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Journal of Physics B Atomic Molecular and Optical Physics

Phase sensitive coherent control of atomic excitation in the presence of static electric fields: a frame transformation Stark theory approach

S. Cohen

Published Sep 29, 2011• 2 citations
Publisher

Abstract

Phase sensitive coherent control on atomic Rydberg states and in the presence of a static electric field is theoretically studied using Harmin's frame transformation theory. It is shown that under the presence of the static field, the total excitation rate of an atomic target by a bichromatic laser field (consisting of a fundamental radiation frequency and of its second harmonic) depends on all the elements of the density-of-states matrix dictating the Stark effect. Some of these off-diagonal matrix elements are inaccessible by any other photoexcitation scheme and affect non-trivially the optimum achievable rate modulation contrast. This fact leads to important qualitative and quantitative differences with respect to static-field-free coherent control. The obtained formal expressions for the phase-controlled excitation rate are applied to the lithium target atom. It is demonstrated that the electric field strength can be used as an additional, externally adjustable, control and manipulation parameter. Finally, it is shown that above the saddle point energy, where quasi-discrete and continuum states coexist, the lineshapes of individual Fano-like resonances can be quite efficiently modified by applying this scheme.

DOI
10.1088/0953-4075/44/20/205402

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Phase sensitive coherent control on atomic Rydberg states and in the presence of a static electric field is theoretically studied using Harmin's frame transformation theory. It is shown that under the presence of the static field, the total excitation rate of an atomic target by a bichromatic laser field (consisting of a fundamental radiation frequency and of its second harmonic) depends on all the elements of the density-of-states matrix dictating the Stark effect. Some of these off-diagonal matrix elements are inaccessible by any other photoexcitation scheme and affect non-trivially the optimum achievable rate modulation contrast. This fact leads to important qualitative and quantitative differences with respect to static-field-free coherent control. The obtained formal expressions for the phase-controlled excitation rate are applied to the lithium target atom. It is demonstrated that the electric field strength can be used as an additional, externally adjustable, control and manipulation parameter. Finally, it is shown that above the saddle point energy, where quasi-discrete and continuum states coexist, the lineshapes of individual Fano-like resonances can be quite efficiently modified by applying this scheme.
We experimentally demonstrate one- and two-photon phase sensitive coherent control over the excitation and ionization of Rydberg states of Sr atom in the presence of a static homogeneous electric field. Without the field this excitation scheme can only be employed for the manipulation of angular distributions of photoelectrons and molecular photofragmentation products. Total atomic excitation-ionization yields cannot be modulated because the final states excited by each pathway are orthogonal to each other. When, however, a static electric field is applied, sss, ppp and ddd character is admixed into the final Rydberg state, which has no definite parity anymore. Hence, the excitation of the target Stark state from the ground state is possible with either two (fundamental laser frequency) photons or one (second harmonic frequency) photon and its population and further ionization can be controlled by varying the relative phase between the two radiation fields. The concept is successfully tested below as well as above the classical saddle point and with either mutually crossed or parallel linear laser beam polarizations (while the second harmonic beam polarization vector is always parallel to the static field direction). We examine the behavior of the obtained photoionization signal modulation depth VVV as a function of the static field strength FFF for otherwise identical experimental conditions. The V(F)V(F)V(F) curve exhibits a maximum (typically $\ensuremath{\sim}65%--85%$) at a field strength value that is dictated by the interplay between the employed laser power densities, one- and two-photon transition dipole moments, and relative amounts of field-dependent sss, ppp and ddd character. It is therefore shown that the static field strength may serve as an additional, experimentally adjustable, control parameter in a fashion complementary to both the intensities and relative phase of the two light beams.
The paper is devoted to the theoretical investigation of the phase control of atomic photo-excitation in discrete energy spectrum under the action of bichromatic laser field with the frequency ratio 1:2 in the presence of stationary electric field. The calculations are made for the case of alkali atoms. It is shown that the phase modulation of the photo-excitation strongly depends upon the electric field strength and the ratio between the intensities of the monochromatic components of the radiation. The optimal range of parameters for the effect observation is determined.
