Floquet theory for short laser pulses

We develop adiabatic perturbation theory for quantum systems responding to short laser pulses, with or without a frequency chirp. Our approach rests on lifting the time-dependent Schr?dinger equation to an extended Hilbert space, then applying standard perturbational techniques to Floquet states in this extended space, and finally projecting back to the physical Hilbert space. The same strategy also allows us to construct superadiabatic bases for monitoring the quantum evolution in the course of a pulse. These bases provide a diagnostic tool for improving the efficiency of pulse-induced population transfer. The formalism is applied to the selective excitation of molecular vibrational states by chirped laser pulses, which exploit either successive single-photon resonances or a multiphoton resonance, and by a STIRAP-like process. Received: 23 June 1998 / Revised: 18 August 1998 / Accepted: 25 August 1998     

Limitations of the strong field approximation in ionization of the hydrogen atom by ultrashort pulses

We present a theoretical study of the ionization of hydrogen atoms as a result of the interaction with an ultrashort external electric field. Doubly-differential momentum distributions and angular momentum distributions of ejected electrons calculated in the framework of the Coulomb-Volkov and strong field approximations, as well as classical calculations are compared with the exact solution of the time dependent Schr ödinger equation. We show that in the impulsive limit, the Coulomb-Volkov distorted wave theory reproduces the exact solution. The validity of the strong field approximation is probed both classically and quantum mechanically. We found that classical mechanics describes the proper quantum momentum distributions of the ejected electrons right after a sudden momentum transfer, however pronounced the differences at latter stages that arise during the subsequent electron-nucleus interaction. Although the classical calculations reproduce the quantum momentum distributions, it fails to describe properly the angular momentum distributions, even in the limit of strong fields. The origin of this failure can be attributed to the difference between quantum and classical initial spatial distributions.     

Independent electron theory of multiple ionization of xenon by intense laser pulses

The intensity dependence of the multiphoton ionization spectra of Xe atoms has been investigated with an improved accuracy and well-controlled laser parameters. In particular, we have examined the ionization rates for X³⁺, X²⁻, X⁺ as functions of the laser intensity and the pressure in the target chamber. The apparatus used for these measurements is characterized by a high-energy resolution (better than 200 meV) and a completely digital acquisition system. The time-of-flight spectra clearly show the contributions of the different isotopes present in Xe gas. The laser pulses have been characterized with great accuracy by monitoring the energy, pulse width and divergence shot by shot. The ionization rates of the different ions have been used for testing the basic assumption of the Geltman theory of multiple ionization based on the single electron ionization model. We have found that for the small intensity range investigated the quantity (dXe ⁺/dI)·(dXe ³⁺/dI)/(dXe ²⁺/dI)² appears to be quite close to the value 0.5 predicted by this model.     

Adiabatic population transfer in multistate chains via dressed intermediate states

The well-known process of stimulated Raman adiabatic passage (STIRAP) provides a robust technique for achieving complete population transfer between the first and last state of a three-state chain, with little population, even transiently, in the intermediate state. The extension of STIRAP to general N-state chainwise-linked systems continues to generate interest. Recently Malinovsky and Tannor (Phys. Rev. A 56, 4929 (1997)) have shown with numerical simulation that a resonant pulse sequence, which they term “straddle STIRAP”, can produce (under appropriate conditions, including specific pulse areas) complete population transfer with very little population in intermediate states. Their proposal supplements a pair of counterintuitively ordered delayed laser pulses, driving the first and last transition of the chain and corresponding to the pump and Stokes pulses in STIRAP, with one or more additional strong pulses of longer duration which couple the intermediate transition(s) and overlap both the pump and the Stokes pulses. In this paper, we modify the “straddling” Malinovsky-Tannor pulse sequence so that the intermediate couplings are constant (and strong), at least during the times when the pump and Stokes pulses are present, and the intermediate states therefore act as a strongly coupled subsystem with constant eigenvalues. Under this condition, we show that the original N-state chain is mathematically equivalent to a system comprising N-2 parallel -transitions, in which the initial state is coupled simultaneously to N-2 dressed intermediate states, which in turn are coupled to the final state. The population transfer is optimized by suitably tuning the pump and Stokes frequencies to resonance with one of these dressed intermediate states, which effectively acts as the single intermediate state in a three-state STIRAP-like process. We show that tuning to a dressed intermediate state turns the system (for both odd N and even N) into a three-state system - with all of the properties of conventional STIRAP (complete population transfer, little transient population in the intermediate states, insensitivity to variations in the laser parameters, such as pulse area). The success of the tuning-to-dressed-state idea is explained by using simple analytic approaches and illustrated with numerical simulations for four-, five-, six- and seven-state systems. Received: 17 April 1998 / Accepted: 15 June 1998     

