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C. D. Lin

Publications and source records attributed to C. D. Lin.

At least 19 recordsLinked to original sources

Adaptive Design for Contour Estimation from Computer Experiments with Quantitative and Qualitative Inputs

Computer experiments with quantitative and qualitative inputs are widely used to study many scientific and engineering processes. Much of the existing work has focused on design and modeling or process optimization for such experiments. This paper proposes an adaptive design approach for estimating a contour from computer experiments with quantitative and qualitative inputs. A new criterion is introduced to search for the follow-up inputs. The key features of the proposed criterion are (a) the criterion yields adaptive search regions; and (b) it is region-based cooperative in that for each stage of the sequential procedure, the candidate points in the design space is divided into two disjoint groups using confidence bounds, and within each group, an acquisition function is used to select a candidate point. Among the two selected points, a point that is closer to the contour level with the higher uncertainty or that has higher uncertainty when the distance between its prediction and the contour level is within a threshold is chosen. The proposed approach provides empirically more accurate contour estimation than existing approaches as illustrated in numerical examples and a real application. Theoretical justification of the proposed adaptive search region is given.

stat.ME

Extension of all-optical reconstruction method for isolated attosecond pulses using high-harmonic generation streaking spectra

An all-optical method for directly reconstructing the spectral phase of isolated attosecond pulse (IAP) has been proposed recently [New J. Phys. 25, 083003 (2023)]. This method is based on the high-harmonic generation (HHG) streaking spectra generated by an IAP and a time-delayed intense infrared (IR) laser, which can be accurately simulated by an extended quantitative rescattering model. Here we extend the retrieval algorithm in this method to successfully retrieve the spectral phase of an shaped IAP, which has a spectral minimum, a phase jump about $\pi$, and a "split" temporal profile. We then reconstruct the carrier-envelope phase of IR laser from HHG streaking spectra. And we finally discuss the retrieval of the phase of high harmonics by the intense IR laser alone using the Fourier transform of HHG streaking spectra.

physics.optics

Quantifying Robustness of Attosecond Transient Absorption Spectroscopy for Vibronic Coherence in Charge Migration

Probing vibronic coherence in molecules has been a central topic in ultrafast science, as it is an essential prerequisite to monitoring electronic motion. While experiments have demonstrated that attosecond transient absorption spectroscopy (ATAS) can probe the vibronic coherence in a few molecules, its robustness remains largely unexplored. In this Letter, we develop a comprehensive theory for ATAS which accounts for the orientation dependence of the density matrix of a pumped molecule. We apply our theory to N$_2^+$ formed by multiorbital tunnel ionization under a few-cycle intense near-infrared laser pulse. The simulated x-ray absorption spectrum shows clear signatures of the vibronic coherence between the $A^2\Pi_u$ and $B^2\Sigma_u^+$ states of N$_2^+$, which was predicted to be absent by a previous theory. We further define a coherence contrast factor to quantify the robustness of ATAS. This work advances the theoretical foundation of ATAS and paves the way for monitoring electronic motion in generic molecules.

physics.atom-ph

Coherence from multiorbital tunneling ionization of molecules

We present a simple and general coherence model for multiorbital tunnel ionization of molecules, which we incorporate into our previously developed density matrix approach for sequential double ionization [Yuen and Lin, Phys. Rev. A 106, 023120 (2022)]. The influence of this coherence is investigated through simulations of single ionization and sequential double ionization of N$_2$ and O$_2$ using few-cycle near-infrared laser pulses. In the case of single ionization, our results reveal the crucial role played by this coherence in generating population inversion in N$_2^+$, suggesting a potential mechanism for air lasing. Regarding sequential double ionization, we observe only minor changes in the kinetic energy release spectra when the coherence is included, while noticeable differences in the angle-dependent dication yield for both N$_2$ and O$_2$ are found. Based on these findings, we recommend the inclusion of multiorbital tunnel ionization coherence in models for single ionization of general molecules, while suggesting that it can be safely neglected in the case of sequential double ionization.

physics.atom-ph

Probing Vibronic Coherence in Charge Migration of Molecules Using Strong Field Sequential Double Ionization

We propose a novel scheme for probing vibronic coherence in charge migration in molecules utilizing strong field sequential double ionization. To demonstrate the feasibility of this approach, we perform full simulations of a pump-probe scheme employing few-cycle intense infrared pulses for N$_2$ and O$_2$. We predict that the vibronic coherence between the pumped states will be directly imprinted in experimental observables such as kinetic energy release spectra and branching ratios of the dissociative dications. Our simulations are based on the recently developed DM-SDI model, which is capable of efficiently accounting for molecular orientations and enabling direct comparison with experimental results. Our findings strongly encourage the use of this probing scheme in future charge migration experiments.

