Search Results
Valley control by linearly polarized laser pulses: example of WSe2
Electrons at the band edges of materials are endowed with a valley index, a quantum number locating the band edge within the Brillouin zone. An important question is then how this index may be controlled by laser pulses, with current understanding that it couples exclusively via circularly polarized light. Employing both tight-binding and state-of-the-art time dependent density function theory, we show that on femtosecond time scales valley coupling is a much more general effect. We find that two time separated linearly polarized pulses allow almost complete control over valley excitation, with the pulse time difference and polarization vectors emerging as key parameters for valley control. Our findings highlight the possibility of controlling coherent electronic excitation by successive femtosecond laser pulses, and offer a route towards valleytronics in two-dimensional materials.
Electron dynamics in laser-driven atoms near the continuum threshold
Strong-field ionization and Rydberg-state excitation (RSE) near the continuum threshold exhibit two phenomena that have attracted a lot of recent attention: the low-energy structure (LES) just above and frustrated tunneling ionization just below the threshold. The former becomes apparent for longer laser wavelengths, while the latter has been especially investigated in the near infrared; both have been treated as separate phenomena so far. Here we present a unified perspective based on electron trajectories, which emphasizes the very important role of the electron-ion Coulomb interaction as expected in this energy region. Namely, those trajectories that generate the LES can also be recaptured into a Rydberg state. The coherent superposition of the contributions of such trajectories with different travel times (each generating one of the various LES peaks) causes an oscillation in the intensity dependence of the RSE yield, which is especially noticeable for longer wavelengths. The theory is illustrated by RSE experiments at 1800 nm, which agree very well with the theory with respect to position and period of the oscillation. The wavelength scaling of the RSE oscillation is also discussed. Our work establishes a solid relationship between processes below and above the threshold and sheds new light on atomic dynamics driven by intense laser fields in this critical energy region.
Compact intense extreme-ultraviolet source
High-intensity laser pulses covering the ultraviolet to terahertz spectral regions are nowadays routinely generated in a large number of laboratories. In contrast, intense extreme-ultraviolet (XUV) pulses have only been demonstrated using a small number of sources including free-electron laser facilities [1-3] and long high-harmonic generation (HHG) beamlines [4-9]. Here we demonstrate a concept for a compact intense XUV source based on HHG that is focused to an intensity of $2 \times 10^{14}$ W/cm$^2$, with a potential increase up to $10^{17}$ W/cm$^2$ in the future. Our approach uses tight focusing of the near-infrared (NIR) driving laser and minimizes the XUV virtual source size by generating harmonics several Rayleigh lengths away from the NIR focus. Accordingly, the XUV pulses can be refocused to a small beam waist radius of 600 nm, enabling the absorption of up to four XUV photons by a single Ar atom in a setup that fits on a modest (2 m) laser table. Our concept represents a straightforward approach for the generation of intense XUV pulses in many laboratories, providing novel opportunities for XUV strong-field and nonlinear optics experiments, for XUV-pump XUV-probe spectroscopy and for the coherent diffractive imaging of nanoscale structures.
Sub-cycle valleytronics: control of valley polarization using few-cycle linearly polarized pulses
So far, it has been assumed that selective excitation of a desired valley in the Brillouin zone of a hexagonal two-dimensional material has to rely on using circularly polarized fields. We theoretically demonstrate a way to control the valley excitation in hexagonal 2D materials on a few-femtosecond timescale using a few-cycle, linearly polarized pulse with controlled carrier–envelope phase. The valley polarization is mapped onto the strength of the perpendicular harmonic signal of a weak, linearly polarized pulse, which allows to read this information all-optically without destroying the valley state and without relying on the Berry curvature, making our approach potentially applicable to inversion-symmetric materials. We show applicability of this method to hexagonal boron nitride and MoS2.
