The amplitude and frequency of laser light can be routinely measured and controlled on a femtosecond (10(-15) s) timescale. However, in pulses comprising just a few wave cycles, the amplitude envelope and carrier frequency are not sufficient to characterize and control laser radiation, because evolution of the light field is also influenced by a shift of the carrier wave with respect to the pulse peak. This so-called carrier-envelope phase has been predicted and observed to affect strong-field phenomena, but random shot-to-shot shifts have prevented the reproducible guiding of atomic processes using the electric field of light. Here we report the generation of intense, few-cycle laser pulses with a stable carrier envelope phase that permit the triggering and steering of microscopic motion with an ultimate precision limited only by quantum mechanical uncertainty. Using these reproducible light waveforms, we create light-induced atomic currents in ionized matter; the motion of the electronic wave packets can be controlled on timescales shorter than 250 attoseconds (250 x 10(-18) s). This enables us to control the attosecond temporal structure of coherent soft X-ray emission produced by the atomic currents--these X-ray photons provide a sensitive and intuitive tool for determining the carrier-envelope phase.

A novel type of Fourier-transform infrared spectrometer (FTIR) is demonstrated. It is based on two Ti:sapphire lasers emitting femtosecond pulse trains with slightly different repetition frequencies. Two mid-infrared beams-derived from those lasers by rectification in GaSe-are superimposed upon a detector to produce purely time-domain interferograms that encode the infrared spectrum. The advantages of this spectrometer compared with the common FTIR include ease of operation (no moving parts), speed of acquisition (100 micros demonstrated), and not-yet-shown collimated long-distance propagation, diffraction-limited microscopic probing, and electronically controllable chemometric factoring. Extending time-domain frequency-comb spectroscopy to lower (terahertz) or higher (visible, ultraviolet) frequencies should be feasible.

Since 1998, the interaction of precision spectroscopy and ultrafast laser science has led to several notable accomplishments. Femtosecond laser optical frequency 'combs' (evenly spaced spectral lines) have revolutionized the measurement of optical frequencies and enabled optical atomic clocks. The same comb techniques have been used to control the waveform of ultrafast laser pulses, which permitted the generation of single attosecond pulses, and have been used in a recently demonstrated 'oscilloscope' for light waves. Here we demonstrate intra-cavity high harmonic generation in the extreme ultraviolet, which promises to lead to another joint frontier of precision spectroscopy and ultrafast science. We have generated coherent extreme ultraviolet radiation at a repetition frequency of more than 100 MHz, a 1,000-fold improvement over previous experiments. At such a repetition rate, the mode spacing of the frequency comb, which is expected to survive the high harmonic generation process, is large enough for high resolution spectroscopy. Additionally, there may be many other applications of such a quasi-continuous compact and coherent extreme ultraviolet source, including extreme ultraviolet holography, microscopy, nanolithography and X-ray atomic clocks.

The remarkable precision of frequency-comb (FC) lasers is transferred to the extreme ultraviolet (XUV, wavelengths shorter than 100 nm), a frequency region previously not accessible to these devices. A frequency comb at XUV wavelengths near 51 nm is generated by amplification and coherent upconversion of a pair of pulses originating from a near-infrared femtosecond FC laser. The phase coherence of the source in the XUV is demonstrated using helium atoms as a ruler and phase detector. Signals in the form of stable Ramsey-like fringes with high contrast are observed when the FC laser is scanned over P states of helium, from which the absolute transition frequency in the XUV can be extracted. This procedure yields a 4 He ionization energy at h  5 945 204 212ð6Þ MHz, improved by nearly an order of magnitude in accuracy, thus challenging QED calculations of this two-electron system. Mode-locked frequency-comb (FC) lasers [1,2] have revolutionized the field of precision laser spectroscopy. Optical atomic clocks using frequency combs are about to redefine the fundamental standard of frequency and time [3]. FC lasers have also vastly contributed to attosecond science by providing a way to synthesize electric fields at optical frequencies [4], made long distance absolute length measurements possible [5], and have recently been employed to produce ultracold molecules [6]. FC based precision spectroscopy on simple atomic systems has provided one of the most stringent tests of bound state quantum electrodynamics (QED) as well as upper bounds on the drift of fundamental constants [7]. Extending these methods into the extreme ultraviolet (XUV, wavelengths below 100 nm) spectral region is highly desirable since this would, for example, allow novel precision QED tests [8].Currently the wavelength range below 120 nm is essentially inaccessible to precision frequency metrology applications due to a lack of power of single frequency lasers and media for frequency up-conversion. Spectroscopic studies on neutral helium using amplified nanosecond laser pulses [9,10] are notoriously plagued by frequency chirping during amplification and harmonic conversion which limits the accuracy. These kind of transient effects can be avoided if a continuous train of high power laser pulses (produced by a FC) can be coherently up-converted. This would transfer the FC modes, at frequencies f n ¼ f CEO þ nf rep , where f CEO is the carrier-envelope offset frequency, f rep is the repetition frequency of the pulses, and n an integer mode number, to the XUV. Similar to what was shown in the visible [11,12], the up-converted pulse train could be used to directly excite a transition, with each of the up-converted modes acting like a single frequency laser.By amplification of a few pulses from the train, and producing low harmonics in crystals and gasses, sufficient coherence has been demonstrated down to 125 nm to perform spectroscopic experiments [13,14]. To reach wavelengths below 120 nm in the extreme ultraviolet or even x rays, high harmonic generati...