X-ray pulses approaching the attosecond frontier

Single soft-x-ray pulses of approximately 90-electron volt (eV) photon energy are produced by high-order harmonic generation with 7-femtosecond (fs), 770-nanometer (1.6 eV) laser pulses and are characterized by photoionizing krypton in the presence of the driver laser pulse. By detecting photoelectrons ejected perpendicularly to the laser polarization, broadening of the photoelectron spectrum due to absorption and emission of laser photons is suppressed, permitting the observation of a laser-induced downshift of the energy spectrum with sub-laser-cycle resolution in a cross correlation measurement. We measure isolated x-ray pulses of 1.8 (+0.7/-1.2) fs in duration, which are shorter than the oscillation cycle of the driving laser light (2.6 fs). Our techniques for generation and measurement offer sub-femtosecond resolution over a wide range of x-ray wavelengths, paving the way to experimental attosecond science. Tracing atomic processes evolving faster than the exciting light field is within reach.     

Steering attosecond electron wave packets with light

Photoelectrons excited by extreme ultraviolet or x-ray photons in the presence of a strong laser field generally suffer a spread of their energies due to the absorption and emission of laser photons. We demonstrate that if the emitted electron wave packet is temporally confined to a small fraction of the oscillation period of the interacting light wave, its energy spectrum can be up- or downshifted by many times the laser photon energy without substantial broadening. The light wave can accelerate or decelerate the electron's drift velocity, i.e., steer the electron wave packet like a classical particle. This capability strictly relies on a sub-femtosecond duration of the ionizing x-ray pulse and on its timing to the phase of the light wave with a similar accuracy, offering a simple and potentially single-shot diagnostic tool for attosecond pump-probe spectroscopy.     

Generation of femtosecond pulses of synchrotron radiation

Femtosecond synchrotron pulses were generated directly from an electron storage ring. An ultrashort laser pulse was used to modulate the energy of electrons within a 100-femtosecond slice of the stored 30-picosecond electron bunch. The energy-modulated electrons were spatially separated from the long bunch and used to generate approximately 300-femtosecond synchrotron pulses at a bend-magnet beamline, with a spectral range from infrared to x-ray wavelengths. The same technique can be used to generate approximately 100-femtosecond x-ray pulses of substantially higher flux and brightness with an undulator. Such synchrotron-based femtosecond x-ray sources offer the possibility of applying x-ray techniques on an ultrafast time scale to investigate structural dynamics in condensed matter.     

Generation of an artificial aurora

On 26 January 1969 an Aerobee 350 rocket was fired from Wallops Island, Virginia, carrying an electron accelerator. Above 230 kilometers the electron guns put out a beam of 0.5 ampere of 10 kev electrons in pulses of 1-second duration aimed downward along the earth's magnetic field lines. The interaction of electron beam with the atmosphere at an altitude of about 100 kilometers generated enough light so that the auroral rays produced could be photographed on the ground by television camera systems.     

Isolated single-cycle attosecond pulses

We generated single-cycle isolated attosecond pulses around approximately 36 electron volts using phase-stabilized 5-femtosecond driving pulses with a modulated polarization state. Using a complete temporal characterization technique, we demonstrated the compression of the generated pulses for as low as 130 attoseconds, corresponding to less than 1.2 optical cycles. Numerical simulations of the generation process show that the carrier-envelope phase of the attosecond pulses is stable. The availability of single-cycle isolated attosecond pulses opens the way to a new regime in ultrafast physics, in which the strong-field electron dynamics in atoms and molecules is driven by the electric field of the attosecond pulses rather than by their intensity profile.     

Melanopsin (Opn4) requirement for normal light-induced circadian phase shifting

The master circadian oscillator in the hypothalamic suprachiasmatic nucleus is entrained to the day/night cycle by retinal photoreceptors. Melanopsin (Opn4), an opsin-based photopigment, is a primary candidate for photoreceptor-mediated entrainment. To investigate the functional role of melanopsin in light resetting of the oscillator, we generated melanopsin-null mice (Opn4-/-). These mice entrain to a light/dark cycle and do not exhibit any overt defect in circadian activity rhythms under constant darkness. However, they display severely attenuated phase resetting in response to brief pulses of monochromatic light, highlighting the critical role of melanopsin in circadian photoentrainment in mammals.     

