arXiv subjects

Yuhai Jiang

Publications and source records attributed to Yuhai Jiang.

16 recordsLinked to original sources

arXiv2026

Tailoring optical Schrödinger cat states via orientation-dependent high-harmonic generation in $\rm{H}_2^+$

We theoretically demonstrate that the molecular orientation angle $θ$ provides a structurally intrinsic, continuously tunable control parameter for engineering optical Schrödinger cat states via high-harmonic generation (HHG) in H$_2^+$. Coupling time-dependent Schrödinger equation simulations to the fully quantized HHG framework, we evaluate the Wigner functions of the post-selected harmonic-mode states under two complementary conditioning strategies. Conditioning on resonance-enhanced low-order harmonics exploits the complementary dipole selection rules of the $1σ_g\to1σ_u$ and $1σ_g\to1π_u$ transitions, driving a kitten-cat crossover whose direction is opposite in the two channels as $θ$ is varied. Conditioning on plateau harmonics instead exploits two-center destructive interference, producing a reentrant cat$\to$kitten$\to$cat transition controlled by the order-dependent interference angle $θ^*(q)$. In both cases the crossover is decoupled from the laser intensity, focal geometry, and molecular density, offering a degree of control with no counterpart in atomic targets.

quant-ph↗

arXiv2026

Observation of Strong Electron Correlation in Planetary Atomic Structure

Unravelling two-electron correlation is a long-standing challenge at the heart of few-body quantum physics, underlying correlated phenomena across atomic, molecular and condensed-matter science. In prototypical three-body Coulomb systems, such strong correlation in doubly excited states (DESs) of planetary atomic systems leaves distinct signatures in nonsequential above-threshold double ionization (NS-ATDI) driven by coherent laser fields, yet such targeted study has long remained elusive. Here we present kinematically complete measurements of multi-photon double ionization in cold strontium atoms. Our results reveal a dominant NS-ATDI channel exhibiting well-defined band structures that encode pronounced energy and angular correlations between the two emitted electrons. Autoionization spectra confirm the presence of DESs as transition states that effectively promote the NS-ATDI process. These observations provide direct evidence that both electrons are synchronously excited and ionized via resonant high-lying DES transitions, meaning the structure-linked two-electron correlation of DES is preserved and propagated in the laser-driven time-dependent three-body system. Our work transcends the traditional paradigm of multi-photon double ionization, and fundamentally reshapes the core understanding of intrinsic electron correlation governing many-body systems in nature.

physics.atom-ph↗

arXiv2026

Symmetry-Breaking Electron Dynamics Enable Ultrabroadband Optical-Field Sampling via Second-Harmonic Generation

Optical-field sampling using second-harmonic generation (SHG) from strong-field ionization enables ultrabroadband terahertz detection, but the microscopic origin of the SHG signal and its ultrabroadband response have been unclear. Here we show that the target field lifts the half-cycle cancellation of photoelectron dipole emission, generating the SHG signal used for field sampling. Time-dependent Schrodinger-equation simulations, supported by classical-trajectory Monte Carlo analysis, demonstrate that the SHG yield directly encodes the instantaneous target electric field at the ionization time, enabling waveform retrieval by scanning the probe-target delay. Because the SHG response is gated by a subcycle ionization window rather than the probe envelope, the detection bandwidth can extend far beyond the probe duration. We further quantify practical constraints on retrieval, including intrinsic probe asymmetry and SHG back-action, providing a predictive framework to optimize sensitivity, temporal resolution, and fidelity through controlled electron dynamics.

physics.optics↗

arXiv2026

Experimental Realization of All-Optical Terahertz Attoclock

The attoclock is a powerful tool for probing ultrafast electron dynamics with attosecond precision.Here, we demonstrate an all-optical terahertz (THz) attoclock that reconstructs photoionization dynamics by detecting the THz radiation emitted from Ar atoms ionized by two-color (800 nm/400 nm) laser fields. In this approach, the polarization direction of the emitted THz field reflects the direction of the photoelectron drift velocity and thus serves as a direct observable that encodes the effective ionization delay, analogous to the angular deflection of photoelectrons in conventional attoclocks. By precisely tailoring the relative phase and ellipticity of the driving fields, we observe intensity-dependent rotations of the THz polarization. These rotations, which reveal changes of the effective delay, are consistent with both conventional attoclock measurements and time-dependent Schrödinger equation simulations. Our experiment establishes the feasibility of the THz attoclock as a vacuum-free and contactless probe of tunneling dynamics, offering a transformative alternative for investigating condensed-matter systems where photoelectron detection is challenging.

