Controlled terahertz emission and electron localization dynamics in semiconductors.

Dynamic localization has been thoroughly studied since 1986 by Dunlap in superlattice structures. However, its implications for terahertz (THz) radiation have not been fully explored. Here, we investigate the interplay between dynamic localization and THz radiation generation in semiconductor structures. Utilizing a two-color laser field, we reveal that intraband current is the primary source of THz radiation. Furthermore, we identify minima in THz radiation yield at specific laser field strengths, indicating the presence of dynamic localization. The relative phase of the two-color laser field and dephasing time can manipulate the extent and range of dynamic localization, thereby influencing the efficiency of THz radiation. Our findings provide valuable insights into simultaneous investigations on materials across different time scales.

Raman time-delay in attosecond transient absorption of strong-field created krypton vacancy.

Strong field ionization injects a transient vacancy in the atom which is entangled to the outgoing photoelectron. When the electron is finally detached, the ion is populated at different excited states with part of coherence information lost. The preserved coherence of matter after interacting with intense short pulses has important consequences on the subsequent nonequilibrium evolution and energy relaxation. Here we employ attosecond transient absorption spectroscopy to measure the time-delay of resonant transitions of krypton vacancy during their creation. We have observed that the absorptions by the two spin-orbit split states are modulated at different paces when varying the time-delay between the near-infrared pumping pulse and the attosecond probing pulse. It is shown that the coupling of the ions with the remaining field leads to a suppression of ionic coherence. Comparison between theory and experiments uncovers that coherent Raman coupling induces time-delay between the resonant absorptions, which provides insight into laser-ion interactions enriching attosecond chronoscopy.

The thermodynamic-pathway-determined microstructure evolution of copper under shock compression.

Shock-induced structural transformations in copper exhibit notable directional dependence and anisotropy, but the mechanisms that govern the responses of materials with different orientations are not yet well understood. In this study, we employ large-scale non-equilibrium molecular dynamics simulations to investigate the propagation of a shock wave through monocrystal copper and analyse the structural transformation dynamics in detail. Our results indicate that anisotropic structural evolution is determined by the thermodynamic pathway. A shock along the [Formula: see text] orientation causes a rapid and instantaneous temperature spike, resulting in a solid-solid phase transition. Conversely, a liquid metastable state is observed along the [Formula: see text] orientation due to thermodynamic supercooling. Notably, melting still occurs during the [Formula: see text]-oriented shock, even if it falls below the supercooling line in the thermodynamic pathway. These results highlight the importance of considering anisotropy, the thermodynamic pathway and solid-state disordering when interpreting phase transitions induced by shock. This article is part of the theme issue 'Dynamic and transient processes in warm dense matter'.

Destructive interference in N2+ lasing.

We report an unexpected experimental observation in rotation-resolved N2+ lasing that the R-branch lasing intensity from a single rotational state in the vicinity of 391 nm can be greatly stronger than the P-branch lasing intensity summing over the total rotational states at suitable pressures. According to a combined measurement of the dependence of the rotation-resolved lasing intensity on the pump-probe delay and the rotation-resolved polarization, we speculate that the destructive interference can be induced for the spectrally-indistinguishable P-branch lasing due to the propagation effect while the R-branch lasing is little affected due to its discrete spectral property, after precluding the role of rotational coherence. These findings shed light on the air-lasing physics, and provide a feasible route to manipulate air lasing intensity.

Strongly anisotropic ultrafast dynamic behavior of GaTe dominated by the tilted and flat bands.

The anisotropic transport properties of gallium telluride (GaTe) have been reported by several experiments, giving rise to many debates recently. The anisotropic electronic band structure of GaTe shows the extreme difference between the flat band and tilted band in two distinct directions,Γ¯-X¯andΓ¯-Y¯, and which we called as the mixed flat-tilted band (MFTB). Focusing on such two directions, the relaxation of photo-generated carriers has been studied using the non-adiabatic molecular dynamics (NAMD) method to investigate the anisotropic behavior of ultrafast dynamics. The results show that the relaxation lifetime is different in flat band direction and tilted band direction, which is evidence for the existence of anisotropic behavior of the ultrafast dynamic, and such anisotropic behavior comes from the different intensities of electron-phonon coupling of the flat band and tilted band. Furthermore, the ultrafast dynamic behavior is found to be affected strongly by spin-orbit coupling (SOC) and such anisotropic behavior of the ultrafast dynamic can be reversed by SOC. The tunable anisotropic ultrafast dynamic behavior of GaTe is expected to be detected in ultrafast spectroscopy experiments and it may provide a tunable application in nanodevice design. The results may also provide a reference for the investigation of MFTB semiconductors.

