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High-harmonic generation (HHG) traditionally combines ~100 near-infrared laser photons to generate bright, phase-matched, extreme ultraviolet beams when the emission from many atoms adds constructively. Here, we show that by guiding a mid-infrared femtosecond laser in a high-pressure gas, ultrahigh harmonics can be generated, up to orders greater than 5000, that emerge as a bright supercontinuum that spans the entire electromagnetic spectrum from the ultraviolet to more than 1.6 kilo-electron volts, allowing, in principle, the generation of pulses as short as 2.5 attoseconds. The multiatmosphere gas pressures required for bright, phase-matched emission also support laser beam self-confinement, further enhancing the x-ray yield. Finally, the x-ray beam exhibits high spatial coherence, even though at high gas density the recolliding electrons responsible for HHG encounter other atoms during the emission process.

Attosecond pulses are central to the investigation of valence- and core-electron dynamics on their natural timescales 1 – 3 . The reproducible generation and characterization of attosecond waveforms has been demonstrated so far only through the process of high-order harmonic generation 4 – 7 . Several methods for shaping attosecond waveforms have been proposed, including the use of metallic filters 8 , 9 , multilayer mirrors 10 and manipulation of the driving field 11 . However, none of these approaches allows the flexible manipulation of the temporal characteristics of the attosecond waveforms, and they suffer from the low conversion efficiency of the high-order harmonic generation process. Free-electron lasers, by contrast, deliver femtosecond, extreme-ultraviolet and X-ray pulses with energies ranging from tens of microjoules to a few millijoules 12 , 13 . Recent experiments have shown that they can generate subfemtosecond spikes, but with temporal characteristics that change shot-to-shot 14 – 16 . Here we report reproducible generation of high-energy (microjoule level) attosecond waveforms using a seeded free-electron laser 17 . We demonstrate amplitude and phase manipulation of the harmonic components of an attosecond pulse train in combination with an approach for its temporal reconstruction. The results presented here open the way to performing attosecond time-resolved experiments with free-electron lasers. Generation of intense attosecond waveforms with independently controllable amplitude and phase is performed by using a seeded free-electron laser.

Molecular electronic states energetically below the highest occupied molecular orbital (HOMO) should contribute to laser-driven high harmonic generation (HHG), but this behavior has not been observed previously. Our measurements of the HHG spectrum of N2 molecules aligned perpendicular to the laser polarization showed a maximum at the rotational half-revival. This feature indicates the influence of electrons occupying the orbital just below the N2 HOMO, referred to as the HOMO-1. Such observations of lower-lying orbitals are essential to understanding subfemtosecond/subangstrom electronic motion in laser-excited molecules.

The series of precisely spaced, sharp spectral lines that form an optical frequency comb is enabling unprecedented measurement capabilities and new applications in a wide range of topics that include precision spectroscopy, atomic clocks, ultracold gases, and molecular fingerprinting. A new optical frequency comb generation principle has emerged that uses parametric frequency conversion in high resonance quality factor (Q) microresonators. This approach provides access to high repetition rates in the range of 10 to 1000 gigahertz through compact, chip-scale integration, permitting an increased number of comb applications, such as in astronomy, microwave photonics, or telecommunications. We review this emerging area and discuss opportunities that it presents for novel technologies as well as for fundamental science.

Achieving on-chip optical signal isolation is a fundamental difficulty in integrated photonics 1 . The need to overcome this difficulty is becoming increasingly urgent, especially with the emergence of silicon nano-photonics 2 , 3 , 4 , which promises to create on-chip optical systems at an unprecedented scale of integration. Until now, there have been no techniques that provide complete on-chip signal isolation using materials or processes that are fundamentally compatible with silicon CMOS processes. Based on the effects of photonic transitions 5 , 6 , we show here that a linear, broadband and non-reciprocal isolation can be accomplished by spatial–temporal refractive index modulations that simultaneously impart frequency and wavevector shifts during the photonic transition process. We further show that a non-reciprocal effect can be accomplished in dynamically modulated micrometre-scale ring-resonator structures. This work demonstrates that on-chip isolation can be accomplished with dynamic photonic structures in standard material systems that are widely used for integrated optoelectronic applications. The realization of a chip-based, broadband optical isolator is of considerable interest for integrated photonics. To date, no technique has been shown to be able to do this using materials and processes that are CMOS-compatible. Now, scientists propose that the use of direction-dependent photonic mode transitions in silicon nanophotonic structures could be the solution.

