arXiv subjects

Zengxiu Zhao

Publications and source records attributed to Zengxiu Zhao.

At least 19 recordsLinked to original sources

arXiv2025

Terahertz frequency conversion at plasma-induced time boundary

We report on the frequency conversions of terahertz (THz) waves at ultrafast time boundaries created via femtosecond laser-induced air-to-plasma phase transitions. Our combined experimental and theoretical approach reveals that the abrupt change in refractive index at the ultrafast time boundaries drives both the red and blue shifts over the broadband THz spectrum due to the dispersive plasma, with distinctive amplitude variations. The present study contrasts these effects with those from spatial boundaries, highlighting the superior efficacy of temporal manipulations for spectral engineering. These findings not only deepen the understanding of light-matter interactions in time-varying media but also pave the way for innovative applications in THz technology and lay the groundwork for the observation of temporal reflection effects, photonic time crystals, and spatio-temporally modulated matter.

physics.optics↗

arXiv2024

Electronic-vibrational dynamics and coherence in x-ray transient absorption of N2+ induced by strong-field ionization

Attosecond transient absorption spectroscopy (ATAS) is becoming an indispensable and powerful tool in the emerging field of attochemistry, while the interpretation of measurements often requires full considerations of the coupling among various freedoms of motion. Here we develop the ionization-coupling model to incorporate the transient absorption and explore the coupled electronic-vibrational dynamics of nitrogen ions induced by strong-field ionization (SFI), which has been investigated in the recent transient x-ray K-edge absorption experiment [PRL 129, 123002 (2022)]. It is found the coherent vibrational wave packet on the involved electronic state is created with broad distribution of vibrational levels which leads to the spectral overlap on the K-edge absorption. By identifying the contributions of each electronic state, the study provides a different interpretation revealing the significant role of the excited state $A^2Π_u$ arising from the electronic-vibrational coupling in strong laser fields. We uncover new features of absorption from forbidden transitions during the laser pulse and confirm the vibronic coherence induced modulations of absorbance after SFI. A new scheme is proposed to avoid the spectral overlap and determine the population among the states which is crucial to resolve the debate on nitrogen air lasing. The work lays down the framework to research the ionic coherence in ATAS and offers valuable insights into the intricate interplay between electronic and vibrational dynamics.

physics.optics↗

arXiv2024

On the Nonlinear Excitation of Phononic Frequency Combs in Molecules

The mechanical analog of optical frequency combs, phononic frequency combs (PFCs), has recently been demonstrated in mechanical resonators via nonlinear coupling among multiple phonon modes. However, for exciting phononic combs in molecules, the requisite strong nonlinear couplings need not be readily present. To overcome this limitation, this paper introduces an alternative route for the generation of phononic combs in polar molecules. Theoretically, we investigated the radiation and phononic spectra generated from CO molecule possessing relatively large permanent dipole moment with density matrix formalism. By considering rovibronic excitation of the ground-state CO molecule while avoiding the electronic excitation, the contribution of the permanent dipole moment and electric dipole polarizability to the creation of PFCs is demonstrated and distinguished. The finding could motivate the possible extension of combs to molecular systems to offer new avenues in molecular sciences.

cond-mat.mes-hall↗

arXiv2024

Theoretical evidence of H-He demixing under Jupiter and Saturn conditions

The immiscibility of hydrogen-helium mixture under the temperature and pressure conditions of planetary interiors is crucial for understanding the structures of gas giant planets (e.g., Jupiter and Saturn). While the experimental probe at such extreme conditions is challenging, theoretical simulation is heavily relied in an effort to unravel the mixing behavior of hydrogen and helium. Here we develop a method via a machine learning accelerated molecular dynamics simulation to quantify the physical separation of hydrogen and helium under the conditions of planetary interiors. The immiscibility line achieved with the developed method yields substantially higher demixing temperatures at pressure above 1.5 Mbar than earlier theoretical data, but matches better to the experimental estimate. Our results suggest a possibility that H-He demixing takes place in a large fraction of the interior radii of Jupiter and Saturn, i.e., 27.5% in Jupiter and 48.3% in Saturn. This indication of an H-He immiscible layer hints at the formation of helium rain and offers a potential explanation for the decrease of helium in the atmospheres of Jupiter and Saturn.

physics.comp-ph↗

arXiv2024

Coherent XUV super continuum emission from atomic bound states

Coherent supercontinuum radiation in the extreme-ultraviolet (XUV) range is indispensable for synthesizing attosecond light pulses and for exploring transient atomic structures. Here, we report the striking observations of coherent XUV supercontinuum (XSC) extended from below to far above the ionization threshold, which exhibits completely different temporal and spatial properties comparing to the conventional rescattering induced high harmonic generation (HHG). We demonstrate that the strong-field created coherence among bound orbitals strongly distort the atomic transition energies during the pulse, leading to coherent emission spanning tens of electron-volts, in contrast to the line emission via free-induction decay occurring after the pulse. The supposed non-radiating bound dark states contribute as well by emitting dressed energy through dark-to-bright emission mechanism. All the processes modulated at sub-cycle time scale jointly form this new-type coherent XSC. This work achieves the strong-field attosecond control of the exotic atomic radiation dynamics and provides the means of simultaneous generation of separated attosecond sources, i.e., XSC and HHG, with potential advancing attosecond interferometry.