Fast phase retrieval for broadband attosecond pulse characterization.

Efficient characterization method for broadband attosecond pulses has become more and more essential, since attosecond pulses with bandwidth spanning few-hundreds electron-volts have been generated. Here we propose a fast phase retrieval algorithm for broadband attosecond pulse characterization with an omega oscillation filtering technique. We introduce a new error function to improve the accuracy of the retrieved phases. More importantly, it can be solved by the steepest descent methods with iterative algorithm, which is much faster than genetic algorithm adopted previously. An experimental spectrogram for isolated attosecond pulses with photon energy covering 52-127 eV and a pulse width of 71 as was successfully retrieved with this method as demonstrated. The proposed technique will help provide real-time feedback on atto-chirp compensation for ultrashort isolated attosecond pulse generation.

Broadband Terahertz Detection by Laser Plasma with Balanced Optical Bias.

Using a controlled optical bias and balanced geometry, we propose a new scheme for broadband terahertz detection by laser-gas interaction without high-voltage manipulation. Compared to the conventional optical bias scheme, the common noise is reduced and the dynamic range as well as the signal-to-noise ratio are doubled. It provides a simple alternative for coherent broadband terahertz detection. The influence of optical bias on terahertz waveform is also investigated, and the evolution of the terahertz-induced second harmonic with probe delay is further revealed. This new detection scheme for broadband terahertz will boost the application of terahertz time-domain spectroscopy for its miniaturization and integrability.

Proposal for High-Energy Cutoff Extension of Optical Harmonics of Solid Materials Using the Example of a One-Dimensional ZnO Crystal.

We propose a novel approach based on the subcycle injection of carriers to extend the high-energy cutoff in solid-state high harmonics. The mechanism is first examined by employing the standard single-cell semiconductor Bloch equation (SC SBE) method for one-dimensional (1D) Mathieu potential model for ZnO subjected to the intense linearly polarized midinfrared laser field and extreme-ultraviolet pulse. Then, we use coupled solution of Maxwell propagation equation and SC SBE to propagate the fundamental laser field through the sample, and find that the high-harmonics pulse train from the entrance section of the sample can inject carriers to the conduction bands with attosecond timing, subsequently leading to a dramatic extension of high-energy cutoff in harmonics from the backside. We predict that for a peak intensity at 2×10^{11} W/cm^{2}, as a result of the self-seeding, the high-energy cutoff shifts from 20th (7.75 eV) order to around 50th (19.38 eV) order harmonics.

Ultraviolet supercontinuum generation driven by ionic coherence in a strong laser field.

Supercontinuum (SC) light sources hold versatile applications in many fields ranging from imaging microscopic structural dynamics to achieving frequency comb metrology. Although such broadband light sources are readily accessible in the visible and near infrared regime, the ultraviolet (UV) extension of SC spectrum is still challenging. Here, we demonstrate that the joint contribution of strong field ionization and quantum resonance leads to the unexpected UV continuum radiation spanning the 100 nm bandwidth in molecular nitrogen ions. Quantum coherences in a bunch of ionic levels are found to be created by dynamic Stark-assisted multiphoton resonances following tunneling ionization. We show that the dynamical evolution of the coherence-enhanced polarization wave gives rise to laser-assisted continuum emission inside the laser field and free-induction decay after the laser field, which jointly contribute to the SC generation together with fifth harmonics. As proof of principle, we also show the application of the SC radiation in the absorption spectroscopy. This work offers an alternative scheme for constructing exotic SC sources, and opens up the territory of ionic quantum optics in the strong-field regime.

Novel Braceletlike BiSbX3 (X = S, Se) Monolayers with an In-Plane Negative Poisson's Ratio and Anisotropic Photoelectric Properties.

