Summary form only given. Fundamental processes in atoms, molecules, as well as condensed matter are triggered or mediated by the motion of electrons inside or between atoms. Electronic dynamics on atomic length scales tends to unfold within tens to thousands of attoseconds (1 attosecond [as] = 10-18 s). Recent breakthroughs in laser science are now opening the door to watching and controlling these hitherto inaccessible microscopic dynamics. The key to accessing the attosecond time domain is the control of the electric field of (visible) light, which varies its strength and direction within less than a femtosecond (1 femtosecond = 1000 attoseconds). Atoms exposed to a few oscillations cycles of intense laser light are able to emit a single extreme ultraviolet (XUV) burst lasting less than one femtosecond. Full control of the evolution of the electromagnetic field in laser pulses comprising a few wave cycles have recently allowed the reproducible generation and measurement of isolated sub-femtosecond XUV pulses, demonstrating the control of microscopic processes (electron motion and photon emission) on an attosecond time scale. These tools have enabled us to visualize the oscillating electric field of visible light with an attosecond "oscilloscope", to control single-electron and probe multi-electron dynamics in atoms, molecules and solids. Recent experiments hold promise for the development of an attosecond X-ray source, which may pave the way towards 4D electron imaging with sub-atomic resolution in space and time.

Attosecond Physics

Nonlinear optics plays a central role in the advancement of optical science and laser-based technologies. We report on the confinement of the nonlinear interaction of light with matter to a single wave cycle and demonstrate its utility for time-resolved and strong-field science. The electric field of 3.3-femtosecond, 0.72-micron laser pulses with a controlled and measured waveform ionizes atoms near the crests of the central wave cycle, with ionization being virtually switched off outside this interval. Isolated sub-100-attosecond pulses of extreme ultraviolet light (photon energy {approx} 80 electron volts), containing {approx} 0.5 nanojoule of energy, emerge from the interaction with a conversion efficiency of {approx} 10{sup -6}. These tools enable the study of the precision control of electron motion with light fields and electron-electron interactions with a resolution approaching the atomic unit of time ({approx} 24 attoseconds).

/pdf/single-cycle-nonlinear-optics-2w4hkpvunv.pdf

Single-cycle nonlinear optics.

The long-standing scientific quest of real-time tracing electronic motion and dynamics in all states of matter has been remarkably benefited by the development of intense laser-based pulsed sources with a temporal resolution in the attosecond [1 attosecond = 10−18 s] time scale. Nowadays, attosecond pulses are routinely produced in laboratories by the synthesis of the frequency components of broadband coherent extreme ultraviolet (XUV) radiation generated by the interaction of matter with intense femtosecond (fs) pulses. Attosecond pulse metrology aims at the accurate and complete determination of the temporal and phase characteristics of attosecond pulses and is one of the most innovative challenges in the broad field of ultrashort pulse metrology. For more than two decades since coherent high-brilliance broadband XUV sources have become available, fascinating advances in attosecond pulse metrology have led to the development of remarkable techniques for pulse duration measurements as well as the complete reconstruction of those pulses. Nonetheless, new challenges born from diverse fields call upon for additional efforts and continuously innovative ideas in the field. In this perspective article, we follow the history of ultrashort pulse technology tracing attosecond pulse production and characterization approaches, focus on the operation principles of the most commonly used techniques in the region where they interact with matter, address their limitations, and discuss future prospects as well as endeavors of the field to encounter contemporary scientific progress.

/pdf/attosecond-pulse-metrology-5ff7orrqd1.pdf

Attosecond pulse metrology

We use semiconductor (Si) and metallic (Al, Zr) transmission filters to shape, in amplitude and phase, high-order harmonics generated from the interaction of an intense titanium sapphire laser field with a pulsed neon gas target. Depending on the properties of the filter, the emitted attosecond pulses can be optimized in bandwidth and/or pulse length. We demonstrate the generation of attosecond pulses centered at energies from 50 to 80 eV, with bandwidths as large as 45 eV and with pulse durations compressed to 130 as.

Broadband attosecond pulse shaping.

We study experimentally the ionization of argon atoms by a train of attosecond pulses in the presence of a strong infrared laser field, using a velocity map imaging technique. The recorded momentum distribution strongly depends on the delay between the attosecond pulses and the laser field. We interpret the interference patterns observed for different delays using numerical and analytical calculations within the strong field approximation.

Angularly resolved electron wave packet interferences

We present experimental measurements of attosecond pulse trains. The characterization of the pulses uses a spectral interferometry technique that is implemented with a Mach-Zehnder interferometer. This allows us to manipulate independently the pump and probe pulses for a wide range of applications. By letting the attosecond pulses pass through metallic films, we can in particular compensate for the intrinsic chirp of the attosecond pulses corresponding to the plateau spectral region, thus getting pulses as short as 170 attoseconds- only 1.2 optical cycles at the central frequency. The measurement technique is also applicable for determination of the group delay of thin XUV-transparent films and relative delay in the photoionization process. Our experimental method is applied to attosecond pulse trains created by 35- and 9-fs laser pulses, and the shortest train observed consists of three or four pulses.

Experimental studies of attosecond pulse trains

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Experimental studies of attosecond pulse trains