Editor’s note

The past two decades have witnessed great progress in development of ultrashort laser pulse in laser science, often at an unexpected speed. It has found various applications, both theoretical and practical, in the frontiers of science.     

An optical lattice clock

The precision measurement of time and frequency is a prerequisite not only for fundamental science but also for technologies that support broadband communication networks and navigation with global positioning systems (GPS). The SI second is currently realized by the microwave transition of Cs atoms with a fractional uncertainty of 10(-15) (ref. 1). Thanks to the optical frequency comb technique, which established a coherent link between optical and radio frequencies, optical clocks have attracted increasing interest as regards future atomic clocks with superior precision. To date, single trapped ions and ultracold neutral atoms in free fall have shown record high performance that is approaching that of the best Cs fountain clocks. Here we report a different approach, in which atoms trapped in an optical lattice serve as quantum references. The 'optical lattice clock' demonstrates a linewidth one order of magnitude narrower than that observed for neutral-atom optical clocks, and its stability is better than that of single-ion clocks. The transition frequency for the Sr lattice clock is 429,228,004,229,952(15) Hz, as determined by an optical frequency comb referenced to the SI second.     

Molecular fingerprinting with the resolved modes of a femtosecond laser frequency comb

The control of the broadband frequency comb emitted from a mode-locked femtosecond laser has permitted a wide range of scientific and technological advances--ranging from the counting of optical cycles for next-generation atomic clocks to measurements of phase-sensitive high-field processes. A unique advantage of the stabilized frequency comb is that it provides, in a single laser beam, about a million optical modes with very narrow linewidths and absolute frequency positions known to better than one part in 10(15) (ref. 5). One important application of this vast array of highly coherent optical fields is precision spectroscopy, in which a large number of modes can be used to map internal atomic energy structure and dynamics. However, an efficient means of simultaneously identifying, addressing and measuring the amplitude or relative phase of individual modes has not existed. Here we use a high-resolution disperser to separate the individual modes of a stabilized frequency comb into a two-dimensional array in the image plane of the spectrometer. We illustrate the power of this technique for high-resolution spectral fingerprinting of molecular iodine vapour, acquiring in a few milliseconds absorption images covering over 6 THz of bandwidth with high frequency resolution. Our technique for direct and parallel accessing of stabilized frequency comb modes could find application in high-bandwidth spread-spectrum communications with increased security, high-resolution coherent quantum control, and arbitrary optical waveform synthesis with control at the optical radian level.     

Nonlinear optics in the extreme ultraviolet

Nonlinear responses to an optical field are universal in nature but have been difficult to observe in the extreme ultraviolet (XUV) and soft X-ray regions owing to a lack of coherent intense light sources. High harmonic generation is a well-known nonlinear optical phenomenon and is now drawing much attention in attosecond pulse generation. For the application of high harmonics to nonlinear optics in the XUV and soft X-ray regime, optical pulses should have both large pulse energy and short pulse duration to achieve a high optical electric field. Here we show the generation of intense isolated pulses from a single harmonic (photon energy 27.9 eV) by using a sub-10-femtosecond blue laser pulse, producing a large dipole moment at the relatively low (ninth) harmonic order nonadiabatically. The XUV pulses with pulse durations of 950 attoseconds and 1.3 femtoseconds were characterized by an autocorrelation technique, based on two-photon above-threshold ionization of helium atoms. Because of the small cross-section for above-threshold ionization, such an autocorrelation measurement of XUV pulses with photon energy larger than the ionization energy of helium has not hitherto been demonstrated. The technique can be extended to the characterization of higher harmonics at shorter wavelengths.     

Direct frequency comb spectroscopy in the extreme ultraviolet

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. 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. 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 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, experimental tests of bound-state and many-body quantum electrodynamics in singly ionized helium and neutral helium, the development of next-generation 'nuclear' clocks and searches for variation of fundamental constants using the enhanced sensitivity of highly charged ions.     

