Phase-matched generation of coherent soft X-rays

Phase-matched harmonic conversion of visible laser light into soft x-rays was demonstrated. The recently developed technique of guided-wave frequency conversion was used to upshift light from 800 nanometers to the range from 17 to 32 nanometers. This process increased the coherent x-ray output by factors of 10(2) to 10(3) compared to the non-phase-matched case. This source uses a small-scale (sub-millijoule) high repetition-rate laser and will enable a wide variety of new experimental investigations in linear and nonlinear x-ray science.     

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.     

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.     

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.     

High-gain harmonic-generation free-electron laser

A high-gain harmonic-generation free-electron laser is demonstrated. Our approach uses a laser-seeded free-electron laser to produce amplified, longitudinally coherent, Fourier transform-limited output at a harmonic of the seed laser. A seed carbon dioxide laser at a wavelength of 10.6 micrometers produced saturated, amplified free-electron laser output at the second-harmonic wavelength, 5.3 micrometers. The experiment verifies the theoretical foundation for the technique and prepares the way for the application of this technique in the vacuum ultraviolet region of the spectrum, with the ultimate goal of extending the approach to provide an intense, highly coherent source of hard x-rays.     

Soft x-ray lasers and their applications

The emerging technology of soft x-ray lasers has novel applications to microscopy, lithography, and other fields. This article describes the status of soft x-ray laser research with the aim of bringing the rapid developments in this field to the attention of potential users in other disciplines. The different techniques for generating a population inversion and producing a soft x-ray laser are reviewed. The status of current research in the field and the near-term prospects are described. It is expected that the range of potential applications of soft x-ray lasers will increase as their performance improves. Work aimed at increasing the output power and progressing to shorter wavelengths with these devices is also reviewed.     

Charge exchange-induced X-ray emission from comet C/1999 S4 (LINEAR)

Using soft x-ray observations of the bright new comet C/1999 S4 (LINEAR) with the Chandra x-ray observatory, we have detected x-ray line emission created by charge exchange between highly ionized solar wind minor ions and neutral gases in the comet's coma. The emission morphology was symmetrically crescent shaped and extended out to 300,000 kilometers from the nucleus. The emission spectrum contains 6 lines at 320, 400, 490, 560, 600, and 670 electron volts, attributable to electron capture and radiative deexcitation by the solar wind species C(+5), C(+6), N(+7), O(+7), and O(+8). A contemporaneous 7-day soft x-ray light curve obtained using the Extreme Ultraviolet Explorer demonstrates a large increase in the comet's emission coincident with a strong solar flare on 14 and 15 July 2000.     

Soft X-ray-driven femtosecond molecular dynamics

The direct observation of molecular dynamics initiated by x-rays has been hindered to date by the lack of bright femtosecond sources of short-wavelength light. We used soft x-ray beams generated by high-harmonic upconversion of a femtosecond laser to photoionize a nitrogen molecule, creating highly excited molecular cations. A strong infrared pulse was then used to probe the ultrafast electronic and nuclear dynamics as the molecule exploded. We found that substantial fragmentation occurs through an electron-shakeup process, in which a second electron is simultaneously excited during the soft x-ray photoionization process. During fragmentation, the molecular potential seen by the electron changes rapidly from nearly spherically symmetric to a two-center molecular potential. Our approach can capture in real time and with angstrom resolution the influence of ionizing radiation on a range of molecular systems, probing dynamics that are inaccessible with the use of other techniques.     

Energy spectra of a number of celestial x-ray sources in the energy range from 2 to 60 kiloelectron volts

The emission of 20 to 60 kev x-rays by an astronomical object in the constellation of Cygnus has been observed with a balloon-borne x-ray telescope flown from Hyderabad, India. The balloon data, used in conjunction with data pertaining to the flux in the wavelength range from 2 to 10 A can be fitted by a power law in photon energy varying as (h(v))-(1.7). The Cygnus object is the brightest object in the sky in the hard x-ray wavelength range and has the hardest spectrum of all observed objects that emit x-rays. The astronomical object should be capable of accelerating protons up to energies of the order of 10(18) electron volts. Upper limits to the hard x-ray fluxes from Sco XR-1, Cyg XR-2, Oph XR-1, and Ser XR-1 are established; it is shown that the Sco XR-1 spectrum is very soft.     

Bright coherent ultrahigh harmonics in the keV x-ray regime from mid-infrared femtosecond lasers

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.     

Two-dimensional x-ray waveguides and point sources

We show that resonant coupling of synchrotron beams into suitable nanostructures can be used for the generation of coherent x-ray point sources. A two-dimensionally confining x-ray waveguide structure has been fabricated by e-beam lithography. By shining a parallel undulator beam onto the structure, a discrete set of resonant modes can be excited in the dielectric cavity, depending on the two orthogonal coupling angles between the beam and the waveguide interfaces. The resonant excitation of the modes is evidenced from the characteristic set of coupling angles as well as the observed far-field pattern. The x-ray nanostructure may be used as coherent x-ray point sources with a beam cross section in the nanometer range.     

