We apply attosecond transient absorption spectroscopy (ATAS) to explore the effects of a nonzero permanent dipole on electron dynamics at the subfemtosecond scale, exemplified in the polar LiF molecule. In contrast with nonpolar systems, a familiar feature of the ATA spectra--the light-induced structures--are observed adjacent to a bright state. Moreover, a previously unobserved ladder structure is identified. The new observations are analyzed in the context of a model based on fixed-nuclei adiabatic states, supported by full numerical simulations. Analytic calculations originating in the adiabatic model shed light on the nature and origins of the new findings.
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 populatio…
The nature of light-induced structures in attosecond transient absorption spectroscopy of molecular systems is investigated theoretically. It is shown how nuclear dynamics affect these structures. We find that a theoretical three-surface model captures the main characteristics in the calculated spectra. Based on this model, nuclear dynamics is divided into different categories, each category having unique signatures in the absorption spectra. Finally, we discuss the possibility for experimental observation of light-induced structures in molecules.
King’s College London（伦敦国王学院）；University of California, Berkeley（加州大学伯克利分校）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；Max-Born-Institut（马克斯·玻恩研究所）
Attosecond transient-absorption spectroscopy (ATAS) is an established method for exploring electron dynamics on the subfemtosecond time-scale. ATAS spectra contain certain ubiquitous features, such as oscillating fringes, light-induced structures and hyperbolic sidebands, representing physical processes. We derive closed analytical expressions describing these features, based on a three-level system responding adiabatically to the influence of an infrared field in conjunction with an extreme ultraviolet pulse, and use He to illustrate the theory. The validity of the formulas is substantiated b…
Strong-field manipulation of autoionizing states is a crucial aspect of electronic quantum control. Recent measurements of the attosecond transient absorption spectrum of helium dressed by a few-cycle visible pulse [Ott et al., arXiv:1205.0519[physics.atom-ph] ] provide evidence of novel ultrafast resonant phenomena, namely, two-photon Rabi oscillations between doubly-excited states and the inversion of Fano profiles. Here we present the results of accurate \emph{ab-initio} calculations that agree with these observations and in addition predict that (i) inversion of Fano profiles is actually p…
Tunable attosecond transient absorption spectroscopy is an ideal tool for studying and manipulating autoionization dynamics in the continuum. We investigate near-resonant two-photon couplings between the bright 3s^-1 4p and dark 3s^-1 4f autoionizing states of argon that lead to Autler-Townes like interactions, forming entangled light-matter states, or polaritons. We observe that one-photon couplings with intermediate dark states play an important role in this interaction, leading to the formation of multiple polaritonic branches whose energies exhibit avoided crossings as a function of the dr…
Laser assisted photoemission by a chirped subfemtosecond extreme ultraviolet (XUV) pulse is considered within an exactly solvable quantum-mechanical model. Special emphasis is given to the energy dependence of photoexcitation cross-section. The streaked spectra are analyzed within the classical picture of initial time-momentum distribution r_ini(p,t) of photoelectrons mapped to the final energy scale. The actual time-momentum distribution in the absence of the probe laser field is shown to be a poor choice for r_ini, and a more adequate ansatz is suggested. The semiclassical theory offers a si…
We study effects of nonadiabatic couplings in a model of a diatomic molecule in the context of attosecond transient absorption spectroscopy. By using a model system consisting of four diabatic electronic states and with a variable strength of the diabatic coupling, we can explore attosecond transient absorption spectra in different regimes of the vibronic couplings between the electronic and nuclear dynamics, and determine when nonadiabatic couplings can be ignored or when they have a substantial effect. The findings are rationalized in terms of a multilevel model, which captures aspects of bo…
We investigate the characteristic effects of nuclear motion on attosecond transient absorption spectra in molecules by calculating the spectrum for different model systems. Two models of the hydrogen molecular ion are considered: one where the internuclear separation is fixed, and one where the nuclei are free to vibrate. The spectra for the fixed nuclei model are similar to atomic spectra reported elsewhere, while the spectra obtained in the model including nuclear motion are very different and dominated by extremely broad absorption features. These broad absorption features are analyzed and …
