Strong-laser-field physics, non-classical light states and quantum information science.

Strong-laser-field physics is a research direction that relies on the use of high-power lasers and has led to fascinating achievements ranging from relativistic particle acceleration to attosecond science. On the other hand, quantum optics has been built on the use of low photon number sources and has opened the way for groundbreaking discoveries in quantum technology, advancing investigations ranging from fundamental tests of quantum theory to quantum information processing. Despite the tremendous progress, until recently these directions have remained disconnected. This is because the majority of the interactions in the strong-field limit have been successfully described by semi-classical approximations treating the electromagnetic field classically, as there was no need to include the quantum properties of the field to explain the observations. The link between strong-laser-field physics, quantum optics, and quantum information science has been developed in the recent past. Studies based on fully quantized and conditioning approaches have shown that intense laser-matter interactions can be used for the generation of controllable entangled and non-classical light states. These achievements open the way for a vast number of investigations stemming from the symbiosis of strong-laser-field physics, quantum optics, and quantum information science. Here, after an introduction to the fundamentals of these research directions, we report on the recent progress in the fully quantized description of intense laser-matter interaction and the methods that have been developed for the generation of non-classical light states and entangled states. Also, we discuss the future directions of non-classical light engineering using strong laser fields, and the potential applications in ultrafast and quantum information science.

Α 10-gigawatt attosecond source for non-linear XUV optics and XUV-pump-XUV-probe studies.

The quantum mechanical motion of electrons and nuclei in systems spatially confined to the molecular dimensions occurs on the sub-femtosecond to the femtosecond timescales respectively. Consequently, the study of ultrafast electronic and, in specific cases, nuclear dynamics requires the availability of light pulses with attosecond (asec) duration and of sufficient intensity to induce two-photon processes, essential for probing the intrinsic system dynamics. The majority of atoms, molecules and solids absorb in the extreme-ultraviolet (XUV) spectral region, in which the synthesis of the required attosecond pulses is feasible. Therefore, the XUV spectral region optimally serves the study of such ultrafast phenomena. Here, we present a detailed review of the first 10-GW class XUV attosecond source based on laser driven high harmonic generation in rare gases. The pulse energy of this source largely exceeds other laser driven attosecond sources and is comparable to the pulse energy of femtosecond Free-Electron-Laser (FEL) XUV sources. The measured pulse duration in the attosecond pulse train is 650 ± 80 asec. The uniqueness of the combined high intensity and short pulse duration of the source is evidenced in non-linear XUV-optics experiments. It further advances the implementation of XUV-pump-XUV-probe experiments and enables the investigation of strong field effects in the XUV spectral region.

Quantum Optical Signatures in a Strong Laser Pulse after Interaction with Semiconductors.

Electrodynamical processes induced in complex systems like semiconductors by strong electromagnetic fields have traditionally been described using semiclassical approaches. Although these approaches allowed the investigation of ultrafast dynamics in solids culminating in multipetahertz electronics, they do not provide any access to the quantum-optical nature of the interaction, as they treat the driving field classically and unaffected by the interaction. Here, using a full quantum-optical approach, we demonstrate that the subcycle electronic response in a strongly driven semiconductor crystal is imprinted in the quantum state of the driving field resulting in nonclassical light states carrying the information of the interaction. This vital step towards strong-field ultrafast quantum electrodynamics unravels information inaccessible by conventional approaches and leads to the development of a new class of nonclassical light sources.

Next Generation Driver for Attosecond and Laser-plasma Physics.

The observation and manipulation of electron dynamics in matter call for attosecond light pulses, routinely available from high-order harmonic generation driven by few-femtosecond lasers. However, the energy limitation of these lasers supports only weak sources and correspondingly linear attosecond studies. Here we report on an optical parametric synthesizer designed for nonlinear attosecond optics and relativistic laser-plasma physics. This synthesizer uniquely combines ultra-relativistic focused intensities of about 1020 W/cm2 with a pulse duration of sub-two carrier-wave cycles. The coherent combination of two sequentially amplified and complementary spectral ranges yields sub-5-fs pulses with multi-TW peak power. The application of this source allows the generation of a broad spectral continuum at 100-eV photon energy in gases as well as high-order harmonics in relativistic plasmas. Unprecedented spatio-temporal confinement of light now permits the investigation of electric-field-driven electron phenomena in the relativistic regime and ultimately the rise of next-generation intense isolated attosecond sources.

