United time-frequency spectroscopy for dynamics and global structure

Ultrashort laser pulses have thus far been used in two distinct modes. In the time domain, the pulses have allowed probing and manipulation of dynamics on a subpicosecond time scale. More recently, phase stabilization has produced optical frequency combs with absolute frequency reference across a broad bandwidth. Here we combine these two applications in a spectroscopic study of rubidium atoms. A wide-bandwidth, phase-stabilized femtosecond laser is used to monitor the real-time dynamic evolution of population transfer. Coherent pulse accumulation and quantum interference effects are observed and well modeled by theory. At the same time, the narrow linewidth of individual comb lines permits a precise and efficient determination of the global energy-level structure, providing a direct connection among the optical, terahertz, and radio-frequency domains. The mechanical action of the optical frequency comb on the atomic sample is explored and controlled, leading to precision spectroscopy with an appreciable reduction in systematic errors.     

Carrier-envelope phase control of femtosecond mode-locked lasers and direct optical frequency synthesis

We stabilized the carrier-envelope phase of the pulses emitted by a femtosecond mode-locked laser by using the powerful tools of frequency-domain laser stabilization. We confirmed control of the pulse-to-pulse carrier-envelope phase using temporal cross correlation. This phase stabilization locks the absolute frequencies emitted by the laser, which we used to perform absolute optical frequency measurements that were directly referenced to a stable microwave clock.     

Measurement of ultrafast phenomena in the femtosecond time domain

Considerable progress has taken place in the generation and application of ultrashort optical pulses. The methods and techniques for extending time-resolved measurements into the femtosecond (10(-15) second) time domain are described, and recent applications and fertile areas for investigation with femtosecond pulses are discussed.     

Parametric Generation of Tunable Light from Continuous-Wave to Femtosecond Pulses

By exploiting nonlinear optical effects, a technology of unprecedented flexibility for the production of tunable coherent light has been developed. Referred to as optical parametric generation, it provides sources with spectral coverage extending all the way from the ultraviolet to the mid-infrared, and with temporal coverage extending over all time domains from the femtosecond pulse to the continuous wave. Such sources generate coherent light of outstanding optical quality and are now finding wide-ranging applications.     

Investigation of ultrafast phenomena in the femtosecond time domain

Rapid progress has taken place in the generation and application of femtosecond optical pulses. The impact of these developments is being felt in a broad range of scientific fields, including physics, chemistry, biology, and engineering. These rapidly evolving techniques have been applied to such diverse problems as phase transitions in highly excited semiconductors, molecular photofragment spectroscopy, impulsive phonon generation in solids, and optical radar ranging through biological tissue.     

Ultrafast optical kerr effect in liquids and solids

In the optical Kerr effect, the electric field of light incident on a transparent sample induces an anisotropic refractive index, which is measured by its effect on the passage of a second light beam. The advent of lasers powerful enough to generate a measurable effect, and which can be pulsed on femtosecond time scales, has made the optical Kerr effect into a practical technology for investigating the molecular structure and interactions of condensed systems such as pure liquids, liquid solutions, and plastic crystals.     

飞秒激光处理对水稻种子发芽和苗期生长的影响

以水稻品种龙稻5号种子为试材,以波长800 nm、光斑半径2 mm、功率650 mw、频率1000 Hz的飞秒激光分别辐照3、5、7、9、11和13 s后,研究飞秒激光辐照处理对水稻种子发芽和苗期生长的影响.结果表明:飞秒激光辐照处理可以刺激水稻发芽和幼苗的生长.3～9 s飞秒激光辐照处理,水稻发芽势和发芽率增高,而随...     

Real-time observation of bimodal proton transfer in acid-base pairs in water

The neutralization reaction between an acid and a base in water, triggered after optical excitation, was studied by femtosecond vibrational spectroscopy. Bimodal dynamics were observed. In hydrogen-bonded acid-base complexes, the proton transfer proceeds extremely fast (within 150 femtoseconds). In encounter pairs formed by diffusion of uncomplexed photoacid and base molecules, the reaction upon contact was an order of magnitude slower, in agreement with earlier reported values. These results call for a refinement of the traditional Eigen-Weller picture of acid-base reactions: A three-stage model is introduced to account for all observed dynamics.     