By coupling a high-power, high-repetition-rate near-infrared frequency comb to a femtosecond optical cavity, a frequency comb operating in the extreme-ultraviolet spectral range has been produced, by high harmonic generation, and provides high-resolution spectroscopy in this spectral region. Precision spectroscopy in the extreme UV Laser-based optical frequency combs, so called because they emit evenly spaced spectral lines, are used in precision spectroscopy and other applications requiring accurate measurements, such as atomic clocks. Efforts to extend this capability to shorter wavelengths in the extreme ultraviolet — which would open up exciting new applications, including searches for variation in fundamental constants — have lacked sufficient power for the purpose until now. Jun Ye and co-workers demonstrate a new approach, using a high-power, high-repetition pulsed infrared laser coupled into an optical cavity, to produce an improved extreme UV comb. In a first precision spectroscopy demonstration, they use direct frequency comb spectroscopy to determine argon and neon atomic transitions with ultra-high precision. The development of the optical frequency comb (a spectrum consisting of a series of evenly spaced lines) has revolutionized metrology and precision spectroscopy owing to its ability to provide a precise and direct link between microwave and optical frequencies 1 , 2 . A further advance in frequency comb technology is the generation of frequency combs in the extreme-ultraviolet spectral range by means of high-harmonic generation in a femtosecond enhancement cavity 3 , 4 . Until now, combs produced by this method have lacked sufficient power for applications, a drawback that has also hampered efforts to observe phase coherence of the high-repetition-rate pulse train produced by high-harmonic generation, which is an extremely nonlinear process. Here we report the generation of extreme-ultraviolet frequency combs, reaching wavelengths of 40 nanometres, by coupling a high-power near-infrared frequency comb 5 to a robust femtosecond enhancement cavity. These combs are powerful enough for us to observe single-photon spectroscopy signals for both an argon transition at 82 nanometres and a neon transition at 63 nanometres, thus confirming the combs’ coherence in the extreme ultraviolet. The absolute frequency of the argon transition has been determined by direct frequency comb spectroscopy. The resolved ten-megahertz linewidth of the transition, which is limited by the temperature of the argon atoms, is unprecedented in this spectral region and places a stringent upper limit on the linewidth of individual comb teeth. Owing to the lack of continuous-wave lasers, extreme-ultraviolet frequency combs are at present the only promising route to extending ultrahigh-precision spectroscopy to the spectral region below 100 nanometres. At such wavelengths there is a wide range of applications, including the spectroscopy of electronic transitions in molecules 6 , experimental tests of bound-state and many-body quantum electrodynamics in singly ionized helium and neutral helium 7 , 8 , 9 , the development of next-generation ‘nuclear’ clocks 10 , 11 , 12 and searches for variation of fundamental constants 13 using the enhanced sensitivity of highly charged ions 14 .

The attosecond time-scale electron-recollision process that underlies high harmonic generation has uncovered extremely rapid electronic dynamics in atoms and diatomics. We showed that high harmonic generation can reveal coupled electronic and nuclear dynamics in polyatomic molecules. By exciting large amplitude vibrations in dinitrogen tetraoxide, we showed that tunnel ionization accesses the ground state of the ion at the outer turning point of the vibration but populates the first excited state at the inner turning point. This state-switching mechanism is manifested as bursts of high harmonic light that is emitted mostly at the outer turning point. Theoretical calculations attribute the large modulation to suppressed emission from the first excited state of the ion. More broadly, these results show that high harmonic generation and strong-field ionization in polyatomic molecules undergoing bonding or configurational changes involve the participation of multiple molecular orbitals.

