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. We also report on the time delays at which broadening occurs, which do not coincide with any of the molecular rotational constants. Further, we encounter that maximum frequency shifts occur when the signal and pump have perpendicular polarization instead of parallel.

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. Here, we build upon the work in VMI lens design and 3D VMI measurement by using a plano-convex thick-lens (PCTL) VMI in conjunction with an event-driven camera (TPX3CAM) providing TOF information for high resolution 3D electron momentum measurements. We perform simulations to show that, with the addition of a mesh electrode to the thick-lens geometry, the resulting plano-convex electrostatic field extends the detectable electron cutoff energy range while retaining the high resolution. This design also extends the electron TOF range, allowing for a better momentum resolution along this axis. We experimentally demonstrate these capabilities by examining above-threshold ionization in xenon, where the apparatus is shown to collect electrons of energy up to ∼7 eV with a TOF spread of ∼30 ns, both of which are improved compared to a previous work by factors of ∼1.4 and ∼3.75, respectively. Finally, the PCTL-VMI is equipped with a coincident ion TOF spectrometer, which is shown to effectively extract unique 3D momentum distributions for different ionic species in a gas mixture. These techniques have the potential to lend themselves to more advanced measurements involving systems where the electron momentum distributions possess non-trivial symmetries.

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. Here we report on the use of poly-crystalline zinc selenide as a universal nonlinear crystal in the frequency resolved optical gating characterization technique from the near to long-wavelength infrared. Due to its property of random quasi-phase-matching it's capable of phase matching second-harmonic and sum-frequency generation of ultra-broadband pulses in the near and long wavelength infrared, while being crystal orientation independent. With the majority of ultra-fast laser sources being in this span of wavelengths, this work demonstrates a greatly simplified approach towards ultra-fast pulse characterization spanning from the near to the long-wavelength infrared. To our knowledge there is no single optical technique capable of such flexible capabilities.

A simple approach for characterizing the spatially varying sensitivity of microchannel plate detectors.

We present a simple approach to characterize the spatial variation of the gain in microchannel plate (MCP) coupled to phosphor detectors using single electron or photon hits. The technique is easy to implement and general enough to be extended to other kinds of detectors. We demonstrate the efficacy of the approach on both laboratory and Monte Carlo generated datasets. Furthermore, we use the approach to measure the variation in gain over time as the MCP is exposed to an increasing number of electrons.

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. Here, we present a method to increase the effective bit-depth of SLMs, which utilizes a linear slope, as is commonly applied to deal with the zeroth-order effect. This technique was tested using two interferometric transient absorption spectroscopy setups. Through the high harmonic generation in gases producing a train of attosecond pulses and harmonics from solids in the ultraviolet, two pulses are generated that interfere in the far field providing a measurement of the optical phase. An increase in the precision far beyond the limit dictated by the digital processor in the bit-depth was found.

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 3.5 mJ of signal and idler, while the low energy arm outputs 1.5 mJ, with the entire system being pumped with a 1 kHz, 18 mJ Ti:Sapphire laser. Both arms are independently tunable from 1080 nm-2600 nm. The combination of relative phase locking, high output power and peak intensity, and large tunability makes our OPA an ideal tool for use in difference frequency generation (DFG) in the strong pump regime, and for high peak field waveform synthesis in the near-infrared. To demonstrate this ability we generate terahertz radiation through two color waveform synthesis in air plasma and show the influence of the relative phase on the generated terahertz intensity. The ability to phase lock multiple incommensurate wavelengths at high energies opens the door to a multitude of possibilities of strong pump DFG and waveform synthesis.

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 (C2H4Br2). We demonstrate that the three-body breakup channel, C2H4+ + Br+ + Br+, contains signatures of both sequential and concerted breakup, which are decoupled to distinguish the geometries of two conformational isomers and to quantify their relative abundance. The sensitivity of our method to quantify these yields is established by measuring the relative abundance change with sample temperature, which agrees well with calculations. Our study paves the way for using Coulomb explosion imaging to track subtle molecular structural changes.

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 (10-21 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. An attosecond pulse train emerges from each focus through the process of high harmonic generation. The two attosecond pulse trains from each focus interfere in the far field producing a clear interference pattern in the extreme ultraviolet region. By controlling the relative optical phase (carrier envelope phase for pulsed fields) between the two driving laser pulses we are able to actively influence the delay between the pulses and are able to perform very stable and precise pump-probe experiments. Because of the phase shaping operation occurs homogeneously across the entire spatial profile, we effectively create two indistinguishable intense laser pulses or a common path interferometer for attosecond pulses. Commonality across the two beams means that they are extremely stable to environmental and mechanical fluctuations up to a Rayleigh range from the focus. In our opinion this represents an ideal source for homodyne and heterodyne spectroscopic measurements with sub-attosecond precision.

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. With this tool, we measure the phase and amplitude of the angle dependent multiorbital HHG emission in molecular nitrogen.

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. When focused, this source can ionize gas targets, which we demonstrate here through the ionization of atomic xenon at wavelengths ranging from 5 µm to 9 µm. This opens up new opportunities for fundamental atomic and molecular physics, enabling experimental tests of strong-field ionization theories in the extreme long-wavelength, few-cycle limit and the direct excitation of vibrational transitions in organic molecules.

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) (C2H2Cl2) and 2-butene (C4H8). 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. We report our findings through the ionization yields and the ratio (trans/cis) of each stereoisomer pair as a function of intensity.

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. The resulting focal profiles are characterized in detail using an accurate high dynamic range imaging technique. Quantitatively, we introduce a metric (R0.8) which defines the spot-size containing 80% of the total energy. Our setup overcomes the typical compromise between long working distances and small spot sizes. This is particularly relevant for strong-field physics where most experiments must operate in vacuum.

Carrier-envelope-phase stabilized terawatt class laser at 1 kHz with a wavelength tunable option.

We demonstrate a chirped-pulse-amplified Ti:Sapphire laser system operating at 1 kHz, with 20 mJ pulse energy, 26 femtosecond pulse duration (0.77 terawatt), and excellent long term carrier-envelope-phase (CEP) stability. A new vibrational damping technique is implemented to significantly reduce vibrational noise on both the laser stretcher and compressor, thus enabling a single-shot CEP noise value of 250 mrad RMS over 1 hour and 300 mrad RMS over 9 hours. This is, to the best of our knowledge, the best long term CEP noise ever reported for any terawatt class laser. This laser is also used to pump a white-light-seeded optical parametric amplifier, producing 6 mJ of total energy in the signal and idler with 18 mJ of pumping energy. Due to preservation of the CEP in the white-light generated signal and passive CEP stability in the idler, this laser system promises synthesized laser pulses spanning multi-octaves of bandwidth at an unprecedented energy scale.

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. We present results on the damage threshold of gold (Au) nanowires when illuminated by intense femtosecond pulses. These nanowires were synthesized via the directed electrochemical nanowire assembly (DENA) process in two configurations: (1) free-standing Au nanowires on tungsten (W) electrodes and (2) Au nanowires attached to fused silica slides. In both cases the wires have a single-crystalline structure. For 790 nm laser pulses with durations of 108 fs and 32 fs at a repetition rate of 2 kHz, we find that the free-standing nanowires melt at intensities close to 3 TW/cm2 (194 mJ/cm2) and 7.5 TW/cm2 (144 mJ/cm2), respectively. The Au nanowires attached to silica slides melt at slightly higher intensities, just above 10 TW/cm2 (192 mJ/cm2) for 32 fs pulses. Our results can be explained with an electron-phonon interaction model that describes the absorbed laser energy and subsequent heat conduction across the wire.