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Rydberg states of helium in electric and magnetic fields of arbitrary relative orientation

Ondřej Tkáč, Matija Žeško, Josef A. Agner, Hansjürg Schmutz, Frédéric Merkt

Published Apr 1, 2016• 5 citations
Publisher

Abstract

A spectroscopic study of Rydberg states of helium (n = 30 and 45) in magnetic, electric and combined magnetic and electric fields with arbitrary relative orientations of the field vectors is presented. The emphasis is on two special cases where (i) the diamagnetic term is negligible and both paramagnetic Zeeman and Stark effects are linear (n = 30, B ≤ 120 mT and F = 0-78 V cm⁻¹), and (ii) the diamagnetic term is dominant and the Stark effect is linear (n = 45, B = 277 mT and F = 0-8 V cm⁻¹). Both cases correspond to regimes where the interactions induced by the electric and magnetic fields are much weaker than the Coulomb interaction, but much stronger than the spin-orbit interaction. The experimental spectra are compared to spectra calculated by determining the eigenvalues of the Hamiltonian matrix describing helium Rydberg states in the external fields. The spectra and the calculated energy-level diagrams in external fields reveal avoided crossings between levels of different m ₗ values and pronounced m ₁-mixing effects at all angles between the electric- and magnetic-field vectors other than 0. These observations are discussed in the context of the development of a method to generate dense samples of cold atoms and molecules in a magnetic trap following Rydberg-Stark deceleration.

DOI
10.3929/ethz-a-010893670

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Abstract A spectroscopic study of Rydberg states of helium ( n = 30 and 45) in magnetic, electric and combined magnetic and electric fields with arbitrary relative orientations of the field vectors is presented. The emphasis is on two special cases where (i) the diamagnetic term is negligible and both paramagnetic Zeeman and Stark effects are linear ( n = 30, B ≤ 120 mT and F = 0–78 V cm −1 ), and (ii) the diamagnetic term is dominant and the Stark effect is linear ( n = 45, B = 277 mT and F = 0–8 V cm −1 ). Both cases correspond to regimes where the interactions induced by the electric and magnetic fields are much weaker than the Coulomb interaction, but much stronger than the spin–orbit interaction. The experimental spectra are compared to spectra calculated by determining the eigenvalues of the Hamiltonian matrix describing helium Rydberg states in the external fields. The spectra and the calculated energy-level diagrams in external fields reveal avoided crossings between levels of different m l values and pronounced m l -mixing effects at all angles between the electric- and magnetic-field vectors other than 0. These observations are discussed in the context of the development of a method to generate dense samples of cold atoms and molecules in a magnetic trap following Rydberg–Stark deceleration.

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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.