Rotational quantum beat lasing without inversion
In standard lasers, light amplification requires population inversion between an upper and a lower state to break the reciprocity between absorption and stimulated emission. However, in a medium prepared in a specific superposition state, quantum interference may fully suppress absorption while leaving stimulated emission intact, opening the possibility of lasing without inversion. Here we show that lasing without inversion arises naturally during propagation of intense femtosecond laser pulses in air. It is triggered by the combination of molecular ionization and molecular alignment, both unavoidable in intense light fields. The effect could enable inversionless amplification of broadband radiation in many molecular gases, opening unusual opportunities for remote sensing. © 2020 Optical Society of America
Tm3+-doped calcium lithium tantalum gallium garnet (Tm:CLTGG): novel laser crystal
We report on the development of a novel laser crystal with broadband emission properties at ∼2 µm – a Tm3+,Li+-codoped calcium tantalum gallium garnet (Tm:CLTGG). The crystal is grown by the Czochralski method. Its structure (cubic, sp. gr. 𝐼𝑎3¯𝑑, a = 12.5158(0) Å) is refined by the Rietveld method. Tm:CLTGG exhibits a relatively high thermal conductivity of 4.33 Wm-1K-1. Raman spectroscopy confirms a weak concentration of vacancies due to the charge compensation provided by Li+ codoping. The transition probabilities of Tm3+ ions are determined using the modified Judd-Ofelt theory yielding the intensity parameters Ω2 = 5.185, Ω4 = 0.650, Ω6 = 1.068 [10−20 cm2] and α = 0.171 [10−4 cm]. The crystal-field splitting of the Tm3+ multiplets is revealed at 10 K. The first diode-pumped Tm:CLTGG laser generates 1.08 W at ∼2 µm with a slope efficiency of 23.8%. The Tm3+ ions in CLTGG exhibit significant inhomogeneous spectral broadening due to the structure disorder (a random distribution of Ta5+ and Ga3+ cations over octahedral and tetrahedral lattice sites) leading to smooth and broad gain profiles (bandwidth: 130 nm) extending well above 2 µm and rendering Tm:CLTGG suitable for femtosecond pulse generation.
Attosecond investigation of extreme-ultraviolet multi-photon multi-electron ionization
Multi-electron dynamics in atoms and molecules very often occur on sub- to few-femtosecond time scales. The available intensities of extreme-ultraviolet (XUV) attosecond pulses have previously allowed the time-resolved investigation of two-photon, two-electron interactions. Here we study double and triple ionization of argon atoms involving the absorption of up to five XUV photons using a pair of intense attosecond pulse trains (APTs). By varying the time delay between the two APTs with attosecond precision and the spatial overlap with nanometer precision, we obtain information on complex nonlinear multi-photon ionization pathways. Our experimental and numerical results show that Ar2+ is predominantly formed by a sequential two-photon process, whereas the delay dependence of the Ar3+ ion yield exhibits clear signatures of the involvement of a simultaneous two-photon absorption process. Our experiment suggests that it is possible to investigate multi-electron dynamics using attosecond pulses for both pumping and probing the dynamics.
In situ temporal measurement of ultrashort laser pulses at full power during high-intensity laser–matter interactions
In laser-matter interaction experiments, it is of paramount importance to characterize the laser pulse on target (in situ) and at full power. This allows pulse optimization and meaningful comparison with theory, and it can shed fundamental new light on pulse distortions occurring in or on the target.Here we introduce and demonstrate a new technique based on dispersion-scan using the concurrent third harmonic emission from the target that permits the full (amplitude and phase), in situ, in-parallel characterization of ultrashort laser pulses in a gas or solid target over a very wide intensity range encompassing the 1013-1015Wcm-2regime of high harmonic generation and other important strong-field phenomena, with possible extension to relativistic intensities presently inaccessible to other diagnostics. © 2020 OSA - The Optical Society. All rights reserved.
Spectroscopy of solid-solution transparent sesquioxide laser ceramic Tm:LuYO3
We report on a detailed spectroscopic study of a Tm3+-doped transparent sesquioxide ceramic based on a solid-solution (lutetia – yttria, LuYO3) composition. The ceramic was fabricated using commercial oxide powders by hot isostatic pressing at 1600°C for 3 h at 190 MPa argon pressure. The most intense Raman peak in Tm:LuYO3 at 385.4 cm−1 takes an intermediate position between those for the parent compounds and is notably broadened (linewidth: 12.8 cm−1). The transition intensities of Tm3+ ions were calculated using the Judd-Ofelt theory; the intensity parameters are W2 = 2.537, W4 = 1.156 and W6 = 0.939 [1020 cm2]. For the 3F4 → 3H6 transition, the stimulated-emission cross-section amounts to 0.27 × 10−20 cm2 at 2059nm and the reabsorption-free luminescence lifetime is 3.47 ms (the 3F4 radiative lifetime is 3.85 ± 0.1 ms). The Tm3+ ions in the ceramic exhibit long-wave multiphonon-assisted emission extending up to at least 2.35 µm; a phonon sideband at 2.23 µm is observed and explained by coupling between electronic transitions and the dominant Raman mode of the sesquioxides. Low temperature (12 K) spectroscopy reveals a significant inhomogeneous spectral broadening confirming formation of a substitutional solid-solution. The mixed ceramic is promising for ultrashort pulse generation at >2 µm.