Dynamic optical response of solids following 1-fs-scale photoinjection.

Photoinjection of charge carriers profoundly changes the properties of a solid. This manipulation enables ultrafast measurements, such as electric-field sampling1,2, advanced recently to petahertz frequencies3-7, and the real-time study of many-body physics8-13. Nonlinear photoexcitation by a few-cycle laser pulse can be confined to its strongest half-cycle14-16. Describing the associated subcycle optical response, vital for attosecond-scale optoelectronics, is elusive when studied with traditional pump-probe metrology as the dynamics distort any probing field on the timescale of the carrier, rather than that of the envelope. Here we apply field-resolved optical metrology to these dynamics and report the direct observation of the evolving optical properties of silicon and silica during the first few femtoseconds following a near-1-fs carrier injection. We observe that the Drude-Lorentz response forms within several femtoseconds-a time interval much shorter than the inverse plasma frequency. This is in contrast to previous measurements in the terahertz domain8,9 and central to the quest to speed up electron-based signal processing.

Optical Gain in Solids after Ultrafast Strong-Field Excitation.

Multiphoton excitation of a solid by a few-cycle, intense laser pulse forms a very nonequilibrium distribution of charge carriers, where occupation probabilities do not necessarily decrease with energy. Within a fraction of the pulse, significant population inversion can emerge between pairs of valence-band states with a dipole-allowed transition between them. This population inversion leads to stimulated emission in a laser-excited solid at frequencies where the unperturbed solid is transparent. We establish the optimal conditions for observing this kind of strong-field-induced optical gain.

Controlling dielectrics with the electric field of light.

The control of the electric and optical properties of semiconductors with microwave fields forms the basis of modern electronics, information processing and optical communications. The extension of such control to optical frequencies calls for wideband materials such as dielectrics, which require strong electric fields to alter their physical properties. Few-cycle laser pulses permit damage-free exposure of dielectrics to electric fields of several volts per ångström and significant modifications in their electronic system. Fields of such strength and temporal confinement can turn a dielectric from an insulating state to a conducting state within the optical period. However, to extend electric signal control and processing to light frequencies depends on the feasibility of reversing these effects approximately as fast as they can be induced. Here we study the underlying electron processes with sub-femtosecond solid-state spectroscopy, which reveals the feasibility of manipulating the electronic structure and electric polarizability of a dielectric reversibly with the electric field of light. We irradiate a dielectric (fused silica) with a waveform-controlled near-infrared few-cycle light field of several volts per angström and probe changes in extreme-ultraviolet absorptivity and near-infrared reflectivity on a timescale of approximately a hundred attoseconds to a few femtoseconds. The field-induced changes follow, in a highly nonlinear fashion, the turn-on and turn-off behaviour of the driving field, in agreement with the predictions of a quantum mechanical model. The ultrafast reversibility of the effects implies that the physical properties of a dielectric can be controlled with the electric field of light, offering the potential for petahertz-bandwidth signal manipulation.

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 100 gigahertz, but electric interconnects may hamper progress towards reaching the terahertz (10(12) hertz) 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 1 femtosecond, 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 (10(15) hertz) domain.

Strong-Field Resonant Dynamics in Semiconductors.

We predict that a direct band gap semiconductor (GaAs) resonantly excited by a strong ultrashort laser pulse exhibits a novel regime: kicked anharmonic Rabi oscillations. In this regime, Rabi oscillations are strongly coupled to intraband motion, and interband transitions mainly take place when electrons pass near the Brillouin zone center where electron populations undergo very rapid changes. The asymmetry of the residual population distribution induces an electric current controlled by the carrier-envelope phase of the driving pulse. The predicted effects are experimentally observable using photoemission and terahertz spectroscopies.

Real-time observation of valence electron motion.

