Nicholas Karpowicz

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.

Optical-field-induced current in dielectrics

The time it takes to switch on and off electric current determines the rate at which signals can be processed and sampled in modern information technology. Field-effect transistors are able to control currents at frequencies of the order of or higher than 100u2009gigahertz, but electric interconnects may hamper progress towards reaching the terahertz (1012u2009hertz) range. All-optical injection of currents through interfering photoexcitation pathways or photoconductive switching of terahertz transients has made it possible to control electric current on a subpicosecond timescale in semiconductors. Insulators have been deemed unsuitable for both methods, because of the need for either ultraviolet light or strong fields, which induce slow damage or ultrafast breakdown, respectively. Here we report the feasibility of electric signal manipulation in a dielectric. A few-cycle optical waveform reversibly increases—free from breakdown—the a.c. conductivity of amorphous silicon dioxide (fused silica) by more than 18 orders of magnitude within 1u2009femtosecond, allowing electric currents to be driven, directed and switched by the instantaneous light field. Our work opens the way to extending electronic signal processing and high-speed metrology into the petahertz (1015u2009hertz) domain.

Carrier-envelope-phase-stable, 1.2 mJ, 1.5 cycle laser pulses at 2.1 μm

We produce 1.5 cycle (10.5 fs), 1.2 mJ, 3 kHz carrier-envelope-phase-stable pulses at 2.1 μm carrier wavelength, from a three-stage optical parametric chirped-pulse amplifier system, pumped by an optically synchronized 1.6 ps Yb:YAG thin disk laser. A chirped periodically poled lithium niobate crystal is used to generate the ultrabroad spectrum needed for a 1.5 cycle pulse through difference frequency mixing of spectrally broadened pulse from a Ti:sapphire amplifier. It will be an ideal tool for producing isolated attosecond pulses with high photon energies.

Optical attosecond pulses and tracking the nonlinear response of bound electrons.

The time it takes a bound electron to respond to the electromagnetic force of light sets a fundamental speed limit on the dynamic control of matter and electromagnetic signal processing. Time-integrated measurements of the nonlinear refractive index of matter indicate that the nonlinear response of bound electrons to optical fields is not instantaneous; however, a complete spectral characterization of the nonlinear susceptibility tensors—which is essential to deduce the temporal response of a medium to arbitrary driving forces using spectral measurements—has not yet been achieved. With the establishment of attosecond chronoscopy, the impulsive response of positive-energy electrons to electromagnetic fields has been explored through ionization of atoms and solids by an extreme-ultraviolet attosecond pulse or by strong near-infrared fields. However, none of the attosecond studies carried out so far have provided direct access to the nonlinear response of bound electrons. Here we demonstrate that intense optical attosecond pulses synthesized in the visible and nearby spectral ranges allow sub-femtosecond control and metrology of bound-electron dynamics. Vacuum ultraviolet spectra emanating from krypton atoms, exposed to intense waveform-controlled optical attosecond pulses, reveal a finite nonlinear response time of bound electrons of up to 115 attoseconds, which is sensitive to and controllable by the super-octave optical field. Our study could enable new spectroscopies of bound electrons in atomic, molecular or lattice potentials of solids, as well as light-based electronics operating on sub-femtosecond timescales and at petahertz rates.

Attosecond nonlinear polarization and light-matter energy transfer in solids

Electric-field-induced charge separation (polarization) is the most fundamental manifestation of the interaction of light with matter and a phenomenon of great technological relevance. Nonlinear optical polarization produces coherent radiation in spectral ranges inaccessible by lasers and constitutes the key to ultimate-speed signal manipulation. Terahertz techniques have provided experimental access to this important observable up to frequencies of several terahertz. Here we demonstrate that attosecond metrology extends the resolution to petahertz frequencies of visible light. Attosecond polarization spectroscopy allows measurement of the response of the electronic system of silica to strong (more than one volt per ångström) few-cycle optical (about 750u2009nanometres) fields. Our proof-of-concept study provides time-resolved insight into the attosecond nonlinear polarization and the light-matter energy transfer dynamics behind the optical Kerr effect and multi-photon absorption. Timing the nonlinear polarization relative to the driving laser electric field with sub-30-attosecond accuracy yields direct quantitative access to both the reversible and irreversible energy exchange between visible-infrared light and electrons. Quantitative determination of dissipation within a signal manipulation cycle of only a few femtoseconds duration (by measurement and ab initio calculation) reveals the feasibility of dielectric optical switching at clock rates above 100 terahertz. The observed sub-femtosecond rise of energy transfer from the field to the material (for a peak electric field strength exceeding 2.5 volts per ångström) in turn indicates the viability of petahertz-bandwidth metrology with a solid-state device.

