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.

We study the generation of high harmonic radiation by Bloch electrons in a model transparent solid driven by a strong mid-infrared laser field. We solve the single-electron time-dependent Schrödinger equation (TDSE) using a velocity-gauge method [New J. Phys. 15, 013006 (2013)] that is numerically stable as the laser intensity and number of energy bands are increased. The resulting harmonic spectrum exhibits a primary plateau due to the coupling of the valence band to the first conduction band, with a cutoff energy that scales linearly with field strength and laser wavelength. We also find a weaker second plateau due to coupling to higher-lying conduction bands, with a cutoff that is also approximately linear in the field strength. To facilitate the analysis of the time-frequency characteristics of the emitted harmonics, we also solve the TDSE in a time-dependent basis set, the Houston states [Phys. Rev. B 33, 5494 (1986)], which allows us to separate inter-band and intra-band contributions to the time-dependent current. We find that the inter-band and intraband contributions display very different time-frequency characteristics. We show that solutions in these two bases are equivalent under an unitary transformation but that, unlike the velocity gauge method, the Houston state treatment is numerically unstable when more than a few low lying energy bands are used.

Natural nacre, which consists of almost 95 vol % inorganic content (calcium carbonate) and 5 vol % elastic biopolymers, possesses a unique combination of remarkable strength and toughness, [1] which is attributed to its hierarchical nano-/ microscale structure and precise inorganic-organic interface. [2] Inspired by the intrinsic relationship between the structures and the mechanical properties lying in the natural nacre, different types of nacre-like layered nanocomposites have been fabricated with two-dimensional (2D) inorganic additives, including glass flake, [3] alumina flake, [4] graphene oxide, [5] layered double hydroxides, [6] nanoclay, [7] and flattened double-walled carbon nanotubes. [8] Although great progress has been achieved in tensile mechanical properties, [7b,c, 8, 9] in only very rare cases are artificial layered composites with excellent toughness are obtained. [6,10] One of the most important causes is the relatively low interfacial strength between interlayers of artificial nacre. Recently, 2D graphene has attracted much research interest owing to its outstanding electrical, thermal, and mechanical properties, [11] and many graphene-based devices have been fabricated, [12] such as bulk composites, [13] one-dimensional fibers, [14] supercapacitors. [15] As the water-soluble derivative of graphene,

Attosecond transient absorption is one of the promising new techniques being developed to exploit the availability of sub-femtosecond extreme ultraviolet (XUV) pulses to study the dynamics of the electron on its natural time scale. The temporal resolution in a transient absorption setup comes from the control of the relative delay and coherence between pump and probe pulses, while the spectral resolution comes from the characteristic width of the features that are being probed. In this review we focus on transient absorption scenarios where an attosecond pulse of XUV radiation creates a broadband excitation that is subsequently probed by a few cycle infrared (IR) laser. Because the attosecond XUV pulses are locked to the IR field cycle, the exchange of energy in the laser–matter interaction can be studied with unprecedented precision. We focus on the transient absorption by helium atoms of XUV radiation around the first ionization threshold, where we can simultaneoulsy solve the time-dependent Schrödinger equation for the single atom response and the Maxwell wave equation for the collective response of the nonlinear medium. We use a time-domain method that allows us to treat on an equal footing all the different linear and nonlinear processes by which the medium can exchange energy with the fields. We present several simple models, based on a few-level system interacting with a strong IR field, to explain many of the novel features found in attosecond transient absorption spectrograms. These include the presence of light-induced states, which demonstrate the ability to probe the dressed states of the atom. We also present a time-domain interpretation of the resonant pulse propagation features that appear in absorption spectra in dense, macroscopic media. We close by reviewing several recent experimental results that can be explained in terms of the models we discuss. Our aim is to present a road map for understanding future attosecond transient absorption experiments in more complex systems.

Laser-dressed absorption in atomic helium is studied, both theoretically and experimentally, by transient absorption spectroscopy using isolated 400-as pulses centered at 22 eV and 12-fs near-infrared (NIR) pulses with 780-nm central wavelength. Multiple features in the helium singly excited bound-state spectrum are observed only when the NIR and attosecond pulses are overlapped in time. Theoretical analysis indicates that these light-induced structures (LISs) are the intermediate states in resonant, second-order processes that transfer population to multiple dipole forbidden states. The use of broadband, coherent extreme ultraviolet (XUV) radiation allows observation of these LISs without specifically tuning to a two-photon resonance, as would be required with narrowband XUV light. The strength and position of the LISs depend strongly on the NIR intensity and the pump-probe delay.