arXiv subjects

Ahai Chen

Publications and source records attributed to Ahai Chen.

9 recordsLinked to original sources

arXiv2026

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

We theoretically demonstrate that the molecular orientation angle $\theta$ provides a structurally intrinsic, continuously tunable control parameter for engineering optical Schr\"{o}dinger cat states via high-harmonic generation (HHG) in H$_2^+$. Coupling time-dependent Schr\"{o}dinger 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 $1\sigma_g\to1\sigma_u$ and $1\sigma_g\to1\pi_u$ transitions, driving a kitten-cat crossover whose direction is opposite in the two channels as $\theta$ 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 $\theta^*(q)$. 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↗

arXiv2025

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 Schr\"odinger 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↗

arXiv2025

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↗

arXiv2022

Molecular rotation assisted non-sequential double ionization

A molecular rotation assisted non-sequential double ionization (MR-NSDI) mechanism is identified in the breakup of rotational H$_2$ molecules in a few-cycle intense laser pulse using a semi-classical trajectory Monte Carlo method. Applying a molecular source in an appropriate rotational state could intensively boost NSDI probability, and conclude with an additional small anti-correlated electron momentum distribution. It reveals the critical role of the continuous dynamics of molecular rotation, which assists the recollision process and subsequently releases the excited electron from the potential portal resulted from molecular rotation. Two underlying exit channels are found to contribute to MR-NSDI, i.e. tunneling ionization (dominated by enhanced ionization) and direct ionization. The two channels are confirmed to have different critical breakup internuclear distances. A prominent nuclear emission in $(-30^{\circ},30^{\circ})$ along the laser polarized direction is identified to be a signature of MR-NSDI.

physics.atom-ph↗

arXiv2022

A Smolyak algorithm adapted to a system-bath separation: application to an encapsulated molecule with large amplitude motions

A Smolyak algorithm adapted to system-bath separation is proposed for rigorous quantum simulations. This technique combines a sparse grid method with the system-bath concept in a specific configuration without limitations on the form of the Hamiltonian, thus achieving a highly efficient convergence of the excitation transitions for the "system" part. Our approach provides a general way to overcome the perennial convergence problem for the standard Smolyak algorithm and enables the simulation of floppy molecules with more than a hundred degrees of freedom.The efficiency of the present method is illustrated on the simulation of H$_2$ caged in an sII clathrate hydrate including two kinds of cage modes. The transition energies are converged by increasing the number of normal modes of water molecules. Our results confirm the triplet splittings of both translational and rotational ($j=1$) transitions of the H$_2$ molecule. Furthermore, they show a slight increase of the translational transitions with respect to the ones in a rigid cage.

physics.atom-ph↗

arXiv2021

ElVibRot-MPI: parallel quantum dynamics with Smolyak algorithm for general molecular simulation

A parallelized quantum dynamics package using the Smolyak algorithm for general molecular simulation is introduced in this work. The program has no limitation of the Hamiltonian form and provides high flexibility on the simulation setup to adapt to different problems. Taking advantage of the Smolyak sparse grids formula, the simulation could be performed with high accuracy, and in the meantime, impressive parallel efficiency. The capability of the simulation could be up to tens of degrees of freedom. The implementation of the algorithm and the package usage are introduced, followed by typical examples and code test results.

physics.comp-ph↗