Transient absorption is a very powerful observable in attosecond experiments on atoms, molecules and solids and is frequently used in experiments employing phase-locked few-cycle infrared and XUV laser pulses derived from high harmonic generation. We show numerically and analytically that in non-centrosymmetric systems, such as many polyatomic molecules, which-way interference enabled by the lack of parity conservation leads to new spectral absorption features, which directly reveal the laser electric field. The extension of Attosecond Transient Absorption Spectroscopy (ATAS) to such targets h…
We calculate the transient absorption of an isolated attosecond pulse by helium atoms subject to a delayed infrared (\ir) laser pulse. With the central frequency of the broad attosecond spectrum near the ionization threshold, the absorption spectrum is strongly modulated at the sub-\ir-cycle level. Given that the absorption spectrum results from a time-integrated measurement, we investigate the extent to which the delay-dependence of the absorption yields information about the attosecond dynamics of the atom-field energy exchange. We find two configurations in which this is possible. The first…
Strong-field ionization generally produces ions in a superposition of ionic eigenstates. This superposition is generally not fully coherent und must be described in terms of a density matrix. A recent experiment [E. Goulielmakis et al., Nature 466, 739 (2010)] employed attosecond transient absorption spectroscopy to determine the density matrix of strong-field-generated Kr+ ions. The experimentally observed degree of coherence of the strong-field-generated Kr+ ions is well reproduced by a recently developed multichannel strong-field-ionization theory. But there is significant disagreement betw…
The exact delay-zero calibration in an attosecond pump-probe experiment is important for the correct interpretation of experimental data. In attosecond transient absorption spectroscopy the determination of the delay-zero exclusively from the experimental results is not straightforward and may introduce significant errors. Here, we report the observation of quarter-laser-cycle (4ω) oscillations in a transient absorption experiment in helium using an attosecond pulse train overlapped with a precisely synchronized, moderately strong infrared pulse. We demonstrate how to extract and calibrate the…
We develop theoretically and confirm both numerically and experimentally a comprehensive analytical model which describes the propensity rules in the emission of circularly polarized high harmonics by systems driven by two-color counter-rotating fields, a fundamental and its second harmonic. We identify and confirm the three propensity rules responsible for the contrast between the 3N+1 and 3N+2 harmonic lines in the HHG spectra of noble gas atoms. We demonstrate how these rules depend on the laser parameters and how they can be used in the experiment to shape the polarization properties of th…
We study the influence of polarization effects in streaking by combined atto- and femtosecond pulses. The polarization-induced terms alter the streaking spectrum. The normal streaking spectrum, which maps to the vector potential of the femtosecond pulse, is modified by a contribution following the field instead. We show that polarization effects may lead to an apparent temporal shift, that needs to be properly accounted for in the analysis. The effect may be isolated and studied by angle-resolved photoelectron spectroscopy from oriented polar molecules. We also show that polarization effects w…
Light-induced states are commonly observed in the photoionization spectra of laser-dressed atoms. The properties of autoionizing polaritons, entangled states of light and Auger resonances, however, are largely unexplored. We employ attosecond transient-absorption spectroscopy to study the evolution of autoionizing states in argon, dressed by a tunable femtosecond laser pulse. The avoided crossings between the $3s^{-1}4p$ and several light-induced states indicates the formation of polariton multiplets. We measure a controllable stabilization of the polaritons against ionization, in excellent ag…
We present the first fully ab initio calculations for attosecond transient absorption spectroscopy of atomic krypton with overlapping pump and probe pulses. Within the time-dependent configuration interaction singles (TDCIS) approach, we describe the pump step (strong-field ionization using a near-infrared pulse) as well as the probe step (resonant electron excitation using an extreme- ultraviolet pulse) from first principles. We extent our TDCIS model and account for the spin-orbit splitting of the occupied orbitals. We discuss the spectral features seen in a recent attosecond transient absor…
We propose an experimental arrangement to image, with attosecond resolution, transient surface plasmonic excitations. The required modifications to state-of-the-art setups used for attosecond streaking experiments from solid surfaces only involve available technology. Buildup and life times of surface plasmon polaritons can be extracted and local modulations of the exciting optical pulse can be diagnosed {\it in situ}.
