of spatial light modulators (SLMs) to modify the amplitude and phase of light has proved them invaluable to the optics and photonics community. In many applications, the bit-depth of SLMs is a major limiting factor dictated by a digital processor. As a result, there is usually a compromise between refresh speed and bit-depth.

Random quasi-phase-matching for pulse characterization from the near to the long wavelength infrared.

Experiments requiring ultrafast laser pulses require a full characterization of the electric field to glean meaning from the experimental data. Such characterization typically requires a separate parametric optical process. As the central wavelength range of new sources continues to increase so too does the need for nonlinear crystals suited for characterizing these wavelengths.

Characterization of an aerosolized nanoparticle beam beyond the diffraction limit through strong field ionization.

The study of nanomaterials is an active area of research for technological applications as well as fundamental science. A common method for studying properties of isolated nanoparticles is by an in-vacuum particle beam produced via an aerodynamic lens. Despite being common practice, characterization of such beams has proven difficult as light scattering detection techniques fail for particles with sizes beyond the diffraction limit.

3D velocity map imaging of electrons with TPX3CAM.

We demonstrate three-dimensional velocity map imaging of low energy electrons using a TPX3CAM, where the three-dimensional momentum information [p, p, p] is encoded in position and timing [x, y, t] of hits on the camera sensor. We make use of the camera sensor for the [x, y] information and a constant fraction discriminator and fast time to digital converter in the camera for the time information. We illustrate the capabilities of our apparatus by presenting above threshold ionization measurements of xenon, which produces well defined structures in the momentum resolved photoelectron yield.

Asymmetric high energy dual optical parametric amplifier for parametric processes and waveform synthesis.

We report on an asymmetric high energy dual optical parametric amplifier (OPA) which is capable of having either the idlers, signals, or depleted pumps, relatively phase locked at commensurate or incommensurate wavelengths. Idlers and signals can be locked on the order of 200 mrad rms or better, corresponding to a 212 as jitter at λ=2 µm. The high energy arm of the OPA outputs a combined 3.

Differentiating and Quantifying Gas-Phase Conformational Isomers Using Coulomb Explosion Imaging.

Conformational isomerism plays a crucial role in defining the physical and chemical properties and biological activity of molecules ranging from simple organic compounds to complex biopolymers. However, it is often a significant challenge to differentiate and separate these isomers experimentally as they can easily interconvert due to their low rotational energy barrier. Here, we use the momentum correlation of fragment ions produced after inner-shell photoionization to distinguish conformational isomers of 1,2-dibromoethane (CHBr).

Self referencing attosecond interferometer with zeptosecond precision.

In this work we demonstrate the generation of two intense, ultrafast laser pulses that allow a controlled interferometric measurement of higher harmonic generation pulses with 12.8 attoseconds in resolution (half the atomic unit of time) and a precision as low as 680 zeptoseconds (10 seconds). We create two replicas of a driving femtosecond pulse which share the same optical path except at the focus where they converge to two foci.

High harmonic generation spectroscopy via orbital angular momentum.

We present an experimental technique using orbital angular momentum (OAM) in a fundamental laser field to drive high harmonic generation (HHG). The mixing of beams with different OAM allows us to generate two laser foci tightly spaced which generate harmonics that interfere in the far field. Thus, this technique is an OAM based in situ HHG interferometric spectroscopic method.

An intense, few-cycle source in the long-wave infrared.

For the last several decades, the wavelength range accessible for strong-field, few-cycle studies has remained limited to the visible, near infrared and mid-wave infrared regimes. In particular, sources in the long-wave infrared have been lacking. We report the development of a 1 kHz, few-cycle laser source with up to a 9 μm central wavelength and gigawatt peak powers.

Spatial characterization of Bessel-like beams for strong-field physics.

We present a compact, simple design for the generation and tuning of both the spot size and effective focal length of Bessel-like beams. In particular, this setup provides an important tool for the use of Bessel-like beams with high-power, femtosecond laser systems. Using a shallow angle axicon in conjunction with a spherical lens, we show that it is possible to focus Bessel-like modes to comparable focal spot sizes to sharp axicons while maintaining a long effective focal length.

Ionization Study of Isomeric Molecules in Strong-field Laser Pulses.

Through the use of the technique of time-of-flight mass spectroscopy, we obtain strong-field ionization yields for randomly oriented 1,2-dichloroethylene (1,2-DCE) (CHCl) and 2-butene (CH). We are interested in studying the effect of conformal structure in strong-field ionization and, in particular, the role of molecular polarity. That is, we can perform strong-field ionization studies in polar vs non-polar molecules that have the same chemical composition.

Optical damage threshold of Au nanowires in strong femtosecond laser fields.

Ultrashort, intense light pulses permit the study of nanomaterials in the optical non-linear regime. Non-linear regimes are often present just below the damage threshold thus requiring careful tuning of the laser parameters to avoid melting the materials. Detailed studies of the damage threshold of nanoscale materials are therefore needed.

Strong-field atomic phase matching.

We interpret a learning-control experiment with the goal of optimizing multiphoton population transfer in atomic sodium in the strong-field limit. Despite multiple experimental constraints, a learning algorithm discovers optimal pulses that can be understood in terms of a simple dynamic picture of the atom-field interaction. We show that the shaped pulses counteract the dynamic Stark-induced stimulated emission that would otherwise impede the efficient use of a pi pulse to invert a multiphoton transition.

Transformations to diagonal bases in closed-loop quantum learning control experiments.

This paper discusses transformations between bases used in closed-loop learning control experiments. The goal is to transform to a basis in which the number of control parameters is minimized and in which the parameters act independently. We demonstrate a simple procedure for testing whether a unitary linear transformation (i.