光波干涉采样示波器

光频梳技术是本世纪初随着飞秒激光技术、非线性光学的飞速发展应运而起的一项重要的精密频率测量技术.它跨越了射频和光频电磁波谱之间长期存在的技术鸿沟,通过频率和相位的相干关系将二者巧妙的衔接,在时间频率标准、精密光谱计量以及基础物理学常数的高精度测量等领域具有举足轻重的应用价值.正因为The-odor W.H?nsch(本文第一作者)和John L.Hall以光频梳技术为代表的激光精密测量技术领域的杰出贡献,二人同Roy J.Glauber(光相干量子理论的贡献)共同分享了2005年诺贝尔物理学奖.从光频梳的基本原理出发,解释了光频梳技术基本概念,稳定工作的光频梳以及作为高精密的频率测量技术,光频梳主要的应用领域等.同时回顾了作者研发光频梳技术的初衷,即用于研究氢原子的精密光谱,验证量子电动力学理论,提高里德堡常数和质子电荷半径等物理学基本常数体系的测量精度.介绍了通过双光频梳实现高精密的光谱直接测量技术,包括该技术的原理以及在气体分子精密光谱测量方面的应用,举例说明了基于双光频梳的光谱直接测量技术在频率分辨率和灵敏度方面相对于传统光频梳表现出来的显著优势.实验验证了单光子水平的光频梳光谱测量可行性,指出其在极紫外或甚至在软x射线这些产生少量光子的应用领域的应用前景.最后介绍了微小区域实现厘米级尺寸的光学腔的脉冲激光的激发、片上稳定的双光频梳实现等微型光频梳和片上光谱系统集成等关键技术和解决方案,并分析了片上光频梳光谱测量系统的发展和应用前景.     

Optical frequency comb generation from a monolithic microresonator

Optical frequency combs provide equidistant frequency markers in the infrared, visible and ultraviolet, and can be used to link an unknown optical frequency to a radio or microwave frequency reference. Since their inception, frequency combs have triggered substantial advances in optical frequency metrology and precision measurements and in applications such as broadband laser-based gas sensing and molecular fingerprinting. Early work generated frequency combs by intra-cavity phase modulation; subsequently, frequency combs have been generated using the comb-like mode structure of mode-locked lasers, whose repetition rate and carrier envelope phase can be stabilized. Here we report a substantially different approach to comb generation, in which equally spaced frequency markers are produced by the interaction between a continuous-wave pump laser of a known frequency with the modes of a monolithic ultra-high-Q microresonator via the Kerr nonlinearity. The intrinsically broadband nature of parametric gain makes it possible to generate discrete comb modes over a 500-nm-wide span (approximately 70 THz) around 1,550 nm without relying on any external spectral broadening. Optical-heterodyne-based measurements reveal that cascaded parametric interactions give rise to an optical frequency comb, overcoming passive cavity dispersion. The uniformity of the mode spacing has been verified to within a relative experimental precision of 7.3 x 10(-18). In contrast to femtosecond mode-locked lasers, this work represents a step towards a monolithic optical frequency comb generator, allowing considerable reduction in size, complexity and power consumption. Moreover, the approach can operate at previously unattainable repetition rates, exceeding 100 GHz, which are useful in applications where access to individual comb modes is required, such as optical waveform synthesis, high capacity telecommunications or astrophysical spectrometer calibration.     

Control of the carrier-envelope phases of a synchronously pumped femtosecond optical parametric oscillator and its applications

The intrinsic synchronization, multi-color outputs and related carrier-envelope phases （CEP） among pulses bring advantages to synchronously pumped femtosecond optical parametric oscillators and the pumping sources for broadband frequency comb generation and ultrashort waveform coherent syn-thesis. In this paper, we discuss our latest research results in this field, which cover the following as-pects： the phase relationship and energy conservation law in an OPO and related experimental verifi-cation; control of the pumping Ti-sapphire femtosecond laser＇s CEP by self-referencing technology, and its repetition-rate locking by piezoelectric transducer （PZT）; CEP locking of the pulses from the OPO by beating the non-phase-matched visible outputs against pump supercontinuum to obtain a driving signal for a fast PZT on the OPO end mirror; the generation of a broadband frequency comb spanning from 400 nm to 2.4 μm with 1.2 kHz bandwidth; and the realization of coherent interference between phase controlled pump pulses and signal second harmonic pulses.     

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.     

Direct observation of electron dynamics in the attosecond domain

Dynamical processes are commonly investigated using laser pump-probe experiments, with a pump pulse exciting the system of interest and a second probe pulse tracking its temporal evolution as a function of the delay between the pulses. Because the time resolution attainable in such experiments depends on the temporal definition of the laser pulses, pulse compression to 200 attoseconds (1 as = 10(-18) s) is a promising recent development. These ultrafast pulses have been fully characterized, and used to directly measure light waves and electronic relaxation in free atoms. But attosecond pulses can only be realized in the extreme ultraviolet and X-ray regime; in contrast, the optical laser pulses typically used for experiments on complex systems last several femtoseconds (1 fs = 10(-15) s). Here we monitor the dynamics of ultrafast electron transfer--a process important in photo- and electrochemistry and used in solid-state solar cells, molecular electronics and single-electron devices--on attosecond timescales using core-hole spectroscopy. We push the method, which uses the lifetime of a core electron hole as an internal reference clock for following dynamic processes, into the attosecond regime by focusing on short-lived holes with initial and final states in the same electronic shell. This allows us to show that electron transfer from an adsorbed sulphur atom to a ruthenium surface proceeds in about 320 as.     