High-order harmonic generation from organic molecules in ultra-short pulses

We have studied high-order harmonic generation (HHG) from organic molecules irradiated with near-infrared high intensity laser pulses of 70 fs and 240 fs duration. The molecular systems studied were the aromatics benzene and naphthalene and the alkanes cyclopropane and cyclohexane (cyclic) and n-hexane (linear). Harmonic intensities were measured both as a function of laser intensity (in the range 5×10¹³-5×10¹⁵ W cm^-2) and as a function of ellipticity of the laser field polarisation. The results were compared with those from the xenon atom. For 70 fs pulses, harmonic generation from the organic systems was similar to that of xenon, revealing an atom-like behaviour for molecules when the laser pulse duration is shorter than the fragmentation timescale of the molecule. We note significant differences between molecules with respect to HHG efficiencies and the suppression of HHG in larger species. We discuss these differences in the context of the molecular properties, electronic structure and behaviour of ionisation and fragmentation that result in enhancement of field ionisation in larger systems. Study of the polarisation ellipticity dependence of HHG shows that the harmonic yield in molecules is less sensitive to the polarisation than for atoms (xenon). This is consistent with the expected behaviour given the larger recollision cross-section presented by the core in the molecular system compared to the atom. Our results suggest that study of HHG from molecules exposed to ultra-short pulses is potentially a powerful tool for understanding the electron dynamics of molecules exposed to an intense field. Received 14 September 2000 and Received in final form 6 December 2000     

Perturbative and nonperturbative processes in adiabatic population transfer

With the help of superadiabatic techniques for quantum systems depending slowly on time, we demonstrate how the total transition amplitude, tracked in time in the usual adiabatic basis, can be decomposed into a perturbative part consisting of terms proportional to powers of the adiabaticity parameter, and a nonperturbative component. The interference of both components underlies the oscillations that accompany transitions in the adiabatic basis. Whereas for traditionally considered systems the final nonadiabatic transition probability is determined by the nonperturbative part alone, this is no longer correct for models describing stimulated Raman adiabatic passage (STIRAP). We explain the recently discovered breakdown of the Dykhne-Davis-Pechukas formula on general grounds, and provide simple, but accurate approximations for transition amplitudes in STIRAP systems. Received: 22 January 1998 / Revised: 17 March 1998 / Accepted: 31 March 1998     

Resonance fluorescence spectrum of a three-level atom driven by coherent and stochastic fields

The dressed-state populations and the resonance fluorescence spectrum of a V-type three-level atom driven by a strong coherent field and a weak stochastic one simultaneously are investigated. There can be significant population inversion due to the effect of the stochastic field. The atomic resonance fluorescence spectrum can be controlled by adjusting the frequency difference between the coherent field and the stochastic one and the coherent Rabi frequency. Peak suppression and line narrowing occur under appropriate conditions. Received 23 June 2000 and Received in final form 18 January 2001     

Influence of nonlinear quantum dissipation on the dynamical properties of the f-deformed Jaynes-Cummings model in the dispersive limit

We investigate the effect of a static electric field on photoionization of the He atom in the ground 1S and low-lying 2S and 2P excited states. The field-affected ionization potential and photoionization cross-section are determined from the complex eigenvalues of the time-dependent Schr?dinger equation solved by the complex rotation method in the Floquet ansatz. Accuracy of the method is enhanced by the use of the Hylleraas basis set. For the ground state of helium, we find that the total photoionization cross-section remains constant or decreases as a function of the DC field strength until this field reaches a certain critical value. For the low-lying excited states, effect of the static field is similar to the ordinary DC Stark effect.     

Wavelength control in Er <Emphasis Type="Bold">3+</Emphasis>-doped fluoride glasses laser by a coherent field

A five-level system to control the wavelength of the in-line amplifier by the quantum interference is proposed. It is found that the gains of the first and the second probe can be adjusted by changing the coherent field and the incoherent pumping. The new scheme may find its application in optical switch and optical communications. Received 9 October 2002 Published online 24 April 2003 RID="a" ID="a"e-mail: qol@mail.jlu.edu.cn     

Coherent population trapping involving Rydberg states in xenon probed by ionization suppression

