Shambhu Ghimire

Femtosecond electronic response of atoms to ultra-intense X-rays

An era of exploring the interactions of high-intensity, hard X-rays with matter has begun with the start-up of a hard-X-ray free-electron laser, the Linac Coherent Light Source (LCLS). Understanding how electrons in matter respond to ultra-intense X-ray radiation is essential for all applications. Here we reveal the nature of the electronic response in a free atom to unprecedented high-intensity, short-wavelength, high-fluence radiation (respectively 1018 W cm−2, 1.5–0.6 nm, ∼105 X-ray photons per Å2). At this fluence, the neon target inevitably changes during the course of a single femtosecond-duration X-ray pulse—by sequentially ejecting electrons—to produce fully-stripped neon through absorption of six photons. Rapid photoejection of inner-shell electrons produces ‘hollow’ atoms and an intensity-induced X-ray transparency. Such transparency, due to the presence of inner-shell vacancies, can be induced in all atomic, molecular and condensed matter systems at high intensity. Quantitative comparison with theory allows us to extract LCLS fluence and pulse duration. Our successful modelling of X-ray/atom interactions using a straightforward rate equation approach augurs favourably for extension to complex systems.

Solid-state harmonics beyond the atomic limit

Strong-field laser excitation of solids can produce extremely nonlinear electronic and optical behaviour. As recently demonstrated, this includes the generation of high harmonics extending into the vacuum-ultraviolet and extreme-ultraviolet regions of the electromagnetic spectrum. High harmonic generation is shown to occur fundamentally differently in solids and in dilute atomic gases. How the microscopic mechanisms in the solid and the gas differ remains a topic of intense debate. Here we report a direct comparison of high harmonic generation in the solid and gas phases of argon and krypton. Owing to the weak van der Waals interaction, rare (noble)-gas solids are a near-ideal medium in which to study the role of high density and periodicity in the generation process. We find that the high harmonic generation spectra from the rare-gas solids exhibit multiple plateaus extending well beyond the atomic limit of the corresponding gas-phase harmonics measured under similar conditions. The appearance of multiple plateaus indicates strong interband couplings involving multiple single-particle bands. We also compare the dependence of the solid and gas harmonic yield on laser ellipticity and find that they are similar, suggesting the importance of electron–hole recollision in these solids. This implies that gas-phase methods such as polarization gating for attosecond pulse generation and orbital tomography could be realized in solids.

Single-cycle Terahertz Pulses with >0.2 V/A Field Amplitudes via Coherent Transition Radiation

We demonstrate terahertz pulses with field amplitudes exceeding 0.2 V/A generated by coherent transition radiation. Femtosecond, relativistic electron bunches generated at the Linac Coherent Light Source are passed through a beryllium foil, and the emitted radiation is characterized as a function of the bunch duration and charge. Broadband pulses centered at a frequency of 10 THz with energies of 140 μJ are measured. These far-below-bandgap pulses drive a nonlinear optical response in a silicon photodiode, with which we perform nonlinear autocorrelations that yield information regarding the terahertz temporal profile. Simulations of the spatiotemporal profile agree well with experimental results.

Strong-field and attosecond physics in solids

We review the status of strong-field and attosecond processes in bulk transparent solids near the Keldysh tunneling limit. For high enough fields and low-frequency excitations, the optical and electronic properties of dielectrics can be transiently and reversibly modified within the applied pulse. In Ghimire et al (2011 Phys. Rev. Lett. 107 167407) non-parabolic band effects were seen in photon-assisted tunneling experiments in ZnO crystals in a strong mid-infrared field. Using the same ZnO crystals, Ghimire et al (2011 Nat. Phys. 7 138–41) reported the first observation of non-pertubative high harmonics, extending well above the bandgap into the vacuum ultraviolet. Recent experiments by Schubert et al (2014 Nat. Photonics 8 119–23) showed a carrier envelope phase dependence in the harmonic spectrum in strong-field 30 THz driven GaSe crystals which is the most direct evidence yet of the role of sub-cycle electron dynamics in solid-state harmonic generation. The harmonic generation mechanism is different from the gas phase owing to the high density and periodicity of the crystal. For example, this results in a linear dependence of the high-energy cutoff with the applied field in contrast to the quadratic dependence in the gas phase. Sub-100 attosecond pulses could become possible if the harmonic spectrum can be extended into the extreme ultraviolet (XUV). Here we report harmonics generated in bulk MgO crystals, extending to ∼26 eV when driven by ∼35 fs, 800 nm pulses focused to a ∼1VA −1 peak field. The fundamental strong-field and attosecond response also leads to Wannier–Stark localization and reversible semimetallization as seen in the sub-optical cycle behavior of XUV absorption and photocurrent experiments on fused silica by Schiffrin et al (2013 Nature 493 70–4) and Schultze et al (2013 Nature 493 75–8). These studies are advancing our understanding of fundamental strong-field and attosecond physics in solids with potential applications for compact coherent short-wavelength sources and ultra-high speed optoelectronics.