Optical frequency metrology

Extremely narrow optical resonances in cold atoms or single trapped ions can be measured with high resolution. A laser locked to such a narrow optical resonance could serve as a highly stable oscillator for an all-optical atomic clock. However, until recently there was no reliable clockwork mechanism that could count optical frequencies of hundreds of terahertz. Techniques using femtosecond-laser frequency combs, developed within the past few years, have solved this problem. The ability to count optical oscillations of more than 1015 cycles per second facilitates high-precision optical spectroscopy, and has led to the construction of an all-optical atomic clock that is expected eventually to outperform today's state-of-the-art caesium clocks.     

Ultrafast non-thermal control of magnetization by instantaneous photomagnetic pulses

The demand for ever-increasing density of information storage and speed of manipulation has triggered an intense search for ways to control the magnetization of a medium by means other than magnetic fields. Recent experiments on laser-induced demagnetization and spin reorientation use ultrafast lasers as a means to manipulate magnetization, accessing timescales of a picosecond or less. However, in all these cases the observed magnetic excitation is the result of optical absorption followed by a rapid temperature increase. This thermal origin of spin excitation considerably limits potential applications because the repetition frequency is limited by the cooling time. Here we demonstrate that circularly polarized femtosecond laser pulses can be used to non-thermally excite and coherently control the spin dynamics in magnets by way of the inverse Faraday effect. Such a photomagnetic interaction is instantaneous and is limited in time by the pulse width (approximately 200 fs in our experiment). Our finding thus reveals an alternative mechanism of ultrafast coherent spin control, and offers prospects for applications of ultrafast lasers in magnetic devices.     

Tunable nanowire nonlinear optical probe

One crucial challenge for subwavelength optics has been the development of a tunable source of coherent laser radiation for use in the physical, information and biological sciences that is stable at room temperature and physiological conditions. Current advanced near-field imaging techniques using fibre-optic scattering probes have already achieved spatial resolution down to the 20-nm range. Recently reported far-field approaches for optical microscopy, including stimulated emission depletion, structured illumination, and photoactivated localization microscopy, have enabled impressive, theoretically unlimited spatial resolution of fluorescent biomolecular complexes. Previous work with laser tweezers has suggested that optical traps could be used to create novel spatial probes and sensors. Inorganic nanowires have diameters substantially below the wavelength of visible light and have electronic and optical properties that make them ideal for subwavelength laser and imaging technology. Here we report the development of an electrode-free, continuously tunable coherent visible light source compatible with physiological environments, from individual potassium niobate (KNbO3) nanowires. These wires exhibit efficient second harmonic generation, and act as frequency converters, allowing the local synthesis of a wide range of colours via sum and difference frequency generation. We use this tunable nanometric light source to implement a novel form of subwavelength microscopy, in which an infrared laser is used to optically trap and scan a nanowire over a sample, suggesting a wide range of potential applications in physics, chemistry, materials science and biology.     

Sub-laser-cycle electron pulses for probing molecular dynamics

Experience shows that the ability to make measurements in any new time regime opens new areas of science. Currently, experimental probes for the attosecond time regime (10(-18) 10(-15) s) are being established. The leading approach is the generation of attosecond optical pulses by ionizing atoms with intense laser pulses. This nonlinear process leads to the production of high harmonics during collisions between electrons and the ionized atoms. The underlying mechanism implies control of energetic electrons with attosecond precision. We propose that the electrons themselves can be exploited for ultrafast measurements. We use a 'molecular clock', based on a vibrational wave packet in H(2)(+) to show that distinct bunches of electrons appear during electron ion collisions with high current densities, and durations of about 1 femtosecond (10(-15) s). Furthermore, we use the molecular clock to study the dynamics of non-sequential double ionization.     

