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arXiv:1212.2220 · Physical Review A

Quantum interference and light polarization effects in unresolvable atomic lines: Application to a precise measurement of the 6 , 7 Li D 2 lines

Roger C. Brown, Saijun Wu, J. V. Porto, Craig J. Sansonetti, Clayton E. Simien, Samuel M. Brewer, Joseph N. Tan, John D. Gillaspy

Published Mar 7, 2013• 88 citations
arXivHTMLPDF

Abstract

We characterize the effect of quantum interference on the line shapes and measured line positions in atomic spectra. These effects, which occur when the excited-state splittings are of order of the natural line widths, represent an overlooked but significant systematic effect. We show that excited-state interference gives rise to non-Lorentzian line shapes that depend on excitation polarization, and we present expressions for the corrected line shapes. We present spectra of ${}^{6,7}$Li $D$ lines taken at multiple excitation laser polarizations and show that failure to account for interference changes the inferred line strengths and shifts the line centers by as much as 1 MHz. Using the correct line shape, we determine absolute optical transition frequencies with an uncertainty of $\ensuremath{\le}$25 kHz and provide an improved determination of the difference in mean-square nuclear charge radii between ${}^{6}$Li and ${}^{7}$Li. This analysis should be important for a number of high-resolution spectral measurements that include partially resolvable atomic lines.

DOI
10.1103/physreva.87.032504

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We characterize the effect of quantum interference on the line shapes and measured line positions in atomic spectra. These effects, which occur when the excited-state splittings are of order of the natural line widths, represent an overlooked but significant systematic effect. We show that excited-state interference gives rise to non-Lorentzian line shapes that depend on excitation polarization, and we present expressions for the corrected line shapes. We present spectra of 6,7{}^{6,7}6,7Li DDD lines taken at multiple excitation laser polarizations and show that failure to account for interference changes the inferred line strengths and shifts the line centers by as much as 1 MHz. Using the correct line shape, we determine absolute optical transition frequencies with an uncertainty of \ensuremath≤\ensuremath{\le}\ensuremath≤25 kHz and provide an improved determination of the difference in mean-square nuclear charge radii between 6{}^{6}6Li and 7{}^{7}7Li. This analysis should be important for a number of high-resolution spectral measurements that include partially resolvable atomic lines.
Doppler-free two-photon (DFTP) spectroscopy is a standard technique for precision measurement of transition frequencies of dipole-forbidden transitions. Here, we report the observation of quantum interference (QI) of optical transition pathways in DFTP spectroscopy of the cesium $6S\text{\ensuremath{-}}7D$ transitions chosen as a prototype system. The QI manifests itself as asymmetric line shapes of the hyperfine lines of the 7D7D7D states, observed through spontaneous emission following excitation by a narrow-linewidth cw laser. The interference persists despite the lines being spectrally well resolved. Ignoring the effect and fitting the spectrum to a Voigt profile causes large systematic shifts in the determination of the line centers, while accounting for QI resolves the apparent line shift and enables the precise determination of hyperfine splitting in the 7D7D7D states. We calculate the spectral line shape including the effect of QI and show that it agrees with the experimental observations. Our results are broadly applicable to other species and have implications for portable secondary optical clocks and precision measurements of hyperfine splittings, isotope shifts, and transition frequencies.
Spectroscopic measurements of transition frequencies in various atomic systems are a significant part of modern physics. They enable the testing of fundamental interactions, the determination of physical constants, and the study of fundamental symmetries that occur in nature with unprecedented accuracy. Studies based on two-photon spectroscopy of simple atoms represent some of the most accurate experiments to date. The verification of precision experimental results is largely supported by theoretical analysis, which is most rigorous for light, nonrelativistic atoms and ions. In the last decade, much attention in the literature has been paid to the study of the quantum interference effect (QIE) in hydrogen and hydrogenlike atomic systems. This has made it possible to significantly reduce the experimental error in determining the appropriate transition frequency. The theoretical description of the QIE corresponds to the consideration of similar pathways arising for close-lying resonant states into which the transition frequency is measured. In the present work, the influence of the emission process on the absorption profile formation is investigated. The results of the studies carried out in this work show the need to take into account the effect of quantum interference in cascade radiation for the precise determination of the absorption transition frequency to highly excited states in two-photon spectroscopic experiments.
A theory on interference effects at high photon densities has been developed for two types of a single three-level atom for which transitions occur: (i) from two different upper levels to a common lower one and (ii) from a common upper level to two different lower levels. The excitation spectrum for the interference effects for the two types of atoms results from the symmetric and antisymmetric interference between the two electronic transitions of the system, respectively. The spectral function for the symmetric modes consists of three Lorentzian lines peaked at the frequencies ω = Δ and ω = Δ ± Ω and having spectral widths of the order of γ0 and 3γ0/4, respectively, where Δ is the beat frequency, Ω is the Rabi frequency, and γ0/2 is equal to the natural linewidth for a photon spontaneously emitted from an isolated atom. The antisy mmetric spectrum consists of the peak of ω = Δ, which has a delta-function distribution indicating the stability of the mode in question, and two Lorentzian lines peaked at ω = Δ ± Ω with radiative widths of the order of γ0/2. The excitation spectrum of each type of atom contains also a Lorentzian line describing the very low frequency mode of the system, respectively.
The effects of different laser line shapes on the intensity and spectrum of resonance fluorescence from a two-level atom are investigated. The laser model considered is that of an ideal single-mode laser operating high above threshold, with constant amplitude and undergoing phase-frequency fluctuations analogous to Brownian motion. As the correlation time of the frequency fluctuations increases from zero to infinity, the laser line shape changes from Lorentzian to Gaussian in a continuous way. It is shown that for intermediate and strong fields, the average intensity of fluorescence in the case of a resonant broadband Lorentzian line shape is higher than that in the case of a Gaussian line shape with the same bandwidth and total power. This is in contrast to the weak-field case where the higher peak power of the Gaussian line shape makes it more effective than the Lorentzian line shape. It is also shown that in the case of a nonzero frequency correlation time (non-Lorentzian line shape) the intensity of fluorescence undergoes non-Markovian fluctuations. In relation to the spectrum of resonance fluorescence, it is shown that as the line shape is varied from Lorentzian to Gaussian the following changes take place: In the case of off-resonance excitation, the asymmetry of the spectrum decreases. In the case of resonant excitation, the center-peak to side-peak height ratio for the triplet structure increases. Moreover, the recently predicted center-line dip, which develops in the spectrum in the case of broadband excitation when the Rabi frequency and the bandwidth are nearly equal, becomes increasingly deeper.
We calculate the effect of light-induced forces on the fluorescence line shape of a two-level atom crossing at right angles two counterpropagating light beams of parallel linear polarizations $(\mathrm{lin}\ensuremath{\Vert}\mathrm{lin})$ in a common configuration for ultrahigh-precision optical spectroscopy. For an incident atomic beam with a narrow spread of transverse velocities the dipole force induces a redshift of the fluorescence maximum, while in the reverse case of a wide spread of transverse velocities the radiation-pressure force induces a blueshift of the saturation dip minimum. We then use our theory to explain the blueshift of the saturation line-center dip occurring for the closed transition $2{}^{3}{S}_{1}\ensuremath{\rightarrow}2{}^{3}{P}_{2}$ of a 4He{}^{4}\mathrm{He}4He beam. The observed shift, which is in quite good agreement with the theory, can be of the order of 1/10 of the transition natural linewidth and hence quite important for ultrahigh-precision spectroscopy measurements.