Nonlinear Optics in Relativistic Plasmas and Laser Wake Field Acceleration of Electrons

When a terawatt-peak-power laser beam is focused into a gas jet, an electron plasma wave, driven by forward Raman scattering, is observed to accelerate a naturally collimated beam of electrons to relativistic energies (up to 10(9) total electrons, with an energy distribution maximizing at 2 megaelectron volts, a transverse emittance as low as 1 millimeter-milliradian, and a field gradient of up to 2 gigaelectron volts per centimeter). Electron acceleration and the appearance of high-frequency modulations in the transmitted light spectrum were both found to have sharp thresholds in laser power and plasma density. A hole in the center of the electron beam may indicate that plasma electrons were expelled radially.     

Efficient multistep photoinitiated electron transfer in a molecular pentad

A synthetic five-part molecular device has been prepared that uses a multistep electron transfer strategy similar to that of photosynthetic organisms to capture light energy and convert it to chemical potential in the form of long-lived charge separation. It consists of two covalently linked porphyrin moieties, one containing a zinc ion (P(Zn)) and the other present as the free base (P). The metailated porphyrin bears a carotenoid polyene (C) and the other a diquinone species (Q(A)-Q(B)). Excitation of the free-base porphyrin in a chloroform solution of the pentad yields an initial charge-separated state, C-P(Zn)-P(.+).-Q(A)(-)-Q(B), with a quantum yield of 0.85. Subsequent electron transfer steps lead to a final charge-separated state, C(.+)-P(Zn)-P-Q(A)-Q(B)(.-), which is formed with an overall quantum yield of 0.83 and has a lifetime of 55 microseconds. Irradiation of the free-base form of the pentad, C-P-P-Q(A)-Q(B), gives a similar charge-separated state with a lower quantum yield (0.15 in dichloromethane), although the lifetime is increased to approximately 340 microseconds. The artificial photosynthetic system preserves a significant fraction ( approximately 1.0 electron volt) of the initial excitation energy (1.9 electron volts) in the long-lived, charge-separated state.     

Coherent control of retinal isomerization in bacteriorhodopsin

Optical control of the primary step of photoisomerization of the retinal molecule in bacteriorhodopsin from the all-trans to the 13-cis state was demonstrated under weak field conditions (where only 1 of 300 retinal molecules absorbs a photon during the excitation cycle) that are relevant to understanding biological processes. By modulating the phases and amplitudes of the spectral components in the photoexcitation pulse, we showed that the absolute quantity of 13-cis retinal formed upon excitation can be enhanced or suppressed by +/-20% of the yield observed using a short transform-limited pulse having the same actinic energy. The shaped pulses were shown to be phase-sensitive at intensities too low to access different higher electronic states, and so these pulses apparently steer the isomerization through constructive and destructive interference effects, a mechanism supported by observed signatures of vibrational coherence. These results show that the wave properties of matter can be observed and even manipulated in a system as large and complex as a protein.     

The simplest double slit: interference and entanglement in double photoionization of H2

The wave nature of particles is rarely observed, in part because of their very short de Broglie wavelengths in most situations. However, even with wavelengths close to the size of their surroundings, the particles couple to their environment (for example, by gravity, Coulomb interaction, or thermal radiation). These couplings shift the wave phases, often in an uncontrolled way, and the resulting decoherence, or loss of phase integrity, is thought to be a main cause of the transition from quantum to classical behavior. How much interaction is needed to induce this transition? Here we show that a photoelectron and two protons form a minimum particle/slit system and that a single additional electron constitutes a minimum environment. Interference fringes observed in the angular distribution of a single electron are lost through its Coulomb interaction with a second electron, though the correlated momenta of the entangled electron pair continue to exhibit quantum interference.     

