We present an ab initio approach to solve the time-dependent Schrödinger equation to treat electron and photon impact multiple ionization of atoms or molecules. It combines the already known time scaled coordinate method with a new high order time propagator based on a predictor-corrector scheme. In order to exploit in an optimal way the main advantage of the time scaled coordinate method namely that the scaled wave packet stays confined and evolves smoothly towards a stationary state the modulus square of which being directly proportional to the electron energy spectra in each ionization channel, we show that the scaled bound states should be subtracted from the total scaled wave packet. In addition, our detailed investigations suggest that multi-resolution techniques like for instance, wavelets are the most appropriate ones to represent spatially the scaled wave packet. The approach is illustrated in the case of the interaction of an one-dimensional model atom as well as atomic hydrogen with a strong oscillating field.
We demonstrate that a near-dissociation photoassociation resonance can be used to create a deeply bound molecular sample of ultracold NaCs. To probe the resulting vibrational distribution of the sample, we use a new technique that can be applied to any ultracold molecular system. We utilize a tunable pulsed dye laser to produce efficient spectroscopic scans ($\sim700$ cm$^{-1}$ at a time) in which we observe the $1^{1} Σ^{+}\rightarrow 2^{1}Σ^{+}-2^{3}Π$ vibrational progression, as well as the dissociation limit to the Cs 6$^{2}$P$_{3/2}$ asymptote. We assign $1^{1} Σ^{+}$$(\emph{v}$ = 4, 5, 6…
Aluminum monochloride (AlCl) has been proposed as a promising candidate for laser cooling to ultracold temperatures, and recent spectroscopy results support this prediction. It is challenging to produce large numbers of AlCl molecules because it is a highly reactive open-shell molecule and must be generated in situ. Here we show that pulsed-laser ablation of stable, non-toxic mixtures of Al with an alkali or alkaline earth chlorides, denoted XCln, can provide a robust and reliable source of cold AlCl molecules. Both the chemical identity of XCln and the Al:XCln molar ratio are varied, and the …
Electron-ion-ion coincidence experiments for photofragmentation of polyatomic molecules using pulsed electric fields: treatment of random coincidences
在通过软X射线的分子光致碎裂过程中，可以产生许多离子碎片，每个离子碎片具有不同的丰度和与发射的电子动能的相关性。为了研究这些碎裂过程，电子-离子和电子-离子-离子符合实验是非常强大的，其中使用静电分析仪分析电子的动能，同时使用脉冲电场分析离子的质量。然而，对于这样的测量，随机巧合的贡献是巨大的，并以非平凡的方式影响数据。不能应用简单直观的减法。在本文中，我们描述了这些电子-离子和电子-离子-离子符合实验，以及随机符合贡献的扣除方法。我们提供了一套全面的数据处理方程，包括计算误差条的方程。我们通过将其应用于游离CF $_3$ SF $_5$分子的片段化来证明该方法。
We develop the theory for the Adiabatic Raman Photoassociation (ARPA) of ultracold atoms to form ultracold molecules in the presence of scattering resonances. Based on a computational method in which we replace the continuum with a discrete set of "effective modes", we show that the existence of resonances greatly aids in the formation of deeply bound molecular states. We illustrate our general theory by computationally studying the formation of $^{85}$Rb$_2$ molecules from pairs of colliding ultracold $^{85}$Rb atoms. The single-event transfer yield is shown to have a near-unity value for wid…
We present a new mechanism contributing to the detection of photoassociated long-range Rydberg molecules via pulsed-field ionization: ionic products, created by the decay of a long-range Rydberg molecule, modify the excitation spectrum of surrounding ground-state atoms and facilitate the excitation of further atoms into Rydberg states by the photoassociation light. Such an ion-mediated excitation mechanism has been previously called "Coulomb anti-blockade". Pulsed-field ionisation typically doesn't discriminate between the ionization of a long-range Rydberg molecule and an isolated Rydberg ato…
We analyze electronically excited nuclear wave functions and their coherence when subjecting a molecule to the action of natural, pulsed incoherent solar-like light, and to that of ultrashort coherent light assumed to have the same center frequencies and spectral bandwidths. Specifically, we compute the spatio-temporal dependence of the excited wave packets and their electronic coherence for these two types of light sources, on different electronic potential energy surfaces. The resultant excited state wave functions are shown to be qualitatively different, reflecting the light source from whi…
Nitric oxide (NO) molecules initially traveling at 795 m/s in pulsed supersonic beams have been photoexcited to long-lived hydrogenic Rydberg-Stark states, decelerated and electrostatically trapped in a cryogenically cooled, chip-based transmission-line Rydberg-Stark decelerator. The decelerated and trapped molecules were detected $in$ $situ$ by pulsed electric field ionization. The operation of the decelerator was validated by comparison of the experimental data with the results of numerical calculations of particle trajectories. Studies of the decay of the trapped molecules on timescales up …
We describe a pulsed rotating supersonic beam source, evolved from an ancestral device [M. Gupta and D. Herschbach, J. Phys. Chem. A 105, 1626 (2001)]. The beam emerges from a nozzle near the tip of a hollow rotor which can be spun at high-speed to shift the molecular velocity distribution downward or upward over a wide range. Here we consider mostly the slowing mode. Introducing a pulsed gas inlet system, cryocooling, and a shutter gate eliminated the main handicap of the original device, in which continuous gas flow imposed high background pressure. The new version provides intense pulses, o…
We make use of an inhomogeneous electrostatic dipole field to impart a quantum-state-dependent deflection to a pulsed beam of OCS molecules, and show that those molecules residing in the absolute ground state, $X ^1Σ^+$, $\ket{00^00}$, J=0, can be separated out by selecting the most deflected part of the molecular beam. Past the deflector, we irradiate the molecular beam by a linearly polarized pulsed nonresonant laser beam that impulsively aligns the OCS molecules. Their alignment, monitored via velocity-map imaging, is measured as a function of time, and the time dependence of the alignment …
We show that weakly-bound molecules can be probed by "shaking" in a pulsed nonresonant laser field. The field introduces a centrifugal term which expels the highest vibrational level from the potential that binds it. Our numerical simulations applied to the Rb$_2$ and KRb Feshbach molecules indicate that shaking by feasible laser pulses can be used to accurately recover the square of the vibrational wavefunction and, by inversion, also the long-range part of the molecular potential.