Temporal cavity solitons are packets of light persisting in a continuously driven nonlinear resonator. They are robust attracting states, readily excited through a phase-insensitive and wavelength-insensitive process. As such, they constitute an ideal support for bits in an optical buffer that would seamlessly combine three critical telecommunication functions, namely all-optical storage, all-optical reshaping and wavelength conversion. Here, with standard silica optical fibres, we report the first experimental observation of temporal cavity solitons. The cavity solitons are 4 ps long and are used to demonstrate storage of a data stream for more than a second. We also observe interactions of close cavity solitons, revealing for our set-up a potential capacity of up to 45,000 bits at 25 Gbit s −1 . More fundamentally, cavity solitons are localized dissipative structures. Therefore, given that silica exhibits a pure instantaneous Kerr nonlinearity, our experiment constitutes one of the simplest examples of self-organization phenomena in nonlinear optics. Using standard silica optical fibres, scientists observe temporal cavity solitons — packets of light persisting in a continuously driven nonlinear resonator. Cavity solitons 4 ps long are reported and used to demonstrate storage of a data stream for more than a second. The findings represent one of the simplest examples of self-organization phenomena in nonlinear optics.

High harmonic emission occurs when an electron, liberated from a molecule by an incident intense laser field, gains energy from the field and recombines with the parent molecular ion. The emission provides a snapshot of the structure and dynamics of the recombining system, encoded in the amplitudes, phases and polarization of the harmonic light. Here we show with CO 2 molecules that high harmonic interferometry can retrieve this structural and dynamic information: by measuring the phases and amplitudes of the harmonic emission, we reveal ‘fingerprints’ of multiple molecular orbitals participating in the process and decode the underlying attosecond multi-electron dynamics, including the dynamics of electron rearrangement upon ionization. These findings establish high harmonic interferometry as an effective approach to resolving multi-electron dynamics with sub-Ångström spatial resolution arising from the de Broglie wavelength of the recombining electron, and attosecond temporal resolution arising from the timescale of the recombination event. Electronic movies: attosecond sight The high harmonic emission that accompanies the recombination of an electron with its parent molecular ion in an intense laser field provides a snapshot of the structure and dynamics of the recombining system. Experiments with CO 2 molecules now show that high harmonic interferometry can retrieve this structural and dynamic information by measuring the phases and amplitudes of the harmonic emission. The resulting 'fingerprints' of the multiple molecular orbitals participating in the process can be used to decode the underlying attosecond multi-electron dynamics, including the dynamics of electron rearrangement upon ionization. The light emitted from the system contains images of moving electrons that can be processed into a movie. These findings establish high harmonic interferometry as an effective approach to resolving multi-electron dynamics with sub-Ångström spatial resolution arising from the de-Broglie wavelength of the recombining electron, and attosecond temporal resolution arising from the timescale of the recombination event. The high harmonic emission that accompanies the recombination of an electron with its parent molecular ion in an intense laser field provides a snapshot of the structure and dynamics of the recombining system. Experiments on CO 2 molecules now show how to extract information from the properties of the emitted light about the underlying multi-electron dynamics with sub-Ångström spatial resolution and attosecond temporal resolution

The properties of quantum states have led to the development of new technologies, ranging from quantum information to quantum metrology 1 , 2 , 3 , 4 , 5 , 6 , 7 , 8 , 9 , 10 , 11 , 12 . A recent field of research to emerge is quantum imaging, which aims to overcome the limits of classical imaging by making use of the spatial properties of quantum states of light 13 , 14 , 15 , 16 , 17 , 18 . In particular, quantum correlations between twin beams represent a fundamental resource for these studies 19 , 20 , 21 , 22 , 23 , 24 , 25 , 26 , 27 , 28 , 29 , 30 , 31 , 32 . One of the most interesting proposed schemes takes advantage of the spatial quantum correlations between parametric down-conversion light beams to realize sub-shot-noise imaging of weak absorbing objects 14 , leading ideally to noise-free imaging. Here, we present the first experimental realization of this scheme, showing its potential to achieve a larger signal-to-noise ratio than classical imaging methods. This work represents the starting point for this quantum technology, which we anticipate will have applications when there is a requirement for low-photon-flux illumination (for example for use with biological samples). Sub-shot-noise imaging using spatial quantum correlations between parametric down-conversion light beams is demonstrated. The scheme exhibits a larger signal-to-noise ratio than is possible through classical imaging methods.