Generation of sub-3 fs pulses in the deep ultraviolet

We demonstrate generation and measurement of intense deep-ultraviolet light pulses with a duration of approximately 2.8 fs (FWHM of the intensity envelope) and a wavelength distribution between 230 and 290 nm. They emerge via direct frequency upconversion of sub-4 fs laser pulses of a carrier wavelength of approximately 750 nm focused into an Ne-filled, quasi-static gas cell. Dispersion-free, third-order autocorrelation measurements provide access to their temporal intensity profile.

Attosecond Streaking Enables the Measurement of Quantum Phase

Attosecond streaking, as a measurement technique, was originally conceived as a means to characterize attosecond light pulses, which is a good approximation if the relevant transition matrix elements are approximately constant within the bandwidth of the light pulse. Our analysis of attosecond streaking measurements on systems with a complex response to the photoionizing pulse reveals the relation between the momentum-space wave function of the outgoing electron and the result of conventional retrieval algorithms. This finding enables the measurement of the quantum phase associated with bound-continuum transitions.

Efficient, octave-spanning difference-frequency generation using few-cycle pulses in simple collinear geometry.

We present experimental observations and corresponding numerical simulations illustrating the difference-frequency generation of mid-infrared radiation using few-cycle near-infrared-to-visible pulses, which yields conversion efficiencies above 12% in beta-barium borate crystal. Type I and type II phase-matching are shown to yield qualitatively different intensity-scaling behavior, with the former showing higher overall efficiency, especially with the addition of a zero-order wave plate for modifying the polarization state of the pulse, and the latter having a better stability of the spectrum versus input intensity.

Sub-cycle optical control of current in a semiconductor: from the multiphoton to the tunneling regime

Nonlinear interactions between ultrashort optical waveforms and solids can be used to induce and steer electric current on a femtosecond (fs) timescale, holding promise for electronic signal processing at PHz frequencies [Nature 493, 70 (2013)]. So far, this approach has been limited to insulators, requiring extremely strong peak electric fields and intensities. Here, we show all-optical generation and control of directly measurable electric current in a semiconductor relevant for high-speed and high-power (opto)electronics, gallium nitride (GaN), within an optical cycle and on a timescale shorter than 2 fs, at intensities at least an order of magnitude lower than those required for dielectrics. Our approach opens the door to PHz electronics and metrology, applicable to low-power (non-amplified) laser pulses, and may lead to future applications in semiconductor and photonic integrated circuit technologies.

Soft x-ray excitonics

Consecutive attosecond pulses reveal the dynamics of excitons ensuing from core-electron excitation in silica. A quick glimpse of the x-ray aftermath X-rays pass through your skin to reveal the inner workings below. At the atomic scale, x-rays skip past valence electrons to grab hold of the core electrons closer to the nucleus. Moulet et al. used two successive, extremely short laser pulses (lasting less than a quadrillionth of a second) to initiate and then track this process in a sample of silica. This study uncovered the angular momentum character and relaxation dynamics of the excitons, or electron-hole pairs, ensuing from the x-ray absorption. Science, this issue p. 1134 The dynamic response of excitons in solids is central to modern condensed-phase physics, material sciences, and photonic technologies. However, study and control have hitherto been limited to photon energies lower than the fundamental band gap. Here we report application of attosecond soft x-ray and attosecond optical pulses to study the dynamics of core-excitons at the L2,3 edge of Si in silicon dioxide (SiO2). This attosecond x-ray absorption near-edge spectroscopy (AXANES) technique enables direct probing of the excitons’ quasiparticle character, tracking of their subfemtosecond relaxation, the measurement of excitonic polarizability, and observation of dark core-excitonic states. Direct measurement and control of core-excitons in solids lay the foundation of x-ray excitonics.