R. Ciuryło

Pound-Drever-Hall-locked, frequency-stabilized cavity ring-down spectrometer

We describe a high sensitivity and high spectral resolution laser absorption spectrometer based upon the frequency-stabilized cavity ring-down spectroscopy (FS-CRDS) technique. We used the Pound-Drever-Hall (PDH) method to lock the probe laser to the high-finesse ring-down cavity. We show that the concomitant narrowing of the probe laser line width leads to dramatically increased ring-down event acquisition rates (up to 14.3 kHz), improved spectrum signal-to-noise ratios for weak O(2) absorption spectra at λ = 687 nm and substantial increase in spectrum acquisition rates compared to implementations of FS-CRDS that do not incorporate high-bandwidth locking techniques. The minimum detectable absorption coefficient and the noise-equivalent absorption coefficient for the spectrometer are about 2×10(-10) cm(-1) and 7.5×10(-11) cm(-1)Hz(-1/2), respectively.

Cavity ring-down spectroscopy of the oxygen B-band with absolute frequency reference to the optical frequency comb

Absolute positions of several oxygen B-band lines were measured with the Pound-Drever-Hall-locked frequency-stabilized cavity ring-down spectrometer. The frequency axis of spectra was linked to the optical frequency comb. Achieved uncertainties of line positions are between 0.9 and 2.9 MHz. Self-pressure shifts coefficients are also reported.

Observations of Dicke narrowing and speed dependence in air-broadened CO2 lineshapes near 2.06 μm

Frequency-stabilized cavity ring-down spectroscopy was used to study CO2 lineshapes in the (20013) ← (00001) band centered near 2.06 μm. Two rovibrational transitions were chosen for this study to measure non-Voigt collisional effects for air-broadened lines over the pressure range of 7 kPa-28 kPa. Lineshape analysis for both lines revealed evidence of simultaneous Dicke (collisional) narrowing and speed-dependent effects that would introduce biases exceeding 2% in the retrieved air-broadening parameters if not incorporated in the modeling of CO2 lineshapes. Additionally, correlations between velocity- and phase/state changing collisions greatly reduced the observed Dicke narrowing effect. As a result, it was concluded that the most appropriate line profile for modeling CO2 lineshapes near 2.06 μm was the correlated speed-dependent Nelkin-Ghatak profile, which includes all of the physical effects mentioned above and leads to a consistent set of line shape parameters that are linear with gas pressure.

Active control of the Pound-Drever-Hall error signal offset in high-repetition-rate cavity ring-down spectroscopy

A new approach to realizing the Pound–Drever–Hall (PDH) error signal offset correction is presented. The proposed setup and correction procedure allow one to control not only the effect of amplitude modulation of the error signal, but also other sources of offsets that are present in the PDH feedback loop. This technique significantly improves laser frequency locking in high-repetition-rate cavity ring-down spectroscopy (CRDS) by allowing one to recover a tight PDH lock within 1 ms after switching off the probe laser beam. We apply the PDH error signal offset correction to CRDS measurements of the weak 16O2 B-band R7 Q8 line. The resulting spectra taken at a pressure of 1.2 kPa had a signal-to-noise ratio of ~8000:1.

Strontium optical lattice clocks for practical realization of the metre and secondary representation of the second

We present a system of two independent strontium optical lattice standards probed with a single shared ultranarrow laser. The absolute frequency of the clocks can be verified by the use of Er:fiber optical frequency comb with the GPS-disciplined Rb frequency standard. We report hertz-level spectroscopy of the clock line and measurements of frequency stability of the two strontium optical lattice clocks.