Multiphoton ionization of atoms

Studies of multiphoton ionization of atoms have revealed several unexpected characteristics. The confluence of the experimental evidence leads to the hypothesis that the basic character of the atomic response involves highly organized, coherent motions of entire atomic shells. The important regime, for which the radiative field strength is greater than an atomic unit (e/a(2)(0)), can be viewed in approximate correspondence with the physics of fast (approximately 10 MeV per atomic mass unit) atom-atom scattering. This physical picture provides a basis for the expectation that stimulated emission in the x-ray range can be produced by direct, highly nonlinear coupling of ultraviolet radiation to atoms.     

Ultrashort light pulses

Experimental techniques are now available for the generation of repetitive and single coherent optical pulses of extremely short time duration and high peak power. These pulses should find extensive application in basic and applied research. Additional shortening of optical pulse durations can be obtained by means of the stimulated Raman effect, second-harmonic generation, or amplification with nonlinear laser amplifiers.     

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.     

Self-trapping of dark incoherent light beams

"Dark beams" are nonuniform optical beams that contain either a one-dimensional (1D) dark stripe or a two-dimensional (2D) dark hole resulting from a phase singularity or an amplitude depression in their optical field. Thus far, self-trapped dark beams (dark solitons) have been observed using coherent light only. Here, self-trapped dark incoherent light beams (self-trapped dark incoherent wavepackets) were observed. Both dark stripes and dark holes nested in a broad partially spatially incoherent wavefront were self-trapped to form dark solitons in a host photorefractive medium. These self-trapped 1D and 2D dark beams induced refractive-index changes akin to planar and circular dielectric waveguides. The experiments introduce the possibility of controlling high-power coherent laser beams with low-power incoherent light sources such as light emitting diodes.     

Imaging atomic structure and dynamics with ultrafast x-ray scattering

Measuring atomic-resolution images of materials with x-ray photons during chemical reactions or physical transformations resides at the technological forefront of x-ray science. New x-ray-based experimental capabilities have been closely linked with advances in x-ray sources, a trend that will continue with the impending arrival of x-ray-free electron lasers driven by electron accelerators. We discuss recent advances in ultrafast x-ray science and coherent imaging made possible by linear-accelerator-based light sources. These studies highlight the promise of ultrafast x-ray lasers, as well as the technical challenges and potential range of applications that will accompany these transformative x-ray light sources.     

Tunable Coherent X-rays

A modern 1- to 2-billion-electron-volt synchrotron radiation facility (based on high-brightness electron beams and magnetic undulators) would generate coherent (laser-like) soft x-rays of wavelengths as short as 10 angstroms. The radiation would also be broadly tunable and subject to full polarization control. Radiation with these properties could be used for phase- and element-sensitive microprobing of biological assemblies and material interfaces as well as reserch on the production of electronic microstructures with features smaller than 1000 angstroms. These short wavelength capabilities, which extend to the K-absorption edges of carbon, nitrogen, and oxygen, are neither available nor projected for laboratory XUV lasers. Higher energy storage rings (5 to 6 billion electron volts) would generate significantly less coherent radiation and would be further compromised by additional x-ray thermal loading of optical components.     

Flash X-ray Microscopy

Soft x-ray contact microscopy, utilizing single-shot exposures of approximately 60 nanoseconds duration in polymethyl methacrylate, has been realized with a resolution of 300 angstroms. The radiation spectrum is intense in the "window" between 23 and 44 angstroms where water is transparent compared to biological materials, and therefore permits viewing of wet samples.     

Time-reversed lasing and interferometric control of absorption

In the time-reversed counterpart to laser emission, incident coherent optical fields are perfectly absorbed within a resonator that contains a loss medium instead of a gain medium. The incident fields and frequency must coincide with those of the corresponding laser with gain. We demonstrated this effect for two counterpropagating incident fields in a silicon cavity, showing that scattering [corrected] can be modulated [corrected] by two orders of magnitude, the maximum predicted by theory for our experimental setup. In addition, we showed that absorption can be reduced substantially by varying the relative phase of the incident fields. The device, termed a "coherent perfect absorber," functions as an absorptive interferometer, with potential practical applications in integrated optics.     

Interband electronic excitation-assisted atomic-scale restructuring of metal surfaces by nanosecond pulsed laser light

Interaction of high-power laser light with materials often causes irreversible damage of the near-surface region. It is shown that copper single-crystal surfaces can be patterned by laser light. Irradiation with green light produced adatoms and vacancies, which self-organized into nanoscale pyramids. This restructuring can be removed by annealing. In contrast to green light, infrared laser irradiation at equivalent absorbed energy density did not produce any structural change. This, for metallic systems, unforeseen spectral difference in laser light action points to a concerted process as the source for structural modification, which involves long-lived primary excitation of localized d-electrons through interband transition together with phonon excitation.