We investigate the evolution of extreme ultraviolet (XUV) spectral lineshapes in an optically-thick helium gas under near-infrared (IR) perturbation. In our experimental and theoretical work, we systematically vary the IR intensity, time-delay, gas density and IR polarization parameters to study lineshape modifications induced by collective interactions, in a regime beyond the single atom response of a thin, dilute gas. In both experiment and theory, we find that specific features in the frequency-domain absorption profile, and their evolution with propagation distance, can be attributed to th…
We investigate the attosecond transient absorption spectroscopy (ATAS) of graphene by numerically solving four-band density-matrix equations, which demonstrates apparent fish bone resonance structures. To gain insight into these interesting structures, we exploit a simplified model that only considers the electrons of $Γ$ and M points in the Brillouin zone. With the help of this model, we can analytically express the ATAS spectrum as the sum of zeroth- and first-order Bessel functions in the variables of the strength and frequency of the infrared pump field as well as the effective mass of ele…
Quantum-mechanical investigation is presented to study single attosecond pulse generation by gating high-order harmonic emission from H$_2^+$ molecule in intense laser pulses with time-dependent ellipticity. The high-order harmonic generation from H$_2^+$ molecule in superposition of a left and a right-hand circularly polarized Gaussian pulse is studied and the effect of time duration and carrier-envelope phase of laser field on single attosecond pulse generation is investigated. Using laser field formed by combination of a left and a right-hand elliptically polarized Gaussian pulse, the effec…
A relativistic transient absorption theory is derived, implemented and validated within the dipole approximation based on the time-dependent Dirac equation. Time-dependent simulations have been performed using the Dirac equation and the Schrödinger equation for the Hydrogen atom in two different attosecond transient absorption scenarios. These simulations validate the present relativistic theory. The presented work can be seen as a first step in the development of a more general relativistic attosecond transient absorption spectroscopy method for studying heavy atoms, but it also suggests the …
We report attosecond-scale probing of the laser-induced dynamics in molecules. We apply the method of high-harmonic spectroscopy, where laser-driven recolliding electrons on various trajec- tories record the motion of their parent ion. Based on the transient phase-matching mechanism of high-order harmonic generation, short and long trajectories contributing to the same harmonic order are distinguishable in both the spatial and frequency domains, giving rise to a one-to-one map between time and photon energy for each trajectory. The short and long trajectories in H2 and D2 are used simultaneous…
We demonstrate sub-cycle control of frustrated double ionization (FDI) in the two-electron triatomic molecule D$_3^+$ when driven by two orthogonally polarized two-color laser fields. We employ a three-dimensional semi-classical model that fully accounts for the electron and nuclear motion in strong fields. We control FDI triggered by a strong near-infrared laser field with a weak mid-infrared laser field. This control as a function of the time delay between the two pulses is demonstrated when the FDI probability and the distribution of the momentum of the escaping electron along the mid-infra…
The generation of the shortest isolated attosecond pulses requires both broad spectral bandwidth and control of the spectral phase. Rapid progress has been made in both aspects, leading to the generation of the world-record-shortest 67 as light pulses in 2012, and broadband attosecond continua covering a wide range of extreme ultraviolet and soft x-ray wavelengths. Such pulses have been successfully applied in photoelectron/photoion spectroscopy and the recently developed attosecond transient absorption spectroscopy to study electron dynamics in matter. In this Review, we discuss the significa…
We present transient absorption spectra of an extreme ultraviolet attosecond pulse train in helium dressed by an 800 nm laser field with intensity ranging from $2\times10^{12}$ W/cm$^2$ to $2\times10^{14}$ W/cm$^2$. The energy range probed spans 16-42 eV, straddling the first ionisation energy of helium (24.59 eV). By changing the relative polarisation of the dressing field with respect to the attosecond pulse train polarisation we observe a large change in the modulation of the absorption reflecting the vectorial response to the dressing field. With parallel polarized dressing and probing fie…
The ionization of atoms with sequences of attosecond pulses gives rise to excited ionic states that are entangled with the emitted photoelectron. Still, the ionic ensemble preserves some coherence that can be controlled through the laser parameters. In helium, control of the $2s/2p$ He$^+$ coherence is mediated by the autoionizing states below the $N=2$ threshold [Phys. Rev. Res. {\bf 3}, 023233 (2021)]. In the present work we study the role of the resonances both below and above the $N=3$ threshold on the coherence of the $N=3$ He$^+$ ion, in the attosecond pump-probe ionization of the helium…
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.