physics.atom-ph

Molecular structure retrieval directly from laboratory-frame photoelectron spectra in laser-induced electron diffraction

Ubiquitous to most molecular scattering methods is the challenge to retrieve bond distance and angle from the scattering signals since this requires convergence of pattern matching algorithms or fitting methods. This problem is typically exacerbated when imaging larger molecules or for dynamic systems with little a priori knowledge. Here, we employ laser-induced electron diffraction (LIED) which is a powerful means to determine the precise atomic configuration of an isolated gas-phase molecule with picometre spatial and attosecond temporal precision. We introduce a simple molecular retrieval method, which is based only on the identification of critical points in the oscillating molecular interference scattering signal that is extracted directly from the laboratory-frame photoelectron spectrum. The method is compared with a Fourier-based retrieval method, and we show that both methods correctly retrieve the asymmetrically stretched and bent field-dressed configuration of the asymmetric top molecule carbonyl sulfide (OCS), which is confirmed by our quantum-classical calculations.

physics.atom-ph

How to obtain complex transition dipole moments satisfying crystal symmetry and periodicity from ab-initio calculations

Transition dipole moments (TDM) between energy bands of solids deserve special attention nowadays as intense lasers can easily drive non-adiabatic transitions of excited electron wave packets across the Brillouin zones. The TDM is required to be continuous, satisfying crystal symmetry, and periodic at zone boundaries. While present day ab-initio algorithms are powerful in calculating band structures of solids, they all introduced random phases into the eigenfunctions at each crystal momentum k. In this paper, we show how to choose a ``smooth-periodic'' gauge where TDMs can be smooth versus k, preserving crystal symmetry, as well as maintaining periodic at zone boundaries. Based on band structure and TDMs in the ``smooth-periodic'' gauge calculated from ab-initio algorithms, we revisit high-order harmonic generation from MgO which exhibits inversion symmetry and ZnO which has broken symmetry. The symmetry properties of TDMs with respect to k ensure the absence of even-order harmonics in system with inversion symmetry, while the TDM in the `smooth-periodic'' gauge for ZnO is shown to enhance even harmonics that were underestimated in previous simulations. These results reveal the importance of correctly treating the complex TDMs in nonlinear laser-solid interactions which has been elusive so far.

physics.optics

Crystal Symmetry and Polarization of High-order Harmonics in ZnO

We carried out a joint theoretical and experimental study of the polarization of high-order harmonics generated from ZnO by intense infrared laser pulses. Experimentally we found that the dependence of parallel and perpendicular polarizations on the crystal orientation for all odd harmonics are nearly identical, but they are quite different from even harmonics which also show little order dependence. A one-dimensional two-band model, combined with a linear coupled excitation model, is shown to be able to explain the observed polarization behavior, including low-order harmonics. We further note that the same odd/even order contrast have been reported in a number of other crystals, despite that the harmonics were perceived to be generated via entirely different mechanisms. We demonstrated that this universality is governed by crystal symmetry, not by specific mechanisms. Thus, polarization measurements of harmonics offers a powerful pure optical method for determining the crystal axes as well as monitoring their ultrafast changes when crystals are undergoing deformation. In addition, the ellipticity of harmonic has been studied. It shows that ellipticity of high-order harmonics from solids can be tuned precisely by changing the bond structure of the sample.

physics.optics

Imaging an isolated water molecule using a single electron wave packet

Observing changes in molecular structure requires atomic-scale Ångstrom and femtosecond spatio-temporal resolution. We use the Fourier transform (FT) variant of laser-induced electron diffraction (LIED), FT-LIED, to directly retrieve the molecular structure of ${\rm H_2O^+}$ with picometre and femtosecond resolution without a priori knowledge of the molecular structure nor the use of retrieval algorithms or ab initio calculations. We identify a symmetrically stretched ${\rm H_2O^+}$ field-dressed structure that is most likely in the ground electronic state. We subsequently study the nuclear response of an isolated water molecule to an external laser field at four different field strengths. We show that upon increasing the laser field strength from 2.5 to 3.8 V/Å, the O-H bond is further stretched and the molecule slightly bends. The observed ultrafast structural changes lead to an increase in the dipole moment of water and, in turn, a stronger dipole interaction between the nuclear framework of the molecule and the intense laser field. Our results provide important insights into the coupling of the nuclear framework to a laser field as the molecular geometry of ${\rm H_2O^+}$ is altered in the presence of an external field.