physics.optics↗

arXiv2026

Multiple charge transfer driven complex reaction dynamics: covalent bonding meets van der Waals interactions

Ultrafast charge transfer (CT) processes redistribute electronic charge within and between molecular units and play a central role in many physical, chemical, and biological phenomena. However, the microscopic pathways of multiple CT events, including the coupled structural evolution and energy redistribution, are challenging to disentangle experimentally in complex systems. To obtain controlled insight into such dynamics, well-defined properties are required. Here, we investigate the N2Ar dimer, which combines a covalent bond with a weak van der Waals interaction, using site-selective synchrotron photoionization and coincident detection of electrons and ions. Combined with ab initio calculations, this approach enables step-by-step tracking of ultrafast CT and fragmentation dynamics. We find that the dimer's structural evolution triggers a second CT event, opening complex reaction pathways in which electrons are transferred back and forth between Ar and N2, through two nonadiabatic transitions involving conical intersections. These results demonstrate that sequential multiple CT-induced transitions, even in a simple dimer, provide controlled insight into nonadiabatic reaction mechanisms relevant to complex systems.

physics.chem-ph↗

arXiv2024

Probing Electronic Motion and Core Potential by Coulomb-reshaped Terahertz Radiation

The nature of electronic motion and structural information of atoms and molecules is encoded into strong-field induced radiations ranging from terahertz (THz) to extreme ultraviolet wavelength. The dependence of THz yields in bi-chromatic laser fields on ellipticity and interpulse phase delay were experimentally measured, and the trajectory calculations establish the link between the THz emission and the motion of the photoelectron wave packet. The interaction between the photoelectron and parent core transforms from soft collision to recollision as the laser field tuned from elliptical to linear polarization, which can be reflected in THz emission. The soft collision is found to be more effective in reconstructing electron dynamics through THz polarization, which enables to construct the effective core potential of the generating medium with the Coulomb-reshaped THz radiation in an elliptically polarized laser field. Our work allows designing innovative all-optical THz measurements of electronic and structural dynamics.

physics.atom-ph↗

arXiv2024

Temporal-Spatial Manipulation of Bi-Focal Bi-Chromatic Fields for Terahertz Radiations

Mixing the fundamental ($ω$) and the second harmonic (2$ω$) waves in gas phase is a widely employed technique for emitting terahertz (THz) pulses. The THz generation driven by bi-chromatic fields can be described by the photocurrent model, where the THz generation is attributed to free electrons ionized by the $ω$ field, and the 2$ω$ field provides a perturbation to break the symmetry of the asymptotic momentum of free electrons. However, we find that the THz radiation is amplified by one order of magnitude when driven by bi-focal bi-chromatic fields, contradicting the common understanding of the photocurrent model. Meanwhile, present measurements demonstrate that the THz radiation mainly originates from the plasma created by the 2$ω$ pulses instead of the $ω$ pulses. Energy transfer from the 2$ω$ beam to the THz beam during the THz generation has been observed, validating the major contribution of the 2$ω$ beam. Furthermore, the THz bandwidth has been observed to extensively exceed the bandwidth of the pump pulse, not be explained by the photocurrent model as well. These counterintuitive results indicate that undiscovered physical mechanisms are involved in bi-chromatic THz generation in plasma, presenting a significant challenge for understanding strong-field nonlinear optics and simultaneously expanding various applications.

physics.optics↗

arXiv2023

Magneto-optical trap reaction microscope for photoionization of cold strontium atoms

We developed a magneto-optical trap reaction microscope (MOTREMI) for strontium atoms by combining the multi-particle coincident detection with laser cooling technique. Present compact injection system can provide cold Sr atoms in three modes of 2D MOT, molasses and 3D MOT, delivering targets with adjustable densities and ratios of the ground state $5s^2$ ($^1S_{0}$) and the excited states $5s5p$ ($^{1}P_{1}$ and $^{3}P_{J}$ etc). The target profiles for the temperature, the density and the size of 3D MOT as well as cold atomic flux in 2D MOT model were characterized in details. With present state-of-the-art setup, we demonstrated the single photoionization of Sr atoms with molasses by absorption of few 800-nm photons, where Sr$^+$ and $e$ were detected in coincidence and most of ionization channels were identified taking into account photoelectron energy, laser-intensity dependence, and target dependence. The best momentum resolution of coincident Sr$^+$ and $e$ along time-of-flight are achieved up to 0.12 a.u. and 0.02 a.u., respectively. Present photoelectron momentum distributions ionized from the ground state and a few excited states illuminate unprecedentedly rich landscapes manifesting prominent features for multi-photon absorption. The full vector momenta of electrons and recoil ion in coincidence paves the way to further studying two-electron correlation dynamics and multi-electron effects in the multiple ionization of alkaline-earth atoms in the ultraviolet region.

