We present the results of the detailed experimental study of multiple ionization of Ne and Ar by 25 and 7 fs laser pulses. For Ne the highly correlated "instantaneous" emission of up to four electrons is triggered by a recollisional electron impact, whereas in multiple ionization of Ar different mechanisms, involving field ionization steps and recollision-induced excitations, play a major role. Using few-cycle pulses we are able to suppress those processes that occur on time scales longer than one laser cycle.
We present an experimental investigation of ultrafast-laser driven Rabi oscillations of atomic rubidium. Since the broadband spectrum of an ultrafast laser pulse simultaneously couples all the electronic hyperfine transitions between the excited and ground states, the complex excitation linkages involved with the D1 or D2 transition are energy degenerate. Here, by applying the Morris-Shore transformation, it is shown that this multi-state system is reduced to a set of independent two-state systems and dark states. In experiments performed by ultrafast laser interactions of atomic rubidium in t…
The requirement of high space-time resolution and brightness is a great challenge for imaging atomic motion and making molecular movies. Important breakthroughs in ultrabright tabletop laser, x-ray and electron sources have enabled the direct imaging of evolving molecular structures in chemical processes. And recent experimental advances in preparing ultrafast laser and electron pulses equipped molecular imaging with femtosecond time resolution. This Perspectives present an overview of versatile imaging methods of molecular dynamics. High-order harmonic generation imaging and photoelectron dif…
We propose a new laser cooling method for atomic species whose level structure makes traditional laser cooling difficult. For instance, laser cooling of hydrogen requires single-frequency vacuum-ultraviolet light, while multielectron atoms need single-frequency light at many widely separated frequencies. These restrictions can be eased by laser cooling on two-photon transitions with ultrafast pulse trains. Laser cooling of hydrogen, antihydrogen, and many other species appears feasible, and extension of the technique to molecules may be possible.
We consider the leakage suppression problem of a three-level system in which the first two levels are the qubit system and the third, weakly-coupled to the second, is the leakage state. We show that phase- and amplitude-controlled two (three) pulses are sufficient for arbitrary qubit controls from the ground (an arbitrary) initial state, with leakage suppressed up to the first order of perturbation without additional pulse-area cost. A proof-of-principle experiment was performed with shaped femtosecond optical pulses and atomic rubidium showing a good agreement with the theory.
It is shown that the magnetic state decoherence produced by collisions in a thermal vapor can be suppressed by the application of a train of ultrafast optical pulses.
A universal mechanism of ultrafast two-electron orbital swap is discovered through two-photon sequential double ionization of Li. After a $1s$ electron in Li is ionized by absorbing an EUV photon, the other two bound electrons located on two different shells have either parallel or antiparallel spin orientations. In the latter case, these two electrons are in the superposition of the singlet and triplet states with different energies, forming a quantum beat and giving rise to the two-electron orbital swap with a period of several hundred attoseconds. The orbital swap mechanism can be used to m…
Calculations relating to two experiments that demonstrate coherent control of preformed rubidium-85 molecules in a magneto-optical trap using ultrafast laser pulses are presented. In the first experiment, it is shown that pre-associated molecules in an incoherent mixture of states can be made to oscillate coherently using a single ultrafast pulse. A mechanism that can transfer molecular population to more deeply bound vibrational levels is used in the second. Optimal parameters of the control pulse are presented for the application of the mechanism to molecules in a magneto-optical trap. The c…
We report a study on the ultrafast coherent population oscillations (UCPO) in two level atoms induced by the frequency modulated few-cycle optical pulse train. The phenomenon of UCPO is investigated by numerically solving the optical Bloch equations beyond the rotating wave approximation. We demonstrate that the quantum state of the atoms and the frequency of UCPO may be controlled by controlling the number of pulses in the pulse trains and the pulse repetition time respectively. Moreover, the robustness of the population inversion against the variation of the laser pulse parameters is also in…
We report and propose a simple scheme to achieve the ultrafast and selective population transfer in four-level atoms by utilizing a single frequency chirped few-cycle pulse. It is demonstrated that the almost complete population may be transferred to the preselected state of atoms just by manipulating the so called chirp offset parameter. The robustness of the scheme against the variation of laser pulse parameters is also investigated. The proposed scheme may also be useful for the selective population transfer in molecules.