The complex Kohn variational method is extended to compute light-driven electronic transitions between continuum wavefunctions in atomic and molecular systems. This development enables the study of multiphoton processes in the perturbative regime for arbitrary light polarization. As a proof of principle, we apply the method to compute the photoelectron spectrum arising from the pump-probe two-photon ionization of helium induced by a sequence of extreme ultraviolet and infrared-light pulses. We compare several two-photon ionization pump-probe spectra, resonant with the (2s2p)1P1o Feshbach reson…
Photoinduced quantum dynamics in molecules have hierarchical temporal structures with different energy scales that are associated with electron and nuclear motions. Femtosecond-to-attosecond transient absorption spectroscopy (TAS) using high-harmonic generation (HHG) with a photon energy below 300 eV has been a powerful tool to observe such electron and nuclear dynamics in a table-top manner. However, comprehensive measurements of the electronic, vibrational, and rotational molecular dynamics have not yet been achieved. Here, we demonstrate HHG-based TAS at the nitrogen K-edge (400 eV) for the…
The ability of spatial light modulators (SLMs) to modify the amplitude and phase of light has proved them invaluable to the optics and photonics community. In many applications the bit-depth of SLMs is a major limiting factor dictated by the digital processor. As a result, there is usually a compromise between refresh speed and bit-depth. Here we present a method to increase the effective bit-depth of SLMs which utilizes a linear slope as is commonly applied to deal with the zeroth order effect. This technique was tested using two interferometric transient absorption spectroscopy setups. Throu…
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 lines…
A novel and universal interference structure is found in the photoelectron momentum distribution of atoms in intense infrared laser field. Theoretical analysis shows that this structure can be attributed to a new form of Coulomb-field-driven backward-scattering of photoelectrons in the direction perpendicular to the laser field, in contrast to the conventional rescattering along the laser polarization direction. This transverse backward-scattering process is closely related to a family of photoelectrons initially ionized within a time interval of less than 200 attosecond around the crest of th…
Time-resolved investigations of ultrafast electronic and molecular dynamics were not possible until recently. The typical time scale of these processes is in the picosecond to attosecond realm. The tremendous technological progress in recent years made it possible to generate ultrashort pulses, which can be used to trigger, to watch, and to control atomic and molecular motion. This tutorial focuses on experimental and theoretical advances which are used to study the dynamics of electrons and molecules in the presence of ultrashort pulses. In the first part, the rotational dynamics of molecules…
Chiral light-matter interactions have been investigated for two centuries, leading to the discovery of many chiroptical processes used for discrimination of enantiomers. Whereas most chiroptical effects result from a response of bound electrons, photoionization can produce much stronger chiral signals that manifest as asymmetries in the angular distribution of the photoelectrons along the light propagation axis. Here we implement a self-referenced attosecond photoelectron interferometry to measure the temporal profile of the forward and backward electron wavepackets emitted upon photoionizatio…
Attosecond transient absorption spectroscopy has thus far been lacking the capability to simultaneously characterize the intense laser pulses at work within a time-resolved quantum-dynamics experiment. However, precise knowledge of these pulses is key to extracting quantitative information in strong-field highly nonlinear light-matter interactions. Here, we introduce and experimentally demonstrate an ultrafast metrology tool based on the time-delay-dependent phase shift imprinted on a strong-field driven resonance. Since we analyze the signature of the laser pulse interacting with the absorbin…
The dynamics of autoionizing Rydberg states of oxygen are studied using attosecond transient absorption technique, where extreme ultraviolet (XUV) initiates molecular polarization and near infrared (NIR) pulse perturbs its evolution. Transient absorption spectra show positive optical density (OD) change in the case of $nsσ_g$ and $ndπ_g$ autoionizing states of oxygen and negative OD change for $ndσ_g$ states. Multiconfiguration time-dependent Hartree-Fock (MCTDHF) calculation are used to simulate the transient absorption spectra and their results agree with experimental observations. The time …
Time-dependent Hole States in Multiconfigurational Time-Dependent Hartree-Fock Approaches: Applications in Photoionization of Water Molecule
Shanghai Jiao Tong University（上海交通大学）；RIKEN Center for Interdisciplinary Theoretical and Mathematical Sciences (iTHEMS)（理化学研究所交叉理论数学科学中心（iTHEMS））；RIKEN Center for Computational Science (R-CCS)（理化学研究所计算科学中心（R-CCS））；The University of Tokyo（东京大学）