Attosecond control and measurement: lightwave electronics

Electrons emit light, carry electric current, and bind atoms together to form molecules. Insight into and control of their atomic-scale motion are the key to understanding the functioning of biological systems, developing efficient sources of x-ray light, and speeding up electronics. Capturing and steering this electron motion require attosecond resolution and control, respectively (1 attosecond = 10(-18) seconds). A recent revolution in technology has afforded these capabilities: Controlled light waves can steer electrons inside and around atoms, marking the birth of lightwave electronics. Isolated attosecond pulses, well reproduced and fully characterized, demonstrate the power of the new technology. Controlled few-cycle light waves and synchronized attosecond pulses constitute its key tools. We review the current state of lightwave electronics and highlight some future directions.     

Looking to the future of quantum optics

Light has provided both fundamental phenomenology and enabling technology for scientific discovery for many years, and today it continues to play a central role in fundamental explorations and innovative applications. The ability to manipulate light beams and pulses with the quantum degrees of freedom of optical radiation will add to those advances. The future of quantum optics, which encompasses both the generation and manipulation of nonclassical radiation, as well as its interaction with matter, lies in the rich variety of quantum states that is now becoming feasible to prepare, together with the numerous applications in sensing, imaging, metrology, communications, and information processing that such states enable.     

Picosecond optical switching based on biphotonic excitation of an electron donor-acceptor-donor molecule

An electron donor-acceptor-donor molecule consisting of two porphyrin donors rigidly attached to the two-electron acceptor N,N'-diphenyl-3,4,9,10-perylenebis(dicarboximide) acts as a light intensity-dependent molecular switch on a picosecond time scale. Excitation of the porphyrins within this molecule with subpicosecond laser pulses results in single or double reduction of the acceptor depending on the light intensity. The singly and doubly reduced electron acceptors absorb light strongly at 713 and 546 nanometers, respectively. Because these absorption changes are produced solely by electron transfers, this molecular switch effectively has no moving parts and switches significantly faster than photochromic molecules that must undergo changes in molecular structure.     

HgS/CdS量子线中电子与声子的相互作用

在有限深势阱模型下,求出了考虑到电子-声子相互作用情况下量子线电子基态能、概率分布和禁带宽度,以HgS/CdS量子线为例,研究了电子-声子相互作用对它们的影响.结果表明:电子-声子相互作用会降低电子基态能,在对基态能的影响中以电子与界面光学支声子相互作用的影响最大,而与界面声学支声子相互作用影响最小;电子-声子相互作用的影响和电子由势阱透入有限高势垒的概率以及禁带宽度均随量子导线半径R的减小而增大;电子-声子相互作用不改变禁带宽度随R的变化趋势,仅使其数值减小.     

Harnessing attosecond science in the quest for coherent X-rays

Modern laser technology has revolutionized the sensitivity and precision of spectroscopy by providing coherent light in a spectrum spanning the infrared, visible, and ultraviolet wavelength regimes. However, the generation of shorter-wavelength coherent pulses in the x-ray region has proven much more challenging. The recent emergence of high harmonic generation techniques opens the door to this possibility. Here we review the new science that is enabled by an ability to manipulate and control electrons on attosecond time scales, ranging from new tabletop sources of coherent x-rays to an ability to follow complex electron dynamics in molecules and materials. We also explore the implications of these advances for the future of molecular structural characterization schemes that currently rely so heavily on scattering from incoherent x-ray sources.     

Attosecond synchronization of high-harmonic soft x-rays

Subfemtosecond light pulses can be obtained by superposing several high harmonics of an intense laser pulse. Provided that the harmonics are emitted simultaneously, increasing their number should result in shorter pulses. However, we found that the high harmonics were not synchronized on an attosecond time scale, thus setting a lower limit to the achievable x-ray pulse duration. We showed that the synchronization could be improved considerably by controlling the underlying ultrafast electron dynamics, to provide pulses of 130 attoseconds in duration. We discuss the possibility of achieving even shorter pulses, which would allow us to track fast electron processes in matter.     

