J. J. Rocca

Atomic inner-shell X-ray laser at 1.46 nanometres pumped by an X-ray free-electron laser

Since the invention of the laser more than 50 years ago, scientists have striven to achieve amplification on atomic transitions of increasingly shorter wavelength. The introduction of X-ray free-electron lasers makes it possible to pump new atomic X-ray lasers with ultrashort pulse duration, extreme spectral brightness and full temporal coherence. Here we describe the implementation of an X-ray laser in the kiloelectronvolt energy regime, based on atomic population inversion and driven by rapid K-shell photo-ionization using pulses from an X-ray free-electron laser. We established a population inversion of the Kα transition in singly ionized neon at 1.46 nanometres (corresponding to a photon energy of 849 electronvolts) in an elongated plasma column created by irradiation of a gas medium. We observed strong amplified spontaneous emission from the end of the excited plasma. This resulted in femtosecond-duration, high-intensity X-ray pulses of much shorter wavelength and greater brilliance than achieved with previous atomic X-ray lasers. Moreover, this scheme provides greatly increased wavelength stability, monochromaticity and improved temporal coherence by comparison with present-day X-ray free-electron lasers. The atomic X-ray lasers realized here may be useful for high-resolution spectroscopy and nonlinear X-ray studies.

Table-top soft x-ray lasers

This article reviews the progress in the development of practical table-top sources of soft x-ray laser radiation. The field is rapidly approaching the stage at which soft x-ray lasers sufficiently compact to fit onto a normal optical table will be routinely utilized in science and technology. This is the result of recent advances in the amplification of soft x-ray radiation in both compact laser-pumped and discharge-pumped devices. The use of excitation mechanisms that take full advantage of new ultrafast high power optical laser drivers and multiple pulse excitation schemes has resulted in the demonstration of saturated soft x-ray amplification at wavelengths as short as 14 nm using several Joule of laser-pump energy. Moreover, several schemes have demonstrated significant gain with only a fraction of a Joule of laser-pump energy. In addition, the demonstration of saturated table-top soft x-ray lasers pumped by very compact capillary discharges has shattered the notion that discharge-created plasmas are insufficiently uniform to allow for soft x-ray amplification, opening a route for the development of efficient, high average power soft x-ray lasers. Recently, a table-top capillary discharge laser operating at 46.9 nm has produced millijoule-level laser pulses at a repetition rate of several Hz, with a corresponding spatially coherent average power per unit bandwidth comparable to that of a beam line at a third generation synchrotron facility. This review summarizes fundamental and technical aspects of table-top soft x-ray lasers based on the generation of population inversions in plasmas, and discusses the present status of development of specific laser systems.

Generation of millijoule-level soft-x-ray laser pulses at a 4-Hz repetition rate in a highly saturated tabletop capillary discharge amplifier

Laser pulses with energies of as much as 1 mJ were generated at a wavelength of 46.9 nm by single-pass amplification in a 34.5 cm-long Ne-like Ar capillary discharge plasma. The large gain–length product of this plasma column allows for soft-x-ray amplification in a highly saturated regime, resulting in efficient energy extraction. Average laser output pulse energy of 0.88 mJ and peak power of 0.6 MW were obtained at a repetition rate of 4 Hz. With an estimated peak spectral brightness of ?1×1023 photons/(s mm2 mrad2 0.01% bandwidth) this tabletop laser is one of the brightest soft-x-ray sources to date.

Demonstration of a desk-top size high repetition rate soft x-ray laser.

We have demonstrated a new type of high repetition rate 46.9 nm capillary discharge laser that fits on top of a small desk and that it does not require a Marx generator for its excitation. The relatively low voltage required for its operation allows a reduction of nearly one order of magnitude in the size of the pulsed power unit relative to previous capillary discharge lasers. Laser pulses with an energy of ~ 13 microJ are generated at repetition rates up to 12 Hz. About (2-3) x 10 4 laser shots can be generated with a single capillary. This new type of portable laser is an easily accessible source of intense short wavelength laser light for applications.

Extended phase matching of high harmonics driven by mid-infrared light.

We demonstrate that phase-matched frequency upconversion of ultrafast laser light can be extended to shorter wavelengths by using longer driving laser wavelengths. Experimentally, we show that the phase-matching cutoff for harmonic generation in argon increases from 45 to 100 eV when the driving laser wavelength is increased from 0.8 to 1.3 microm. Phase matching is also obtained at higher pressures using a longer-wavelength driving laser, mitigating the unfavorable scaling of the single-atom response. Theoretical calculations suggest that phase-matched high harmonic frequency upconversion driven by mid-infrared pulses could be extended to extremely high photon energies.

