We investigate computationally a method for ultrafast preparation of alkali metal atoms in their Rydberg states using a three-dimensional model potential in the single active electron approximation. By optimizing laser pulse shapes that can be generated with modern waveform synthesizers, we propose pulses for controlling the population transfer from the ground state to a preselected set of Rydberg states. Dynamical processes under the optimized pulses are shown to be much more complicated than in the traditional optical two-photon preparation of Rydberg states.
We investigate the Rydberg states generation of Hydrogen atoms with intense laser pulses, by solving the time-dependent Schrödinger equation and by means of classical trajectory monte-carlo simulations. Both linearly polarized multi-cycle pulses and pairs of optical half cycle pulses are used. Comparisons between these methods show that both the Coulomb force and initial lateral momentum, which have effects on the $n$-distribution and $l$-distribution of the population of excited states, are important in the generation of Rydberg states.
Population transfer between low lying Rydberg states independent of the initial state is realized using a train of half-cycle pulses with pulse durations much less than the classical orbit period. We demonstrate experimentally the transfer of population from initial states around n=50 down to n<40 as well as up to the continuum. The measured population transfer matches well to a model of the process for 1D atoms.
The dissociation dynamics of diatomic molecules interacting with (near) optical laser pulses of different duration is investigated by an elaborate discussion of the electric field of the laser and by a direct solution of the time-dependent molecular Schrödinger equation. The systematic variation of the pulse duration from the electronic time scale (attoseconds) to the nuclear time scale (femtoseconds) shows that the employed few-cycle laser pulses lead to well-known but quite different dissociation mechanisms. A comparative calculation with a model pulse and an experimentally realized attoseco…
Rydberg atoms have shown significant promise as the basis for highly sensitive detectors of continuous radio-frequency (RF) E-fields. Here, we study their time-dependent response to pulse-modulated RF E-fields at 19.4 GHz using a cesium vapour cell at room temperature. We use density matrix simulations to explain the time scales that shape the transient atomic response under different laser conditions, finding them to be limited by dephasing mechanisms including transit time broadening, Rydberg-Rydberg collisions, and ionization. Using a matched filter, we demonstrate the detection of individu…
An experimental realization of high-precision direct frequency comb spectroscopy using counter-propagating femtosecond pulses on two-photon atomic transitions is presented. Doppler broadened background signal, hampering precision spectroscopy with ultrashort pulses, is effectively eliminated with a simple pulse shaping method. As a result, all four 5S-7S two-photon transitions in a rubidium vapor are determined with both statistical and systematic uncertainties below 10$^{-11}$, which is an order of magnitude better than previous experiments on these transitions.
The kinetic energy distribution of D$^+$ ions resulting from the interaction of a femtosecond laser pulse with D$_2$ molecules is calculated based on the rescattering model. From analyzing the molecular dynamics, it is shown that the recollision time between the ionized electron and the D$_2^+$ ion can be read from the D$^+$ kinetic energy peaks to attosecond accuracy. We further suggest that more precise reading of the clock can be achieved by using shorter fs laser pulses (about 15fs).