The superposition of quantum states drives motion on the atomic and subatomic scales, with the energy spacing of the states dictating the speed of the motion. In the case of electrons residing in the outer (valence) shells of atoms and molecules which are separated by electronvolt energies, this means that valence electron motion occurs on a subfemtosecond to few-femtosecond timescale (1 fs = 10(-15) s). In the absence of complete measurements, the motion can be characterized in terms of a complex quantity, the density matrix. Here we report an attosecond pump-probe measurement of the density matrix of valence electrons in atomic krypton ions. We generate the ions with a controlled few-cycle laser field and then probe them through the spectrally resolved absorption of an attosecond extreme-ultraviolet pulse, which allows us to observe in real time the subfemtosecond motion of valence electrons over a multifemtosecond time span. We are able to completely characterize the quantum mechanical electron motion and determine its degree of coherence in the specimen of the ensemble. Although the present study uses a simple, prototypical open system, attosecond transient absorption spectroscopy should be applicable to molecules and solid-state materials to reveal the elementary electron motions that control physical, chemical and biological properties and processes.

25-Year Storage of Human Choroid Plexus in Methyl Salicylate Preserves Its Antigen Immunoreactivity.

OBJECTIVE: Immunohistochemical investigation of archival histological material is a serious problem, since long-term storage of biological tissues, most often in formalin, leads to a loss of antigenic properties. However, the biological material can also be stored in the clearing agent methyl salicylate. The aim of this study was to assess the antigenicity of the human choroid plexus after extra long-term storage in methyl salicylate. MATERIAL AND METHOD: The study was performed on samples of fixed human choroid plexus (occasionally with attached neighboring pineal gland) stored in either methyl salicylate or paraffin blocks for 25 years. Chromogenic and fluorescence immunohistochemistry of vimentin, GFAP, type IV collagen, ß-catenin, α-smooth muscle actin, von Willebrand factor, CD68, mast cell tryptase, TMEM119, and synaptophysin was carried out. RESULTS: The storage of human choroid plexus in methyl salicylate for 25 years does not impair its histomorphology and preserves the properties of all the antigens assessed, which makes their immunohistochemical visualization possible using both light and fluorescence microscopy. Additionally, we found that long-term storage of human choroid plexus in methyl salicylate does not cause an increase in autofluorescence. CONCLUSION: Methyl salicylate can be recommended as a medium for long-term storage of biological tissue, as it provides excellent brain tissue preservation and retains its antigenic properties for up to 25 years.

Ultra-broadband all-optical sampling of optical waveforms.

Optical-field sampling techniques provide direct access to the electric field of visible and near-infrared light. The existing methods achieve the necessary bandwidth using highly nonlinear light-matter interaction that involves ionization of atoms or generation of charge carriers in solids. We demonstrate an alternative, all-optical approach for measuring electric fields of broadband laser pulses, which offers an advantage in terms of sensitivity and signal-to-noise ratio and extends the detection bandwidth of optical methods to the petahertzdomain.

The emergence of macroscopic currents in photoconductive sampling of optical fields.

Photoconductive field sampling enables petahertz-domain optoelectronic applications that advance our understanding of light-matter interaction. Despite the growing importance of ultrafast photoconductive measurements, a rigorous model for connecting the microscopic electron dynamics to the macroscopic external signal is lacking. This has caused conflicting interpretations about the origin of macroscopic currents. Here, we present systematic experimental studies on the signal formation in gas-phase photoconductive sampling. Our theoretical model, based on the Ramo-Shockley-theorem, overcomes the previously introduced artificial separation into dipole and current contributions. Extensive numerical particle-in-cell-type simulations permit a quantitative comparison with experimental results and help to identify the roles of electron-neutral scattering and mean-field charge interactions. The results show that the heuristic models utilized so far are valid only in a limited range and are affected by macroscopic effects. Our approach can aid in the design of more sensitive and more efficient photoconductive devices.

Attosecond dispersion control by extreme ultraviolet multilayer mirrors.

We report the first experimental demonstration of a-periodic multilayer mirrors controlling the frequency sweep (chirp) of isolated attosecond XUV pulses. The concept was proven with about 200-attosecond pulses in the photon energy range of 100-130 eV measured via photoelectron streaking in neon. The demonstrated attosecond dispersion control is engineerable in a wide range of XUV photon energies and bandwidths. The resultant tailor-made attosecond pulses with highly enhanced photon flux are expected to significantly advance attosecond metrology and spectroscopy and broaden their range of applications.

Attosecond optoelectronic field measurement in solids.