Experimental and theoretical study of the reactions between neutral vanadium oxide clusters and ethane, ethylene, and acetylene.

Reactions of neutral vanadium oxide clusters with small hydrocarbons, namely C2H6, C2H4, and C2H2, are investigated by experiment and density functional theory (DFT) calculations. Single photon ionization through extreme ultraviolet (EUV, 46.9 nm, 26.5 eV) and vacuum ultraviolet (VUV, 118 nm, 10.5 eV) lasers is used to detect neutral cluster distributions and reaction products. The most stable vanadium oxide clusters VO2, V2O5, V3O7, V4O10, etc. tend to associate with C2H4 generating products V(m)O(n)C2H4. Oxygen-rich clusters VO3(V2O5)(n=0,1,2...), (e.g., VO3, V3O8, and V5O13) react with C2H4 molecules to cause a cleavage of the C=C bond of C2H4 to produce (V2O5)(n)VO2CH2 clusters. For the reactions of vanadium oxide clusters (V(m)O(n)) with C2H2 molecules, V(m)O(n)C2H2 are assigned as the major products of the association reactions. Additionally, a dehydration reaction for VO3 + C2H2 to produce VO2C2 is also identified. C2H6 molecules are quite stable toward reaction with neutral vanadium oxide clusters. Density functional theory calculations are employed to investigate association reactions for V2O5 + C2H(x). The observed relative reactivity of C2 hydrocarbons toward neutral vanadium oxide clusters is well interpreted by using the DFT calculated binding energies. DFT calculations of the pathways for VO3+C2H4 and VO3+C2H2 reaction systems indicate that the reactions VO3+C2H4 --> VO2CH2 + H2CO and VO3+C2H2 --> VO2C2 + H2O are thermodynamically favorable and overall barrierless at room temperature, in good agreement with the experimental observations.

High numerical aperture tabletop soft x-ray diffraction microscopy with 70-nm resolution.

Light microscopy has greatly advanced our understanding of nature. The achievable resolution, however, is limited by optical wavelengths to ≈200 nm. By using imaging and labeling technologies, resolutions beyond the diffraction limit can be achieved for specialized specimens with techniques such as near-field scanning optical microscopy, stimulated emission depletion microscopy, and photoactivated localization microscopy. Here, we report a versatile soft x-ray diffraction microscope with 70- to 90-nm resolution by using two different tabletop coherent soft x-ray sources—a soft x-ray laser and a high-harmonic source. We also use field curvature correction that allows high numerical aperture imaging and near-diffraction-limited resolution of 1.5λ. A tabletop soft x-ray diffraction microscope should find broad applications in biology, nanoscience, and materials science because of its simple optical design, high resolution, large depth of field, 3D imaging capability, scalability to shorter wavelengths, and ultrafast temporal resolution.

Polarization switching in vertical-cavity surface emitting lasers observed at constant active region temperature

Polarization switching in gain-guided, vertical-cavity, surface-emitting lasers was studied as a function of the active region temperature. We show that polarization switching occurs even when the active region temperature is kept constant during fast pulse low duty cycle operation. This temperature independent polarization switching phenomenon is explained in terms of a recently developed model.

Single-shot extreme ultraviolet laser imaging of nanostructures with wavelength resolution

We have demonstrated near-wavelength resolution microscopy in the extreme ultraviolet. Images of 50 nm diameter nanotubes were obtained with a single ~1 ns duration pulse from a desktop-size 46.9 nm laser. We measured the modulation transfer function of the microscope for three different numerical aperture zone plate objectives, demonstrating that 54 nm half-period structures can be resolved. The combination of near-wavelength spatial resolution and high temporal resolution opens myriad opportunities in imaging, such as the ability to directly investigate dynamics of nanoscale structures.

Sub-38 nm resolution tabletop microscopy with 13 nm wavelength laser light

We have acquired images with a spatial resolution better than 38 nm by using a tabletop microscope that combines 13 nm wavelength light from a high-brightness tabletop laser and Fresnel zone plate optics. These results open a gateway to the development of compact and widely available extreme-ultraviolet imaging tools capable of inspecting samples in a variety of environments with a 15-20 nm spatial resolution and a picosecond time resolution.