Adrian L. Cavalieri

Attosecond spectroscopy in condensed matter

Comprehensive knowledge of the dynamic behaviour of electrons in condensed-matter systems is pertinent to the development of many modern technologies, such as semiconductor and molecular electronics, optoelectronics, information processing and photovoltaics. Yet it remains challenging to probe electronic processes, many of which take place in the attosecond (1 as = 10-18 s) regime. In contrast, atomic motion occurs on the femtosecond (1 fs = 10-15 s) timescale and has been mapped in solids in real time using femtosecond X-ray sources. Here we extend the attosecond techniques previously used to study isolated atoms in the gas phase to observe electron motion in condensed-matter systems and on surfaces in real time. We demonstrate our ability to obtain direct time-domain access to charge dynamics with attosecond resolution by probing photoelectron emission from single-crystal tungsten. Our data reveal a delay of approximately 100 attoseconds between the emission of photoelectrons that originate from localized core states of the metal, and those that are freed from delocalized conduction-band states. These results illustrate that attosecond metrology constitutes a powerful tool for exploring not only gas-phase systems, but also fundamental electronic processes occurring on the attosecond timescale in condensed-matter systems and on surfaces.

Delay in Photoemission

Defining Time-Zero When a high-energy photon hits an atom and is absorbed, the result can be the excitation and emission of an electron. This photoemission, or photoelectric effect, is generally assumed to occur instantaneously, and represents the definition of “time-zero” in clocking such ultrafast events. Schultze et al. (p. 1658, see the cover; see the Perspective by van der Hart) use ultrafast spectroscopy, with light pulses on the time scale of several tens of attoseconds, to test this assumption directly. They excite neon atoms with 100 eV photons and find that there is a small (20-attosecond) time delay between the emission of electrons from the 2s and 2p orbitals of the atoms. These results should have implications in modeling electron dynamics occurring on ultrafast time scales. Ultrafast metrology reveals a 20-attosecond delay between photoemission from different electronic orbitals in neon atoms. Photoemission from atoms is assumed to occur instantly in response to incident radiation and provides the basis for setting the zero of time in clocking atomic-scale electron motion. We used attosecond metrology to reveal a delay of 21±5 attoseconds in the emission of electrons liberated from the 2p orbitals of neon atoms with respect to those released from the 2s orbital by the same 100–electron volt light pulse. Small differences in the timing of photoemission from different quantum states provide a probe for modeling many-electron dynamics. Theoretical models refined with the help of attosecond timing metrology may provide insight into electron correlations and allow the setting of the zero of time in atomic-scale chronoscopy with a precision of a few attoseconds.

Intense 1.5-cycle near infrared laser waveforms and their use for the generation of ultra-broadband soft-x-ray harmonic continua

We demonstrate sub-millijoule-energy, sub-4?fs-duration near-infrared laser pulses with a controlled waveform comprised of approximately 1.5 optical cycles within the full-width at half-maximum (FWHM) of their temporal intensity profile. We further demonstrate the utility of these pulses for producing high-order harmonic continua of unprecedented bandwidth at photon energies around 100?eV. Ultra-broadband coherent continua extending from 90?eV to more than 130?eV with smooth spectral intensity distributions that exhibit dramatic, never-before-observed sensitivity to the carrier-envelope offset (CEO) phase of the driver laser pulse were generated. These results suggest the feasibility of sub-100-attosecond XUV pulse generation for attosecond spectroscopy in the 100?eV range, and of a simple yet highly sensitive on-line CEO phase detector with sub-50-ms response time.

Femtosecond x-ray pulse length characterization at the Linac Coherent Light Source free-electron laser

Two-color, single-shot time-of-flight electron spectroscopy of atomic neon was employed at the Linac Coherent Light Source (LCLS) to measure laser-assisted Auger decay in the x-ray regime. This x-ray-optical cross-correlation technique provides a straightforward, non-invasive and on-line means of determining the duration of femtosecond (>40?fs) x-ray pulses. In combination with a theoretical model of the process based on the soft-photon approximation, we were able to obtain the LCLS pulse duration and to extract a mean value of the temporal jitter between the optical pulses from a synchronized Ti-sapphire laser and x-ray pulses from the LCLS. We find that the experimentally determined values are systematically smaller than the length of the electron bunches. Nominal electron pulse durations of 175 and 75?fs, as provided by the LCLS control system, yield x-ray pulse shapes of 120?20?fs full-width at half-maximum (FWHM) and an upper limit of 40?20?fs FWHM, respectively. Simulations of the free-electron laser agree well with the experimental results.

Transient Strain Driven by a Dense Electron-Hole Plasma

We measure transient strain in ultrafast laser-excited Ge by time-resolved x-ray anomalous transmission. The development of the coherent strain pulse is dominated by rapid ambipolar diffusion. This pulse extends considerably longer than the laser penetration depth because the plasma initially propagates faster than the acoustic modes. X-ray diffraction simulations are in agreement with the observed dynamics.

Adaptive dispersion compensation for remote fiber delivery of near-infrared femtosecond pulses.

We report on remote delivery of 25-pJ broadband near-infrared femtosecond light pulses from a Ti:sapphire laser through 150 m of single-mode optical fiber. Pulse distortion caused by dispersion is overcome with precompensation by adaptive pulse shaping techniques, while nonlinearities are mitigated by use of an SF10 glass rod for the final stage of pulse compression. A near-transform-limited pulse duration of 130 fs was measured after the final compression.

Advanced Dispersive Optics for the VIS-IR Range

We report on two types of dispersive mirrors: ultrabroadband chirped mirrors with reflectivity and dispersion covering 1.5 octaves (and supporting 2.6-fs pulses), and high-dispersive mirrors for kHz Ti:Sa oscillator-amplifier system and Ti:Sa CPO compressors.

Attosecond Time-Resolved Studies of Electron Dynamics on Surfaces

We report on time-resolved experiments to investigate the attosecond dynamics of photoelectrons generated by ultra-short XUV pulses on clean metal surfaces and in well-defined adsorbate-metal interfaces.

Highly dispersive mirrors for Ti:sapphire laser compressors

We report on two types of dispersive mirrors designed for a 3 kHz Ti:Sa oscillator-amplifier system and Ti:Sa CPO compressors. The mirrors have an average group delay dispersion of -400 fs2 for the 3 kHz Femtopower compact Pro system in the range 730-860 nmand -1300 fs2 for the Ti:Sa CPO (770-820 nm). A hybrid prism-mirror compressor was implemented in the 3kHz, lmJ Femtopower system using 18 highly dispersive mirror reflections.

Stronger seed for a multiterawatt few-cycle pulse OPCPA

Summary form only given. Optical parametric chirped pulse amplification is a unique tool for amplification of ultra-broadband pulses to highest energies. In this this paper, we implement a stronger seed source which delivers muJ -level seed pulses with excellent temporal contrast. A 1 kHz, 1 mJ Ti:sapphire amplifier is used as front-end. The output pulses of the Ti:sapphire amplifier are broadened in a hollow-core fiber (HCF) obtaining ultra-broadband pulses with 400 muJ energy. A fraction of this output (50 muJ) is used to generate the seed for a broadband OPCPA in the near infrared.