High-order harmonics measured by the photon statistics of the infrared driving-field exiting the atomic medium.

High-order harmonics in the extreme-ultraviolet spectral range, resulting from the strong-field laser-atom interaction, have been used in a broad range of fascinating applications in all states of matter. In the majority of these studies the harmonic generation process is described using semi-classical theories which treat the electromagnetic field of the driving laser pulse classically without taking into account its quantum nature. In addition, for the measurement of the generated harmonics, all the experiments require diagnostics in the extreme-ultraviolet spectral region. Here by treating the driving laser field quantum mechanically we reveal the quantum-optical nature of the high-order harmonic generation process by measuring the photon number distribution of the infrared light exiting the harmonic generation medium. It is found that the high-order harmonics are imprinted in the photon number distribution of the infrared light and can be recorded without the need of a spectrometer in the extreme-ultraviolet.

Polarization shaping of high-order harmonics in laser-aligned molecules.

The present work reports on the generation of short-pulse coherent extreme ultraviolet radiation of controlled polarization. The proposed strategy is based on high-order harmonics generated in pre-aligned molecules. Field-free molecular alignment produced by a short linearly-polarized infrared laser pulse is used to break the isotropy of a gas medium. Driving the aligned molecules by a circularly-polarized infrared pulse allows to transfer the anisotropy of the medium to the polarization of the generated harmonic light. The ellipticity of the latter is controlled by adjusting the angular distribution of the molecules at the time they interact with the driving pulse. Extreme ultraviolet radiation produced with high degree of ellipticity (close to circular) is demonstrated.

Quantum optical signatures in strong-field laser physics: Infrared photon counting in high-order-harmonic generation.

We analytically describe the strong-field light-electron interaction using a quantized coherent laser state with arbitrary photon number. We obtain a light-electron wave function which is a closed-form solution of the time-dependent Schrödinger equation (TDSE). This wave function provides information about the quantum optical features of the interaction not accessible by semi-classical theories. With this approach we can reveal the quantum optical properties of high harmonic generation (HHG) process in gases by measuring the photon statistics of the transmitted infrared (IR) laser radiation. This work can lead to novel experiments in high-resolution spectroscopy in extreme-ultraviolet (XUV) and attosecond science without the need to measure the XUV light, while it can pave the way for the development of intense non-classical light sources.

The ion microscope as a tool for quantitative measurements in the extreme ultraviolet.

We demonstrate a tool for quantitative measurements in the extreme ultraviolet (EUV) spectral region measuring spatially resolved atomic ionization products at the focus of an EUV beam. The ionizing radiation is a comb of the 11(th)-15(th) harmonics of a Ti:Sapphire femtosecond laser beam produced in a Xenon gas jet. The spatial ion distribution at the focus of the harmonics is recorded using an ion microscope. Spatially resolved single- and two-photon ionization products of Argon and Helium are observed. From such ion distributions single- and two-photon generalized cross sections can be extracted by a self-calibrating method. The observation of spatially resolved two-EUV-photon ionization constitutes an initial step towards future single-shot temporal characterization of attosecond pulses.

Few-cycle driven relativistically oscillating plasma mirrors: a source of intense isolated attosecond pulses.