We show theoretically the presence of electromagnetically induced transparency (EIT) like feature in a Λ-type atom-molecule coupled system. We demonstrate that EIT in such a systems has a sharp dispersion characteristic which is useful to slow down light propagation in a medium. The results of our model calculations show that, it is possible to achieve a time delay of the order of 1 ms for a probe field propagating a distance of 1 cm through a medium of ultracold diatomic molecules coupled to the continuum of atom-atom collisional states with a control field. This enables one to reduce the gro…
For two-electron diatomic molecules, we investigate magnetic field effects in non-sequential double ionization where recollisions prevail. We do so by formulating a three-dimensional semi-classical model that fully accounts for the Coulomb singularities and for magnetic field effects during time propagation. Using this model, we identify a prominent signature of non-dipole effects. Namely, we demonstrate that the recolliding electron back-scatters along the direction of light propagation. Hence, this electron escapes opposite to the direction of change in momentum due to the magnetic field. Th…
We model the formation of stable heteronuclear molecules via pulsed Raman photoassociation of a two-component Bose-Einstein condensate near a strong Feshbach resonance, for both counterintuitive and intuitive pulse sequencing. Compared to lasers alone, weak Raman photoassociation is enhanced by as much as a factor of ten (five) for a counterintuitive (intuitive) pulse sequence, whereas strong Raman photoassociation is barely enhanced at all--regardless of pulse sequence. Stronger intra-atom, molecule, or atom-molecule collisions lead to an expected decrease in conversion efficiency, but strong…
The ionization energy of D$_2$ has been determined experimentally from measurements involving two-photon Doppler-free vacuum-ultraviolet pulsed laser excitation and near-infrared continuous-wave laser excitation to yield $E_\mathrm{I}(\mathrm{D}_2)=124\,745.393\,739(26)$ \wn. From this value, the dissociation energy of D$_2$ is deduced to be $D_0$(D$_2$) = 36\,748.362\,282(26) \wn, representing a 25-fold improvement over previous values, and found in good agreement (at $1.6σ$) with recent ab initio calculations of the 4-particle nonadiabatic relativistic energy and of quantum-electrodynamic co…
We demonstrate that a bichromatic standing-wave laser field can exert a significantly larger force on a molecule than ordinary radiation pressure. Our experiment measures the deflection of a pulsed supersonic beam of CaF molecules by a two-frequency laser field detuned symmetrically about resonance with the nearly closed $X (v=0) \rightarrow B (v'=0)$ transition. The inferred force as a function of relative phase between the two counterpropagating beams is in reasonable agreement with numerical simulations of the bichromatic force in this multilevel system. The large magnitude of the force, co…
Metastable helium molecules (He$_2^*$) have been generated by striking a discharge in a supersonic expansion of helium gas from a pulsed valve. When operating the pulsed valve at room temperature, 77K, and 10K, the mean velocity of the supersonic beam was measured to be 1900m/s, 980m/s, and 530m/s, respectively. A 55-stage Zeeman decelerator operated in a phase-stable manner was then used to further reduce the beam velocity and tune it in the range between 100 and 150m/s. The internal-state distribution of the decelerated sample was established by photoionization spectroscopy.
Single-photon loading of polar molecules into an optical trap
Van Swinderen Institute for Particle Physics and Gravity, University of Groningen（格罗宁根大学范斯温德伦粒子物理与引力研究所）；Nikhef, National Institute for Subatomic Physics（荷兰国家亚原子物理研究所尼赫夫）；Experimental Physics Department, CERN（欧洲核子研究中心实验物理部）；Department of Physical and Theoretical Chemistry, Comenius University（布拉迪斯拉发康斯坦丁神学院大学物理与理论化学系）
We calculate high-harmonic generation (HHG) by intense infrared lasers in atoms and molecules with the inclusion of macroscopic propagation of the harmonics in the gas medium. We show that the observed experimental spectra can be accurately reproduced theoretically despite that HHG spectra are sensitive to the experimental conditions. We further demonstrate that the simulated (or experimental) HHG spectra can be factored out as a product of a \macroscopic wave packet" and the photo-recombination transition dipole moment where the former depends on the laser properties and the experimental cond…