•Jan 1, 2018•0 citations
A spectroscopic study of Rydberg states of helium (n = 30 and 45) in magnetic, electric and combined magnetic and electric fields with arbitrary relative orientations of the field vectors is presented. The emphasis is on two special cases where (i) the diamagnetic term is negligible and both paramagnetic Zeeman and Stark effects are linear (n = 30, B ≤ 120 mT and F = 0-78 V cm⁻¹), and (ii) the diamagnetic term is dominant and the Stark effect is linear (n = 45, B = 277 mT and F = 0-8 V cm⁻¹). Both cases correspond to regimes where the interactions induced by the electric and magnetic fields are much weaker than the Coulomb interaction, but much stronger than the spin-orbit interaction. The experimental spectra are compared to spectra calculated by determining the eigenvalues of the Hamiltonian matrix describing helium Rydberg states in the external fields. The spectra and the calculated energy-level diagrams in external fields reveal avoided crossings between levels of different m ₗ values and pronounced m ₁-mixing effects at all angles between the electric- and magnetic-field vectors other than 0. These observations are discussed in the context of the development of a method to generate dense samples of cold atoms and molecules in a magnetic trap following Rydberg-Stark deceleration.
Abstract A spectroscopic study of Rydberg states of helium ( n = 30 and 45) in magnetic, electric and combined magnetic and electric fields with arbitrary relative orientations of the field vectors is presented. The emphasis is on two special cases where (i) the diamagnetic term is negligible and both paramagnetic Zeeman and Stark effects are linear ( n = 30, B ≤ 120 mT and F = 0–78 V cm −1 ), and (ii) the diamagnetic term is dominant and the Stark effect is linear ( n = 45, B = 277 mT and F = 0–8 V cm −1 ). Both cases correspond to regimes where the interactions induced by the electric and magnetic fields are much weaker than the Coulomb interaction, but much stronger than the spin–orbit interaction. The experimental spectra are compared to spectra calculated by determining the eigenvalues of the Hamiltonian matrix describing helium Rydberg states in the external fields. The spectra and the calculated energy-level diagrams in external fields reveal avoided crossings between levels of different m l values and pronounced m l -mixing effects at all angles between the electric- and magnetic-field vectors other than 0. These observations are discussed in the context of the development of a method to generate dense samples of cold atoms and molecules in a magnetic trap following Rydberg–Stark deceleration.
The results of an experimental study of the Rydberg spectrum of rubidium in crossed electric and magnetic fields are reported and compared with theoretical predictions. The present investigations have been conducted in the low-field regime in which the paramagnetic and linear Stark interactions are perturbations to the Coulomb energy. When quantum-defect corrections are negligible, the SO(4) symmetry of the Coulomb interaction organizes the hydrogenic energy spectrum according to the law En{\mathit{E}}_{\mathit{n}}En​,k=-R/n2{\mathit{n}}^{2}n2+\ensuremath{\Elzxh}k(${\mathrm{\ensuremath{\omega}}}_{\mathit{L}}^{2}$+${\mathrm{\ensuremath{\omega}}}_{\mathit{S}}^{2}$)1/2{)}^{1/2})1/2, where k is an integer such that -(n-1)\ensuremath{\le}k\ensuremath{\le}(n-1), and ${\mathrm{\ensuremath{\omega}}}_{\mathit{L}}$,${\mathrm{\ensuremath{\omega}}}_{\mathit{S}}$, are, respectively, the Larmor and linear Stark frequencies. The experimental evidence for such a quantization is presented in rubidium Rydberg series using Doppler-free two-photon spectroscopy. The role of quantum defects is incorporated into the theory and experimentally demonstrated.
The problem of Rydberg atomic spectra in crossed electric F and magnetic B fields (combined Stark–Zeeman effects), as well as an oscillating electric field are under consideration. The main problem is the great array of radiative transitions between the Rydberg atomic states. The different versions of semiclassical approaches are applied for the solution of the problem. New approximate selection rules are established to simplify the matrix elements of radiative transitions, making it possible to reduce the complex expressions of Gordon’s hypergeometric series to the trivial trigonometric functions. Simple analytical formulas for the dipole matrix elements of a Rydberg hydrogen-like atom in external crossed electric and magnetic fields for Hnα are obtained. The specific calculations are presented for n = 10 to 9 transition both for parallel and perpendicular orientations of F–B fields. The result of Blokhintsev for a single Stark component in oscillating field is generalized for the array of radiative transitions between Rydberg atomic states. Such spectra with large values of modulation index are compared with static ones.
We study the spectra of diamagnetic rubidium Rydberg atoms in strong magnetic and weak electric parallel fields, in the nnn-mixing regime. Our emphasis is on isolated pairs of near-degenerate, opposite-parity, diamagnetic states that become mixed by the weak electric field. Such level pairs allow for the generation of nondegenerate states with large, tunable permanent electric dipole moments and large optical excitation cross sections from the atomic ground state. We investigate how the dipole moments and the zero-electric-field energy defects of these level pairs can be tuned using small variations of the electric and magnetic fields. Using calculations, we explore the abundance of such level pairs over wide spectral regions for several magnetic quantum numbers. Applications of polar, diamagnetic Rydberg states in Rydberg-atom interaction experiments are briefly discussed.
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.