Abstract

In this Letter, we report on the sub-parts-per-billion-level radiocarbon dioxide detection using cantilever-enhanced photoacoustic spectroscopy. The $^{14}{\rm C/C}$ ratio of samples is measured by targeting a $^{14}{{\rm CO}_2}$ absorption line with minimal interference from other ${{\rm CO}_2}$ isotopes. Using a quantum cascade laser as a light source allows for a compact experimental setup. In addition, measurements of sample gases with $^{14}{{\rm CO}_2}$ concentrations as low as 100 parts-per-trillion (ppt) are presented. The Allan deviation demonstrates a noise equivalent concentration of 30 ppt at an averaging time of 9 min. The achieved sensitivity validates this method as a suitable alternative to more complex optical detection methods for radiocarbon dioxide detection used so far, and it can be envisioned for future in situ radiocarbon detection.

© 2021 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

Radiocarbon is a naturally occurring radioactive isotope of carbon with a natural abundance of 1.2 parts per trillion (ppt). It is mainly produced by the transmutation reaction of thermal neutrons with atmospheric nitrogen. Radiocarbon has a half-life of 5700 years [1] and is the ideal marker of the origin of carbon, as it has totally decayed in carbon of fossil origin, while biogenic carbon contains the natural abundance of radiocarbon. It has thus been widely applied in the fields of archaeology, oceanography, paleoenvironmental studies, and climate sciences [2,3]. It can in particular play an important role in tackling global warming, as it provides a means to determine the biofraction content of various products and to apportion sources of greenhouse gas emissions. Radiocarbon is also used as a tracer in biomedical studies to detect drug pathways in human body [4].

In nuclear facilities, radiocarbon is produced in higher concentrations than its natural abundance [5]. It is one of the main sources of radioactive gaseous emissions, mostly in the form of carbon dioxide or methane [6]. Long-lived radionuclides such as $^{14}{\rm C}$ are problematic because they have a high rate of environmental mobility and can be easily assimilated into living matter. This calls out for the development of new methods for on-line in situ radiocarbon detection.

The state-of-the-art technique for radiocarbon detection is accelerator mass spectrometry, which has a very high sensitivity and is preferentially used for concentrations at or below the natural abundance. Liquid scintillation counting is mostly used in the nuclear industry for measurements of higher concentrations of radiocarbon dioxide [7]. Both methods usually require complex sample preparation, particularly for analysis of gaseous samples, and they are designed for off-site laboratory analysis. These measurement techniques are thus not suitable for in situ $^{14}{{\rm CO}_2}$ measurements. Laser spectroscopy has been established as a versatile method for field-deployable trace gas detection. Owing to the low natural abundance of $^{14}{{\rm CO}_2}$, previous research on optical $^{14}{{\rm CO}_2}$ detection has mostly focused on advanced spectroscopy techniques, such as cavity ring-down spectroscopy (CRDS) [6,813]. The CRDS is highly sensitive and is widely used for numerous applications in trace gas detection. High sensitivity below the ppt level has for instance been achieved for radiocarbon detection using this method [912]; however, this was accomplished using laboratory-based setups, built around bulky optical cavities. To enable in situ radiocarbon detection, it is crucial to build compact, portable, and robust instruments. Cantilever-enhanced photoacoustic spectroscopy (CEPAS) has been recognized in this regard [1416]. In this work, we therefore present, to the best of our knowledge, the first investigation into applying CEPAS for $^{14}{{\rm CO}_2}$ detection, which can enable future in situ radiocarbon detection.

