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arXiv:1203.2828 · Physical Review A

Power-dependent line-shape corrections for quantitative spectroscopy

Thomas M. Stace, Gar-Wing Truong, James D. Anstie, Eric F. May, Andre Nicholas Luiten

Published Jul 17, 2012• 16 citations
arXivHTMLPDF

Abstract

The Voigt profile---a convolution of a Gaussian and a Lorentzian---accurately describes the absorption lines of atomic and molecular gases at low probe powers. Fitting experimental absorption data to such a Voigt profile yields both the Lorentzian natural linewidth and the Gaussian Doppler broadening. However, as the probe power increases, saturation effects change the absorption line shape, such that it is no longer accurately described by a Voigt profile. Naively fitting a simple Voigt profile to the absorption line therefore introduces spurious power dependence into the extracted Doppler component. Using a simple atomic model, we calculate power-dependent corrections to the Voigt profile, which are parametrized by the Gaussian Doppler width, the Lorentzian natural linewidth, and the optical depth. We show numerically and experimentally that including the correction term substantially reduces the spurious power dependence in the fitted Gaussian width.

DOI
10.1103/physreva.86.012506

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The Voigt profile---a convolution of a Gaussian and a Lorentzian---accurately describes the absorption lines of atomic and molecular gases at low probe powers. Fitting experimental absorption data to such a Voigt profile yields both the Lorentzian natural linewidth and the Gaussian Doppler broadening. However, as the probe power increases, saturation effects change the absorption line shape, such that it is no longer accurately described by a Voigt profile. Naively fitting a simple Voigt profile to the absorption line therefore introduces spurious power dependence into the extracted Doppler component. Using a simple atomic model, we calculate power-dependent corrections to the Voigt profile, which are parametrized by the Gaussian Doppler width, the Lorentzian natural linewidth, and the optical depth. We show numerically and experimentally that including the correction term substantially reduces the spurious power dependence in the fitted Gaussian width.
The line shapes of saturation spectroscopy in optically thick two-level media are calculated for atomic and molecular transitions. Line narrowing and distortion effects due to propagation are presented. For Doppler-broadened media it is shown that, due to multiphoton processes, the natural linewidth limits the ultimate narrowing that can be reached. Thus, up to ${\ensuremath{\alpha}}_{0}L=20,$ only when the rate-equation approximation is valid subhomogeneous linewidths are expected.
For pt.I see ibid., vol.8, p.1795 (1975) where the theory of Doppler-free two-photon transitions was discussed for the case of one single laser frequency. Here, the effects of two different frequencies are considered. When the residual Doppler width of the two-photon transition is less than the natural linewidth, the previous results are essentially regained. For large residual Doppler shifts, the absorption profile is a power-broadened Lorentzian if the frequency of the probe field is larger than the frequency of the strong field. In the opposite case, the absorption peak splits because of the AC Stark effect. The high-intensity distortions are minimized when equal frequencies can be used. Power-dependent shifts do not ordinarily occur with a resonantly tuned intermediate level. Some modifications of the spectra are introduced by phase-disturbing collisions.
There is extensive use of monochromatic lasers to select atoms with a narrow range of velocities in many atomic physics experiments. For the commonplace situation of the inhomogeneous Doppler-broadened (Gaussian) linewidth exceeding the homogeneous (Lorentzian) natural linewidth by typically two orders of magnitude, a substantial narrowing of the velocity class of atoms interacting with the light can be achieved. However, this is not always the case, and here we show that for a certain parameter regime there is essentially no selection – all of the atoms interact with the light in accordance with the velocity probability density. An explanation of this effect is provided, emphasizing the importance of the long tail of the constituent Lorentzian distribution in a Voigt profile.
We present a theoretical and experimental study of the line shape of resonant four-wave mixing induced by broad-bandwidth laser radiation that revises the theory of Meacher, Smith, Ewart, and Cooper (MSEC) [Phys. Rev. A 46, 2718 (1992)]. We adopt the same method as MSEC but correct for an invalid integral used to average over the distribution of atomic velocities. The revised theory predicts a Voigt line shape composed of a homogeneous, Lorentzian component, defined by the collisional rate \ensuremath{\Gamma}, and an inhomogeneous, Doppler component, which is a squared Gaussian. The width of the inhomogeneous component is reduced by a factor of \ensuremath{\surd}2 compared to the simple Doppler width predicted by MSEC. In the limit of dominant Doppler broadening, the width of the homogeneous component is predicted to be 4\ensuremath{\Gamma}, whereas in the limit of dominant homogeneous broadening, the predicted width is 2\ensuremath{\Gamma}. An experimental measurement is reported of the line shape of the four-wave-mixing signal using a broad-bandwidth, ``modeless,'' laser resonant with the Q1{\mathit{Q}}_{1}Q1​(6) line of the A2{\mathrm{}}^{2}2\ensuremath{\Sigma}-X2{\mathrm{}}^{2}2\ensuremath{\Pi}(0,0) system of the hydroxyl radical. The measured widths of the Voigt components were found to be consistent with the predictions of the revised theory. \textcopyright{} 1996 The American Physical Society.
This paper presents a theory of lineshapes for molecular Optical-Optical Double Resonance (DR) Spectroscopy with arbitrary strength for both pump and probe fields using the steady-state solutions for the 3-level density matrix. When Doppler broadening can be neglected, the results are analytical, and the probe spectrum is a pair of Lorentzian lines that display Autler-Townes splitting, each with an angular frequency half-width half maximum equal to the relaxation rates, which are assumed to be equal. When Doppler broadening is introduced, one must resort to numerical integration except for the limit of weak pump and probe fields. When the Doppler width is assumed to be much larger than the pump and probe Rabi frequencies and the probe frequency is higher than that of the pump, the calculated DR lineshapes are found to be Lorentzian with a strong pump field limit width that is proportional to the pump Rabi frequency, which is commonly known as power broadening. However, the width does not equal that Rabi frequency and is different for co- and counter-propagating pump and probe fields. Furthermore, that broadening is largely inhomogeneous, despite the Lorentzian shape. The saturation power is found to be about 4 times higher than for the bare probe transition with the same relaxation rate, dramatically lower than that expected if the width is interpreted as homogeneous.
Power broadening-the broadening of the spectral line profile of a two-state quantum transition as the amplitude of the driving field increases-is a well-known and thoroughly examined phenomenon in spectroscopy. It typically occurs in continuous-wave driving when the intensity of the radiation field increases beyond the saturation intensity of the transition. In pulsed-field excitation, linear power broadening occurs for a pulse of rectangular temporal shape. Pulses with smooth shapes are known to exhibit much less power broadening, e.g., logarithmic for a Gaussian pulse shape. It has been predicted, but never experimentally verified, that pulse shapes which vanish in time as ∼|t|^{-λ} should exhibit the opposite effect-power narrowing-in which the postpulse transition line width decreases as the amplitude of the driving pulse increases. In this Letter, power narrowing is demonstrated for a class of powers-of-Lorentzian pulse shapes on the IBM Quantum processor ibmq_manila. Reduction of the line width by a factor of over 10 is observed when increasing the pulse area from π to 7π, in a complete reversal of the power broadening paradigm. Moreover, thorough study is conducted on the truncation of the pulse wings which introduces a (small) power-broadened term which prevents power narrowing from reaching extreme values. In the absence of other power broadening mechanisms, Lorentzian pulses truncated at sufficiently small values can achieve as narrow line profiles as desired.