Millisecond Pulsar PSR 1937+21: A Highly Stable Clock

The stable rotation and sharp radio pulses of PSR 1937+21 make this pulsar a clock whose long-term frequency stability approaches and may exceed that of the best atomic clocks. Improvements in measurement techniques now permit pulse arrival times to be determined in 1 hour at the Arecibo radio telescope with uncertainties of about 300 nanoseconds relative to atomic time. Measurements taken approximately every 2 weeks since November 1982 yield estimates of fractional frequency stability that continue to improve with increasing averaging time. The pulsar's frequency stability is at least as good as 6 x 10(-14) for averaging times longer than 4 months, and over the longest intervals the measurements appear to be limited by the stability of the reference atomic docks. The data yield a firm upper limit of 7 x 10(-36) gram per cubic centimeter for the energy density of a cosmic background of gravitational radiation at frequencies of about 0.23 cycle per year. This limit corresponds to approximately 4 x 10(-7) of the density required to close the universe.     

Synthesized light transients

Manipulation of electron dynamics calls for electromagnetic forces that can be confined to and controlled over sub-femtosecond time intervals. Tailored transients of light fields can provide these forces. We report on the generation of subcycle field transients spanning the infrared, visible, and ultraviolet frequency regimes with a 1.5-octave three-channel optical field synthesizer and their attosecond sampling. To demonstrate applicability, we field-ionized krypton atoms within a single wave crest and launched a valence-shell electron wavepacket with a well-defined initial phase. Half-cycle field excitation and attosecond probing revealed fine details of atomic-scale electron motion, such as the instantaneous rate of tunneling, the initial charge distribution of a valence-shell wavepacket, the attosecond dynamic shift (instantaneous ac Stark shift) of its energy levels, and its few-femtosecond coherent oscillations.     

不同光强与低温交叉胁迫下黄瓜PSⅠ与PSⅡ的光抑制研究

 【目的】探讨低温胁迫下不同光强对黄瓜光系统Ⅰ（PSⅠ）和光系统II（PSⅡ）的影响以及低温胁迫下两个光系统之间的相互作用机制。【方法】以冷敏感黄瓜品种津春4号为试材,通过同时测定黄瓜叶片叶绿素荧光快速诱导动力学曲线和对820 nm光的吸收曲线,结合叶绿素荧光淬灭分析,探讨了低温（4 ℃）与不同光强（0,100,200,400μmol•m-2•s-1）结合处理对黄瓜PSⅠ和PSⅡ活性的影响。【结果】低温下,随过剩激发能（（1-qP）/NPQ）的增加,PSⅡ最大光化学效率（Fv/Fm）持续下降; 在过剩激发能较低时,PSⅠ活性（△I/Io）也随过剩激发能的增加而明显下降,但是当过剩激发能增加到一定程度时,PSⅠ活性不再随过剩激发能的增加而明显下降。【结论】在低温下,过剩激发能不但能够抑制黄瓜PSⅠ的活性也能抑制PSⅡ的活性,但是当过剩激发能增加到一定程度时,PSⅡ光化学活性的显著下降减少了光合电子向PSⅠ的供应,避免了PSⅠ光抑制的进一步加剧。     

棉花花青素能量耗散过程维持光合机构稳定性分析

【目的】研究棉花花青素能量耗散过程维持光合机构稳定性。【方法】选取花青素含量差异较大的棉花为材料,测定花青素含量、光合色素含量、气体交换参数、叶绿素荧光参数、NDH介导的环式电子流活性、ATP合成酶活性、玉米黄质的合成速率等。【结果】随花青素含量升高,吸光能力逐渐增强,而净光合速率逐渐减弱,将面临较多的过剩激发能;NDH介导的环式电子流活性均逐渐增强,并且环式电子调控的ATP合成也逐渐增强;相对于无花青素的棉花,花青素存在的条件下,叶黄素循环的热耗散明显较弱,并且随花青素含量的增多,叶黄素循环的过程逐渐减弱,可能花青素的耗散能力逐渐增强。【结论】花青素能够作为一种光保护机制起到耗散过剩光能有效保护PSI和PSII。