Attosecond control of electronic processes by intense light fields

The amplitude and frequency of laser light can be routinely measured and controlled on a femtosecond (10(-15) s) timescale. However, in pulses comprising just a few wave cycles, the amplitude envelope and carrier frequency are not sufficient to characterize and control laser radiation, because evolution of the light field is also influenced by a shift of the carrier wave with respect to the pulse peak. This so-called carrier-envelope phase has been predicted and observed to affect strong-field phenomena, but random shot-to-shot shifts have prevented the reproducible guiding of atomic processes using the electric field of light. Here we report the generation of intense, few-cycle laser pulses with a stable carrier envelope phase that permit the triggering and steering of microscopic motion with an ultimate precision limited only by quantum mechanical uncertainty. Using these reproducible light waveforms, we create light-induced atomic currents in ionized matter; the motion of the electronic wave packets can be controlled on timescales shorter than 250 attoseconds (250 x 10(-18) s). This enables us to control the attosecond temporal structure of coherent soft X-ray emission produced by the atomic currents--these X-ray photons provide a sensitive and intuitive tool for determining the carrier-envelope phase.     

Attosecond control of electrons emitted from a nanoscale metal tip

Attosecond science is based on steering electrons with the electric field of well controlled femtosecond laser pulses. It has led to the generation of extreme-ultraviolet pulses with a duration of less than 100 attoseconds (ref. 3; 1 as = 10(-18) s), to the measurement of intramolecular dynamics (by diffraction of an electron taken from the molecule under scrutiny) and to ultrafast electron holography. All these effects have been observed with atoms or molecules in the gas phase. Electrons liberated from solids by few-cycle laser pulses are also predicted to show a strong light-phase sensitivity, but only very small effects have been observed. Here we report that the spectra of electrons undergoing photoemission from a nanometre-scale tungsten tip show a dependence on the carrier-envelope phase of the laser, with a current modulation of up to 100 per cent. Depending on the carrier-envelope phase, electrons are emitted either from a single sub-500-attosecond interval of the 6-femtosecond laser pulse, or from two such intervals; the latter case leads to spectral interference. We also show that coherent elastic re-scattering of liberated electrons takes place at the metal surface. Owing to field enhancement at the tip, a simple laser oscillator reaches the peak electric field strengths required for attosecond experiments at 100-megahertz repetition rates, rendering complex amplified laser systems dispensable. Practically, this work represents a simple, extremely sensitive carrier-envelope phase sensor, which could be shrunk in volume to about one cubic centimetre. Our results indicate that the attosecond techniques developed with (and for) atoms and molecules can also be used with solids. In particular, we foresee subfemtosecond, subnanometre probing of collective electron dynamics (such as plasmon polaritons) in solid-state systems ranging in scale from mesoscopic solids to clusters and to single protruding atoms.     

What are Exciting in Laser Science

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光频梳技术在微波光子学中的应用

 光频梳是一种具有若干等频率间隔和窄线宽的相干谱线的一种新型光源。本文介绍了国内外电光调制和非线性微腔等光频梳产生技术,并分析了其在微波光子信号生成、变换和接收等方面的应用及前景。     

Frequency Calibration and Stabilization of the Cooling Laser of Ytterbium Lattice Clock with Molecular Iodine Spectroscopy

In order to apply the frequency comparison among the different optical clocks, transportable optical clocks(TOCs) is suggested as a valuable tool. For transportable clocks, the key technique is how to lock the lasers involved in the whole system. In this paper, we carry out a new way to calibrate and lock the second stage cooling laser of the ytterbium lattice clock with molecular iodine spectroscopy. The locking spectral width of 556 nm laser can be narrowed to 195 kHz, which can be used for frequency control and the stabilization of the second stage cooling. So the new method will make the transportable optical clocks more compact and robust in the future.     

Atomic transient recorder

In Bohr's model of the hydrogen atom, the electron takes about 150 attoseconds (1 as = 10(-18) s) to orbit around the proton, defining the characteristic timescale for dynamics in the electronic shell of atoms. Recording atomic transients in real time requires excitation and probing on this scale. The recent observation of single sub-femtosecond (1 fs = 10(-15) s) extreme ultraviolet (XUV) light pulses has stimulated the extension of techniques of femtochemistry into the attosecond regime. Here we demonstrate the generation and measurement of single 250-attosecond XUV pulses. We use these pulses to excite atoms, which in turn emit electrons. An intense, waveform-controlled, few cycle laser pulse obtains 'tomographic images' of the time-momentum distribution of the ejected electrons. Tomographic images of primary (photo)electrons yield accurate information of the duration and frequency sweep of the excitation pulse, whereas the same measurements on secondary (Auger) electrons will provide insight into the relaxation dynamics of the electronic shell following excitation. With the current approximately 750-nm laser probe and approximately 100-eV excitation, our transient recorder is capable of resolving atomic electron dynamics within the Bohr orbit time.