physics.chem-ph

Imaging the Renner-Teller effect using laser-induced electron diffraction

Structural information on electronically excited neutral molecules can be indirectly retrieved, largely through pump-probe and rotational spectroscopy measurements with the aid of calculations. Here, we demonstrate the direct structural retrieval of neutral carbonyl disulfide (CS$_2$) in the B$^1$B$_2$ excited electronic state using laser-induced electron diffraction (LIED). We unambiguously identify the ultrafast symmetric stretching and bending of the field-dressed neutral CS$_2$ molecule with combined picometer and attosecond resolution using intrapulse pump-probe excitation and measurement. We invoke the Renner-Teller effect to populate the B$^1$B$_2$ excited state in neutral CS$_2$, leading to bending and stretching of the molecule. Our results demonstrate the sensitivity of LIED in retrieving the geometric structure of CS$_2$, which is known to appear as a two-center scatterer.

physics.chem-ph

Influence of orbital symmetry on diffraction imaging with rescattering electron wave packets

The ability to directly follow and time resolve the rearrangement of the nuclei within molecules is a frontier of science that requires atomic spatial and few-femtosecond temporal resolutions. While laser induced electron diffraction can meet these requirements, it was recently concluded that molecules with particular orbital symmetries (such as πg) cannot be imaged using purely backscattering electron wave packets without molecular alignment. Here, we demonstrate, in direct contradiction to these findings, that the orientation and shape of molecular orbitals presents no impediment for retrieving molecular structure with adequate sampling of the momentum transfer space. We overcome previous issues by showcasing retrieval of the structure of randomly oriented O2 and C2H2 molecules, with πg and πu symmetries, respectively, and where their ionisation probabilities do not maximise along their molecular axes. While this removes a serious bottleneck for laser induced diffraction imaging, we find unexpectedly strong back scattering contributions from low-Z atoms.

physics.atom-ph

Unraveling nonadiabatic ionization and Coulomb potential effects in strong-field photoelectron holography

Strong field photoelectron holography has been proposed as a means for interrogating the spatial and temporal information of electrons and ions in a dynamic system. After ionization, part of the electron wave packet may directly go to the detector (the reference wave), while another part may be driven back to the ion where it scatters off (the signal wave). The interference hologram of the two waves may be used to retrieve the target information. However, unlike conventional optical holography, the propagations of electron wave packets are affected by the Coulomb potential as well as by the laser field. In addition, electrons are emitted over the whole laser pulse duration, thus multiple interferences may occur. In this work, we used a generalized quantum-trajectory Monte Carlo method to investigate the effect of Coulomb potential and the nonadiabatic subcycle ionization on the photoelectron hologram. We showed that photoelectron hologram can be well described only when the nonadiabatic effect in ionization is accounted for, and Coulomb potential can be neglected only in the tunnel ionization regime. Our results help establishing photoelectron holography for probing spatial and dynamic properties of atoms and molecules.

physics.atom-ph

Probing dipole-forbidden autoionizing states by isolated attosecond pulses

We propose a general technique to retrieve the information of dipole-forbidden resonances in the autoionizing region. In the simulation, a helium atom is pumped by an isolated attosecond pulse in the extreme ultraviolet (EUV) combined with a few-femtosecond laser pulse. The excited wave packet consists of the $^1S$, $^1P$, and $^1D$ states, including the background continua, near the $2s2p(^1P)$ doubly excited state. The resultant electron spectra with various laser intensities and time delays between the EUV and laser pulses are obtained by a multilevel model and an ab initio time-dependent Schrödinger equation calculation. By taking the ab initio calculation as a "virtual measurement", the dipole-forbidden resonances are characterized by the multilevel model. We found that in contrast to the common assumption, the nonresonant coupling between the continua plays a significant role in the time-delayed electron spectra, which shows the correlation effect between photoelectrons before they leave the core. This technique takes the advantages of ultrashort pulses uniquely and would be a timely test for the current attosecond technology.

physics.atom-ph

Absorption and emission of single attosecond light pulses in an autoionizing gaseous medium dressed by a time-delayed control field

