Use of Co2+:MgAl2O4 transparent ceramics in passive Q-switching of an Er:Glass laser at 1.534†µm.

We present the implementation of Co2+:MgAl2O4 transparent ceramics as passive Q-switching elements in an Er:Glass laser at 1.534 µm. Linearly polarized pulsed output was obtained by Brewster angle inclination of the material Q-switching plate relative to the laser axis. Separate pulses were ∼105 ns long (FWHM), exhibiting ∼6.2 kW peak power at near TEM00 quality. Several fundamental sample properties important for laser intracavity operation were measured; thermo-optic coefficient dn/dT = ( - 3.8 ± 1) × 10-5 °C-1, thermal lensing factor L-1d(nL)/dT = 2.59 × 10-5 °C-1, linear expansion coefficient α = (3.9 ± 0.6) × 10-5 °C-1, polarizability thermal coefficient ϕ = (7.2 ± 2.2) × 10-5 °C-1, and damage threshold ∼6.5 J/cm2.

Competing radiative and nonradiative decay of embedded ions states in dielectric crystals: theory, and application to Co2+:AgCl0.5Br0.5.

We present a generally applicable theoretical model describing excited-state decay lifetime analysis of metal ions in a host crystal matrix. In contrast to common practice, we include multi-phonon non-radiative transitions competitively to the radiative one. We have applied our theory to Co2+ ions in a mixed AgCl0.5Br0.5 crystal, and as opposed to a previous analysis, find excellent agreement between theory and experiment over the entire measured temperature range. The fit predicts a zero absolute temperature radiative lifetime τrad(0) = 5.5 ms, more than three times longer than the measured effective low-temperature one τeff(0) = 1.48 ms. Furthermore, the fit configuration potential dissociation energy has been estimated as D = 2500 cm-1 and the lattice vibrational cutoff frequency as hωco = 180 cm-1. We have experimentally verified the latter by optical reflection measurement in the far-IR.

Creating high-harmonic beams with controlled orbital angular momentum.

A beam with an angular-dependant phase Φ = ℓϕ about the beam axis carries an orbital angular momentum of ℓℏ per photon. Such beams are exploited to provide superresolution in microscopy. Creating extreme ultraviolet or soft-x-ray beams with controllable orbital angular momentum is a critical step towards extending superresolution to much higher spatial resolution. We show that orbital angular momentum is conserved during high-harmonic generation. Experimentally, we use a fundamental beam with |ℓ| = 1 and interferometrically determine that the harmonics each have orbital angular momentum equal to their harmonic number. Theoretically, we show how any small value of orbital angular momentum can be coupled to any harmonic in a controlled manner. Our results open a route to microscopy on the molecular, or even submolecular, scale.

Order-dependent structure of high harmonic wavefronts.

The physics of high harmonics has led to the generation of attosecond pulses and to trains of attosecond pulses. Measurements that confirm the pulse duration are all performed in the far field. All pulse duration measurements tacitly assume that both the beam's wavefront and intensity profile are independent of frequency. However, if one or both are frequency dependent, then the retrieved pulse duration depends on the location where the measurement is made. We measure that each harmonic is very close to a Gaussian, but we also find that both the intensity profile and the beam wavefront depend significantly on the harmonic order. Thus, our findings mean that the pulse duration will depend on where the pulse is observed. Measurement of spectrally resolved wavefronts along with temporal characterization at one single point in the beam would enable complete space-time reconstruction of attosecond pulses. Future attosecond science experiments need not be restricted to spatially averaged observables. Our approach paves the way to recovery of the single molecule response to the strong field.

Oriented rotational wave-packet dynamics studies via high harmonic generation.

We produce oriented rotational wave packets in CO and measure their characteristics via high harmonic generation. The wave packet is created using an intense, femtosecond laser pulse and its second harmonic. A delayed 800 nm pulse probes the wave packet, generating even-order high harmonics that arise from the broken symmetry induced by the orientation dynamics. The even-order harmonic radiation that we measure appears on a zero background, enabling us to accurately follow the temporal evolution of the wave packet. Our measurements reveal that, for the conditions optimum for harmonic generation, the orientation is produced by preferential ionization which depletes the sample of molecules of one orientation.

Probing polar molecules with high harmonic spectroscopy.

We bring the methodology of orienting polar molecules together with the phase sensitivity of high harmonic spectroscopy to experimentally compare the phase difference of attosecond bursts of radiation emitted upon electron recollision from different ends of a polar molecule. This phase difference has an impact on harmonics from aligned polar molecules, suppressing emission from the molecules parallel to the driving laser field while favoring the perpendicular ones. For oriented molecules, we measure the amplitude ratio of even to odd harmonics produced when intense light irradiates CO molecules and determine the degree of orientation and the phase difference of attosecond bursts using molecular frame ionization and recombination amplitudes. The sensitivity of the high harmonic spectrum to subtle phase differences in the emitted radiation makes it a detailed probe of polar molecules and will drive major advances in the theory of high harmonic generation.

Frequency-resolved high-harmonic wavefront characterization.

We introduce and demonstrate a novel concept of frequency-resolved wavefront characterization. Our approach is particularly suitable for high-harmonic, extreme-UV (XUV) and soft X-ray radiation. The concept is based on an analysis of radiation diffracted from a slit scanned in front of a flat-field XUV spectrometer. With the spectrally resolved signal spread across one axis and the spatially resolved diffraction pattern in the other dimension, we reconstruct the wavefront. While demonstrated for high harmonics, the method is not restricted in wavelength.

Femtosecond pulse shaping using a two-dimensional liquid-crystal spatial light modulator.

We introduce a programmable, high-rate scanning femtosecond pulse shaper based on a two-dimensional liquid crystal on a silicon spatial light modulator (SLM). While horizontal resolution of 1920 addressable pixels provides superior fidelity for generating complex waveforms, scanning across the vertical dimension (1080 pixels) has been used to facilitate at least 3 orders of magnitude speed increase as compared with typical liquid-crystal SLM-based pulse shapers. An update rate in excess of 100 kHz is demonstrated.

Femtosecond pulse-shape modulation at nanosecond rates.

We report high-rate, computer-controlled femtosecond pulse shaping by use of an electro-optical gallium arsenide optical phased-array modulator with 2304 controlled waveguides. It provides fast modulation speed of both spectral phases and amplitudes. Limited by the driving electronics of our current setup, we were able to update a pulse shape in approximately 30 ns. This technique paves the way toward individual shaping of every single pulse of typical femtosecond mode-locked oscillators.

Femtosecond pulse-shape modulation at kilohertz rates.

We demonstrate a new scanning femtosecond pulse-shaping technique that allows pulse shapes to be modulated at kilohertz rates. This technique is particularly useful for lock-in measurements in which the signal is synchronized with the alternating pulse shapes. The pulse-shape lock-in technique is demonstrated in resonant coherent anti-Stokes Raman scattering, where it is shown to significantly improve the ratio of the resonant signal to both the nonresonant background and to noise.