4. Survey of Novel Multiphoton Active Materials 1257 4.1. Multiphoton Absorbing Systems 1257 4.2. Organic Molecules 1257 4.3. Organic Liquids and Liquid Crystals 1259 4.4. Conjugated Polymers 1259 4.4.1. Polydiacetylenes 1261 4.4.2. Polyphenylenevinylenes (PPVs) 1261 4.4.3. Polythiophenes 1263 4.4.4. Other Conjugated Polymers 1265 4.4.5. Dendrimers 1265 4.4.6. Hyperbranched Polymers 1267 4.5. Fullerenes 1267 4.6. Coordination and Organometallic Compounds 1271 4.6.1. Metal Dithiolenes 1271 4.6.2. Pyridine-Based Multidentate Ligands 1272 4.6.3. Other Transition-Metal Complexes 1273 4.6.4. Lanthanide Complexes 1275 4.6.5. Ferrocene Derivatives 1275 4.6.6. Alkynylruthenium Complexes 1279 4.6.7. Platinum Acetylides 1279 4.7. Porphyrins and Metallophophyrins 1279 4.8. Nanoparticles 1281 4.9. Biomolecules and Derivatives 1282 5. Nonlinear Optical Characterizations of Multiphoton Active Materials 1282

Multiphoton Absorbing Materials : Molecular Designs, Characterizations, and Applications

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

Gigaelectron volt (GeV) electron accelerators are essential to synchrotron radiation facilities and free-electron lasers, and as modules for high-energy particle physics. Radiofrequency-based accelerators are limited to relatively low accelerating fields (10–50 MV m−1), requiring tens to hundreds of metres to reach the multi-GeV beam energies needed to drive radiation sources, and many kilometres to generate particle energies of interest to high-energy physics. Laser-wakefield accelerators1,2 produce electric fields of the order 10–100 GV m−1 enabling compact devices. Previously, the required laser intensity was not maintained over the distance needed to reach GeV energies, and hence acceleration was limited to the 100 MeV scale3,4,5. Contrary to predictions that petawatt-class lasers would be needed to reach GeV energies6,7, here we demonstrate production of a high-quality electron beam with 1 GeV energy by channelling a 40 TW peak-power laser pulse in a 3.3-cm-long gas-filled capillary discharge waveguide8,9.

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GeV electron beams from a centimetre-scale accelerator

The advent of ultraintense laser pulses generated by the technique of chirped pulse amplification (CPA) along with the development of high-fluence laser materials has opened up an entirely new field of optics. The electromagnetic field intensities produced by these techniques, in excess of ${10}^{18}\phantom{\rule{0.3em}{0ex}}\mathrm{W}∕{\mathrm{cm}}^{2}$, lead to relativistic electron motion in the laser field. The CPA method is reviewed and the future growth of laser technique is discussed, including the prospect of generating the ultimate power of a zettawatt. A number of consequences of relativistic-strength optical fields are surveyed. In contrast to the nonrelativistic regime, these laser fields are capable of moving matter more effectively, including motion in the direction of laser propagation. One of the consequences of this is wakefield generation, a relativistic version of optical rectification, in which longitudinal field effects could be as large as the transverse ones. In addition to this, other effects may occur, including relativistic focusing, relativistic transparency, nonlinear modulation and multiple harmonic generation, and strong coupling to matter and other fields (such as high-frequency radiation). A proper utilization of these phenomena and effects leads to the new technology of relativistic engineering, in which light-matter interactions in the relativistic regime drives the development of laser-driven accelerator science. A number of significant applications are reviewed, including the fast ignition of an inertially confined fusion target by short-pulsed laser energy and potential sources of energetic particles (electrons, protons, other ions, positrons, pions, etc.). The coupling of an intense laser field to matter also has implications for the study of the highest energies in astrophysics, such as ultrahigh-energy cosmic rays, with energies in excess of ${10}^{20}\phantom{\rule{0.3em}{0ex}}\mathrm{eV}$. The laser fields can be so intense as to make the accelerating field large enough for general relativistic effects (via the equivalence principle) to be examined in the laboratory. It will also enable one to access the nonlinear regime of quantum electrodynamics, where the effects of radiative damping are no longer negligible. Furthermore, when the fields are close to the Schwinger value, the vacuum can behave like a nonlinear medium in much the same way as ordinary dielectric matter expanded to laser radiation in the early days of laser research.