physics.atom-ph↗

arXiv2023

Few-photon single ionization of cold rubidium in the over-the-barrier regime

Photoionization of the rubidium (Rb) atoms cooled in a magneto-optical trap, characterized by the coexistence of the ground 5$S_{1/2}$ and the excited 5$P_{3/2}$ states, is investigated experimentally and theoretically with the 400 nm femtosecond laser pulses at intensities of $I=3\times10^9$ W/cm$^2$ - $4.5\times10^{12}$ W/cm$^2$. Recoil-ion momentum distribution (RIMD) of Rb$^+$ exhibits rich ring-like structures and their energies correspond to one-photon ionization of the 5$P_{3/2}$ state, two-photon and three-photon ionizations of the 5$S_{1/2}$ state, respectively. With the increasing of $I$, we find that experimental signals near zero-momentum (NZM) in RIMDs resulted from the 5$P_{3/2}$ state enhance dramatically and its peaked Rb$^+$ momenta dwindle obviously while that from the 5$S_{1/2}$ state is maintained. Meanwhile, the ion-yield ratio of the 5$S_{1/2}$ over the 5$P_{3/2}$ states varies from $I$ to $I^{1.5}$ as $I$ increases. These features indicate a transition from perturbative ionization to strong-perturbative ionization for the 5$P_{3/2}$ state. Numerical simulations by solving the time-dependent Schrödinger equation (TDSE) can qualitatively explain the measurements of RIMD, photoion angular distributions, as well as ion-yield ratio. However, some discrepancies still exist, especially for the NZM dip, which could stem from the electron-electron correlation that is neglected in the present TDSE simulations since we have adopted the single-active-electron approximation.

physics.atom-ph↗

arXiv2023

Coulomb potential determining terahertz polarization in two-color laser field

The orientation and ellipticity of terahertz (THz) polarization generated by two-color strong field not only cast light on underlying mechanisms of laser-matter interaction, but also play an important role for various applications. We develop the Coulomb-corrected classical trajectory Monte Carlo (CTMC) method to well reproduce the joint measurements, that the THz polarization generated by the linearly-polarized 800 nm and circularly-polarized 400 nm fields is independent on two-color phase delay. The trajectory analysis shows that the Coulomb potential twists the THz polarization by deflecting the orientation of asymptotic momentum of electron trajectories. Further, the CTMC calculations predict that, the two-color mid-infrared field can effectively accelerate the electron rapidly away from the parent core to relieve the disturbance of Coulomb potential, and simultaneously create large transverse acceleration of trajectories, leading to the circularly-polarized THz radiation.

physics.optics↗

arXiv2022

Intensity-surged and Bandwidth-extended Terahertz Radiation in Two-foci Cascading Plasmas

The two-color strong-field mixing in gas medium is a widely-used approach to generate bright broadband terahertz (THz) radiation. Here, we present a new and counterintuitive method to promote THz performance in two-color scheme. Beyond our knowledge that the maximum THz generation occurs with two-color foci overlapped, we found that, when the foci of two-color beams are noticeably separated along the propagation axis resulting in cascading plasmas, the THz conversion efficiency is surged by one order of magnitude and the bandwidth is stretched by more than 2 times, achieving $10^{-3}$ conversion efficiency and $>$100 THz bandwidth under the condition of 800/400 nm, $\sim$35 fs driving lasers. With the help of the pulse propagation equation and photocurrent model, the observations can be partially understood by the compromise between THz generation and absorption due to the spatial redistribution of laser energy in cascading plasmas. Present method can be extended to mid-infrared driving laser, and the new records of THz peak power and conversion efficiency are expected.

physics.optics↗

arXiv2022

Observation of photon recoil effects in single-beam absorption spectroscopy with an ultracold strontium gas