We report the observation of pronounced coherent population trapping and dark resonances in Rydberg states of xenon. A weak two-photon coupling with radiation of = 250 nm is induced between the 5p^{6 1} S ₀ ground state of xenon and state 5p ⁵6p[1/2]₀, leading to (2+1) resonantly enhanced three-photon ionization. The state 5p ⁵6p[1/2]₀ is strongly coupled by radiation with ≃ 600 nm to 5p ⁵ ns[J _C]₁ or 5p ⁵ nd[J _C]₁ Rydberg states with principal quantum numbers n in the range 18 ?n? 23 and with the rotational quantum number of the ionic core J _C = 1/2 or J _C = 3/2. The ionization is monitored through observation of the photoelectrons with an energy resolution ΔE = 150 meV which is sufficient to distinguish the ionization processes into the two ionization continua. Pronounced and robust dark resonances are observed in the ionization rate whenever is tuned to resonance with one of the ns- or nd-Rydberg states. The dark resonances are due to efficient population trapping in the atomic ground state 5p^{6 1} S ₀ through the suppression of excitation of the intermediate state 5p ⁵6p[1/2]₀. The resolution is sufficient to resolve the hyperfine structure of the ns-Rydberg levels for odd xenon isotopes. The hyperfine splitting does not vary significantly with n in the given range. Results from model calculations taking the natural isotope abundance into account are in good agreement with the observed spectral structures. Pronounced dark resonances are also observed when the dressing radiation field with is generated from a laser with poor coherence properties. The maximum reduction of the ionization signal clearly exceeds 50%, a value which is expected to be the maximum, when the dip is caused by saturation of the transition rate between the intermediate and the Rydberg state due to incoherent radiation. This work demonstrates the potential of dark resonance spectroscopy of high lying electronic states of rare gas atoms. Received 7 May 2000 and Received in final form 25 June 2001     

Non-adiabatic quantum molecular dynamics: General formalism and case study H<Subscript>2</Subscript><Superscript>+</Superscript> in strong laser fields

In Rydberg atoms subject to static and harmonic collinear electric fields, intrashell transition can be induced by the first order perturbation from a small perpendicular electric or magnetic field, or by effects of the second order in the major fields. Both mechanisms lead to resonances that are suppressed under certain conditions, and high-frequency interference oscillations in case of non-adiabatic field switching. Recent measurements of microwave ionization signals show very rich and fascinating structures similar to the ones predicted for intrashell mixing. We show that the observed ionization structures may be explained by diabatic electric-field ionization and the consistent use of perturbation theory for intrashell mixing. In particular, the dominant oscillation frequency is successfully interpreted in terms of interference between first and second order transition amplitudes. New predictions are provided. The present approach gives a comprehensive picture of intrashell transitions, which may be tested in future experiments designed to observe such transitions directly. Received 2 May 2002 / Received in final form 23 September 2002 Published online 21 January 2003 RID="a" ID="a"e-mail: Valentin.Ostrovsky@pobox.spbu.ru RID="b" ID="b"e-mail: horsdal@ifa.au.dk     

Absorption spectrum of a resonantly driven degenerate V-type atom with a dc-field coupling between excited states

We study the absorption spectra of a degenerate V-type atom, where a resonant driving field and a probe field drive different branches of transitions and a dc field is applied to drive the transition between two excited states. The effects of vacuum induced coherence (VIC) on the absorption spectra are investigated. It is demonstrated that in some special cases the VIC can lead to the depression of absorption and narrow resonance. The origin of these features are discussed. When the pump field and the dc field have the same intensity, it is interesting to find that the whole absorption spectrum comes mainly from the absorptions induced by the interferences among different transitions between dressed states.     

An electromagnetic wave propagation in a non-uniform plasma controlled by EIT

We investigate the conditions in which the propagation of an electromagnetic wave is changed from transparency to cutoff in a non-uniform plasma. The allowed frequency range of the driving wave is obtained for the case that the probe frequency is above the plasma frequency. The effect of the power of the driving field on the range is analyzed. Received 23 May 2001     

Study of width and height of EIT resonance in a Doppler broadened five-level system with varying probe power

We report the experimental observation of electromagnetically induced transparency (EIT) in a Doppler broadened rubidium vapour at room temperature for different probe intensities at a fixed pump intensity in a five-level Λ-type system formed by the D₂ transition of ⁸⁵Rb. For a constant pump intensity, we find that the EIT width and height change with the variation of probe intensity. We observe a nonlinear variation of the height of the EIT peak and a linear variation of the width (FWHM) of the EIT signal with probe intensity. In the Doppler broadened multilevel system, we also observe the velocity selective dips along with the EIT signal. A numerical simulation of the probe response signal based on density matrix representation in a five-level system is carried out to reproduce the experimentally observed spectra.     