Cavity mode-width spectroscopy with widely tunable ultra narrow laser

We explore a cavity-enhanced spectroscopic technique based on determination of the absorbtion coefficient from direct measurement of spectral width of the mode of the optical cavity filled with absorbing medium. This technique called here the cavity mode-width spectroscopy (CMWS) is complementary to the cavity ring-down spectroscopy (CRDS). While both these techniques use information on interaction time of the light with the cavity to determine absorption coefficient, the CMWS does not require to measure very fast signals at high absorption conditions. Instead the CMWS method require a very narrow line width laser with precise frequency control. As an example a spectral line shape of P7 Q6 O₂ line from the B-band was measured with use of an ultra narrow laser system based on two phase-locked external cavity diode lasers (ECDL) having tunability of ± 20 GHz at wavelength range of 687 to 693 nm.

One-dimensional frequency-based spectroscopy

Recent developments in optical metrology have tremendously improved the precision and accuracy of the horizontal (frequency) axis in measured spectra. However, the vertical (typically absorbance) axis is usually based on intensity measurements that are subject to instrumental errors which limit the spectrum accuracy. Here we report a one-dimensional spectroscopy that uses only the measured frequencies of high-finesse cavity modes to provide complete information about the dispersive properties of the spectrum. Because this technique depends solely on the measurement of frequencies or their differences, it is insensitive to systematic errors in the detection of light intensity and has the potential to become the most accurate of all absorptive and dispersive spectroscopic methods. The experimental results are compared to measurements by two other high-precision cavity-enhanced spectroscopy methods. We expect that the proposed technique will have significant impact in fields such as fundamental physics, gas metrology and environmental remote sensing.

Low-pressure line-shape study in molecular oxygen with absolute frequency reference

We present a line-shape analysis of the rovibronic R1 Q2 transition of the oxygen B band resolved by the Pound-Drever-Hall-locked frequency-stabilized cavity ring-down spectroscopy technique in the low pressure range. The frequency axis of the spectra is linked by the ultra-narrow diode laser to the optical frequency comb in order to measure the absolute frequency at each point of the recorded spectra. Experimental spectra are fitted with various line-shape models: the Voigt profile, the Galatry profile, the Nelkin-Ghatak profile, the speed-dependent Voigt profile, and the speed-dependent Nelkin-Ghatak profile with quadratic and hypergeometric approximations for the speed dependence of collisional broadening and shifting. The influences of Dicke narrowing, speed-dependent effects, and correlation between phase- and velocity-changing collisions on the line shape are investigated. Values of line-shape parameters, including the absolute frequency of the transition 435685.24828(46) GHz, are reported.

Non-adiabatic approach to the asymmetry of pressure broadened spectral lines

Abstract A semi-classical formula for the asymmetry of the profile of pressure broadened spectral lines, which takes into account non-adiabatic processes is derived. The resultant spectrum is shown to be given as a linear combination of the Lorentzian and dispersion profiles. The line profile asymmetry can be evaluated in cases when the degeneracy of both the initial and final states is important.

Absolute molecular transition frequencies measured by three cavity-enhanced spectroscopy techniques

Absolute frequencies of unperturbed (12)C(16)O transitions from the near-infrared (3-0) band were measured with uncertainties five-fold lower than previously available data. The frequency axis of spectra was linked to the primary frequency standard. Three different cavity enhanced absorption and dispersion spectroscopic methods and various approaches to data analysis were used to estimate potential systematic instrumental errors. Except for a well established frequency-stabilized cavity ring-down spectroscopy, we applied the cavity mode-width spectroscopy and the one-dimensional cavity mode-dispersion spectroscopy for measurement of absorption and dispersion spectra, respectively. We demonstrated the highest quality of the dispersion line shape measured in optical spectroscopy so far. We obtained line positions of the Doppler-broadened R24 and R28 transitions with relative uncertainties at the level of 10(-10). The pressure shifting coefficients were measured and the influence of the line asymmetry on unperturbed line positions was analyzed. Our dispersion spectra are the first demonstration of molecular spectroscopy with both axes of the spectra directly linked to the primary frequency standard, which is particularly desirable for the future reference-grade measurements of molecular spectra.