We study the field-ionization threshold behavior when a Rydberg atom is ionized by a short single-cycle pulse field. Both hydrogen and sodium atoms are considered. The required threshold field amplitude is found to scale \emph{inversely} with the binding energy when the pulse duration becomes shorter than the classical Rydberg period, and, thus, more weakly bound electrons require larger fields for ionization. This threshold scaling behavior is confirmed by both 3D classical trajectory Monte Carlo simulations and numerically solving the time-dependent Schrödinger equation. More surprisingly, t…
We report on coherent control of excitation processes of translationally ultracold rubidium dimers in a magneto-optical trap by using shaped femtosecond laser pulses. Evolution strategies are applied in a feedback loop in order to optimize the photoexcitation of the Rb2 molecules, which subsequently undergo ionization or fragmentation. A superior performance of the resulting pulses compared to unshaped pulses of the same pulse energy is obtained by distributing the energy among specific spectral components. The demonstration of coherent control to ultracold ensembles opens a path to actively i…
We investigate a long-range interaction between $64D_{5/2}$ Rydberg-atom pairs and antiblockade effect employing a two-color excitation scheme. The first color (pulse A) is set to resonantly excite the Rydberg transition and prepare a few seed atoms, which establish a blockade region due to strong long-range interaction between Rydberg-atom pairs. The second color (pulse B) is blue detuned relative to Rydberg transition and enables further Rydberg excitation of atoms by counteracting the blockade effect. It is found that a few seed atoms lead to a huge difference of the Rydberg excitation with…
We analyze the photoelectron angular distribution in two-pathway interference between non\-resonant one-photon and resonant two-photon ionization of neon. We consider a bichromatic femtosecond XUV pulse whose fundamental frequency is tuned near the $2p^5 3s$ atomic states of neon. The time-dependent Schrödinger equation is solved and the results are employed to compute the angular distribution and the associated anisotropy parameters at the main photoelectron line. We also employ a time-dependent perturbative approach, which allows obtaining information on the process for a large range of puls…
High Harmonic Generation (HHG) creates coherent high frequency radiation via the process of strong field ionization followed by recombination. Recently, a complementary approach based on Frustrated Tunnel Ionization (FTI) was demonstrated (Nature Photonics 12, 620 (2018)). It uses spectrally separated peaks created by lower quantum number Rydberg states to produce coherent extreme ultraviolet (EUV) light. While much is understood about enhancing emission from HHG by controlling recombining electron trajectories, relatively little is known about controlling the quantum number distribution of Ry…
Ionization-free femtosecond UV pulse filamentation resulting from non-perturbative Kerr effect saturation due to transient photoexcitation of molecules
P.N. Lebedev Physical Institute of the Russian Academy of Sciences（俄罗斯科学院列别杰夫物理研究所）
We analyze excitation of two ground state atoms to a double Rydberg state by a two-photon chirped optical pulse in the regime of adiabatic rapid passage. For intermediate Rydberg-Rydberg interaction strengths, relevant for atoms separated by $\sim$ten $μ$m, adiabatic excitation can be achieved at experimentally feasible Rabi frequencies and chirp rates of the pulses, resulting in high transfer efficiencies. We also study the adiabatic transfer between ground and Rydberg states as a means to realize a controlled phase gate between atomic qubits.
We show that a single femtosecond optical frequency comb may be used to induce two-photon transitions between molecular vibrational levels to form ultracold molecules, e.g., KRb. The phase across an individual pulse in the pulse train is sinusoidally modulated with a carefully chosen modulation amplitude and frequency. Piecewise adiabatic population transfer is fulfilled to the final state by each pulse in the applied pulse train providing a controlled population accumulation in the final state. Detuning the pulse train carrier and modulation frequency from one-photon resonances changes the ti…
We show that the use of shaped pulses improves the fidelity of a Rydberg blockade two-qubit entangling gate by several orders of magnitude compared to previous protocols based on square pulses or optimal control pulses. Using analytical Derivative Removal by Adiabatic Gate (DRAG) pulses that reduce excitation of primary leakage states and an analytical method of finding the optimal Rydberg blockade we generate Bell states with a fidelity of $F>0.9999$ in a 300 K environment for a gate time of only $50\;{\rm ns}$, which is an order of magnitude faster than previous protocols. These results esta…
We present direct time- and space- resolved measurements of the electron density of femtosecond laser pulse-induced plasma filaments. The dominant nonlinearity responsible for extended atmospheric filaments is shown to be field-induced rotation of air molecules.
We analyze neutral atom Rydberg $C_Z$ gates based on adiabatic pulses applied symmetrically to both atoms. Analysis with smooth pulse shapes and Cs atom parameters predicts the gates can create Bell states with fidelity ${\mathcal F}>0.999$ using adiabatic rapid passage (ARP) pulses. With globally optimized adiabatic pulse shapes, in a two-photon excitation process, we generate Bell states with fidelity ${\mathcal F}=0.997$. The analysis fully accounts for spontaneous emission from intermediate and Rydberg states, including the Rydberg lifetime in a room temperature environment, but does not i…
We report a study on the optical dipole force on a beam of neutral three-level like atomic system induced by a femtosecond super-Gaussian pulse. We show that maximum coherence between the ground state |1> and the excited state |2> could be achieved using a train of femtosecond pulses. In addition, it is possible to control the trajectory of the atoms in an atomic beam by using the same scheme. The robustness of the scheme against the variation of the pulse parameters is also investigated.