We demonstrate quantum entanglement of two trapped atomic ion qubits using a sequence of ultrafast laser pulses. Unlike previous demonstrations of entanglement mediated by the Coulomb interaction, this scheme does not require confinement to the Lamb-Dicke regime and can be less sensitive to ambient noise due to its speed. To elucidate the physics of an ultrafast phase gate, we generate a high entanglement rate using just 10 pulses, each of $\sim20$ ps duration, and demonstrate an entangled Bell-state with $(76\pm1)$% fidelity. These results pave the way for entanglement operations within a lar…
Generation of 480 nm picosecond pulses for ultrafast excitation of Rydberg atoms
Institute for Molecular Science, National Institutes of Natural Sciences（国立自然科学研究所分子科学研究所）；SOKENDAI (The Graduate University for Advanced Studies)（综合研究大学院大学）
We study a hybrid quantum system composed of an ion and an electric dipole. We show how a trapped ion can be used to measure the small electric field generated by a classical dipole. We discuss the application of this scheme to measure the electric dipole moment of cold polar molecules, whose internal state can be controlled with ultrafast laser pulses, by trapping them in the vicinity of a trapped ion.
We report and propose a simple scheme to achieve efficient and fast coherent population transfer (CPT) by utilizing either a nonlinearly chirped Gaussian shaped few-cycle laser pulse or an unchirped sinc-shaped few-cycle laser pulse. The proposed scheme is shown to be fairly robust against the variation of the laser parameters such as temporal pulse width, chirp rates, carrier envelope phases and Rabi frequencies. We find that compared to the so-called stimulated Raman adiabatic passage (STIRAP) technique, our scheme for complete population transfer with few-cycle Gaussian shaped laser pulses …
Pulsed lasers offer significant advantages over CW lasers in the coherent control of qubits. Here we review the theoretical and experimental aspects of controlling the internal and external states of individual trapped atoms with pulse trains. Two distinct regimes of laser intensity are identified. When the pulses are sufficiently weak that the Rabi frequency $Ω$ is much smaller than the trap frequency $\otrap$, sideband transitions can be addressed and atom-atom entanglement can be accomplished in much the same way as with CW lasers. By contrast, if the pulses are very strong ($Ω\gg \otrap$),…
We report on the comparative experimental investigation on third and fifth harmonic generation (THG and FHG) in atomic and molecular gases driven by mid-infrared ultrafast laser pulses at a wavelength of ~1500 nm. We observe that the conversion efficiencies of both the THG and FHG processes saturate at similar peak intensities close to ~1.5\times1014 W/cm2 for argon, nitrogen, and air, whose ionization potentials are close to each other. Near the saturation intensity, the ratio of yields of the FHG and THG reaches ~10-1 for all the gases. Our results show that high-order Kerr effects do exist,…
We show how to emulate a conventional pump-probe scheme using a single frequency-chirped ultrashort UV pulse to obtain a time-resolved image of molecular ultrafast dynamics. The chirp introduces a spectral phase in time that encodes the delay between the pump and the probe frequencies contained in the pulse. By comparing the results of full dimensional ab initio calculations for the H$^+_2$ molecule with those of a simple sequential model, we demonstrate that, by tuning the chirp parameter, two-photon energy-differential ionization probabilities directly map the wave packet dynamics generated …
Ultrafast electronic dynamics are typically studied using pulsed lasers. We demonstrate a complementary experimental approach: quantum simulation of ultrafast dynamics using trapped ultracold atoms. Counter-intuitively, this technique emulates some of the fastest processes in atomic physics with some of the slowest, leading to a temporal magnification factor of up to twelve orders of magnitude. In these experiments, time-varying forces on neutral atoms in the ground state of a tunable optical trap emulate the electric fields of a pulsed laser acting on bound charged particles. We demonstrate t…
The absorption of a single photon that excites a quantum system from a low to a high energy level is an elementary process of light-matter interaction, and a route towards realizing pure single-photon absorption has both fundamental and practical implications in quantum technology. Due to nonlinear optical effects, however, the probability of pure single-photon absorption is usually very low, which is particularly pertinent in the case of strong ultrafast laser pulses with broad bandwidth. Here we demonstrate theoretically a counterintuitive coherent single-photon absorption scheme by eliminat…
Carrier envelope phase (CEP) stabilized pulses of intense 800 nm light of 5 fs duration are used to probe the dissociation dynamics of dications of isotopically-substituted water, HOD. HOD$^{2+}$ dissociates into either H$^+$ + OD$^+$ or D$^+$ + OH$^+$. The branching ratio for these two channels is CEP-dependent; the OD$^+$/OH$^+$ ratio (relative to that measured with CEP-unstabilized pulses) varies from 150% to over 300% at different CEP values, opening prospects of isotope-dependent control over molecular bond breakage. The kinetic energy released as HOD$^{2+}$ Coulomb explodes is also CEP-d…
