Search

We demonstrate that pulsed THz radiation produced in air by a focused ultrashort laser pulse can be steered to large angles or even in the backward direction with respect to the laser propagation axis. The emission angle is adjusted by the flying focus technique, which determines the speed and direction of the ionization front created by the single-color laser pulse. This easily adjustable THz source, being well separated from the intense laser, opens exciting applications for remote THz spectroscopy., Comment: 8 pages, 5 figures

Electric currents circulating between charged clouds and the earth surface during lightning discharges are responsible for considerable damages and casualties. It is therefore important to develop better protection methods in addition to the traditional Franklin rod. Here we present the first demonstration that filaments formed by short and intense laser pulses can guide lightning discharges over considerable distances. We believe that this experimental breakthrough will lead to progress in lightning protection and lightning physics. An experimental campaign was carried out on the S\"antis Mountain in Northeastern Switzerland during the Summer of 2021 with a high repetition rate terawatt laser. The guiding of an upward negative lightning leader over a distance of 50 m was recorded by two separate high-speed cameras. The guiding of negative lightning leaders by laser filaments was corroborated in three other instances by VHF interferometric measurements, and the number of X-ray bursts detected during guided lightning events was significantly increased. While this research field has been very active for more than 20 years with many research groups around the world working to achieve this goal, this result demonstrates lightning guiding by lasers, which may lead to the development of a laser lightning rod. This work paves the way for new atmospheric applications of ultrashort lasers and represents a significant step forward in the development of a laser based lightning protection for airports, launchpads or large infrastructures., Comment: Laser-guided lightning. Nat. Photon. (2023)

Quantum interference occurs frequently in the interaction of laser radiation with materials, leading to a series of fascinating effects such as lasing without inversion, electromagnetically induced transparency, Fano resonance, etc. Such quantum interference effects are mostly enabled by single-photon resonance with transitions in the matter, regardless of how many optical frequencies are involved. Here, we demonstrate quantum interference driven by multiple photons in the emission spectroscopy of nitrogen ions that are resonantly pumped by ultrafast infrared laser pulses. In the spectral domain, Fano resonance is observed in the emission spectrum, where a laser-assisted dynamic Stark effect creates the continuum. In the time domain, the fast-evolving emission is measured, revealing the nature of free-induction decay (FID) arising from quantum radiation and molecular cooperativity. These findings clarify the mechanism of coherent emission of nitrogen ions pumped with MIR pump laser and are likely to be universal. The present work opens a route to explore the important role of quantum interference during the interaction of intense laser pulses with materials near multiple photon resonance., Comment: 20 pages, 8 figures

Rydberg excitons are, with their ultrastrong mutual interactions, giant optical nonlinearities, and very high sensitivity to external fields, promising for applications in quantum sensing and nonlinear optics at the single-photon level. To design quantum applications it is necessary to know how Rydberg excitons and other excited states relax to lower-lying exciton states. Here, we present photoluminescence excitation spectroscopy as a method to probe transition probabilities from various excitonic states in cuprous oxide, and we show giant Rydberg excitons at $T=38$ mK with principal quantum numbers up to $n=30$, corresponding to a calculated diameter of 3 $\mu$m., Comment: 11 pages, 4 figures

Cavity-free lasing of N$_2^+$ induced by a femtosecond laser pulse at 800~nm is nearly totally suppressed by a delayed twin pump pulse. We explain this surprising effect within the V-scheme of lasing without population inversion. A fast transfer of population between nitrogen ionic states X$^2\Sigma_g^+$ and A$^2\Pi_u$, induced by the second pulse, terminates the conditions for amplification in the system. Appearance of short lasing bursts at delays corresponding to revivals of rotational wave packets are explained along the same lines.

Delayed cavity-free forward lasing at the wavelengths of 391 and 428 nm was observed in recent experiments in air or pure nitrogen pumped with an intense femtosecond laser pulse at wavelength of 800~nm. The mechanism responsible for the lasing is highly controversial. In this article we explain the delayed emission by the presence of long-lived polarizations coupling simultaneously ground state X$^2\Sigma_g^+$ to states A$^2\Pi_u$ and B$^2\Sigma_u^+$ of singly ionized nitrogen molecules N$_2^+$. Ionization of neutral nitrogen molecules in a strong laser field and subsequent ion excitation are described by a system of Bloch equations providing a distribution of ions in the ground and excited states A and B at the end of the laser pulse. The delayed signal amplification at the B-X transition wavelength is described by a system of Maxwell-Bloch equations with polarization coupling maintained by a weak laser post-pulse. Two regimes of signal amplification are identified: a signal of a few ps duration at low gas pressures and a short (sub-picosecond) signal at high gas pressures. The theoretical model compares favorably with experimental results.