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 have studied the effects of chirped femtosecond laser pulses on the formation of ultracold molecules in a Rb magneto-optical trap. We have found that application of chirped femtosecond pulses suppressed the formation of 85Rb-2 and 87Rb-2 lowest triplet state molecules in contrast to comparable non-chirped pulses, cw illumination, and background formation rates. Variation of the amount of chirp indicated that this suppression is coherent in nature, suggesting that coherent control is likely to be useful for manipulating the dynamics of ultracold quantum molecular gases.
An electric analogue of the longitudinal Stern-Gerlach matter-wave interferometer has been realized for atoms in Rydberg states with high principal quantum number, $n$. The experiments were performed with He atoms prepared in coherent superpositions of the $n=55$ and $n=56$ circular Rydberg states in zero electric field by a $π/2$ pulse of resonant microwave radiation. These atoms were subjected to a pulsed inhomogeneous electric field to generate a superposition of momentum states before a $π$ pulse was applied to invert the internal states. The same pulsed inhomogeneous electric field was th…
It is shown that it is feasible to use ultrashort time delay between two XUV femtosecond pulses in order to control two photon resonant ionization. The proposal is demonstrated on the spectrum of Helium, in terms of nonperturbative solutions of the time dependent Schroedinger equation. Comparison with results from second order time dependent perturbation theory provides additional insight.
We extend the powerful frequency-domain analysis of femtosecond two-photon absorption to the intermediate-field regime, which involves both two- and four-photon transitions. Consequently, we find a broad family of shaped pulses that enhance the absorption over the transform-limited pulse. It includes any spectral phase that is anti-symmetric around half the transition frequency. The spectrum is asymmetric around it. The theoretical framework and results for Na are verified experimentally. This work opens the door for rational femtosecond coherent control in a regime of considerable absorption …
We discover a new mechanism of electronic population inversion using strong femtosecond pulses, where the transfer is mediated by vibrational motion on a light-induced potential. The process can be achieved with a single pulse tuning its frequency to the red of the Franck-Condon window. We show the determinant role that the sign of the slope of the transition dipole moment can play on the dynamics, and extend the method to multiphoton processes with odd number of pulses. As an example, we show how the scheme can be applied to population inversion in Na2.
Photoassociation of ultracold rubidium atoms with femtosecond laser pulses is studied theoretically. The spectrum of the pulses is cut off in order to suppress pulse amplitude at and close to the atomic resonance frequency. This leads to long tails of the laser pulse as a function of time giving rise to coherent transients in the photoassociation dynamics. They are studied as a function of cutoff position and chirp of the pulse. Molecule formation in the electronically excited state is attributed to off-resonant excitation in the strong-field regime.
We report on the generation of intense extreme ultraviolet (EUV) supercontinuum with photon energies spanning from 35 eV to 50 eV (i. e., supporting an isolated attosecond pulse with a duration of ~271 as) by loosely focusing 35 fs, 11 mJ pulses from a femtosecond laser amplifier into a 10-mm long gas cell filled with krypton gas. The dramatic change of spectral and temporal properties of the driver pulses after passing through the gas cell indicates that propagation effects play a significant role in promoting the generation of the EUV supercontinuum.
We propose a new technique to fully characterize the temporal structure of extreme ultraviolet pulses by ionizing a bound coherent electronic wavepacket. The populated energy levels make it possible to interfere different spectral components leading to quantum beats in the photoelectron spectrum as a function of the delay between ionization and initiation of the wavepacket. The influence of the dipole phase, which is the main obstacle for state-of-the-art pulse characterization schemes, can be eliminated by angle integration of the photoelectron spectrum. We show that particularly atomic Rydbe…
We study the photon statistics of weak coherent pulses propagating through a cold Rydberg atomic ensemble in the regime of Rydberg electromagnetically induced transparency. We show experimentally that the value of the second-order autocorrelation function of the transmitted light strongly depends on the position within the pulse and heavily varies during the transients of the pulse. In particular, we show that the falling edge of the transmitted pulse displays much lower values than the rest of the pulse. We derive a theoretical model that quantitatively predicts our results and explains the p…
Multiphoton detachment of F$^-$ by strong few-cycle laser pulses was studied by Shearer and Monteith using a Keldysh-type approach [Phys. Rev. A 88, 033415 (2013)]. We believe that this work contained errors in the calculation of the detachment amplitude and photoelectron spectra. We describe the necessary corrections to the theory and show that the results, in particular, the interference features of the photoelectron spectra, appear noticeably different.
