Time-resolved holography with photoelectrons

Ionization is the dominant response of atoms and molecules to intense laser fields and is at the basis of several important techniques, such as the generation of attosecond pulses that allow the measurement of electron motion in real time. We present experiments in which metastable xenon atoms were ionized with intense 7-micrometer laser pulses from a free-electron laser. Holographic structures were observed that record underlying electron dynamics on a sublaser-cycle time scale, enabling photoelectron spectroscopy with a time resolution of almost two orders of magnitude higher than the duration of the ionizing pulse.     

Attosecond control and measurement: lightwave electronics

Electrons emit light, carry electric current, and bind atoms together to form molecules. Insight into and control of their atomic-scale motion are the key to understanding the functioning of biological systems, developing efficient sources of x-ray light, and speeding up electronics. Capturing and steering this electron motion require attosecond resolution and control, respectively (1 attosecond = 10(-18) seconds). A recent revolution in technology has afforded these capabilities: Controlled light waves can steer electrons inside and around atoms, marking the birth of lightwave electronics. Isolated attosecond pulses, well reproduced and fully characterized, demonstrate the power of the new technology. Controlled few-cycle light waves and synchronized attosecond pulses constitute its key tools. We review the current state of lightwave electronics and highlight some future directions.     

Attosecond synchronization of high-harmonic soft x-rays

Subfemtosecond light pulses can be obtained by superposing several high harmonics of an intense laser pulse. Provided that the harmonics are emitted simultaneously, increasing their number should result in shorter pulses. However, we found that the high harmonics were not synchronized on an attosecond time scale, thus setting a lower limit to the achievable x-ray pulse duration. We showed that the synchronization could be improved considerably by controlling the underlying ultrafast electron dynamics, to provide pulses of 130 attoseconds in duration. We discuss the possibility of achieving even shorter pulses, which would allow us to track fast electron processes in matter.     

X-ray pulses approaching the attosecond frontier

Single soft-x-ray pulses of approximately 90-electron volt (eV) photon energy are produced by high-order harmonic generation with 7-femtosecond (fs), 770-nanometer (1.6 eV) laser pulses and are characterized by photoionizing krypton in the presence of the driver laser pulse. By detecting photoelectrons ejected perpendicularly to the laser polarization, broadening of the photoelectron spectrum due to absorption and emission of laser photons is suppressed, permitting the observation of a laser-induced downshift of the energy spectrum with sub-laser-cycle resolution in a cross correlation measurement. We measure isolated x-ray pulses of 1.8 (+0.7/-1.2) fs in duration, which are shorter than the oscillation cycle of the driving laser light (2.6 fs). Our techniques for generation and measurement offer sub-femtosecond resolution over a wide range of x-ray wavelengths, paving the way to experimental attosecond science. Tracing atomic processes evolving faster than the exciting light field is within reach.     

Generation and photonic guidance of multi-octave optical-frequency combs

Ultrabroad coherent comb-like optical spectra spanning several octaves are a chief ingredient in the emerging field of attoscience. We demonstrate generation and guidance of a three-octave spectral comb, spanning wavelengths from 325 to 2300 nanometers, in a hydrogen-filled hollow-core photonic crystal fiber. The waveguidance results not from a photonic band gap but from the inhibited coupling between the core and cladding modes. The spectrum consists of up to 45 high-order Stokes and anti-Stokes lines and is generated by driving the confined gas with a single, moderately powerful (10-kilowatt) infrared laser, producing 12-nanosecond-duration pulses. This represents a reduction by six orders of magnitude in the required laser powers over previous equivalent techniques and opens up a robust and much simplified route to synthesizing attosecond pulses.     

Ultrafast lasers. Strobe light breaks the attosecond barrier

On page 1689 of this issue, physicists report creating the fastest strobe light ever made, with individual pulses lasting just 220 attoseconds, or 220 billionths of a billionth of a second. These unimaginably short pulses are the first to be confirmed as breaking the attosecond barrier, a goal of high-speed-laser researchers for nearly a decade. Such pulses may one day serve as an ultrafast camera, allowing researchers to freeze action and perhaps to spot the gyrations of individual electrons whirling around an atomic nucleus.     