We report on observing photon recoil effects in the absorption of a single monochromatic light at 689~nm through an ultracold $^{88}$Sr gas, where the recoil frequency is comparable to natural linewidth of the narrow-line transition $5\mathrm{s^2}\, ^1\textrm{S}_0 - 5\mathrm{s}5\mathrm{p}\, ^3\textrm{P}_1$ in strontium. In the regime of high-saturation, the absorption profile becomes asymmetric due to the photon-recoil shift, which is of the same order as the natural linewidth. The lineshape is described by an extension of the optical Bloch equations including the momentum transfers to atoms during emission and absorption of photons. Our work reveals the photon recoil effects in a simplest single-beam absorption setting, which is of significant relevance to other applications such as saturation spectroscopy, Ramsey interferometry, and absorption imaging.

physics.atom-ph↗

arXiv2020

Ellipticity-dependent sequential over-barrier ionization of cold rubidium

We perform high-resolution measurements of momentum distribution on Rb$^{n+}$ recoil ions up to charge state $n=4$, where laser-cooled rubidium atoms are ionized by femtosecond elliptically polarized lasers with the pulse duration of 35 fs and the intensity of 3.3$\times$10$^{15}$ W/cm$^2$ in the over-barrier ionization (OBI) regime. The momentum distributions of the recoil ions are found to exhibit multi-band structures as the ellipticity varies from the linear to circular polarizations. The origin of these band structures can be explained quantitatively by the classical OBI model and dedicated classical trajectory Monte Carlo simulations with Heisenberg potential. Specifically, with back analysis of the classical trajectories, we reveal the ionization time and the OBI geometry of the sequentially released electrons, disentangling the mechanisms behind the tilted angle of the band structures. These results indicate that the classical treatment can describe the strong-field multiple ionization processes of alkali atoms.

physics.atom-ph↗

arXiv2020

Momentum spectroscopy for multiple ionization of cold rubidium in the elliptically polarized laser field

Employing recent developed magneto-optical trap recoil ion momentum spectroscopy (MOTRIMS) combining cold atom, strong laser pulse, and ultrafast technologies, we study momentum distributions of the multiply ionized cold rubidium (Rb) induced by the elliptically polarized laser pulses (35 fs, $1.3 \times 10^{15}$ W/cm$^2$). The complete vector momenta of Rbn+ ions up to charge state n = 4 are recorded with extremely high resolution (0.12 a.u. for Rb$^+$). Variations of characteristic multi-bands displayed in momentum distributions, as the ellipticity varies from the linear to circular polarization, are interpreted qualitatively with the classical over-barrier ionization model. Present momentum spectroscopy of cold heavy alkali atoms presents novel strong-field phenomena beyond the noble gases.

physics.atom-ph↗

arXiv2019

Strong-field extreme-ultraviolet dressing of atomic double excitation

We report on the experimental observation of strong-field dressing of an autoionizing two-electron state in helium with intense extreme-ultraviolet laser pulses from a free-electron laser. The asymmetric Fano line shape of this transition is spectrally resolved, and we observe modifications of the resonance asymmetry structure for increasing free-electron-laser pulse energy on the order of few tens of $μ$J. A quantum-mechanical calculation of the time-dependent dipole response of this autoionizing state, driven by classical extreme-ultraviolet (XUV) electric fields, reveals a direct link between strong-field-induced energy and phase shifts of the doubly excited state and the Fano line-shape asymmetry. The experimental results obtained at the Free-Electron Laser in Hamburg (FLASH) thus correspond to transient energy shifts on the order of few meV, induced by strong XUV fields. These results open up a new way of performing non-perturbative XUV nonlinear optics for the light-matter interaction of resonant electronic transitions in atoms at short wavelengths.

physics.atom-ph↗

arXiv2012

Noisy pulses enhance temporal resolution in pump-probe spectroscopy

Time-resolved measurements of quantum dynamics are based on the availability of controlled events (e.g. pump and probe pulses) that are shorter in duration than the typical evolution time scale of the dynamical processes to be observed. Here we introduce the concept of noise-enhanced pump-probe spectroscopy, allowing the measurement of dynamics significantly shorter than the average pulse duration by exploiting randomly varying, partially coherent light fields consisting of bunched colored noise. It is shown that statistically fluctuating fields can be superior by more than a factor of 10 to frequency-stabilized fields, with important implications for time-resolved pump-probe experiments at x-ray free-electron lasers (FELs) and, in general, for measurements at the frontiers of temporal resolution (e.g. attosecond spectroscopy). As an example application, the concept is used to explain the recent experimental observation of vibrational wave packet motion in a deuterium molecular ion on time scales shorter than the average pulse duration.

physics.optics↗