In this work we present a scheme to control the optical dipole trap potential in an N-type four-level atomic system by using chirped femtosecond Gaussian pulses. The spatial size of the trap can be well controlled by tuning the beam waist of the Gaussian pulse and the detuning frequency. The trapping potential splits with increasing Rabi frequency about the center of the trap, a behavior analogous to the one observed experimentally in the context of trapping of nanoparticles with femtosecond pulses. An attempt is made to explain the physics behind this phenomenon by studying the spatial probab…
We introduce a new scheme for generating short-wavelength coherent broadband radiation with well-controlled spectral characteristics. It is based on shaping long-wavelength femtosecond pulse to coherently control atomic resonance-mediated (2+1) three-photon excitation to a broad far-from-resonance continuum. Here, the spectrum (central frequency and bandwidth) of deep-ultraviolet coherent broadband radiation generated in Na vapor is experimentally controlled by tuning the linear chirp we apply to the driving phase-shaped near-infrared femtosecond pulse. This is a first step in implementing the…
We experimentally investigate various processes present in the photoassociative interaction of an ultracold atomic sample with shaped femtosecond laser pulses. We demonstrate the photoassociation of pairs of rubidium atoms into electronically excited, bound molecular states using spectrally cut femtosecond laser pulses tuned below the rubidium D1 or D2 asymptote. Time-resolved pump-probe spectra reveal coherent oscillations of the molecular formation rate, which are due to coherent transient dynamics in the electronic excitation. The oscillation frequency corresponds to the detun-ing of the sp…
This work investigates the utility of femtosecond pulse shaping in increasing the efficiency of Raman excitation of molecules in the strong-field interaction regime. We study experimentally and theoretically the effect of pulse shaping on the strength of non-resonant coherent anti-Stokes Raman scattering in iodine vapor at laser intensities exceeding $10^{13}$ W/cm$^2$. We show that unlike the perturbative case, shaping strong non-resonant laser pulses can increase the signal strength beyond that observed with the transform-limited excitation. Both adiabatic and non-adiabatic schemes of excita…
Fewer-qubit quantum logic gate, serving as a basic unit for constructing universal multiqubit gates, has been widely applied in quantum computing and quantum information. However, traditional constructions for fewer-qubit gates often utilize a multi-pulse protocol which inevitably suffers from serious intrinsic errors during the gate execution. In this article, we report an optimal model about universal two- and three-qubit CNOT gates mediated by excitation to Rydberg states with easily-accessible van der Waals interactions. This gate depends on a global optimization to implement amplitude and…
We explore the effects of ultrafast shaped pulses for two-level systems that do not have a single photon resonance by developing a multiphoton density-matrix approach. We take advantage of the fact that the dynamics of the intermediate virtual states are absent within our laser pulse timescales. Under these conditions, the multiphoton results are similar to the single photon and that it is possible to extend the single photon coherent control ideas to develop multiphoton coherent control.
Metal atoms in solid and liquid helium-4 have attracted some interest either as a way to keep the atoms in a weakly perturbing matrix, or using them as a probe for the helium host medium. Laser sputtering with nanosecond pulsed lasers is the most often used method for atom production, resulting however in a substantial perturbation of the matrix. We show that a much weaker perturbation can be obtained by using femtosecond laser pulses with energy as low as 10 $μ$J. As an unexpected benefit, the atomic density produced is much higher.
We investigate the dynamics of molecular photoexcitation by unchirped femtosecond laser pulses using RbCs as a model system. This study is motivated by a goal of optimizing a two-color scheme of transferring vibrationally-excited ultracold molecules to their absolute ground state. In this scheme the molecules are initially produced by photoassociation or magnetoassociation in bound vibrational levels close to the first dissociation threshold. We analyze here the first step of the two-color path as a function of pulse intensity from the low-field to the high-field regime. We use two different a…