We study the use of frequency upconversion schemes of near-IR picosecond laser pulses and compare their ability to guide and trigger electric discharges through filamentation in air. Upconversion, such as Second Harmonic Generation, is favorable for triggering electric discharges for given amount of available laser energy, even taking into account the losses inherent to frequency conversion. We focus on the practical question of optimizing the use of energy from a given available laser system and the potential advantage to use frequency conversion schemes.

Cuprous oxide (Cu$_2$O) is a semiconductor with large exciton binding energy and significant technological importance in applications such as photovoltaics and solar water splitting. It is also a superior material system for quantum optics that enabled the observation of two intriguing phenomena, i.e. Rydberg excitons as solid-state analogue to highly-excited atomic states and dense exciton gases showing quantum degeneracy when approaching the phase transition to Bose-Einstein condensation. Previous experiments focused on natural bulk crystals due to major difficulties in growing high-quality synthetic samples. Here, we present Cu$_2$O microcrystals with excellent optical material quality capable of hosting both quantum-degenerate excitons and excited Rydberg states. Growth of Cu$_2$O with exceedingly low point defect levels was achieved on silicon by a scalable thermal oxidation process compatible with lithographic patterning. Using the latter, we demonstrate Rydberg excitons in site-controlled Cu$_2$O microstructures, paving the way for a plethora of applications in integrated quantum photonics.

A cavity-free laser in the sky could lead to revolutionary improvements in optical remote sensing for atmospheric science. Abundant in air, nitrogen molecules are prime candidates as an active medium for such a laser. Nitrogen molecules, either neutral or singly ionized, exhibit a significant optical gain in the UV regime when pumped by an intense femtosecond laser. Despite numerous works, the physical origin of this lasing is still not understood. Here we offer a consistent interpretation of all experimental facts by introducing a concept drawn from the field of quantum optics: transient lasing without inversion. Our experiments and simulations identify the crucial role of macroscopic coherence, instead of population inversion, in the nitrogen ions lasing system. Manipulating the macroscopic coherence provides a new level of control over nitrogen air lasing and offers new perspectives for the generation of very short wavelength laser where population inversion is difficult to achieve.

We report on the observation of backward lasing at 391.4 nm of nitrogen ions pumped by linearly polarized intense femtosecond pulses at 800 nm. The strongly enhanced spectral intensity at 391.4 nm, as well as the amplification of an externally injected backward seeding pulse, confirm that the backward 391.4 nm signal is due to optical amplification in the gas plasma. Compared to the forward emission at 391.4 nm, the optimal backward emission is achieved at a lower gas pressure around 10 mbar, which is due to asymmetry of the backward and forward directions rooted in the traveling excitation geometry. This method, using the widely available 800 nm femtosecond pulses as a pump laser, provides a promising scheme for the generation of backward air laser, which holds a unique potential for optical remote sensing.

We investigate experimentally the plasma dynamics of a centimeter-scale, laser filamentation-guided spark discharge. Using electrical and optical diagnostics to study monopolar discharges with varying current pulses we show that plasma decay is dominated by free electron recombination if the current decay time is shorter than the recombination characteristic time. In the opposite case, the plasma electron density closely follows the current evolution. We demonstrate that this criterion holds true in the case of damped AC sparks, and that alternative current is the best option to achieve a long plasma lifetime for a given peak current., Comment: 5 pages, 5 figures

Acoustic signals generated by filamentation of ultrashort TW laser pulses in water are characterized experimentally. Measurements reveal a strong influence of input pulse duration on the shape and intensity of the acoustic wave. Numerical simulations of the laser pulse nonlinear propagation and the subsequent water hydrodynamics and acoustic wave generation show that the strong acoustic emission is related to the mechanism of superfilamention in water. The elongated shape of the plasma volume where energy is deposited drives the far-field profile of the acoustic signal, which takes the form of a radially directed pressure wave with a single oscillation and a very broad spectrum., Comment: 9 pages, 12 figures