The sub-cycle interaction of light and matter is one of the key frontiers of inquiry made accessible by attosecond science. Here, we show that when light excites a pair of charge carriers inside of a solid, the transition probability is strongly localized to instants slightly after the extrema of the electric field. The extreme temporal localization is utilized in a simple electronic circuit to record the waveforms of infrared to ultraviolet light fields. This form of petahertz-bandwidth field metrology gives access to both the modulated transition probability and its temporal offset from the laser field, providing sub-fs temporal precision in reconstructing the sub-cycle electronic response of a solid state structure.

The robustness of attosecond streaking measurements.

We investigate attosecond streaking measurements, where a spectrogram is described by an ensemble of electron wave packets. Such a description may be required for processes more complex than direct photoemission from an isolated atom; an ensemble of wave packets may also be needed to describe the role of shot-to-shot fluctuations or a non-uniform spatio-temporal profile of attosecond light pulses. Under these conditions, we examine the performance of conventional (FROG) analysis of attosecond streaking measurements.

Enhanced phase-matching for generation of soft X-ray harmonics and attosecond pulses in atomic gases.

Focus Serial: Frontiers of Nonlinear Optics

Nanoscopy of Phase Separation in InxGa1-xN Alloys.

Phase separations in ternary/multinary semiconductor alloys is a major challenge that limits optical and electronic internal device efficiency. We have found ubiquitous local phase separation in In1-xGaxN alloys that persists to nanoscale spatial extent by employing high-resolution nanoimaging technique. We lithographically patterned InN/sapphire substrates with nanolayers of In1-xGaxN down to few atomic layers thick that enabled us to calibrate the near-field infrared response of the semiconductor nanolayers as a function of composition and thickness. We also developed an advanced theoretical approach that considers the full geometry of the probe tip and all the sample and substrate layers. Combining experiment and theory, we identified and quantified phase separation in epitaxially grown individual nanoalloys. We found that the scale of the phase separation varies widely from particle to particle ranging from all Ga- to all In-rich regions and covering everything in between. We have found that between 20 and 25% of particles show some level of Ga-rich phase separation over the entire sample region, which is in qualitative agreement with the known phase diagram of In1-xGaxN system.

Atomic-scale diffractive imaging of sub-cycle electron dynamics in condensed matter.

For interaction of light with condensed-matter systems, we show with simulations that ultrafast electron and X-ray diffraction can provide a time-dependent record of charge-density maps with sub-cycle and atomic-scale resolutions. Using graphene as an example material, we predict that diffraction can reveal localised atomic-scale origins of optical and electronic phenomena. In particular, we point out nontrivial relations between microscopic electric current and density in undoped graphene.

Use of electron correlation to make attosecond measurements without attosecond pulses.

We describe how correlations between electrons can be used to trace the dynamics of correlated two-electron ionization with attosecond precision, without using attosecond pulses. The approach is illustrated using the example of Auger or Coster-Kronig decay triggered by photoionization with an extreme ultraviolet pulse. It requires correlated measurements of angle-resolved energy spectra of both the photo- and Auger electrons in the presence of a laser pulse. To reconstruct the dynamics, we use not only classical time and energy correlation, but also entanglement between the two electrons.

Monolithic carrier-envelope phase-stabilization scheme.

A new scheme for stabilizing the carrier-envelope (CE) phase of a few-cycle laser pulse train is demonstrated. Self-phase modulation and difference-frequency generation in a single periodically poled lithium niobate crystal that transmits the main laser beam allows CE phase locking directly in the usable output. The monolithic scheme obviates the need for splitting off a fraction of the laser output for CE phase control, coupling into microstructured fiber, and separation and recombination of spectral components. As a consequence, the output yields 6-fs, 800-nm pulses with an unprecedented degree of short- and long-term reproducibility of the electric field waveform.

High harmonic imaging of few-cycle laser pulses.

We show that the strength of the central electric field peaks in a few-cycle laser pulse can be recovered from a frequency-time image of the high harmonic spectrum generated in a gas volume. Pulse intensity, duration, and also the carrier-envelope phase phi(CE) can be determined. A simple and robust observable is defined that provides a gauge of phi(CE) for pulse durations up to three optical cycles, corresponding to 7.8 fs FWHM at the Ti:sapphire wavelength of 800 nm.