When the light of suitable wavelength is irradiated on a sample in the photoacoustic (PA) cell, the absorption of the radiation heats up the gas increasing both temperature and pressure. By modulating the laser wavelength, pressure waves are created throughout the sample, forming acoustic waves [17]. In CEPAS, these acoustic waves bend the cantilever in the cell, and the displacement of its free end is measured via a compact laser interferometer. The PA signal measured by the cantilever, expressed by $S$, is given by

$$S = {S_m}P{C_{{\rm cell}}}{N_{{\rm tot}}}{c_m}\sigma ,$$
where ${S_m}$ is the cantilever sensitivity in mV/Pa, $P$ is the optical power of the incident light in W, ${C_{{\rm cell}}}$ is the PA cell response constant in ${{\rm Pa/cm}^{- 1}}\;{\rm W}$, ${N_{{\rm tot}}}$ is the number density of molecules in ${{\rm molecule/cm}^3}$, ${c_m}$ is the concentration given as volume mixing ratio, and $\sigma$ is the absorption cross section in ${{\rm cm}^2}/{\rm molecule}$ [18].

Like other spectroscopy techniques, CEPAS is very selective as lasers with narrow linewidth allow high-resolution probing of spectral lines. For CEPAS, no optical cavity is needed, resulting in a comparatively less complex and robust system with a simpler alignment. The PA sample cell volume is small (only a few milliliters) allowing to build a compact system. Another advantage of CEPAS is that the signal strength scales with the incident light power [Eq. (1)]. Furthermore, the detection scheme of CEPAS is independent of the wavelength making it ideal for the detection of a variety of molecules, and it will be used here to address the fundamental vibrational band of $^{14}{{\rm CO}_2}$ at 4.5 µm.

The $^{14}{\rm C}$ content of the sample can be accurately determined by targeting an absorption line of $^{14}{{\rm CO}_2}$ with minimal interference from other ${{\rm CO}_2}$ isotopologues. We have chosen the P(20) line at $2209.1\;{{\rm cm}^{- 1}}$ for $^{14}{{\rm CO}_2}$ detection [1921], similarly to previous studies using CRDS. Its line intensity is $2.8 \times {10^{- 18}}\;{{\rm cm}^{- 1}}/{\rm mol}\;{{\rm cm}^{- 2}}$ in case of a pure $^{14}{{\rm CO}_2}$ sample. Although absorption lines of other ${{\rm CO}_2}$ isotopologues are typically weak in this wavelength region, the target radiocarbon dioxide concentration is also low, and interfering lines pose a challenge. Previous studies on PAS have mostly focused on isolated absorption lines. Here, we are targeting an absorption line surrounded by more potentially interfering lines, and measurements are carried out at low pressure to improve spectral selectivity. For these reasons, achieving high sensitivity with CEPAS is demanding.

 figure: Fig. 1.

Fig. 1. Simulated absorption spectra for 1 ppb of $^{14}{{\rm CO}_2}$ at a pressure of 20 mbar and 70 mbar are shown in orange and blue, respectively, in (a). $\alpha$ denotes the normalized absorption coefficient. A simulation of ${2}f$ wavelength-modulated spectrum at 70 mbar and a modulation amplitude of $0.01\;{{\rm cm}^{- 1}}$ are presented in (b).

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We use wavelength modulation spectroscopy (WMS): the laser wavelength is modulated, and the nominal wavelength of the laser is scanned across the absorption spectra simultaneously. The modulation shifts the absorption spectra to higher discrete harmonics less affected by acoustic noise (often referred to as ${1/}f$ noise). Spectra are recorded at the second harmonic (${2}f$) of the modulation frequency $f$. The ${2}f$ wavelength-modulated spectra were simulated using a model based on Voigt profiles developed by Westberg et al. [22,23]. Figure 1 presents a comparison of simulated spectra for direct absorption (DA) and ${2}f$ Voigt profile. In the DA spectrum, the $^{14}{{\rm CO}_2}$ line cannot be resolved at a pressure ${\gt}{20}\;{\rm mbar}$, while it is resolved even at 70 mbar with scanning-wavelength modulation. Moreover, a significant background from Lorentzian wings of strong lines can be observed in the DA spectrum, which diminishes with wavelength modulation.