The conditions required for the production of isolated attosecond pulses from relativistically oscillating mirrors (ROM) are investigated numerically and experimentally. In simulations, carrier-envelope-phase-stabilized three-cycle pulses are found to be sufficient to produce isolated attosecond pulses, while two-cycle pulses will predominantly lead to isolated attosecond pulses even in the absence of carrier-envelope stabilization. Using a state-of-the-art laser system delivering three-cycle pulses at multiple-terawatt level, we have generated higher harmonics up to 70 eV photon energy via the ROM mechanism. The observed spectra are in agreement with theoretical expectations and highlight the potential of few-cycle-driven ROM harmonics for intense isolated attosecond pulse generation for performing extreme ultraviolet-pump extreme ultraviolet-probe experiments.

A compact collinear polarization gating scheme for many cycle laser pulses.

We demonstrate the generation of a broadband coherent continuum extreme-ultraviolet (XUV) radiation produced by the interaction of gases with a many-cycle infrared (IR) laser field, utilizing a compact collinear many cycle-polarization gating (CMC-PG) device. The spectral width of the XUV radiation can support isolated pulses of 200 asec duration. The CMC-PG device forms a high energy content ultra-short temporal gate in a many-cycle laser pulse, within which the XUV emission is taking place. The gate width has been measured and is in agreement with the theoretical calculations. The simplicity, the compactness, the long term stability, and the high IR energy output within the gate, make the CMC-PG device an ideal tool for generating energetic isolated attosecond pulses and measure the carrier-envelope phase of a high-power many-cycle laser field.

Tracking autoionizing-wave-packet dynamics at the 1-fs temporal scale.

We present time-resolved studies and Fourier transform spectroscopy of inner-shell excited states undergoing Auger decay and doubly excited autoionizing states, utilizing coherent extreme-ultraviolet (XUV) radiation continua. Series of states spanning a range of ∼4 eV are excited simultaneously. An XUV probe pulse tracks the oscillatory and decaying evolution of the formed wave packet. The Fourier transform of the measured trace reproduces the spectrum of the series. The present work paves the way for ultrabroadband XUV spectroscopy and studies of ultrafast dynamics in all states of matter.

Coherent continuum extreme ultraviolet radiation in the sub-100-nJ range generated by a high-power many-cycle laser field.

High-energy coherent continuum radiation is generated by the interaction of rare gases with a high-power many-cycle laser field, utilizing the interferometric polarization gating technique. A narrow temporal gate is formed in the laser pulse within which the extreme ultraviolet (XUV) emission is restricted. An analytical expression for the gate function is derived. A super-XUV continuum down to 15 nm, broad enough to support synthesis of single pulses of 260 as duration and a few tens of nanojoule energy, has been measured. These results directly challenge the perspectives of single-attosecond pulse XUV-pump-XUV-probe applications.

Spectral phase distribution retrieval through coherent control of harmonic generation.

The temporal intensity distribution of the third harmonic of a Ti:sapphire laser generated in Xe gas is fully reconstructed from its spectral phase and amplitude distributions. The spectral phases are retrieved by cross correlating the fundamental laser frequency field with that of the third harmonic, in a three laser versus one harmonic photon coupling scheme. The third harmonic spectral amplitude distribution is extracted from its field autocorrelation. The measured pulse duration is found to be in agreement with that expected from lowest order perturbation theory both for unstretched and chirped pulses.

Second order autocorrelation of an XUV attosecond pulse train.

Temporal widths of an attosecond (asec) XUV radiation pulse train, formed by the superposition of higher order harmonics, have been recently determined utilizing a 2nd order autocorrelation measurement. An assessment of the validity of the approach, for the broadband XUV radiation of asec pulses, is implemented through ab initio calculations modeling the spectral and temporal response of the two-XUV-photon He ionization detector employed. The measured width of the asec bursts is discussed in terms of the spectral phases of the individual harmonics, as well as in terms of the spatially modulated temporal width of the radiation, and is found in reasonable agreement with the expected duration.

Direct observation of attosecond light bunching.

