The performance of time-resolved photoemission experiments at fs-pulsed photon sources is ultimately limited by the e-e Coulomb interaction, downgrading energy and momentum resolution. Here, we present an approach to effectively suppress space-charge artifacts in momentum microscopes and photoemission microscopes. A retarding electrostatic field generated by a special objective lens repels slow electrons, retaining the k-image of the fast photoelectrons. The suppression of space-charge effects scales with the ratio of the photoelectron velocities of fast and slow electrons. Fields in the range from -20 to -1100 V/mm for Ekin = 100 eV to 4 keV direct secondaries and pump-induced slow electrons back to the sample surface. Ray tracing simulations reveal that this happens within the first 40 to 3 μm above the sample surface for Ekin = 100 eV to 4 keV. An optimized front-lens design allows switching between the conventional accelerating and the new retarding mode. Time-resolved experiments at Ekin = 107 eV using fs extreme ultraviolet probe pulses from the free-electron laser FLASH reveal that the width of the Fermi edge increases by just 30 meV at an incident pump fluence of 22 mJ/cm2 (retarding field -21 V/mm). For an accelerating field of +2 kV/mm and a pump fluence of only 5 mJ/cm2, it increases by 0.5 eV (pump wavelength 1030 nm). At the given conditions, the suppression mode permits increasing the slow-electron yield by three to four orders of magnitude. The feasibility of the method at high energies is demonstrated without a pump beam at Ekin = 3830 eV using hard x rays from the storage ring PETRA III. The approach opens up a previously inaccessible regime of pump fluences for photoemission experiments.

We report observation of x-ray and optical sum frequency generation. An ultrafast optical pulse drives charge oscillations to the chemical bonds in diamond. A co-propagating x-ray pulse probes the accompanying atomic-scale chemical bond distortion.

We report the generation of high power extreme ultraviolet frequency combs at 154 MHz repetition rate. The XUV combs are characterized by conducting high resolution spectroscopy and observing the heterodyne beats between two independent systems

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Light-matter interactions are ubiquitous, and underpin a wide range of basic research fields and applied technologies. Although optical interactions have been intensively studied, their microscopic details are often poorly understood and have so far not been directly measurable. X-ray and optical wave mixing was proposed nearly half a century ago as an atomic-scale probe of optical interactions but has not yet been observed owing to a lack of sufficiently intense X-ray sources. Here we use an X-ray laser to demonstrate X-ray and optical sum-frequency generation. The underlying nonlinearity is a reciprocal-space probe of the optically induced charges and associated microscopic fields that arise in an illuminated material. To within the experimental errors, the measured efficiency is consistent with first-principles calculations of microscopic optical polarization in diamond. The ability to probe optical interactions on the atomic scale offers new opportunities in both basic and applied areas of science.

Through a combined experimental and theoretical approach, we study the nonadiabatic dynamics of the prototypical ethylene (C(2)H(4)) molecule upon π → π(∗) excitation with 161 nm light. Using a novel experimental apparatus, we combine femtosecond pulses of vacuum ultraviolet and extreme ultraviolet (XUV) radiation with variable delay to perform time resolved photo-ion fragment spectroscopy. In this second part of a two part series, the XUV (17 eV < hν < 23 eV) probe pulses are sufficiently energetic to break the C-C bond in photoionization, or to photoionize the dissociation products of the vibrationally hot ground state. The experimental data is directly compared to excited state ab initio molecular dynamics simulations explicitly accounting for the probe step. Enhancements of the CH(2)(+) and CH(3)(+) photo-ion fragment yields, corresponding to molecules photoionized in ethylene (CH(2)CH(2)) and ethylidene (CH(3)CH) like geometries are observed within 100 fs after π → π(∗) excitation. Quantitative agreement between theory and experiment on the relative CH(2)(+) and CH(3)(+) yields provides experimental confirmation of the theoretical prediction of two distinct conical intersections and their branching ratio [H. Tao, B. G. Levine, and T. J. Martinez, J. Phys. Chem. A. 113, 13656 (2009)]. Evidence for fast, non-statistical, elimination of H(2) molecules and H atoms is observed in the time resolved H(2)(+) and H(+) signals.

We achieve 10dB suppression of phase-noise in a Yb-based frequency comb with 300kHz bandwidth by implementing robust intensity servo. The results are important for precision comb applications including femtosecond enhancement cavities.

Intrinsic to the process of high-order harmonic generation is the creation of plasma and the resulting spatiotemporal distortions of the driving laser pulse. Inside a high-finesse cavity where the driver pulse and gas medium are reused, this can lead to optical bistability of the cavity-plasma system, accumulated self-phase modulation of the intracavity pulse, and coupling to higher-order cavity modes. We present an experimental and theoretical study of these effects and discuss their implications for power scaling of intracavity high-order harmonic generation and extreme ultraviolet frequency combs.