The experimental setup is very compact with approximate dimensions of ${45} \times {35} \times {15}\;{\rm cm}$, including the laser. The main components shown in Fig. 2 are a 4.5 µm continuous-wave quantum cascade laser (QCL) from Hamamatsu (LE0907), a photoacoustic cell from Gasera Ltd. (PA201), a lock-in amplifier from SRS Instruments (SR-830), and a data acquisition card. A 30 Hz sinusoidal modulation on top of a 15 mHz triangular ramp was applied to the QCL current to simultaneously modulate the laser wavelength and scan it over the spectral region of interest. The incident laser power reaching the cell was 40 mW. Two mirrors were used to align the beam into the PA cell cavity. A third mirror was placed at the end of the cavity to send the beam back into the cell, with an aim double the optical power and increase the photoacoustic signal. The signal from the cantilever was demodulated at the second harmonic of the 30 Hz modulation using a lock-in amplifier with a time constant of 300 ms. The lock-in amplifier output was recorded by a 14-bit data acquisition card (DAQ). A leakage from one mirror was sent into an infrared photovoltaic detector through a 50.8-mm-long germanium etalon to calibrate the non-linear relationship between driving current and laser wavelength. The cell pressure was regulated by adjusting the computer-controlled input and output valves of the PA cell, and measurements were carried out in static conditions. The analog lock-in output was sampled with a 2 kHz rate (i.e., the Nyquist rate of the DAQ input filter of 1 kHz). The signal was then digitally down-sampled by a factor of 2000 to a sampling rate of 1 Hz corresponding to two times the lock-in bandwidth.

 figure: Fig. 2.

Fig. 2. Experimental setup comprises a quantum cascade laser, a photoacoustic cell, a lock-in amplifier, and a data acquisition card. The photoacoustic signal is recorded at the second harmonic of the modulation frequency.

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The system was characterized using a standardized dry gas sample with elevated levels of $^{14}{{\rm CO}_2}$, which was produced at the National Physical Laboratory (NPL) with a known $^{14}{\rm C/C}$ fraction of $1.01 \pm 0.085\;{\rm ppb}$ [6]. Figure 3 shows experimental spectra with the P(20) line of $^{14}{{\rm CO}_2}$ and the neighboring $^{13}{{\rm CO}_2}$ absorption lines at different pressures and modulation amplitudes. The photoacoustic signal in general increases with pressure [Eq. (1)]. However, at higher pressure, the absorption line width is dominated by pressure broadening and the different lines overlap with each other. Low pressure is thus required to resolve the lines, at the cost of decreased signal strength and worsened signal-to-noise (SNR) ratio. Similarly, the modulation amplitude must be carefully optimized. These effects were studied experimentally as shown in Fig. 3. The optimum combination of modulation amplitude and pressure was empirically found to be $0.009\;{{\rm cm}^{- 1}}$ and 60 mbar, respectively.

 figure: Fig. 3.

Fig. 3. Experimental spectra for different pressures with a constant modulation amplitude of $0.009\;{{\rm cm}^{- 1}}$ are presented in (a). The spectra for different modulation amplitudes at a constant pressure of 60 mbar are shown in (b). The solid lines act as a guide to the eye. All the spectra are averaged over 30 scans for an acquisition time of 33 min.

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To investigate the linearity of the system, samples with different concentrations of $^{14}{{\rm CO}_2}$ were prepared by mixing the NPL sample with inactive ${{\rm CO}_2}$. Experimental spectra were recorded at optimum pressure and modulation amplitude. The spectra averaged over 30 scans together with corresponding fits are depicted in Fig. 4(a). These spectra were fitted by a sum of wavelength-modulated Voigt profiles using a non-linear least-square-fitting routine [22,23]. A total of five absorption lines of the ${{\rm CO}_2}$ isotopologues identified from the HITRAN database [2426], listed in the Supplement 1, were added to the fitting routine. The line broadenings and line positions were determined empirically under different conditions based on the HITRAN data. The line intensities, the center laser frequency, constant linear background, and the pressure were fitted. The ${{\rm N}_2}{\rm O}$ absorption lines were situated in the same wavelength range, but their intensity was negligible for short measurement times, when only a small amount of outside air leaked into the cell. A quadratic function was used to calibrate the frequency axis. The fit residuals, shown in (b), are dominated by white noise from the PA cell that is limiting the achievable sensitivity. The white noise behavior was experimentally verified by comparing individual consecutive scans, as seen in Fig. S2 of the Supplement 1 and by the Allan plot presented below in Fig. 5:

$${\rm NNEA} = {\alpha _{{\rm min}}}P\sqrt t ,$$
where ${\alpha _{{\rm min}}} = \alpha /{\rm SNR}$ is the noise equivalent absorption coefficient, and the SNR is the ratio of the signal peak-to-peak amplitude and the standard deviation of the fit residual in Fig. 4(b). The normalized absorption coefficient $\alpha$ is calculated using the line parameters from the HITRAN database, the sample pressure, temperature, and the wavenumber range. $P$ is the incident laser power, and $t$ the acquisition time [18]. The normalized noise-equivalent absorption for the system is $8 \times {10^{- 9}}\;{\rm W}\;{{\rm cm}^{- 1}}\;{{\rm Hz}^{- 1/2}}$, which is similar to the previously reported values [27], albeit at a lower pressure and with more interfering absorption lines. The $^{14}{\rm C/C}$ ratios as a function of the sample-mixing ratios are presented in Fig. 4(c). The isotopic ratio is obtained by calculating the ratio of the $^{14}{{\rm CO}_2}$ and $^{13}{{\rm CO}_2}$ absorption line areas, normalized using the 1 ppb sample at a mixing ratio of 1. It demonstrates that the system has a good linearity. The maximum concentration of $^{14}{{\rm CO}_2}$ that can be detected with this system is estimated to be 100 ppm. This was calculated assuming a 20% maximum absorption, above which nonlinear effects start to affect the line shape.
 figure: Fig. 4.

Fig. 4. Experimental spectra for 1000, 500, 100, and 0 ppt of a $^{14}{{\rm CO}_2}$ sample are presented in blue, orange, yellow, and purple, respectively, in (a). The corresponding fit through these points are depicted by a solid line. The fit residuals are shown in (b). The $^{14}{\rm C/C}$ ratio determined by computing the ratio of absorption line areas from the experimental data as a function of mixing ratio are plotted in (c), with the black line depicting the expected linear behavior.

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 figure: Fig. 5.

Fig. 5. Allan deviation plot for 1 ppb and 500 ppt of $^{14}{{\rm CO}_2}$. The sample gas pressure at the start of the measurement is 40 mbar. The noise equivalent concentration (NEC) for 1 ppb of $^{14}{{\rm CO}_2}$ is 30 ppt at an averaging time of 9 min. The expected $1/\sqrt t$ behavior for a white-noise-dominated system is depicted by the grey dashed line.

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To determine the stability and sensitivity of the system, 2-h-long measurements for 1 ppb and 500 ppt of $^{14}{{\rm CO}_2}$ were recorded at an initial pressure of 40 mbar. A full spectrum was recorded every 66 s, and the $^{14}{\rm C/C}$ ratio was calculated after fitting the absorption lines. These isotopic ratios were then used to compute the Allan deviations shown in Fig. 5. The photoacoustic cell used in these experiments is not optimized for low pressure, and outside air leaks inside the cell during the measurement. The pressure after 2 h was approximately 100 mbar. However, pressure changes affect all lines in a similar fashion and measurement of the isotopic ratio will partly overcome this issue. The noise equivalent concentration (NEC) is found to be 140 ppt at the averaging time of 66 s and 30 ppt at 9 min for 1 ppb of $^{14}{{\rm CO}_2}$. Comparison of the measured Allan deviation and the ideal white noise behavior (dashed line) shows that the system is white noise limited up to 528 s. However, the pressure leak of the system hinders longer measurement times, as the lines cannot be resolved at higher pressure. Hence, overcoming this limiting factor can lead to increased sensitivity in the future.