We propose a new mechanism to explain the origin of optical gain in the transitions between excited and ground state of the ionized nitrogen molecule following irradiation of neutral nitrogen molecules with an intense ultra short laser pulse. An efficient transfer of population to the excited state is achieved via field-induced multiple recollisions. We show that the proposed excitation mechanism must lead to a super-radiant emission, a feature that we confirm experimentally., Comment: 15 pages, 4 figures

Laser filamentation is responsible for the deposition of a significant part of the laser pulse energy in the propagation medium. We found that using terawatt laser pulses and relatively tight focusing conditions in air, resulting in a bundle of co-propagating multifilaments, more than 60 % of the pulses energy is transferred to the medium, eventually degrading into heat. This results in a strong hydrodynamic reaction of air with the generation of shock waves and associated underdense channels for each short-scale filament. In the focal zone, where filaments are close to each other, these discrete channels eventually merge to form a single cylindrical low-density tube over a $\sim 1 \mu\mathrm{s}$ timescale. We measured the maximum lineic deposited energy to be more than 1 J/m., Comment: 7 pages, 7 figures

We show experimental and numerical evidence of spontaneous self-symmetrization of focused laser beams experiencing multi-filamentation in air. The symmetrization effect is observed as the multiple filaments generated prior to focus approach the focal volume. This phenomenon is attributed to the nonlinear interactions amongst the different parts of the beam mediated by the optical Kerr effect, which leads to a symmetric redistribution of the wave vectors even when the beam consists of a bundle of many filaments., Comment: 9 pages, 7 figures

Using femtosecond laser pulses at 800 and 400 nm, we characterize the formation of underdense channels in air generated by laser filamentation at the millijoule energy level by means of transverse interferometry. We find that using tight focusing conditions, filamentation generates a shock wave and that the resulting low-density channel lasts for more than 90 ms. Comparison of these results with hydrodynamic simulations using an Eulerian hydrodynamic code gives an good agreement and allows us to estimate the initial gas peak temperature at $\sim$ 1000 K. The influence of experimental parameters such as the focusing conditions for the ultrashort laser pulse, its polarization or the wavelength is studied and linked to previous characterizations of filamentation-generated plasma columns., Comment: 9 pages, 9 figures

We present a space and time resolved interferometric plasma diagnostic for use on plasmas where neutral-bound electron contribution to the refractive index cannot be neglected. By recording simultaneously the plasma optical index at 532 and 1064 nm, we are able to extract independently the neutral and free electron density profiles. We report a phase resolution of 30 mrad, corresponding to a maximum resolution on the order of $4\times10^{23}~\mathrm{m}^{-3}$ for the electron density, and of $10^{24} ~ \mathrm{m}^{-3}$ for the neutral density. The interferometer is demonstrated on centimeter-scale sparks triggered by laser filamentation in air with typical currents of a few tens of A., Comment: 10 pages, 11 figures

The interaction between a large number of laser filaments brought together using weak external focusing leads to the emergence of few filamentary structures reminiscent of standard filaments, but carrying a higher intensity. The resulting plasma is measured to be one order of magnitude denser than for short-scale filaments. This new propagation regime is dubbed superfilamentation. Numerical simulations of a nonlinear envelope equation provide good agreement with experiments., Comment: 5 pages, 4 figures

Recently, S. Mitryukovskiy et al. presented experimental evidence showing that backward stimulated radiation at 337 nm can be obtained from plasma filaments in nitrogen gas pumped by circularly polarized 800 nm femtosecond pulses (Opt. Express, 22, 12750 (2014)). Here, we report that this backward stimulated radiation is enhanced by a factor of ~ 16 in the presence of a seed pulse. This enhanced stimulated radiation can be either linearly or circularly polarized, dictated by the seeding pulse, which is distinct from the non-polarized nature of the ASE without seeding pulse. We also measured the spatial profile and estimated the energy of the radiation. This seeding effect confirms unambiguously the existence of population inversion between the C3{\Pi}u and B3{\Pi}g state of nitrogen molecules inside plasma filament and provides a possible solution to control the properties of this backward stimulated radiation., Comment: 6 pages, 5 figures