We address technical impediments to the generation of high-photon flux XUV frequency combs through cavity-enhanced high harmonic generation. These difficulties arise from mirror damage, cavity nonlinearity, the intracavity plasma generated during the HHG process, and imperfect phase-matching. By eliminating or minimizing each of these effects we have developed a system capable of generating > 200 μW and delivering ~20 μW of average power for each spectrally separated harmonic (wavelengths ranging from 50 nm - 120 nm), to actual comb-based spectroscopy experiments.

We report a simple technique to suppress high-frequency phase noise of a Yb-based fiber optical frequency comb using an active intensity noise servo. Out-of-loop measurements of the phase noise using an optical heterodyne beat with a cw laser show suppression of phase noise by ≥7 dB out to Fourier frequencies of 100 kHz with a unity-gain crossing of ∼700 kHz. These results are enabled by the strong correlation between the intensity and phase noise of the laser. Detailed measurements of intensity and phase noise spectra, as well as transfer functions, reveal that the dominant phase and intensity noise contribution above ∼100 kHz is due to amplified spontaneous emission or other quantum noise sources.

Using a combined theoretical and experimental approach, we investigate the non-adiabatic dynamics of the prototypical ethylene (C(2)H(4)) molecule upon π → π∗ excitation. In this first part of a two part series, we focus on the lifetime of the excited electronic state. The femtosecond time-resolved photoelectron spectrum (TRPES) of ethylene is simulated based on our recent molecular dynamics simulation using the ab initio multiple spawning method with multi-state second order perturbation theory [H. Tao, B. G. Levine, and T. J. Martinez, J. Phys. Chem. A 113, 13656 (2009)]. We find excellent agreement between the TRPES calculation and the photoion signal observed in a pump-probe experiment using femtosecond vacuum ultraviolet (hν = 7.7 eV) pulses for both pump and probe. These results explain the apparent discrepancy over the excited state lifetime between theory and experiment that has existed for ten years, with experiments [e.g., P. Farmanara, V. Stert, and W. Radloff, Chem. Phys. Lett. 288, 518 (1998) and K. Kosma, S. A. Trushin, W. Fuss, and W. E. Schmid, J. Phys. Chem. A 112, 7514 (2008)] reporting much shorter lifetimes than predicted by theory. Investigation of the TRPES indicates that the fast decay of the photoion yield originates from both energetic and electronic factors, with the energetic factor playing a larger role in shaping the signal.

We combine different wavelengths from an intense high-order harmonics source with variable delay at the focus of a split-mirror interferometer to conduct pump-probe experiments on gas-phase molecules. We report measurements of the time resolution (<44 fs) and spatial profiles (4 μm × 12 μm) at the focus of the apparatus. We demonstrate the utility of this two-color, high-order-harmonic technique by time resolving molecular hydrogen elimination from C(2)H(4) excited into its absorption band at 161 nm.

The ensemble of lower orders produced in high order harmonic generation can be efficiently temporally separated by propagation in a fluoride window while still preserving their femtosecond pulse duration. We present calculations for MgF2, CaF2, and LiF windows for the third, fifth, and seventh harmonics of 800 nm. We use this simple and inexpensive technique in a pump/probe experiment to resolve femtosecond dynamics in the ethylene molecule.

Ultrafast X-ray science is an exciting frontier that promises the visualization of electronic, atomic and molecular dynamics on atomic time and length scales. A largely unexplored area of ultrafast X-ray science is the use of light to control how X-rays interact with matter. To extend control concepts established for long-wavelength probes to the X-ray regime, the optical control field must drive a coherent electronic response on a timescale comparable to femtosecond core-hole lifetimes. An intense field is required to achieve this rapid response. Here, an intense optical control pulse is observed to efficiently modulate photoelectric absorption for X-rays and to create an ultrafast transparency window. We demonstrate an application of X-ray transparency relevant to ultrafast X-ray sources: an all-photonic temporal cross-correlation measurement of a femtosecond X-ray pulse. The ability to control X-ray–matter interactions with light will create new opportunities for present and next-generation X-ray light sources. Intense optical beams can alter the way that a material interacts with X-ray radiation. This is now demonstrated by experiments that use femtosecond laser pulses to affect inner-shell processes in neon atoms, increasing the transmission of X-rays. This could allow imprinting of optical pulse trains onto much longer X-ray pulses.

We report, to our knowledge, the first dressed absorption spectrum at an X-ray probe wavelength. An ultrafast optical pulse induces transparency for X-rays, demonstrating a promising route to femtosecond X-ray pulse shaping and measurement.