Characterization of laser-induced ionization dynamics in solid dielectrics
Peter Jürgens, Benjamin Liewehr, Björn Kruse, Christian Peltz, Tobias Witting, Anton Husakou, Arnaud Rouzee, Mikhail Ivanov, Thomas Fennel, Marc. J. J. Vrakking… 展开作者
Peter Jürgens, Benjamin Liewehr, Björn Kruse, Christian Peltz, Tobias Witting, Anton Husakou, Arnaud Rouzee, Mikhail Ivanov, Thomas Fennel, Marc. J. J. Vrakking, Alexandre Mermillod-Blondin
The formation of an electron-hole plasma during the interaction of intense femtosecond laser pulses with transparent solids lies at the heart of femtosecond laser processing. Advanced micro- and nanomachining applications require improved control over the excitation characteristics. Here, we relate the emission of low-order harmonics to the strong laser-field-induced plasma formation. Together with a measurement of the total plasma density we identify the contribution of two competing ionization mechanisms - strong-field and electron-impact ionization.
We develop a new model of laser-matter interaction based on Optical Bloch Equations, which includes photo-ionization, impact ionization, and various relaxation processes typical of dielectric materials. This approach is able to describe the temporal evolution of the electron dynamics in the conduction band driven by few-cycle laser pulses of any wavelength. Moreover, the nonlinear polarization response of both centrosymmetric and non-centrosymmetric materials can be described while ensuring the proper selection rules for the harmonics emission.
In the absence of external excitation, light trapped within a dielectric medium generally decays by leaking out, and also by getting absorbed within the medium. We analyze the leaky modes of solid dielectric spheres by examining solutions of Maxwell's equations for simple homogeneous, isotropic, linearly dispersive media that admit complex-valued oscillation frequencies. We show that, under appropriate circumstances, these leaky modes constitute a complete set into which an initial electromagnetic field distribution inside a dielectric sphere can be expanded. We provide the outline of a comple…
High harmonic generation in solids is becoming an important method for strong field solid state physics research. The power scale relationship between high harmonics and the driving laser is investigated both experimentally and theoretically. Results of the power scale dependence clearly divided the interaction into two regimes. The modification of the bandgap by intense laser proved to be very important for theoretically reproducing the experimental result. Combining with the Keldysh theory analysis, the harmonic generation process is found to be transitioned from multiphoton excitations to t…
The limited resolution of a conventional optical microscope stems from the fact that the subwavelength information of an object is carried by evanescent waves, which exponentially decays in space and cannot reach the imaging plane. We introduce here a metamaterial solid immersion lens (mSIL), which utilizes closely-packed high-index nanoparticles as a composite media to effectively convert and transport evanescent waves from near-field to far-field. About 20% of evanescent wave energy of an ideal point source can be directed into far-field by mSIL. This has led to the exceptional imaging perfo…
Experimental and theoretical studies of laser-induced breakdown in dielectrics provide conflicting conclusions about the possibility to trigger ionization avalanche on the sub-picosecond time scale and the relative importance of carrier-impact ionization over field ionization. On the one hand, current models based on single ionization-rate equations do not account for the gradual heating of the charge carriers which, for short laser pulses, might not be sufficient to start an avalanche. On the other hand, models based on multiple rate equations that track the carriers kinetics rely on several …
The mechanism of ablation of solids by intense femtosecond laser pulses is described in an explicit analytical form. It is shown that at high intensities when the ionization of the target material is complete before the end of the pulse, the ablation mechanism is the same for both metals and dielectrics. The physics of this new ablation regime involves ion acceleration in the electrostatic field caused by charge separation created by energetic electrons escaping from the target. The formulae for ablation thresholds and ablation rates for metals and dielectrics, combining the laser and target p…
The use of relatively simple structures to achieve high performance refractive index sensors has always been urgently needed. In this work, we propose a lithography-free sensing platform based on metal-dielectric cavity, the sensitivity of our device can reach 1456700 nm/RIU for solution and 1596700 nm/RIU for solid material, and the FOM can be up to 1234500 /RIU for solution and 1900800 /RIU for solid material, which both are much higher than most sensing methods. This sensor has excellent sensing performance in both TE and TM light, and suitable for integrated microfluidic channels. Our sche…
We report the first experimental demonstration of a TE-polarization photonic band gap (PBG) in a 2D isotropic hyperuniform disordered solid (HUDS) made of dielectric media with a index contrast of 1.6:1, very low for PBG formation. The solid is composed of a connected network of dielectric walls enclosing air-filled cells. Direct comparison with photonic crystals and quasicrystals permitted us to investigate band-gap properties as a function of increasing rotational isotropy. We present results from numerical simulations proving that the PBG observed experimentally for HUDS at low index contra…