Two strong nonlinearity regimes in cold molecule formation

Two distinct strongly non-linear scenarios of molecule formation in an atomic Bose-Einstein condensate (either by photoassociation or Feshbach resonance) corresponding to large and small field detuning are revealed. By examining arbitrary external field configurations, we show that the association process in the first case is almost non-oscillatory in time while in the second case the evolution of the system displays strongly pronounced Rabi-type oscillations. We construct highly accurate approximate solutions for both limit cases. We show that at strong coupling limit the non-crossing models are able to provide conversion of no more than one third of the initial atomic population. Finally, we show that for constant-amplitude models involving a finite final detuning the strong interaction limit is not optimal for molecule formation.     

Phase control of maximal atomic coherence

The atomic coherence in a three-level Λ atom is studied, in which each optical transition is driven by a coherent field and the metastable states are coupled to each other via a microwave field. It’s shown that the atomic coherence crucially depends on the relative phase delay between the envelopes of the amplitudes of the three coupling fields. In particular, when the phase delay is adjusted to 0 or π, the maximal atomic coherence arises, while the maximal atomic coherence doesn’t occur once the phase delay is changed to π/2. The maximal atomic coherence is attributed to the trapping of the population in the lower sublevels.     

Ionization of Rydberg atoms in THz-laser fields at the transition from low to high scaled frequencies

We have studied the ionization of Rydberg-excited xenon atoms in THz-laser fields and by quantum dynamical calculations. The experimental threshold laser field strength for 10% ionization probability follows an n^*-1.68 (1.04 THz) dependence (n^* effective principal quantum number) with additional weak resonance structures and shows that ionization does not occur by a Landau-Zener mechanism. At scaled frequencies of to 5.6 the simulated threshold fields for ionization in oscillatory fields show a dependence on the principal quantum number n of n^-4.1 to n^-1.35. Received: 17 February 1998 / Revised: 20 April 1998 / Accepted: 21 April 1998     

Coherent control of stimulated emission inside one dimensional photonic crystals: strong coupling regime

The present paper discusses the stimulated emission, in strong coupling regime, of an atom embedded inside a one dimensional (1D) Photonic Band Gap (PBG) cavity which is pumped by two counter-propagating laser beams. Quantum electrodynamics is applied to model the atom-field interaction, by considering the atom as a two level system, the e.m. field as a superposition of normal modes, the coupling in dipole approximation, and the equations of motion in Wigner-Weisskopf and rotating wave approximations. In addition, the Quasi Normal Mode (QNM) approach for an open cavity is adopted, interpreting the local density of states (LDOS) as the local density of probability to excite one QNM of the cavity; and therefore rendering this LDOS dependent on the phase difference of the two laser beams. In this paper we demonstrate that the strong coupling regime occurs at high values of the LDOS. In accordance with the results of the literature, the emission probability of the atom decays with an oscillatory behaviour, so that the atomic emission spectrum exhibits two peaks (Rabi splitting). The novelty of this work is that the phase difference of the two laser beams can produce a coherent control of both the oscillations for the atomic emission probability and, as a consequence, of the Rabi splitting in the emission spectrum. Possible criteria to design active delay lines are finally discussed.     

Enhanced narrow spectral line and double electromagnetically induced two-photon transparency induced by double dark resonances

We theoretically investigate the features of two-photon absorption in a five-level atomic system with interacting dark resonances. It is found that two-photon absorption can be completely suppressed at two different frequencies due to the application of two coherent coupling fields and the atomic system exhibits double electromagnetically induced transparency windows against two-photon absorption. The position and width of the double two-photon transparency windows can be controlled via properly adjusting the frequency detuning and the intensities of the two coupling fields. In addition, one enhanced narrow central line can be observed in the two-photon absorption spectra, which may find applications in high-precision spectroscopy. Form a physical point of view, we explicitly explain these results in terms of quantum interference induced by three different two-photon excitation channels in the dressed-state picture.     

Quasiclassical dynamics of resonantly driven Rydberg states

We present a semiclassical analysis of the dynamics of Rydberg states of atomic hydrogen driven by a resonant microwave field of linear polarization. The semiclassical quasienergies of the atom in the field are found to be in very good agreement with the exact quantum solutions. The ionization rates of individual eigenstates of the atom dressed by the field reflect their quasiclassical dynamics along classical periodic orbits in the near integrable regime, but exhibit a transition to nonspecific rates when global chaos takes over in phase space. We concentrate both on the principal resonance where the unperturbed Kepler frequency is equal to the driving field frequency and on the higher primary resonance The latter case allows for the construction of nondispersive wave packets which propagate along Kepler ellipses of intermediate eccentricity. Received: 23 June 1998 / Accepted: 10 November 1998