The use of coherent phase control of multiphoton ionization to measure the refractive indices of H2 and Ar between 1100 and 1150 Å

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Abstract
We have used the method of coherent phase modulation, first proposed by Brumer and Shapiro for controlling the rates of chemical reactions, to measure the refractive index of a gas in the vacuum ultraviolet. In these experiments we populated a Rydberg state of HCl or CO by simultaneous absorption of one VUV photon and three UV photons. Molecular ions were generated by absorption of an additional UV photon and detected with a time‐of‐flight mass spectrometer. The phase difference for the UV and VUV beams was altered by passing them through a cell containing either H2 or Ar. By varying the pressure in the cell we could control this phase difference and thereby modulate the ion signal. From the modulation frequency of the signal it was possible to determine the difference between the refractive indices of the gas at the UV and VUV wavelengths. Using reliable refractive indices in the UV, we extracted from our data values for the VUV indices. These values are in quantitative agreement with a calculation that uses dipole oscillator strengths constructed using constrained oscillator strength methods, taking into account the dispersion resulting from individual rotational transitions. The experimental method can be used very close to an optical transition of the refractive medium, provided that the refractive index does not vary appreciably across the bandwidth of the VUV laser.