Most optical systems involve a combination of lenses separated by free-space regions where light acquires the required angle-dependent phase delay for a certain functionality. Very recently, flat-optics structures have been proposed to compress these large free-space volumes and miniaturize the overall optical system. However, these early designs can only replace free-space volumes of limited length, or operate in a very narrow angular range, or require a high-index background. These issues raise questions about the applicability of these devices in practical scenarios. Here, we first derive a…
The release of conduction-band electrons from a metal surface by a sub-femtosecond extreme ultraviolet (XUV) pulse, and their propagation through the solid, provokes a dielectric response in the solid that acts back on the photoelectron wave packet. We calculated the (wake) potential associated with this photoelectron self-interaction in terms of bulk and surface plasmon excitations and show that it induces a considerable, XUV-frequency-dependent temporal shift in laser-streaked XUV photoemission spectra, suggesting the observation of the ultrafast solid-state dielectric response in contempora…
The Keldysh theory of photoionization in a solid dielectric is generalized to the case of arbitrarily short driving pulses of arbitrary pulse shape. We derive a closed-form solution for the nonadiabatic ionization rate in a transparent solid with a periodic dispersion relation, which reveals ultrafast ionization dynamics within the field cycle and recovers the key results of the Keldysh theory in the appropriate limiting regimes.
We report enhanced broadband Terahertz (THz) generation and detailed characterization from the interaction of femtosecond two colour laser pulses with thin transparent dielectric tape target in ambient air. The proposed source is easy to implement, exhibits excellent scalability with laser energy. Spectral characterization using Fourier transform spectrometer reveals yield enhancement of more than 150 % in the THz region of 0.1 - 10 THz with respect to conventional two-colour laser plasma source in ambient air. Further, the source spectrum extends up to 40 THz with an enhancement of flux > 30 …
We use finite-difference time-domain modelling to investigate plasma generation induced by multi-photon absorption of intense laser light in dielectrics with tiny inhomogenities. Plasma generation is found to be strongly amplified around nanometer-sized inhomogeneities as present in glasses. Each inhomogeneity acts as the seed of a plasma structure growing against the direction of light propagation. Plasma structures originating from randomly distributed inhomogeneities are found to interact strongly and to organize in regularly spaced planes oriented perpendicularly to the laser polarization.…
The aim of this work is to find analytical expressions of the radiation force and potential densities arising from a laser pulse propagating in a dielectric media. In the femtosecond region the force becomes strong enough to confine neutral particles into the pulse envelope and translate them with the group velocity in gases. Additionally, if the trapped particles are with high density, the probability of collision with the free atoms and molecules in air become significant. The collision energies are in the range of 12 - 24 GeV and high enough to ionize the neutral atoms. Thus, a new type of …
The generation of high-order harmonics in bulk solids subjected to intense ultrashort laser pulses has opened up new avenues for research in extreme nonlinear optics and light-matter interaction on sub-cycle timescales. Despite significant advancement over the past decade, a complete understanding of the involved phenomena is still lacking. High-harmonic generation in solids is currently understood as arising from nonlinear intraband currents, interband recollision and ionization-related phenomena. As all of these mechanisms involve or rely upon laser-driven excitation we combine measurements …
The recent observation of high-harmonic generation from solids creates a new possibility for engineering fundamental strong-field processes by patterning the solid target with subwavelength nanostructures. All-dielectric metasurfaces exhibit high damage thresholds and strong enhancement of the driving field, making them attractive platforms to control high-harmonics and other high-field processes at nanoscales. Here we report enhanced non-perturbative high-harmonic emission from a Si metasurface that possesses a sharp Fano resonance resulting from a classical analogue of electromagnetically in…
We revisit the mechanism of high harmonic generation (HHG) from solids by comparing HHG in laser fields with different ellipticities but constant maximum amplitude. It is shown that the cutoff of HHG is strongly extended in a circularly polarized field. Moreover, the harmonic yield with large ellipticity is comparable to or even higher than that in the linearly polarized field. To understand the underlying physics, we develop a reciprocal-space-trajectory method, which explains HHG in solids by a trajectory ensemble from different ionization times and different initial states in the reciprocal…