In this work, we predict two novel two-dimensional (2D) auxetic materials, BiSbX3 (X = S, Se) monolayers, through first-principles calculations. Attributed to their special braceletlike structure, the in-plane negative Poisson's ratio (NPR) of BiSbS3 and BiSbSe3 monolayers are as high as -0.25 and -0.26, respectively. The phonon dispersion calculations, ab initio molecular dynamics simulations, and elastic constants calculations demonstrate that these two monolayers possess excellent dynamic, thermal, and mechanical stabilities. The band gap values of BiSbS3 and BiSbSe3 calculated at the HSE level by considering the spin-orbit coupling (SOC) effect are 1.68 and 1.20 eV. The anisotropic carrier mobility and superior optical absorption indicate that they may shine in the next generation of electronic and optoelectronic devices. All of these discoveries not only enrich the types of auxetic materials but also provide a structural reference for designing new auxetic materials on the molecular level. Furthermore, they can provide theoretical guidance for future applications of BiSbX3 (X = S, Se) monolayers in various fields.

Revealing Molecular Strong Field Autoionization Dynamics.

The novel strong field autoionization (SFAI) dynamics is identified and investigated by channel-resolved angular streaking measurements of two electrons and two ions for the double-ionized CO. Comparing with the laser-assisted autoionization calculations, we demonstrate the electrons from SFAI are generated from the field-induced decay of the autoionizing state with a following acceleration in the laser fields. The energy-dependent photoelectron angular distributions further reveal that the subcycle ac-Stark effect modulates the lifetime of the autoionizing state and controls the emission of SFAI electrons in molecular frame. Our results pave the way to control the emission of resonant high-harmonic generation and trace the electron-electron correlation and electron-nuclear coupling by strong laser fields. The lifetime modulation of quantum systems in the strong laser field has great potential for quantum manipulation of chemical reactions and beyond.

Photon retention in coherently excited nitrogen ions.

Quantum coherence in quantum optics is an essential part of optical information processing and light manipulation. Alkali metal vapors, despite the numerous shortcomings, are traditionally used in quantum optics as a working medium due to convenient near-infrared excitation, strong dipole transitions and long-lived coherence. Here, we proposed and experimentally demonstrated photon retention and subsequent re-emittance with the quantum coherence in a system of coherently excited molecular nitrogen ions (N2+) which are produced using a strong 800 nm femtosecond laser pulse. Such photon retention, facilitated by quantum coherence, keeps releasing directly-unmeasurable coherent photons for tens of picoseconds, but is able to be read out by a time-delayed femtosecond pulse centered at 1580 nm via two-photon resonant absorption, resulting in a strong radiation at 329.3 nm. We reveal a pivotal role of the excited-state population to transmit such extremely weak re-emitted photons in this system. This new finding unveils the nature of the coherent quantum control in N2+ for the potential platform for optical information storage in the remote atmosphere, and facilitates further exploration of fundamental interactions in the quantum optical platform with strong-field ionized molecules..

Enhanced resonant vibrational Raman scattering of N2+ induced by self-seeding ionic lasers created in polarization-modulated intense laser fields.

We report on an experimental investigation of the five vibrational Raman lines at 358 nm, 388 nm, 391 nm, 428 nm, and 471 nm of N2+ resonantly driven by the self-seeding ionic lasers generated by a polarization-modulated (PM) or alternatively a linearly polarized (LP) femtosecond laser. It was found that the spectral intensities of several Raman lines can be dramatically enhanced by exploiting the PM laser pulses in comparison to the LP laser pulses. The evaluated Raman conversion efficiency reaches ∼10-2 for some lasing lines at suitable pressures. Moreover, the role of interplay between the seed amplification and the resonant vibrational Raman scattering processes in inducing the gain of N2+ lasing is characterized for the first time. The developed vibrational Raman spectroscopy with intense ultrafast lasers provides an additional approach to interrogate the products in a femtosecond filament, and it therefore can be a powerful tool for identifying chemical species at remote distances in the atmosphere.

Time-resolved recombination by attosecond-controlled high harmonic generation.

We theoretically investigate the coherent control of strong-field high-harmonic generation in the presence of an isolated attosecond pulse. It is found that the rapid modulation of the controlled signal exhibits interference fringe structures in the delay-dependent spectra. By comparing the classical trajectory model with quantum mechanical calculation, it is demonstrated that the fringes are resulted from the interference between the photon- and the tunnelling-initiated recombination pathways. The relative recombination times for the two paths are reconstructed from the interference fringes, which provides a novel scheme for optical observation of the interplay of the photionization and tunneling ionization electron dynamics in attosecond resolution.

Mechanism and control of rotational coherence in femtosecond laser-driven N2.