Temporal probing of a number of fundamental dynamical processes requires intense pulses at femtosecond or even attosecond (1 as = 10(-18) s) timescales. A frequency 'comb' of extreme-ultraviolet odd harmonics can easily be generated in the interaction of subpicosecond laser pulses with rare gases: if the spectral components within this comb possess an appropriate phase relationship to one another, their Fourier synthesis results in an attosecond pulse train. Laser pulses spanning many optical cycles have been used for the production of such light bunching, but in the limit of few-cycle pulses the same process produces isolated attosecond bursts. If these bursts are intense enough to induce a nonlinear process in a target system, they can be used for subfemtosecond pump-probe studies of ultrafast processes. To date, all methods for the quantitative investigation of attosecond light localization and ultrafast dynamics rely on modelling of the cross-correlation process between the extreme-ultraviolet pulses and the fundamental laser field used in their generation. Here we report the direct determination of the temporal characteristics of pulses in the subfemtosecond regime, by measuring the second-order autocorrelation trace of a train of attosecond pulses. The method exhibits distinct capabilities for the characterization and utilization of attosecond pulses for a host of applications in attoscience.

Two-Photon Ionization of He through a Superposition of Higher Harmonics.

We present experimental results and theoretical analysis of two-photon ionization of He by a superposition of the 7th to the 13th harmonic of a Ti:sapphire laser. Solving the time-dependent Schrödinger equation for He in a coherent polychromatic field, the He+ yield is calculated. From this yield the number of He+ ions produced has been estimated and found in reasonable agreement with its measured value. The present results establish the feasibility of a second-order autocorrelation measurement of superposition of harmonics, and thus they represent the precursor towards the direct temporal characterization of attosecond pulse trains.

Femtosecond laser time-of-flight mass spectrometry of labile molecular analytes: laser-desorbed nitro-aromatic molecules.

Femtosecond laser time-of-flight mass spectra of solid samples of trinitrobenzene (TNB), trinitrotoluene (TNT) and trinitrophenol (TNP) have been recorded. Desorption of the solid samples was enacted by the fourth harmonic output (266 nm) of a 5 ns Nd:YAG laser. Subsequent femtosecond post-ionisation of the plume of neutral molecules was achieved using 800 nm laser pulses of 80 fs duration. Mass spectra have been recorded for desorption laser intensities from 2-6 x 10(9) W cm(-2) with ionisation laser intensities between 2 x 10(14) and 6 x 10(15) W cm(-2). Femtosecond laser ionisation has been shown to be capable of generating precursor and characteristic high-mass fragment ions for labile nitro-aromatic molecules commonly used in high-explosive materials. This feature is critical in the future development of femtosecond laser-based analytical instruments that can be used for complex molecular identification and quantitative analysis of environmentally important labile molecules. Furthermore, a comparison of femtosecond post-ionisation mass spectra with standard 70 eV electron impact data has revealed similarities in the spectra and hence the fragmentation processes.

The onset of coulomb explosions in polyatomic molecules

With the development of high intensity femtosecond lasers, the ionisation and dissociation dynamics of molecules has become an area of considerable interest. Using the technique of femtosecond laser mass spectrometry (FLMS), the molecules carbon disulphide, pyrimidine, toluene, cyclohexanone and benzaldehyde are studied with pulse widths of 50 fs in the near infrared (IR) wavelength region (790 nm). Results are presented and contrasted for laser beam intensities around 10(15) and 10(16) W cm(-2). For the lower intensities, the mass spectra yield dominant singly charged parent ions. Additionally, the appearance of doubly charged parent ions is evident for carbon disulphide, toluene and benzaldehyde with envelopes of doubly charged satellite species existing in these local regions. Carbon disulphide also reveals a small triply charged component. Such atomic-like features are thought to be a strong fingerprint of FLMS at these intensities. However, upon increasing the laser intensity to approximately 10(16) W cm(-2), parent ion dominance decreases and the appearance of multiply charged atomic species occurs, particularly carbon. This phenomenon has been attributed to Coulomb explosions in which the fast absorption of many photons may produce transient highly ionised parent species which can subsequently blow apart. Copyright 1999 John Wiley & Sons, Ltd.