physics.atom-ph↗

arXiv2023

Enhanced Population on Ionic Excited States by Synchronized Ionization and Multiphoton Resonance

We study population distributions and lasing actions of N_2^+ driven by femtosecond lasers with various wavelengths, and uncover an efficient ionic excitation mechanism induced by synchronized ionization and multiphoton resonance. Our results show that the strongest N_2^+ lasing appears around 1000 nm pump wavelength. At the optimal wavelength, the pump-energy threshold for air lasing generation is reduced by five folds compared with that required by the previous 800 nm pump laser. Simulations based on the ionization-coupling model indicate that although the Stark-assisted three-photon resonance can be satisfied within a broad pump wavelength range, the optimal pump wavelength arises when the dynamic three-photon resonance temporally synchronizes with the ionization injection. In this case, the ionic dipoles created at each half optical cycle have the same phase. The dipole phase locking promotes the continuous population transfer from ionic ground state to the excited state, giving rise to a dramatic increase of excited-state population. This work provides new insight on the photoexcitation mechanism of ions in strong laser fields, and opens up a route for optimizing ionic radiations.

physics.atom-ph↗

arXiv2022

Multiband dynamics of extended harmonic generation in solids under ultraviolet injection

Using one-dimensional semiconductor Bloch equations, we investigate the multiband dynamics of electrons in a cutoff extension scheme employing an infrared pulse with additional UV injection. An extended three-step model is firstly validated to play a dominant role in emitting harmonics in the second plateau. Surprisingly, further analysis employing the acceleration theorem shows that though harmonics in both the primary and secondary present positive and negative chirps, the positive (negative) chirp in the first region is related to the so-called short (long) trajectory, while that in the second region is emitted through `general' trajectory, where electrons tunnelling earlier and recombining earlier contribute significantly. The novel characteristics deepen the understanding of high harmonic generation in solids and may have great significance in attosecond science and reconstruction of band dispersion beyond the band edge.

physics.optics↗

arXiv2022

Multiple-Photon Resonance Enabled Quantum Interference in Emission Spectroscopy of N_2^+

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.

physics.optics↗

arXiv2022

Storage and manipulation of single x-ray photons via nuclear hyperfine splitting

We introduce a technique to store and manipulate single x-ray photons which relies on dynamically controlled absorption via nuclear hyperfine magnetic splitting. This scheme is inherently suitable for storage, on-demand generation and dynamical manipulation of single x-ray photons, for instance, the manipulation of the temporal shape, temporal splitting, the interference between x-ray photons and the control of the polarization. Our approach opens up new paths in x-ray quantum information.

quant-ph↗

arXiv2021

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.

quant-ph↗

arXiv2020

Role of rotational coherence in femtosecond-pulse-driven nitrogen ion lasing

We experimentally investigated the rotationally resolved polarization characteristics of N$_2^+$ lasing at 391 and 428 nm using a pump-seed scheme. By varying the relative angle between the linear polarizations of the pump and seed, it is found that the polarizations of the P and R branches of 391-nm lasing are counter-rotated. By contrast, both branches of 428-nm lasing remain polarized along the pump. The origin of the puzzled abnormal polarization characteristics is found based on a complete physical model that simultaneously includes the transient photoionization and the subsequent coupling among the electronic, vibrational and rotational quantum states of ions.It suggests that the cascaded resonant Raman processes following ionization create negative coherence between the rotational states of $J$ and $J$+2 in the ionic ground state X$^2Σ_g^+(ν=0)$, which leads to mirror-symmetrical polarization for the P and R branches of 391-nm lasing. Both the experiment and theory indicate that the demonstrated rotational coherence plays an extremely pivotal role in clarifying the gain mechanism of N$_2^+$ lasing and opens up the route toward quantum optics under ultrafast strong fields.

physics.atom-ph↗

arXiv2019

Sub-cycle coherent control of ionic dynamics via transient ionization injection

We investigate the interwoven dynamic evolutions of neutral nitrogen molecules together with nitrogen ions created through transient tunnel ionization in an intense laser field. By treating the molecules as open quantum systems, it is found that considering real-time injection of ions and strong couplings among their electronic states, nitrogen molecular ions are primarily populated in the electronically excited states, rather than staying in the ground state as predicted by the well-known tunneling theory. The unexpected result is attributed to sub-cycle switch-on of time-dependent polarization by transient ionization and dynamic Stark shift mediated near-resonant multiphoton transitions. Their combined contribution also causes that the vibrational distribution of N$_2^+$ does not comply with Franck-Condon principle. These findings corroborate the mechanism of nitrogen molecular ion lasing and are likely to be universal. The present work opens a new route to explore the important role of transient ionization injection in strong-field induced non-equilibrium dynamics.

