We experimentally investigate the process of intramolecular quantum interference in high-order harmonic generation in impulsively aligned CO2 molecules. The recombination interference effect is clearly seen through the order dependence of the harmonic yield in an aligned sample. The experimental results can be well modeled assuming that the effective de Broglie wavelength of the returning electron wave is not significantly altered by the Coulomb field of the molecular ion. We demonstrate that such interference effects can be effectively controlled by changing the ellipticity of the driving laser field.

Wavelength scaling of high harmonic generation efficiencyUsing longer wavelength laser drivers for high harmonic generation is desirable because the highest extreme ultraviolet frequency scales as the square of the wavelength. Recent numerical studies predict that high harmonic efficiency falls dramatically with increasing wavelength, with a very unfavorable Àð5À6Þ scaling. We performed an experimental study of the high harmonic yield over a wavelength range of 800-1850 nm. A thin gas jet was employed to minimize phase matching effects, and the laser intensity and focal spot size were kept constant as the wavelength was changed. Ion yield was simultaneously measured so that the total number of emitting atoms was known. We found that the scaling at constant laser intensity is À6:3AE1:1 in Xe and À6:5AE1:1 in Kr over the wavelength range of 800-1850 nm, somewhat worse than the theoretical predictions.

Using quadrupole scan measurements we show laser-wakefield accelerated electrons to have a normalized transverse emittance of 0:21 þ0:01 À0:02 mm mrad at 245 MeV. We demonstrate a multishot and a single-shot method, the mean emittance values for both methods agree well. A simple model of the beam dynamics in the plasma density downramp at the accelerator exit matches the source size and divergence values inferred from the measurement. In the energy range of 245 to 300 MeV the normalized emittance remains constant.Laser-wakefield acceleration (LWFA) [1,2] can deliver ultrarelativistic electron beams in a compact setup with unique features [3][4][5][6]. It is receiving particular attention as a source or driver for ultrashort x-ray beams [7,8] and for its potential for realizing a tabletop free-electron laser (FEL) [9]. The electron bunch duration has recently been measured to be only a few femtoseconds long [10,11] which results in peak beam currents on the order of kiloamperes. An essential parameter for the performance of x-ray sources, FELs, or linear colliders is the transverse electron beam emittance. Previous emittance measurements of LWFA electron beams have used the pepperpot method [12][13][14] giving normalized emittances of $2:2 mm mrad with single shots down to the resolution limit of 1:1 mm mrad. As these measurements are not spectrally resolved, they rely on a low energy spread to give a meaningful normalized emittance. For LWFA beams which fluctuate in energy and energy spread, a simultaneous measurement of the spectrum is required. This technique is also limited to electron energies that can be sufficiently scattered by the pepper-pot mask; to date, measurements of a 508 MeV beam have been carried out [15]. Experiments characterizing the betatron radiation emitted by the electron beam while it is in the plasma suggest the beam size there to be & 1 m [16,17], which in combination with a divergence measurement give an estimated emittance of <0:5 mm mrad [18]. However, inferring the emittance from the electron beam size in the plasma and its downstream divergence in the vacuum can be unreliable as this neglects the plasma-vacuum density transition at the accelerator exit; here the decreasing strength of the plasma focusing forces result in an increase in beam size and decrease in divergence [13]. This publication reports on direct measurements of the emittance of LWFA electrons that are both energy resolved and that include the beam transport of the density downramp at the accelerator exit. This is achieved by analyzing their beam size around a focus using a quadrupole lens scan method [19].The transverse phase space of an electron beam is often specified using the Twiss parameters , , , and the natural emittance ". These parameters describe the volume and orientation of the particle distribution in phase space. The beam size at a particular position ðs 1 Þ is related to the Twiss parameters at s 0 by [20] ðs 1 Þ 2 ¼ M 2 11 ðs 0 Þ À2M 11 M 12 ðs 0 Þþ M 2 12 ðs 0 Þ: (1)Here M ij refers to the ij eleme...

Understanding the role of coherent electronic motion is expected to resolve general questions of importance in macromolecular energy transfer. We demonstrate a novel nonlinear optical method, angle-resolved coherent wave mixing, that separates out coherently coupled electronic transitions and energy transfers in an instantaneous two-dimensional mapping. Angular resolution of the signal is achieved by using millimeter laser beam waists at the sample and by signal relay to the far field; for this we use a high energy, ultrabroadband hollow fiber laser source. We reveal quantum electronic beating with a time-ordered selection of transition energies in a photosynthetic complex.

We produce oriented rotational wave packets in CO and measure their characteristics via high harmonic generation. The wavepacket 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. Laser-assisted molecular alignment has become an enabling tool for molecular frame studies in physics and chemistry [1]. Field-free molecular alignment plays a particularly important role in attosecond and recollision science, facilitating, for example, high harmonic orbital tomography [2,3], and laser induced electron diffraction experiments [4]. For polar molecules, in addition to alignment, it is important to orient the sample to avoid averaging over two opposite molecular orientations.Since the work of Friedrich and Herschach [5] on orientation of molecules in the presence of a strong DC field, several field-free orientation techniques have been demonstrated. Orientation methods include using a combination of a static electric field and a non-resonant femtosecond laser excitation [6][7][8]; using a combination of an electrostatic field and an intense nonresonant rapidly turnedoff laser field [9]; using an IR and UV pulse pair [10]; using THz pulses [11]; and using two-color laser fields [12,13]. To date orientation has been achieved in low gas densities [7] or with such a small degree of orientation [6,7,11] that high harmonics experiments have not been feasible.We demonstrate field-free orientation of CO molecules by using two-color (ω + 2ω) laser fields. The degree of orientation of the sample is probed by a second, delayed, probe pulse that generates high harmonic radiation (HHG). HHG in an isotropic gas produces odd harmonics of the laser frequency because alternate halfcycles of the laser field produce attosecond pulses with alternating sign. Anisotropy in the medium, produced for example by oriented molecules, breaks the strict alternation of sign, leading to the appearance of even harmonics of the laser frequency. Because there is no background Black line E total (t) = Eω cos(ωt) + E2ω cos(2ωt + ϕ2ω), ϕ2ω = 0, E2ω = 0.43Eω -the total field in the pump beam. The relative field ratio shown in the plot is the same as used in our experiment. (b) Half cycle total ionization rate of CO molecule as a function of angle between the molecular axis and the electric force calculated for intensity 1.5 × 10 14 W/cm 2 at 800 nm. -C-side points toward 0 • .at the spectral position of the even harmonics, HHG is a very sensitive measure of orientation.There are two contributing mechanisms of two-color laser fields th...

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.

We review recent progress towards imaging the electronic wavefunctions and nuclear dynamics of small molecules using the high order harmonics emitted when a molecule experiences an intense laser field. We illustrate that the essence of high harmonic emission is contained in the recombination amplitude between the continuum portion of the electronic wavefunction, that is formed through field ionization and which is accelerated and driven back to recollide in the laser field, and the bound electronic state. We review for the non-specialist some recent experimental and theoretical work dealing with high harmonic generation (HHG) in molecules. Particular attention is paid to two types of experiment recently performed in our group. The first of these types of experiment is the measurement of signatures of molecular electronic structure using HHG from molecules with a fixed orientation in space. The second is the use of HHG to track extremely fast proton rearrangement following ionization in light molecules, using the intrinsic temporal variation of the recolliding electron energy to extract these dynamics from measurements of the high harmonics.

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