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Optics in the relativistic regime

The field of laser-matter interaction traditionally deals with the response of atoms, molecules, and plasmas to an external light wave. However, the recent sustained technological progress is opening up the possibility of employing intense laser radiation to trigger or substantially influence physical processes beyond atomic-physics energy scales. Available optical laser intensities exceeding ${10}^{22}\text{ }\text{ }\mathrm{W}/{\mathrm{cm}}^{2}$ can push the fundamental light-electron interaction to the extreme limit where radiation-reaction effects dominate the electron dynamics, can shed light on the structure of the quantum vacuum, and can trigger the creation of particles such as electrons, muons, and pions and their corresponding antiparticles. Also, novel sources of intense coherent high-energy photons and laser-based particle colliders can pave the way to nuclear quantum optics and may even allow for the potential discovery of new particles beyond the standard model. These are the main topics of this article, which is devoted to a review of recent investigations on high-energy processes within the realm of relativistic quantum dynamics, quantum electrodynamics, and nuclear and particle physics, occurring in extremely intense laser fields.

Extremely high-intensity laser interactions with fundamental quantum systems

Novel methods for particle-in-cell simulation of plasma-based amplification using a moving window

Accelerators driven by 10s TW-class lasers can produce electron bunches with femtosecond-scale duration and energy of 100s of MeV. A potential application of such short bunches is high-dose rate radiotherapy, which could transition to FLASH radiotherapy if a sufficiently large dose is delivered in a single shot. Here we present Monte Carlo simulations to study the bunch length evolution of an electron beam propagating in a water phantom. We show that for electron energies above 100 MeV the bunch lengthens to 1–10 ps duration after interaction with a 30 cm long water phantom, both for a collimated and weakly focused geometry. The corresponding dose rates are on the order of 200 Gy/s per primary electron, much higher than in conventional radiotherapy.

Focused beam dosimetry of short VHEE bunches

Temporally modulated optical media are important in both abstract and applied applications, such as spacetime transformation optics, relativistic laser-plasma interactions, and dynamic metamaterials. Here we investigate the behaviour of temporal boundaries, and show that traditional approaches that assume constant dielectric properties, with loss incorporated as an imaginary part, necessarily lead to unphysical solutions. Further, although physically reasonable predictions can be recovered with a narrowband approximation, we show that appropriate models should use materials with a temporal response and dispersive behaviour.

Temporal boundaries in electromagnetic materials

The ion-channel laser (ICL) has been proposed as an alternative to the free-electron laser (FEL), replacing the deflection of electrons by the periodic magnetic field of an undulator with the periodic betatron motion in an ion channel. Ion channels can be generated by passing dense energetic electron bunches or intense laser pulses through plasma. The ICL has potential to replace FELs based on magnetic undulators, leading to very compact coherent X-ray sources. In particular, coupling the ICL with a laser plasma wakefield accelerator would reduce the size of a coherent light source by several orders of magnitude. An important difference between FEL and ICL is the wavelength of transverse oscillations: In the former it is fixed by the undulator period, whereas in the latter it depends on the betatron amplitude, which therefore has to be treated as variable. Even so, the resulting equations for the ICL are formally similar to those for the FEL with space charge taken into account, so that the well-developed formalism for the FEL can be applied. The amplitude dependence leads to additional requirements compared to the FEL, e.g. a small spread of betatron amplitudes. We shall address these requirements and the resulting practical considerations for realizing an ICL, and give parameters for operation at UV fundamental wavelength, with harmonics extending into X-rays.

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Dino A. Jaroszynski

Papers

Novel methods for particle-in-cell simulation of plasma-based amplification using a moving window

Focused beam dosimetry of short VHEE bunches

Temporal boundaries in electromagnetic materials

Practical considerations for the ion channel free-electron laser

Narrow-band operation of FELIX☆