It is confirmed that the sub-parts-per-billion level radiocarbon dioxide can be detected using cantilever-enhanced photoacoustic spectroscopy. This detection level is already sufficient for monitoring of $^{14}{{\rm CO}_2}$ in nuclear facilities [28]. It is comparable to our previous work using CRDS [6,13], albeit with a simpler instrumentation. A number of improvements can in the future increase the sensitivity of the method. For instance, almost all the weak lines around $2209\;{{\rm cm}^{- 1}}$ are hot transitions whose strength decreases at lower temperature [20]. Thus, by cooling down the sample, the intensity of the interfering ${{\rm CO}_2}$ lines substantially decreases (in particular the $^{13}{{\rm CO}_2}$ line at $2209.116\;{{\rm cm}^{- 1}}$), and the P(20) line can be detected more easily. The PA signal can also be enhanced by increasing the optical power, either by using a more powerful laser source or by building a compact optical cavity around the PA cell. Cavity-enhanced CEPAS, the combination of CEPAS with passive optical enhancement cavity, has the potential to increase the sensitivity by at least two orders of magnitude [29]. CEPAS can therefore in the future become an alternative to other radiocarbon detection techniques and contribute to applications where sub-ppt level radiocarbon detection is required, e.g.,  biofraction measurements, source apportionment, or biomedical labeling [30,31]. It has the potential to offer an even more compact, robust, and affordable method than other currently explored optical techniques for radiocarbon detection.

Funding

Academy of Finland (314363, 320168).

Acknowledgment

The authors thank Ville Ulvila for his contribution for the initial idea to this work.

Disclosures

The authors declare no conflicts of interest.

Data Availability

Data underlying the results presented in this paper are not publicly available at this time but may be obtained from the authors upon reasonable request.

Supplemental document

See Supplement 1 for supporting content.

REFERENCES

1. W. Kutschera, Int. J. Mass Spectrom. 349, 203 (2013). [CrossRef]  

2. H. D. Graven, Proc. Natl. Acad. Sci. USA 112, 9542 (2015). [CrossRef]  

3. J. Mohn, S. Szidat, K. Zeyer, and L. Emmenegger, Waste Manage. 32, 1516 (2012). [CrossRef]  

4. G. Lappin and L. Stevens, Expert. Opin. Drug Metab. Toxicol. 4, 1021 (2008). [CrossRef]  

5. M.-S. Yim and F. Caron, Prog. Nucl. Energy 48, 2 (2006). [CrossRef]  

6. G. Genoud, M. Vainio, H. Phillips, J. Dean, and M. Merimaa, Opt. Lett. 40, 1342 (2015). [CrossRef]  

7. J. M. Passmann, N. S. Radin, and J. A. D. Cooper, Anal. Chem. 28, 484 (1956). [CrossRef]  

8. D. Romanini, A. Kachanov, N. Sadeghi, and F. Stoeckel, Chem. Phys. Lett. 264, 316 (1997). [CrossRef]  

9. I. Galli, S. Bartalini, S. Borri, P. Cancio, D. Mazzotti, P. De Natale, and G. Giusfredi, Phys. Rev. Lett. 107, 270802 (2011). [CrossRef]  

10. A. McCartt, T. Ognibene, G. Bench, and K. Turteltaub, Nucl. Instrum. Methods Phys. Res., Sect. B 361, 277 (2015). [CrossRef]  

11. I. Galli, S. Bartalini, R. Ballerini, M. Barucci, P. Cancio, M. D. Pas, G. Giusfredi, D. Mazzotti, N. Akikusa, and P. D. Natale, Optica 3, 385 (2016). [CrossRef]  

12. A. Fleisher, D. Long, Q. Liu, L. Gameson, and J. Hodges, J. Phys. Chem. Lett. 8, 4550 (2017). [CrossRef]  

13. G. Genoud, J. Lehmuskoski, S. Bell, V. Palonen, M. Oinonen, M.-L. Koskinen-Soivi, and M. Reinikainen, Anal. Chem. 91, 12315 (2019). [CrossRef]  

14. J. