Long range propagation of ultrafast, ionizing laser pulses in a resonant nonlinear medium
G. Demeter, J. T. Moody, M. Aladi, A. -M. Bachmann, F. Batsch, F. Braunmuller, G. P. Djotyan, V. Fedosseev, F. Friebel, S. Gessner, E. Granados, E. Guran, M. Hu… 展开作者
G. Demeter, J. T. Moody, M. Aladi, A. -M. Bachmann, F. Batsch, F. Braunmuller, G. P. Djotyan, V. Fedosseev, F. Friebel, S. Gessner, E. Granados, E. Guran, M. Huther, M. A. Kedves, M. Martyanov, P. Muggli, E. Oz, H. Panuganti, B. Raczkevi, L. Verra, G. Zevi Della Porta
We study the propagation of 0.05-1 TW power, ultrafast laser pulses in a 10 meter long rubidium vapor cell. The central wavelength of the laser is resonant with the $D_2$ line of rubidium and the peak intensity in the $10^{12}-10^{14} ~W/cm^2$ range, enough to create a plasma channel with single electron ionization. We observe the absorption of the laser pulse for low energy, a regime of transverse confinement of the laser beam by the strong resonant nonlinearity for higher energies and the transverse broadening of the output beam when the nonlinearity is saturated due to full medium ionization. We compare experimental observations of transmitted pulse energy and transverse fluence profile with the results of computer simulations modeling pulse propagation. We find a qualitative agreement between theory and experiment that corroborates the validity of our propagation model. While the quantitative differences are substantial, the results show that the model can be used to interpret the observed phenomena in terms of self-focusing and channeling of the laser pulses by the saturable nonlinearity and the transparency of the fully ionized medium along the propagation axis.
We present a combined theoretical and experimental study of spatio-temporal propagation effects in terahertz (THz) generation in gases using two-color ionizing laser pulses. The observed strong broadening of the THz spectra with increasing gas pressure reveals the prominent role of spatio-temporal reshaping and of a plasma-induced blue-shift of the pump pulses in the generation process. Results obtained from (3+1)-dimensional simulations are in good agreement with experimental findings and clarify the mechanisms responsible for THz emission.
We investigate the propagation of ultra-short laser pulses in atomic rubidium vapor. The pulses are intensive enough to ionize the atoms and are directly resonant with the 780 nm $D_2$ line. We derive a relatively simple theory for computing the nonlinear optical response of atoms and investigate the competing effects of strong resonant nonlinearity and ionization in the medium using computer simulations. A nonlinear self-channeling of pulse energy is found to produce a continuous plasma channel with complete ionization. We evaluate the length, width and homogeneity of the resulting plasma cha…
Filming atomic motion within molecules is an active pursuit of molecular physics and quantum chemistry. A promising method is laser-induced Coulomb Explosion Imaging (CEI) where a laser pulse rapidly ionizes many electrons from a molecule, causing the remaining ions to undergo Coulomb repulsion. The ion momenta are used to reconstruct the molecular geometry which is tracked over time (i.e. filmed) by ionizing at an adjustable delay with respect to the start of interatomic motion. Results are distorted, however, by ultrafast motion during the ionizing pulse. We studied this effect in water and …
We demonstrate generation of a pulsed stream of electrically triggered single photons in resonance fluorescence, by applying high frequency electrical pulses to a single quantum dot in a p-i-n diode under resonant laser excitation. Single photon emission was verifed, with the probability of multiple photon emission reduced to 2.8%. We show that despite the presence of charge noise in the emission spectrum of the dot, resonant excitation acts as a filter to generate narrow bandwidth photons.
We demonstrate how the technique of ultrafast resonant x-ray scattering can be applied to imaging dynamics of electronic wave packets in crystals. We study scattering patterns from crystals with electron dynamics in valence bands taking into account that inelastic and elastic scattering events induced by a broad-band probe pulse cannot be separated through the spectroscopy of the scattered photon. As a result, scattering patterns are not determined by the structure factor at the time of measurement, but can encode the instantaneous electron current between scattering atoms. We provide examples…
We present a theoretical description of resonant radiofrequency (RF) deflecting cavities in TM$_{110}$ mode as dynamic optical elements for ultrafast electron microscopy. We first derive the optical transfer matrix of an ideal pillbox cavity and use a Courant-Snyder formalism to calculate the 6D phase space propagation of a Gaussian electron distribution through the cavity. We derive closed, analytic expressions for the increase in transverse emittance and energy spread of the electron distribution. We demonstrate that for the special case of a beam focused in the center of the cavity, the low…
We present space and time resolved measurements of the air hydrodynamics induced by ultrafast laser pulse excitation of the air gap between two electrodes at high potential difference. We explore both plasma-based and plasma-free gap excitation. The former uses the plasma left in the wake of femtosecond filamentation, while the latter exploits air heating by multiple-pulse resonant excitation of quantum molecular wavepackets. We find that the cumulative electrode-driven air density depression channel initiated by the laser plays the dominant role in the gap evolution leading to breakdown.
Ultrashort photoemitted electron bunches can provide high electron currents within sub-picosecond timeframes, enabling time-resolved investigations of ultrafast physical processes with nanoscale resolution. Non-resonant conductive nanotips are typically employed to realize nanoscale photoelectron sources with high brightness. However, such emitters require complex non-scalable fabrication procedures featuring poor reproducibility. Planar resonant antennas fabricated via photolithography have been recently investigated, also because of their superior field enhancement properties. Nevertheless, …
Single-photon emitters in solid-state systems are important building blocks for scalable quantum technologies. Recently, quantum light emitters have been discovered in the wide-gap van der Waals insulator hBN. These color centers have attracted considerable attention due to their quantum performance at elevated temperatures and wide range of transition energies. Here, we demonstrate coherent state manipulation of a single hBN color center with ultrafast laser pulses and investigate in our joint experiment-theory study the coupling between the electronic system and phonons. We demonstrate that …
The functionalities of a wide range of optical and opto-electronic devices are based on resonance effects and active tuning of the amplitude and wavelength response is often essential. Plasmonic nanostructures are an efficient way to create optical resonances, a prominent example is the extraordinary optical transmission (EOT) through arrays of nanoholes patterned in a metallic film. Tuning of resonances by heating, applying electrical or optical signals has proven to be more elusive, due to the lack of materials that can induce modulation over a broad spectral range and/or at high speeds. Her…
The Raman effect -- inelastic scattering of light by lattice vibrations (phonons) -- produces an optical response closely tied to a material's crystal structure. Here we show that resonant optical excitation of IR and Raman phonons gives rise to a Raman scattering effect that can induce giant shifts to the refractive index and induce new optical constants that are forbidden in the equilibrium crystal structure. We complete the description of light-matter interactions mediated by coupled IR and Raman phonons in crystalline insulators -- currently the focus of numerous experiments aiming to dyna…
Vacuum polarization, an effect predicted nearly 70 years ago, is still yet to be directly detected despite significant experimental effort. Previous attempts have made use of large liquid-helium cooled electromagnets which inadvertently generate spurious signals that mask the desired signal. We present a novel approach for the ultra-sensitive detection of optical birefringence that can be usefully applied to a laboratory detection of vacuum polarization. The new technique has a predicted birefringence measurement sensitivity of $Δn \sim 10^{20}$ in a 1 second measurement. When combined with th…
Ultrashort electron beams with femtosecond to picosecond bunch durations offer unique opportunities to explore active research areas ranging from ultrafast structural dynamics to ultra-high dose-rate radiobiological studies. We present a straightforward method to generate MeV-ranged electron beams in ambient air through the tight focusing of a few-cycle, mJ-class femtosecond IR laser. At one meter from the source, the highest measured dose rate of 0.15 Gy/s exceeds the yearly dose limit in less than one second and warrants the implementation of radiation protection. Two-dimensional Particle-In…
The quest to improve density, speed and energy efficiency of magnetic memory storage has led to exploration of new ways of optically manipulating magnetism at the ultrafast time scale, in particular in ferrimagnetic alloys. While all-optical magnetization switching is well-established on the femtosecond timescale, lateral nanoscale confinement and thus potential significant reduction of the size of the magnetic element remains an outstanding challenge. Here we employ resonant electromagnetic energy-funneling plasmon nanoantennas to influence the demagnetization dynamics of a ferrimagnetic TbCo…
Prior to the invention of holography or lasers, Bragg's X-ray microscope opened the door to optical computation in short-wavelength studies using spatially coherent visible light, including phase retrieval methods. This optical approach lost ground to semiconductor detection and digital computing in the 1960s. Since then, visible optics including spatial light modulators (SLMs), array detectors and femtosecond lasers have become widely available, routinely allowing versatile and computer-interfaced imposition of optical phase, molecular coherent control, and detection. Today, high brilliance X…
Nowadays, via controlling surface plasmons (SPs) on elaborate man-made structures, plasmonics aiming at manipulating light beyond the diffraction limit has aroused great interest. Here, nevertheless, we demonstrate in short-pulse laser ablation ultrafast active plasmonic structures spontaneously generate in virtue of plasmonic effects rather than human ingenuity. First, the splitting of laser-induced subwavelength gratings that is experimentally evidenced on ZnO, Si, and GaAs, is confirmed to originate in the conversion of SP modes from the resonant to the nonresonant mode and further to the i…
We study how the color and polarization of ultrashort pulses of visible light can be used to control the demagnetization processes of the antiferromagnetic insulator Cr$_2$O$_3$. We utilize time-resolved second harmonic generation (SHG) to probe how changes in the magnetic and structural state evolve in time. We show that, varying the pump photon-energy to excite either localized transitions within the Cr or charge transfer states, leads to markedly different dynamics. Through a full polarization analysis of the SHG signal, symmetry considerations and density functional theory calculations, we…
We experimentally demonstrate the efficient generation of circularly polarized pulses tunable from the vacuum to deep ultraviolet (160-380 nm) through resonant dispersive wave emission from optical solitons in a gas-filled hollow capillary fiber. In the deep ultraviolet we measure up to 13 microjoule of pulse energy, and from numerical simulations, we estimate the shortest output pulse duration to be 8.5 fs. We also experimentally verify that simply scaling the pulse energy by 3/2 between linearly and circularly polarized pumping closely reproduces the soliton and dispersive wave dynamics. Bas…
Exploration of a new ultrafast-ultrasmall frontier in atomic and molecular physics has begun. Not only is is possible to control outer-shell electron dynamics with intense ultrafast optical lasers, but now control of inner-shell processes has become possible by combining intense infrared/optical lasers with tunable sources of x-ray radiation. This marriage of strong-field laser and x-ray physics has led to the discovery of methods to control reversibly resonant x-ray absorption in atoms and molecules on ultrafast timescales. Using a strong optical dressing field, resonant x-ray absorption in a…
We report on the broadband transient optical response from anisotropic nanobrick amorphous silicon particles, exhibiting Mie-type resonances. A quantitative model is developed to identify and disentangle the three physical processes that govern the ultrafast changes of the nanobrick optical properties, namely two-photon absorption, free-carrier relaxation, and lattice heating. We reveal a set of operating windows where ultrafast all-optical modulation of transmission is achieved with full return to zero in 20 ps. This is made possible due to the interplay between the competing nonlinear proces…
Optically generated electron-hole plasma in high-index dielectric nanostructures was demonstrated as a means of tuning of their optical properties. However, until now an ultrafast operation regime of such plasma driven nanostructures has not been attained. Here, we perform pump-probe experiments with resonant silicon nanoparticles and report on dense optical plasma generation near the magnetic dipole resonance with ultrafast (about 2.5 ps) relaxation rate. Basing on experimental results, we develop an analytical model describing transient response of a nanocrystalline silicon nanoparticle to a…
Trapped ions are one of the most promising approaches for the realization of a universal quantum computer. Faster quantum logic gates could dramatically improve the performance of trapped-ion quantum computers, and require the development of suitable high repetition rate pulsed lasers. Here we report on a robust frequency upconverted fiber laser based source, able to deliver 2.5 ps ultraviolet (UV) pulses at a stabilized repetition rate of 300.00000 MHz with an average power of 190 mW. The laser wavelength is resonant with the strong transition in Ytterbium (Yb+) at 369.53 nm and its repetitio…
Deep ultraviolet (DUV) laser pulses with tuneable wavelength and very short duration are a key enabling technology for next-generation technology and ultrafast science. Their generation has been the subject of extensive experimental effort, but no technique demonstrated thus far has been able to meet all requirements in one light source. Here we demonstrate a bright, efficient, and compact source of tuneable deep ultraviolet ultrafast laser pulses based on resonant dispersive wave emission in hollow capillary fibre. In a total footprint of only 120 x 75 cm, including the ytterbium-based drive …
Strain engineering has been extended recently to the ultrafast timescales, driving metal-insulator phase transitions and the propagation of ultrasonic demagnetization fronts. However, the non-linear lattice dynamics underpinning interfacial optoelectronic phase switching have not yet been addressed. Here we focus on the lattice dynamics initiated by impulsive resonant excitation of polar lattice vibrations in LaAlO$_3$ single crystals, one of the most widely utilized substrates for oxide electronics. We show that ionic Raman scattering drives coherent oxygen octahedra rotations around a high-s…
The nonlinear optical dynamics of nano-materials comprised of plasmons interacting with quantum emitters is investigated by a self-consistent model based on the coupled Maxwell-Liouville-von Neumann equations. It is shown that ultra-short resonant laser pulses significantly modify the optical properties of such hybrid systems. It is further demonstrated that the energy transfer between interacting molecules and plasmons occurs on a femtosecond time scale and can be controlled with both material and laser parameters.
Controlling Ultrafast Excitations in Germanium:The Role of Pump-Pulse Parameters and Multi-Photon Resonances
Università degli Studi di Salerno（萨莱诺大学）；CNR-SPIN, Unità di Salerno（意大利国家研究委员会自旋物理研究所萨莱诺分部）；CNISM, Unità di Salerno, Università degli Studi di Salerno（意大利凝聚态物质创新科学中心萨莱诺分部，萨莱诺大学）
Materials with thermal-invariant elastic properties of materials are of interest for resonant device frequency and dimensional stability of precision devices. Here, we demonstrate that the temperature coefficient of elasticity (TCE) of amorphous silica can be locally reduced using femtosecond laser irradiation. Notably, a self-organized laser-induced modification shows a decrease of the TCE beyond 50%. The origin of this dramatic decrease is attributed to the presence of sub-micron permanent densified zones within the fine multi-layers structure of the laser-modified zone.
Spectral anti-crossings between the fundamental guided mode and core wall resonances alter the dispersion in hollow-core anti-resonant-reflection photonic crystal fibers. Here we study the effect of this dispersion change on the nonlinear propagation and dynamics of ultrashort pulses. We find that it causes emission of narrow spectral peaks through a combination of four-wave mixing and dispersive wave emission. We further investigate the influence of the anti-crossings on nonlinear pulse propagation and show that their impact can be minimized by adjusting the core-wall thickness in such a way …
We study ultrafast ionization dynamics using orthogonally polarized two-color (OTC) laser pulses involving the resonant "first plus second" ($ω+2ω$) scheme. The scheme is illustrated by numerical simulations of the time-dependent Schrödinger equation and recording the photoelectron momentum distribution. On the basis of the simulations of this resonant ionization, we identify signatures of the dynamic Autler-Townes effect and dynamic interference, in which their characterization is not possible in spectral domain. Taking advantage of the OTC scheme we show that these dynamical effects, which o…
Ultrafast tuning of the focusing efficiency of a nonlinear atomically thin lens
Friedrich Schiller University Jena（耶拿弗里德里希·席勒大学）；Van der Waals-Zeeman Institute, Institute of Physics, University of Amsterdam（阿姆斯特丹大学物理学院范德瓦尔斯-塞曼研究所）；Abbe Center of Photonics, Friedrich Schiller University Jena（耶拿弗里德里希·席勒大学阿贝光子学中心）
We demonstrate the controlled creation of a $\mathrm{^{174}Yb^{2+}}$ ion by photo-ionizing $\mathrm{^{174}Yb^+}$ with weak continuous-wave lasers at ultraviolet wavelengths. The photo-ionization is performed by resonantly exciting transitions of the $\mathrm{^{174}Yb^+}$ ion in three steps. Starting from an ion crystal of two laser-cooled $\mathrm{^{174}Yb^+}$ ions localized in a radio-frequency trap, the verification of the ionization process is performed by characterizing the properties of the resulting mixed-species ion-crystal. The obtained results facilitate fundamental studies of physics…
We present a laboratory system for single-shot magneto-optical (MO) imaging of ultrafast magnetization dynamics with high-sensitivity of MO rotation. We create a stack of MO images repeatedly employing a single pair of a pump and defocused probe pulses to induce and visualize MO changes in the sample. Both laser beams are independently wavelength-tunable allowing for a flexible, resonant adjustable two-color pump and probe scheme. To increase the MO contrast the probe beam is spatially filtered. We performed the all-optical switching experiment in Co-doped yttrium iron garnet films (YIG:Co) to…
Laser printing with a spatial light modulator (SLM) has several advantages over conventional raster-writing and dot-matrix display (DMD) writing: multiple pixel exposure, high power endurance and existing software for computer generated holograms (CGH). We present a technique for the design and manufacturing of plasmonic metasurfaces based on ultrafast laser printing with an SLM. As a proof of principle, we have used this technique to laser print a plasmonic metalens as well as high resolution plasmonic color decorations. The high throughput holographic resonant laser printing (HRLP) approach …
The requirement for optical-electrical-optical conversion of signals in optical technologies is often one of the majors bottleneck in terms of speed and energy consumption. The use of dressed photons (also called polaritons), that allows for intrinsic sizable interactions, could significantly improve the performances of optical integrated elements such as switches or optical gates. In this work we demonstrate the ultrafast switch of a laser coupled into a polaritonic waveguide triggered by an optical pulse resonant with the same dispersion but at a lower energy. Our experiments show two effect…