Synopsis Photoionization microscopy (PM) is employed for imaging the flux of slow (meV) electrons ejected via atomic photoionization in the presence of a static electric field. Just above the ionization limit continuum and quasi-disrete states are degenerate. In hydrogen atom resonant excitation dominates over the continuum one, while the reverse holds for more complex atoms. We demonstrate theoretically that by using a bichromatic ω/2ω laser field and by applying phase sensitive coherent control techniques it is possible to unbury and isolate other-wise obscured resonant features in PM images.
A new method for coherent phase control of excitation of atoms in a discrete spectrum under the action of bichromatic laser radiation with the frequency ratio 1 : 2 is analysed. An important feature of this control method is the presence of a electrostatic field, which removes the parity selection rule for one of the control channels. It is shown that for the phase difference between the monochromatic radiation components, corresponding to the destructive interference between channels, there exists the electrostatic field strength at which the excited atomic transition is `bleached'. It is proposed to use luminescence at the adjacent atomic transition for detecting the phase dependence of optical excitation.
In this work, numerical calculations were implemented based on the diagonalisation of a matrix representation of the Stark Hamiltonian on a subset of the basis given by the zero-field Hamiltonian. Dipole matrix elements between the involved states were calculated, which allow for the prediction of transition strengths to Stark shifted Rydberg states. The applicability of the numerical methods were confirmed experimentally by precision spectroscopy in a rubidium vapour cell with electrodes using electromagnetically induced transparency (EIT). The numerical methods were then extended to predict ionisation rates of Rydberg states in the highly Stark shifted regime beyond the classical ionisation threshold. For this purpose, a complex absorbing potential (CAP) was specifically adjusted to the Stark Hamiltonian. An experiment was conducted, in which cold atoms from a magneto-optical trap (MOT) were excited to Stark shifted Rydberg states and the arising ions were detected. The obtained ionisation spectra agree well with the results from the numerical calculations. Another extension of the numerical methods was implemented for crossed electric and magnetic fields. This was used for approximate calculations of the motional Stark effect (MSE), which acts on atoms moving through static magnetic fields and thereby experiencing a Lorentz electric field. In a precision spectroscopy, once more using EIT in a vapour cell, the MSE was observed in low magnetic fields for the first time in rubidium. The spectral shift, which is caused by the MSE, matches the prediction from the numerical calculations. In a final experiment, the practical use of the knowledge of several properties of Stark shifted Rydberg states was illustrated. The numerical methods including the CAP were used to specifically select states for their optical accessibility, permanent electric dipole moments and ionisation rates. In the experiment, atoms from a MOT were excited to these states to observe different characteristics of the dipole blockade effect. The detection scheme for this experiment was realised by controlled ionisation using only small changes in the external electric field.
A novel theoretical study of the control of translational motion of atomic and molecular Rydberg states in inhomogeneous static electric fields is presented. Simulations have been carried out demonstrating that, under realistic conditions, the deflection and focusing of Rydberg atoms and molecules should be achievable. Advantage is taken of the high susceptibility of the Rydberg states to external electric fields, allowing the use of much smaller fields than would be necessary for ground state neutrals. The simulations presented are for trajectories of Rydberg states with n = 18-20 in the fields of an electric dipole, quadrupole and hexapole. A deflection of 7 mm is predicted for n = 18 Rydberg states travelling parallel to the dipole after 100 µs time of flight. In the hexapole n = 20 Rydberg states are refocused to a spot size of the order of the laser beam waist (10 µm) after 20 µs. It is demonstrated that the hexapole can also act as a cylindrical lens if its axis is perpendicular to the Rydberg beam direction. Spontaneous emission and black-body decay rates are also calculated, and their variation with the applied field is investigated. The potential applications of this work might include the use of focusing and deflection for controlled low-energy collisions of Rydberg molecules with surfaces.