Synthesized light transients

Manipulation of electron dynamics calls for electromagnetic forces that can be confined to and controlled over sub-femtosecond time intervals. Tailored transients of light fields can provide these forces. We report on the generation of subcycle field transients spanning the infrared, visible, and ultraviolet frequency regimes with a 1.5-octave three-channel optical field synthesizer and their attosecond sampling. To demonstrate applicability, we field-ionized krypton atoms within a single wave crest and launched a valence-shell electron wavepacket with a well-defined initial phase. Half-cycle field excitation and attosecond probing revealed fine details of atomic-scale electron motion, such as the instantaneous rate of tunneling, the initial charge distribution of a valence-shell wavepacket, the attosecond dynamic shift (instantaneous ac Stark shift) of its energy levels, and its few-femtosecond coherent oscillations.     

Observation of a train of attosecond pulses from high harmonic generation

In principle, the temporal beating of superposed high harmonics obtained by focusing a femtosecond laser pulse in a gas jet can produce a train of very short intensity spikes, depending on the relative phases of the harmonics. We present a method to measure such phases through two-photon, two-color photoionization. We found that the harmonics are locked in phase and form a train of 250-attosecond pulses in the time domain. Harmonic generation may be a promising source for attosecond time-resolved measurements.     

Generation of femtosecond pulses of synchrotron radiation

Femtosecond synchrotron pulses were generated directly from an electron storage ring. An ultrashort laser pulse was used to modulate the energy of electrons within a 100-femtosecond slice of the stored 30-picosecond electron bunch. The energy-modulated electrons were spatially separated from the long bunch and used to generate approximately 300-femtosecond synchrotron pulses at a bend-magnet beamline, with a spectral range from infrared to x-ray wavelengths. The same technique can be used to generate approximately 100-femtosecond x-ray pulses of substantially higher flux and brightness with an undulator. Such synchrotron-based femtosecond x-ray sources offer the possibility of applying x-ray techniques on an ultrafast time scale to investigate structural dynamics in condensed matter.     

Generation of an artificial aurora

On 26 January 1969 an Aerobee 350 rocket was fired from Wallops Island, Virginia, carrying an electron accelerator. Above 230 kilometers the electron guns put out a beam of 0.5 ampere of 10 kev electrons in pulses of 1-second duration aimed downward along the earth's magnetic field lines. The interaction of electron beam with the atmosphere at an altitude of about 100 kilometers generated enough light so that the auroral rays produced could be photographed on the ground by television camera systems.     

Time-resolved investigation of coherently controlled electric currents at a metal surface

Studies of current dynamics in solids have been hindered by insufficiently brief trigger signals and electronic detection speeds. By combining a coherent control scheme with photoelectron spectroscopy, we generated and detected lateral electron currents at a metal surface on a femtosecond time scale with a contact-free experimental setup. We used coherent optical excitation at the light frequencies omega(a) and omega(a)/2 to induce the current, whose direction was controlled by the relative phase between the phase-locked laser excitation pulses. Time- and angle-resolved photoelectron spectroscopy afforded a direct image of the momentum distribution of the excited electrons as a function of time. For the first (n = 1) image-potential state of Cu(100), we found a decay time of 10 femtoseconds, attributable to electron scattering with steps and surface defects.     

Steering attosecond electron wave packets with light

Photoelectrons excited by extreme ultraviolet or x-ray photons in the presence of a strong laser field generally suffer a spread of their energies due to the absorption and emission of laser photons. We demonstrate that if the emitted electron wave packet is temporally confined to a small fraction of the oscillation period of the interacting light wave, its energy spectrum can be up- or downshifted by many times the laser photon energy without substantial broadening. The light wave can accelerate or decelerate the electron's drift velocity, i.e., steer the electron wave packet like a classical particle. This capability strictly relies on a sub-femtosecond duration of the ionizing x-ray pulse and on its timing to the phase of the light wave with a similar accuracy, offering a simple and potentially single-shot diagnostic tool for attosecond pump-probe spectroscopy.     

The future of attosecond spectroscopy

Attoscience is the study of physical processes that occur in less than a fraction of a cycle of visible light, in times less than a quadrillionth of a second. The motion of electrons inside atoms and molecules that are undergoing photoionization or chemical change falls within this time scale, as does the plasma motion that causes the reflectivity of metals. The techniques to study motion on this scale are based on careful control of strong-field laser-atom interactions. These techniques and new research opportunities in attosecond spectroscopy are reviewed.     