An extreme ultraviolet (EUV) single attosecond pulse passing through a laser-dressed dense gas is studied theoretically. The weak EUV pulse pumps the helium gas from the ground state to the 2s2p(1P) autoionizing state, which is coupled to the 2s2(1S) autoionizing state by a femtosecond infrared laser with the intensity in the order of 10^{12} W/cm2. The simulation shows how the transient absorption and emission of the EUV are modified by the coupling laser. A simple analytical expression for the atomic response derived for delta-function pulses reveals the strong modification of the Fano lineshape in the spectra, where these features are quite universal and remain valid for realistic pulse conditions. We further account for the propagation of pulses in the medium and show that the EUV signal at the atomic resonance can be enhanced in the gaseous medium by more than 50% for specifically adjusted laser parameters, and that this enhancement persists as the EUV propagates in the gaseous medium. Our result demonstrates the high-level control of nonlinear optical effects that are achievable with attosecond pulses.

physics.atom-ph

Resonant enhancement of a single attosecond pulse in a gas medium by a time-delayed control field

An optical coherent control scheme has been proposed and theoretically investigated where an extreme ultraviolet single attosecond pulse (SAP) propagates through a dense helium gas dressed by a time-delayed femtosecond laser pulse. The laser pulse couples the 2s2p(^1P) and 2s^2(^1S) autoionizing states when the SAP excites the 2s2p state. After going through the gas, the spectral and temporal profiles of the SAP are strongly distorted. A narrowed but enhanced spike in the spectrum shows up for specific intensities and time delays of the laser, which exemplifies the control of a broadband photon wave packet by an ultrashort dressing field for the first time. We analyze the photon and electron dynamics and conclude on the dressing condition that maximizes this enhancement. The result demonstrates new possibilities of attosecond optical control.

physics.atom-ph

Theory of ultrafast autoionization dynamics of Fano resonances

We study atomic autoionization processes in the time domain. With the emerging attosecond extreme vacuum ultraviolet and soft x-ray pulses, we first address how to characterize the time evolution of the decay of a discrete state into a degenerate continuum. A short pump beam generates a number of resonance states in a series and the nearby background continuum, and the resultant wave packet evolves with time until the full decay of the bound states. Taking the 2pns(^1P^o) resonance series embedded in the 2sEp(^1P^o) continuum in beryllium atom as an example, the time evolution of the autoionizing wave packet in energy domain and in coordinate space is calculated and analyzed, where Fano profiles build up in the photoelectron energy during the process. A proposed pump-probe scheme assumes that the probe beam ionizes the 2s inner electron in the wave packet. The lifetimes of the resonances and the photoelectron energy distribution can be obtained from the ionization yield versus the time delay of the probe.

physics.atom-ph

Laser-assisted-autoionization dynamics of helium resonances with single attosecond pulses

The strong coupling between two autoionizing states in helium is studied theoretically with the pump-probe scheme. An isolated 100-as XUV pulse is used to excite helium near the 2s2p(1P) resonance state in the presence of an intense infrared (IR) laser. The laser field introduces strong coupling between 2s2p(1P) and 2p^2(1S) states. The IR also can ionize helium from both autoionizing states. By changing the time delay between the XUV and the IR pulses, we investigated the photoelectron spectra near the two resonances. The results are used to explain the recent experiment by Gilbertson et al. [Phys. Rev. Lett. 105, 263003 (2010)]. Using the same isolated attosecond pulse and a 540-nm laser, we also investigate the strong coupling between 2s2p(1P) and 2s^2(1S) by examining how the photoelectron spectra are modified versus the time delay and the possibility of observing Autler-Townes doublet in such experiments.

physics.atom-ph

Photoabsorption of attosecond XUV light pulses by two strongly laser-coupled autoionizing states

We study theoretically the photoabsorption spectra of an attosecond XUV pulse by a laserdressed atomic system. A weak XUV excites an autoionizing state which is strongly coupled to another autoionizing state by a laser. The theory was applied to explain two recent experiments [Loh, Greene, and Leone, Chem. Phys. 350, 7 (2008); Wang, Chini, Chen, Zhang, Cheng, He, Cheng, Wu, Thumm, and Chang, Phys. Rev. Lett. 105 143002 (2010)] where the absorption spectra of the XUV lights were measured against the time delay between the laser and the XUV. In another example, we study an attosecond pulse exciting the 2s2p(1P) resonance of helium which is resonantly coupled to the 2s2(1S) resonance by a moderately intense 540 nm laser. The relation between the photoabsorption spectra and the photoelectron spectra and the modification of the transmitted lights in such an experiment are analyzed. The role of Rabi flopping between the two autoionizing states within their lifetimes is investigated with respect to the laser intensity and detuning.

physics.atom-ph