physics.atom-ph↗

arXiv2016

High-harmonic and terahertz wave spectroscopy (HATS) for aligned molecules

We present the experimental and theoretical details of our recent published letter [Phys. Rev. Lett. 115. 123002] on synchronized high-harmonic and terahertz-wave spectroscopy (HATS) from nonadiabatically aligned nitrogen molecules in dual-color laser fields. Associating the alignment-angle dependent terahertz wave generation with the synchronizing high-harmonic signal, the angular differential photoionization cross section (PICS) for molecules can be reconstructed, and the minima of the angle on PICS show great convergence between the theoretical predictions and the experimental deduced results. We also show the optimal relative phase between the dual-color laser fields for terahertz wave generation dose not change with the alignment angle at a precision of $50$ attoseconds. This all-optical method provides an alternative for investigating molecular structures and dynamics.

physics.atom-ph↗

arXiv2016

Strong-field ionization inducing multi-electron-hole coherence probed by attosecond pulses

We propose a new scenario to apply IR-pump-XUV-probe schemes to resolving strong field ionization induced and attosecond pulse driven electron-hole dynamics and coherence in real time. The coherent driving of both the infrared laser and the attoscond pulse correlates the dynamics of the core-hole and the valence-hole which leads to the otherwise forbidden absorption and emission of XUV photon. An analytical model is developed based on the strong-field approximation by taking into account of the essential multielectron configurations. The emission spectra from the core-valence transition and the core-hole recombination are found modulating strongly as functions of the time delay between the two pulses, which provides a unique insight into the instantaneous ionization and the interplay of the multi-electron-hole coherence.

physics.atom-ph↗

arXiv2015

Theoretical study of terahertz generation from atoms and aligned molecules driven by two-color laser fields

We study the generation of terahertz radiation from atoms and molecules driven by an ultrashort fundamental laser and its second harmonic field by solving time-dependent Schrödinger equation (TDSE). The comparisons between one-, two-, and three- dimensional TDSE numerical simulations show that initial ionized wave-packet and its subsequent acceleration in the laser field and rescattering with long-range Coulomb potential play key roles. We also present the dependence of the optimum phase delay and yield of terahertz radiation on the laser intensity, wavelength, duration, and the ratio of two-color laser components. Terahertz wave generation from model hydrogen molecules are further investigated by comparing with high harmonic emission. It is found that the terahertz yield is following the alignment dependence of ionization rate, while the optimal two-color phase delays varies by a small amount when the alignment angle changes from 0 to 90 degrees, which reflects alignment dependence of attosecond electron dynamics. Finally we show that terahertz emission might be used to clarify the origin of interference in high harmonic generation from aligned molecules by coincidently measuring the angle-resolved THz yields.

physics.atom-ph↗

arXiv2015

Analysis of interference in attosecond transient absorption in adiabatic condition

We simulate the transient absorption of attosecond pulses of infrared-laser-dressed atoms by considering a three-level system with the adiabatic approximation. The delay-dependent interference features are investigated from the perspective of the coherent interaction processes between the attosecond pulse and the quasi-harmonics. We find that many features of the interference fringes in the absorption spectra of the attosecond pulse can be attributed to the coherence phase difference. However, the modulation signals of laser-induced sidebands of the dark state is found related to the population dynamics of the dark state by the dressing field.

physics.atom-ph↗

arXiv2014

Rydberg states generation of Hydrogen atoms with intense laser pulses: the roles of Coulomb force and initial lateral momentum

We investigate the Rydberg states generation of Hydrogen atoms with intense laser pulses, by solving the time-dependent Schrödinger equation and by means of classical trajectory monte-carlo simulations. Both linearly polarized multi-cycle pulses and pairs of optical half cycle pulses are used. Comparisons between these methods show that both the Coulomb force and initial lateral momentum, which have effects on the $n$-distribution and $l$-distribution of the population of excited states, are important in the generation of Rydberg states.

physics.atom-ph↗

arXiv2014

Dynamic orbitals in high-harmonic generation from CO molecules

We identify that both the dynamic core polarization and dynamic orbital deformation are important in the orientation-dependent high-harmonic generation of CO molecules subjected to intense few cycle laser fields. These polarization dynamics allow for the observation of strong orientation effects and dynamic minimum in the harmonic spectra. The generated attosecond pulses can be greatly affected by these multielectron effects. This work sheds light on future development of dynamic orbital imaging on attosecond time scale.

physics.atom-ph↗