Laser waveform control of extreme ultraviolet high harmonics from solids

Solid-state high-harmonic sources offer the possibility of compact, high-repetition-rate attosecond light emitters. However, the time structure of high harmonics must be characterized at the sub-cycle level. We use strong two-cycle laser pulses to directly control the time-dependent nonlinear current in single-crystal MgO, leading to the generation of extreme ultraviolet harmonics. We find that harmonics are delayed with respect to each other, yielding an atto-chirp, the value of which depends on the laser field strength. Our results provide the foundation for attosecond pulse metrology based on solid-state harmonics and a new approach to studying sub-cycle dynamics in solids.

High-harmonic generation in amorphous solids

High-harmonic generation in isolated atoms and molecules has been widely utilized in extreme ultraviolet photonics and attosecond pulse metrology. Recently, high-harmonic generation has been observed in solids, which could lead to important applications such as all-optical methods to image valance charge density and reconstruct electronic band structures, as well as compact extreme ultraviolet light sources. So far these studies are confined to crystalline solids; therefore, decoupling the respective roles of long-range periodicity and high density has been challenging. Here we report the observation of high-harmonic generation from amorphous fused silica. We decouple the role of long-range periodicity by comparing harmonics generated from fused silica and crystalline quartz, which contain the same atomic constituents but differ in long-range periodicity. Our results advance current understanding of the strong-field processes leading to high-harmonic generation in solids with implications for the development of robust and compact extreme ultraviolet light sources.Although higher harmonic generation from solids has become of interest in many fields, its observation is typically limited to crystalline solids. Here, the authors demonstrate that higher harmonics can be generated from amorphous solids.

Scaling of High-Order Harmonic Generation in the Long Wavelength Limit of a Strong Laser Field

The development of intense, ultrashort, table-top lasers operating in the mid-infrared spectral region, offers many new avenues for strong-field physics. Atoms submitted to such radiation allow photoelectrons to acquire huge quiver energies well over an order of magnitude larger than the binding energy of the neutral. Consequently, many interesting phenomena arise. First, wavelength offers a convenient experimental knob to tune the ionization regime by controlling the Keldysh parameter. Second, high harmonic generation depends directly on the quiver energy and can, therefore, be pushed to unprecedented limits. Third, wavelength controls the spectral phase of harmonics, and hence the possibility to improve the generation of pulses in the attosecond regime. The use of long wavelength lasers is critical to studying high-order harmonic generation in condensed phase systems, because they facilitate harmonic generation within the transmission window of the material and increase the damage threshold. We review some of the recent discoveries in long wavelength driven high-order harmonic generation in the case of isolated atoms, bulk crystals, and liquid.

Below gap optical absorption in GaAs driven by intense, single-cycle coherent transition radiation.

Single-cycle terahertz fields generated by coherent transition radiation from a relativistic electron beam are used to study the high field optical response of single crystal GaAs. Large amplitude changes in the sub-band-gap optical absorption are induced and probed dynamically by measuring the absorption of a broad-band optical beam generated by transition radiation from the same electron bunch, providing an absolutely synchronized pump and probe geometry. This modification of the optical properties is consistent with strong-field-induced electroabsorption. These processes are pertinent to a wide range of nonlinear terahertz-driven light-matter interactions anticipated at accelerator-based sources.

High-order harmonic generation in solid argon

We report on the generation of high-order harmonics in bulk solid argon at the highest laser intensity of 3 × 10¹³ w/cm² without damage. The measured 7^th and 9^th order harmonics have similar strengths.

High-harmonic generation from an atomically thin semiconductor [Observation of high harmonics from an atomically thin semiconductor]

Observations of high-harmonic generation from a single layer of a transition metal dichalcogenide opens the door to studying strong-field and attosecond phenomena in two-dimensional materials.