We analyze numerically and experimentally the effect of the input pulse chirp on the nonlinear energy deposition from $5\ \mu$J fs-pulses at $800$ nm to water. Numerical results are also shown for pulses at $400$ nm, where linear losses are minimized, and for different focusing geometries. Input chirp is found to have a big impact on the deposited energy and on the plasma distribution around focus, thus providing a simple and effective mechanism to tune the electron density and energy deposition. We identify three relevant ways in which plasma features may be tuned., Comment: 9 pages, 7 figures

We report on strong backward stimulated emission at 337 nm in Nitrogen gas pumped by circularly polarized femtosecond laser pulses at 800 nm. A distinct dependence of the backward UV spectrum on pump laser polarization and intensity is observed, pointing to the occurrence of backward amplified spontaneous emission inside filaments. We attribute the population inversion to inelastic collision between the free electrons produced by the pump laser and neutral N2 molecules. The addition of Oxygen molecules is detrimental for the gain, reducing it to near threshold at atmospheric concentration.

We report on the lasing action of atmospheric air pumped by an 800 nm femtosecond laser pulse with peak power up to 4 TW. Lasing emission at 428 nm increases rapidly over a small range of pump laser power, followed by saturation above ~ 1.5 TW. The maximum lasing pulse energy is measured to be 2.6 uJ corresponding to an emission power in the MW range, while a maximum conversion efficiency of is measured at moderate pump pulse energy. The optical gain inside the filament plasma is estimated to be excess of 0.7/cm. The lasing emission shows a doughnut profile, reflecting the spatial distribution of the pump-generated white-light continuum that acts as a seed for the lasing. We attribute the pronounced saturation to the defocusing of the seed in the plasma amplifying region and to the saturation of the seed intensity.

We report on the lasing in air and pure nitrogen gas pumped by a single 800 nm femtosecond laser pulse. Depending on gas pressure, incident laser power and beam convergence, different lasing lines are observed in the forward direction with rapid change of their relative intensities. The lines are attributed to transitions between vibrational and rotational levels of the first negative band of the singly charged nitrogen molecule-ion. We show that self-seeding plays an important role in the observed intensity changes., Comment: 9 pages, 4 figures

The balance of the linear photon momentum in multiphoton ionization is studied experimentally. In the experiment argon and neon atoms are singly ionized by circularly polarized laser pulses with a wavelength of 800 nm and 1400 nm in the intensity range of 10^{14} - 10^{15} W/cm^2. The photoelectrons are measured using velocity map imaging. We find that the photoelectrons carry linear momentum corresponding to the photons absorbed above the field free ionization threshold. Our finding has implications for concurrent models of the generation of terahertz radiation in filaments., Comment: 4 pages, 3 figures

We report on the observation of the yellow exciton Lyman series up to the fourth term in Cu2O by time-resolved mid-infrared spectroscopy. The dependence of the oscillator strength on the principal quantum number n can be well reproduced using the hydrogenic model including an AC dielectric constant, and precise information on the electronic structure of the 1s exciton state can be obtained. A Bohr radius a_{1s}=7.9 A and a 1s-2p transition dipole moment \mu_{1s-2p}= 4.2 eA were found.

Using time-resolved $1s$-$2p$ excitonic Lyman spectroscopy, we study the orthoexciton-to-paraexcitons transfer, following the creation of a high density population of ultracold $1s$ orthoexcitons by resonant two-photon excitation with femtosecond pulses. An observed fast exciton-density dependent conversion rate is attributed to spin exchange between pairs of orthoexcitons. Implication of these results on the feasibility of BEC of paraexcitons in Cu$_2$O is discussed.

In view of the recent experiments of O'Hara, et al. on excitons in Cu_2O, we examine the interconversion between the angular-momentum triplet-state excitons and the angular-momentum singlet-state excitons by a spin-exchange process which has been overlooked in the past. We estimate the rate of this particle-conserving mechanism and find a substantially higher value than the Auger process considered so far. Based on this idea, we give a possible explanation of the recent experimental observations, and make certain predictions, with the most important being that the singlet-state excitons in Cu_2O is a very serious candidate for exhibiting the phenomenon of Bose-Einstein condensation., Comment: 4 pages, RevTex, 1 ps figure