Single-cycle nonlinear optics

Nonlinear optics plays a central role in the advancement of optical science and laser-based technologies. We report on the confinement of the nonlinear interaction of light with matter to a single wave cycle and demonstrate its utility for time-resolved and strong-field science. The electric field of 3.3-femtosecond, 0.72-micron laser pulses with a controlled and measured waveform ionizes atoms near the crests of the central wave cycle, with ionization being virtually switched off outside this interval. Isolated sub-100-attosecond pulses of extreme ultraviolet light (photon energy approximately 80 electron volts), containing approximately 0.5 nanojoule of energy, emerge from the interaction with a conversion efficiency of approximately 10(-6). These tools enable the study of the precision control of electron motion with light fields and electron-electron interactions with a resolution approaching the atomic unit of time ( approximately 24 attoseconds).     

Femtosecond phase-coherent two-dimensional spectroscopy

Femtosecond phase-coherent two-dimensional (2D) spectroscopy has been experimentally demonstrated as the direct optical analog of 2D nuclear magnetic resonance. An acousto-optic pulse shaper created a collinear three-pulse sequence with well-controlled and variable interpulse delays and phases,which interacted with a model atomic system of rubidium vapor. The desired nonlinear polarization was selected by phase cycling (coadding experimental results obtained with different interpulse phases). This method may enhance our ability to probe the femtosecond structural dynamics of macromolecules.     

Ultrafast hydrogen-bond dynamics in the infrared spectroscopy of water

We investigated rearrangements of the hydrogen-bond network in water by measuring fluctuations in the OH-stretching frequency of HOD in liquid D2O with femtosecond infrared spectroscopy. Using simulations of an atomistic model of water, we relate these frequency fluctuations to intermolecular dynamics. The model reveals that OH frequency shifts arise from changes in the molecular electric field that acts on the proton. At short times, vibrational dephasing reflects an underdamped oscillation of the hydrogen bond with a period of 170 femtoseconds. At longer times, vibrational correlations decay on a 1.2-picosecond time scale because of collective structural reorganizations.     

Phase-coherent optical pulse synthesis from separate femtosecond lasers

We generated a coherently synthesized optical pulse from two independent mode-locked femtosecond lasers, providing a route to extend the coherent bandwidth available for ultrafast science. The two separate lasers (one centered at 760 nanometers wavelength, the other at 810 nanometers) are tightly synchronized and phase-locked. Coherence between the two lasers is demonstrated via spectral interferometry and second-order field cross-correlation. Measurements reveal a coherently synthesized pulse that has a temporally narrower second-order autocorrelation width and that exhibits a larger amplitude than the individual laser outputs. This work represents a new and flexible approach to the synthesis of coherent light.     

Generation of megawatt optical solitons in hollow-core photonic band-gap fibers

The measured dispersion of a low-loss, hollow-core photonic band-gap fiber is anomalous throughout most of the transmission band, and its variation with wavelength is large compared with that of a conventional step-index fiber. For an air-filled fiber, femtosecond self-frequency--shifted fundamental solitons with peak powers greater than 2megawatts can be supported. For Xe-filled fibers, nonfrequency-shifted temporal solitons with peak powers greater than 5.5 megawatts can be generated, representing an increase in the power that can be propagated in an optical fiber of two orders of magnitude. The results demonstrate a unique capability to deliver high-power pulses in a single spatial mode over distances exceeding 200 meters.     

Spatiotemporal coherent control of lattice vibrational waves

We achieved automated optical control over coherent lattice responses that were both time- and position-dependent across macroscopic length scales. In our experiments, spatiotemporal femtosecond pulse shaping was used to generate excitation light fields that were directed toward distinct regions of crystalline samples, producing terahertz-frequency lattice vibrational waves that emanated outward from their multiple origins at lightlike speeds. Interferences among the waves resulted in fully specified far-field responses, including tilted, focusing, or amplified wavefronts. Generation and coherent amplification of terahertz traveling waves and terahertz phased-array generation also were demonstrated.     