A wavelength-degenerate pump-probe spectroscopy is used to study the ultrafast dynamics of strong-field ionization in femtosecond-laser subwavelength-structured fused silica. The comparative spectra demonstrate that femtosecond-laser subwavelength structuring always give rise to great enhancement for strong-field ionization as well as third-order nonlinear optical effects, which is the direct evidence of great local field enhancement in subwavelength apertures of fs-laser highly-excited surface. In short, the study shows the prominent subwavelength spatial effect of strong-field ionization in …
The textbook-accepted formulation of electromagnetic force was proposed by Lorentz in the 19th century, but its validity has been challenged due to incompatibility with the special relativity and momentum conservation. The Einstein-Laub formulation, which can reconcile those conflicts, was suggested as an alternative to the Lorentz formulation. However, intense debates on the exact force are still going on due to lack of experimental evidence. Here, we report the first experimental investigation of angular symmetry of optical force inside a solid dielectric, aiming to distinguish the two formu…
We describe laser systems for photoionization, Doppler cooling and quantum state manipulation of beryllium ions. For photoionization of neutral beryllium, we have developed a continuous-wave 235 nm source obtained by two stages of frequency doubling from a diode laser at 940 nm. The system delivers up to 400 mW at 470 nm and 28 mW at 235 nm. For control of the beryllium ion, three laser wavelengths at 313 nm are produced by sum-frequency generation and second-harmonic generation from four infrared fiber lasers. Up to 7.2 W at 626 nm and 1.9 W at 313 nm are obtained using two pump beams at 1051…
In this work, we present an in-depth experimental and numerical study of the short-range THz communications links that use subwavelength dielectric fibers for information transmission and define main challenges and tradeoffs in the link implementation. Particularly, we use air or foam-cladded polypropylene-core subwavelength dielectric THz fibers of various diameters (0.57-1.75 mm) to study link performance as a function of the link length of up to ~10 m, and data bitrates of up to 6 Gbps at the carrier frequency of 128 GHz (2.34 mm wavelength). We find that depending on the fiber diameter, th…
We show, via simulations, that an optical fiber taper waveguide can be an efficient tool for photoluminescence and resonant, extinction spectroscopy of single emitters, such as molecules or colloidal quantum dots, deposited on the surface of a thin dielectric membrane. Placed over a high refractive index membrane, a tapered fiber waveguide induces the formation of hybrid mode waves, akin to dielectric slotted waveguide modes, that provide strong field confinement in the low index gap region. The availability of such gap-confined waves yields potentially high spontaneous emission enhancement fa…
We investigate numerically effects related to ``single-cycle'' ionization of dense matter by an ultra-short laser pulse. The strongly non-adiabatic response of electrons leads to generation of a megagauss steady magnetic field in laser-solid interaction. By using two-beam interference, it is possible to create periodic density structures able to trap light and to generate relativistic ionization fronts
A nonlocal quantum model is presented for calculating the atomic dielectric response to a strong laser electric field. By replacing the Coulomb potential with a nonlocal potential in the Schrodinger equation, a 3+1D calculation of the time-dependent electric dipole moment can be replaced with a 0+1D integral equation, offering significant computational savings. The model is benchmarked against an established ionization model and \textit{ab initio} simulation of the time-dependent Schrodinger equation. The reduced computational overhead makes the model a promising candidate to incorporate full …
Nanoparticles levitated in vacuum can be set to spin at ultimate frequencies, limited only by the tensile strength of the material. At such high frequencies, drastic changes to the dynamics of solid-state quantum excitations are to be expected. Here, we theoretically describe the interaction between acoustic phonons and the rotation of a nanoparticle around its own axis, and model how the acoustic and optical properties of the nanoparticle change when it rotates at a fixed frequency. As an example, we analytically predict the scaling of the shape, the acoustic eigenmode spectrum, the permittiv…
We find that, for sufficiently strong mid-IR fields, transitions between different conduction bands play an important role in the generation of high-order harmonics in a dielectric. The transitions make a significant contribution to the harmonic signal, and they can create a single effective band for the motion of an electron wave packet. We show how high harmonic spectra produced during the interaction of ultrashort laser pulses with periodic solids provide a spectroscopic tool for understanding the effective band structure that controls electron dynamics in these media.
The force of electromagnetic radiation on a dielectric medium may be derived by a direct application of the Lorentz law of classical electrodynamics. While the light's electric field acts upon the (induced) bound charges in the medium, its magnetic field exerts a force on the bound currents. We use the example of a wedge-shaped solid dielectric, immersed in a transparent liquid and illuminated at Brewster's angle, to demonstrate that the linear momentum of the electromagnetic field within dielectrics has neither the Minkowski nor the Abraham form; rather, the correct expression for momentum de…