The multielectron ionization dynamics underlying attosecond strong-field spectroscopies

Subcycle strong-field ionization (SFI) underlies many emerging spectroscopic probes of atomic or molecular attosecond electronic dynamics. Extending methods such as attosecond high harmonic generation spectroscopy to complex polyatomic molecules requires an understanding of multielectronic excitations, already hinted at by theoretical modeling of experiments on atoms, diatomics, and triatomics. Here, we present a direct method which, independent of theory, experimentally probes the participation of multiple electronic continua in the SFI dynamics of polyatomic molecules. We use saturated (n-butane) and unsaturated (1,3-butadiene) linear hydrocarbons to show how subcycle SFI of polyatomics can be directly resolved into its distinct electronic-continuum channels by above-threshold ionization photoelectron spectroscopy. Our approach makes use of photoelectron-photofragment coincidences, suiting broad classes of polyatomic molecules.     

Picosecond optical switching based on biphotonic excitation of an electron donor-acceptor-donor molecule

An electron donor-acceptor-donor molecule consisting of two porphyrin donors rigidly attached to the two-electron acceptor N,N'-diphenyl-3,4,9,10-perylenebis(dicarboximide) acts as a light intensity-dependent molecular switch on a picosecond time scale. Excitation of the porphyrins within this molecule with subpicosecond laser pulses results in single or double reduction of the acceptor depending on the light intensity. The singly and doubly reduced electron acceptors absorb light strongly at 713 and 546 nanometers, respectively. Because these absorption changes are produced solely by electron transfers, this molecular switch effectively has no moving parts and switches significantly faster than photochromic molecules that must undergo changes in molecular structure.     

Cherenkov radiation at speeds below the light threshold: phonon-assisted phase matching

Charged particles traveling through matter at speeds larger than the phase velocity of light in the medium emit Cherenkov radiation. Calculations reveal that a given angle of the radiation conical wavefront is associated with two velocities, one above and one below a certain speed threshold. Emission at subluminal but not superluminal speeds is predicted and verified experimentally for relativistic dipoles generated with an optical method based on subpicosecond pulses moving in a nonlinear medium. The dipolar Cherenkov field, in the range of infrared-active phonons, is identical to that of phonon polaritons produced by impulsive laser excitation.     

Picosecond coherent optical manipulation of a single electron spin in a quantum dot

Most schemes for quantum information processing require fast single-qubit operations. For spin-based qubits, this involves performing arbitrary coherent rotations of the spin state on time scales much faster than the spin coherence time. By applying off-resonant, picosecond-scale optical pulses, we demonstrated the coherent rotation of a single electron spin through arbitrary angles up to pi radians. We directly observed this spin manipulation using time-resolved Kerr rotation spectroscopy and found that the results are well described by a model that includes the electronnuclear spin interaction. Measurements of the spin rotation as a function of laser detuning and intensity confirmed that the optical Stark effect is the operative mechanism.     

Bright coherent ultrahigh harmonics in the keV x-ray regime from mid-infrared femtosecond lasers

High-harmonic generation (HHG) traditionally combines ~100 near-infrared laser photons to generate bright, phase-matched, extreme ultraviolet beams when the emission from many atoms adds constructively. Here, we show that by guiding a mid-infrared femtosecond laser in a high-pressure gas, ultrahigh harmonics can be generated, up to orders greater than 5000, that emerge as a bright supercontinuum that spans the entire electromagnetic spectrum from the ultraviolet to more than 1.6 kilo-electron volts, allowing, in principle, the generation of pulses as short as 2.5 attoseconds. The multiatmosphere gas pressures required for bright, phase-matched emission also support laser beam self-confinement, further enhancing the x-ray yield. Finally, the x-ray beam exhibits high spatial coherence, even though at high gas density the recolliding electrons responsible for HHG encounter other atoms during the emission process.     

A quantum dot single-photon turnstile device

Quantum communication relies on the availability of light pulses with strong quantum correlations among photons. An example of such an optical source is a single-photon pulse with a vanishing probability for detecting two or more photons. Using pulsed laser excitation of a single quantum dot, a single-photon turnstile device that generates a train of single-photon pulses was demonstrated. For a spectrally isolated quantum dot, nearly 100% of the excitation pulses lead to emission of a single photon, yielding an ideal single-photon source.     

Generation of megawatt optical solitons in hollow-core photonic band-gap fibers

The measured dispersion of a low-loss, hollow-core photonic band-gap fiber is anomalous throughout most of the transmission band, and its variation with wavelength is large compared with that of a conventional step-index fiber. For an air-filled fiber, femtosecond self-frequency--shifted fundamental solitons with peak powers greater than 2megawatts can be supported. For Xe-filled fibers, nonfrequency-shifted temporal solitons with peak powers greater than 5.5 megawatts can be generated, representing an increase in the power that can be propagated in an optical fiber of two orders of magnitude. The results demonstrate a unique capability to deliver high-power pulses in a single spatial mode over distances exceeding 200 meters.