The first step in vision: femtosecond isomerization of rhodopsin

The kinetics of the primary event in vision have been resolved with the use of femtosecond optical measurement techniques. The 11-cis retinal prosthetic group of rhodopsin is excited with a 35-femtosecond pump pulse at 500 nanometers, and the transient changes in absorption are measured between 450 and 580 nanometers with a 10-femtosecond probe pulse. Within 200 femtoseconds, an increased absorption is observed between 540 and 580 nanometers, indicating the formation of photoproduct on this time scale. These measurements demonstrate that the first step in vision, the 11-cis----11-trans torsional isomerization of the rhodopsin chromophore, is essentially complete in only 200 femtoseconds.     

Deep-ultraviolet quantum interference metrology with ultrashort laser pulses

Precision spectroscopy at ultraviolet and shorter wavelengths has been hindered by the poor access of narrow-band lasers to that spectral region. We demonstrate high-accuracy quantum interference metrology on atomic transitions with the use of an amplified train of phase-controlled pulses from a femtosecond frequency comb laser. The peak power of these pulses allows for efficient harmonic upconversion, paving the way for extension of frequency comb metrology in atoms and ions to the extreme ultraviolet and soft x-ray spectral regions. A proof-of-principle experiment was performed on a deep-ultraviolet (2 x 212.55 nanometers) two-photon transition in krypton; relative to measurement with single nanosecond laser pulses, the accuracy of the absolute transition frequency and isotope shifts was improved by more than an order of magnitude.     

啁啾和色散对光接收机灵敏度的影响研究

研究了啁啾高斯光脉冲信号对带前置放大器光接收机灵敏度的影响,进行了理论分析和数值摸拟,并以常见的G652A光纤为例研究了啁啾、群速度色散、光信号码元速率和高斯光脉冲信号的占空比对光接收机灵敏度恶化量的影响。研究表明,适当选取高斯光脉冲信号的占空比、啁啾、光接收机均衡滤波器输出的升余弦波形滚降因子的值可以提高光接收机灵敏度;群速度色散存在时,占空比的减小反而导致灵敏度恶化量的增加,说明光信号脉冲宽度并非越小越好。适当选取啁啾、群速度色散的参量β2和风以及占空比的值可以使光接收机灵敏度的恶化量降低。该研究结果对光接收机的分析和设计有一定的指导意义。     

Observing the multiexciton state in singlet fission and ensuing ultrafast multielectron transfer

Multiple exciton generation (MEG) refers to the creation of two or more electron-hole pairs from the absorption of one photon. Although MEG holds great promise, it has proven challenging to implement, and questions remain about the underlying photo-physical dynamics in nanocrystalline as well as molecular media. Using the model system of pentacene/fullerene bilayers and femtosecond nonlinear spectroscopies, we directly observed the multiexciton (ME) state ensuing from singlet fission (a molecular manifestation of MEG) in pentacene. The data suggest that the state exists in coherent superposition with the singlet populated by optical excitation. We also found that multiple electron transfer from the ME state to the fullerene occurs on a subpicosecond time scale, which is one order of magnitude faster than that from the triplet exciton state.     

Real-time observation of the vibration of a single adsorbed molecule

The newly developed femtosecond field emission camera was used to observe the time dependence of field emission through a single copper phthalocyanine molecule adsorbed on a tungsten tip. In many of the individual 212-picosecond-long recordings, the field emission was found to oscillate with a frequency between 5 x 10(10) and 20 x 10(10) hertz. The oscillations, which were not observed from a bare tip, are believed to arise from the vibration of a single molecule with respect to the surface. Numerical simulations confirmed the statistical significance of the data.     

Hertz-level measurement of the optical clock frequency in a single 88Sr+ ion

The frequency of the 5s 2S(1/2)-4d 2D(5/2) electric quadrupole clock transition in a single, trapped, laser-cooled 88Sr+ ion has been measured by using an optical frequency comb referenced to a cesium fountain primary frequency standard. The frequency of the transition is measured as 444,779,044,095,484.6 (1.5) hertz, with a fractional uncertainty within a factor of 3 of that of the cesium standard. Improvements required to obtain a cesium-limited frequency measurement are described and are expected to lead to a 88Sr+ optical clock with stability and reproducibility exceeding that of the primary cesium standard.