We investigate the formation of rotational coherence of N2+ resonantly interacting with an intense femtosecond laser field by numerical simulations based on a strong-field ionization-coupling model described with the density matrix formalism. The created N2+ system is unique in many aspects: the variable total population within the pump duration due to the intensity-dependent ionization injection, the readily accessible resonance owing to the effect of Stark shift, and the involvement of a few dozen of quantum states. By regarding the N2+ system as an open and non-stationary Λ-type cascaded multi-level system, we quantitatively studied the dependence of rotational coherence in different electronic-vibrational states of N2+ on the alignment angle θ and the pumping intensity. Our simulation results indicate that the quantum coherence between the neighbouring rotational states of J, J+2 in the vibrational state ν=0, 1 of the ground state of N2+ can be changed from a negative to a positive. The significant contribution of rotational coherence to inducing an extra gain or absorption of N2+ air lasing is further verified by solving the Maxwell's propagating equation. The finding provides crucial clues on how to manipulate N2+ lasing by controlling the rotational coherence and paves the way to studying strong-field quantum optics effects such as lasing without inversion and electromagnetically induced transparency in molecular ionic systems.

Erratum: Extremely Low Electron-ion Temperature Relaxation Rates in Warm Dense Hydrogen: Interplay between Quantum Electrons and Coupled Ions [Phys. Rev. Lett. 122, 015001 (2019)].

This corrects the article DOI: 10.1103/PhysRevLett.122.015001.

Extremely Low Electron-ion Temperature Relaxation Rates in Warm Dense Hydrogen: Interplay between Quantum Electrons and Coupled Ions.

Theoretical and computational modeling of nonequilibrium processes in warm dense matter represents a significant challenge. The electron-ion relaxation process in warm dense hydrogen is investigated here by nonequilibrium molecular dynamics using the constrained electron force field (CEFF) method. CEFF evolves wave packets that incorporate dynamic quantum diffraction that obviates the Coulomb catastrophe. Predictions from this model reveal temperature relaxation times as much as three times longer than prior molecular dynamics results based on quantum statistical potentials. Through analyses of energy distributions and mean free paths, this result can be traced to delocalization. Finally, an improved GMS [Gericke, Murillo, and Schlanges, Phys. Rev. E 78, 025401 (2008)PRESCM1539-375510.1103/PhysRevE.78.025401] model is proposed, in which the Coulomb logarithms are in good agreement with CEFF results.

In situ spatial mapping of Gouy phase slip with terahertz generation in two-color field.

We establish a one-to-one mapping between the local phase slip and the spatial position near the focus by scanning a thin jet along the propagation direction of laser beams. The measurement shows that the optimal phase of terahertz can be utilized to characterize in situ the spatially dependent relative phase of the two-color field. We also investigate the role of the Gouy phase shift on terahertz generation from two-color laser-induced plasma. The result is of critical importance for phase-dependent applications of two-color laser-field, including high-order harmonic and terahertz generation.

Coherence and resonance effects in the ultra-intense laser-induced ultrafast response of complex atoms.

Both coherent pumping and energy relaxation play important roles in understanding physical processes of ultra-intense coherent light-matter interactions. Here, using a large-scale quantum master equation approach, we describe dynamical processes of practical open quantum systems driven by both coherent and stochastic interactions. As examples, two typical cases of light-matter interactions are studied. First, we investigate coherent dynamics of inner-shell electrons of a neon gas irradiated by a high-intensity X-ray laser along with vast number of decaying channels. In these single-photon dominated processes, we find that, due to coherence-induced Rabi oscillations and power broadening effects, the photon absorptions of a neon gas can be suppressed resulting in differences in ionization processes and final ion-stage distributions. Second, we take helium as an example of multiphoton and multichannel interference dominated electron dynamics, by investigating the transient absorption of an isolated attosecond pulse in the presence of a femtosecond infrared laser pulse.

Joint Measurements of Terahertz Wave Generation and High-Harmonic Generation from Aligned Nitrogen Molecules Reveal Angle-Resolved Molecular Structures.

We report the synchronized measurements of terahertz wave generation and high-harmonic generation from aligned nitrogen molecules in dual-color laser fields. Both yields are found to be alignment dependent, showing the importance of molecular structures in the generation processes. By calibrating the angular ionization rates with the terahertz yields, we present a new way of retrieving the angular differential photoionization cross section (PICS) from the harmonic signals which avoids specific model calculations or separate measurements of the alignment-dependent ionization rates. The measured PICS is found to be consistent with theoretical predications, although some discrepancies exist. This all-optical method provides a new alternative for investigating molecular structures.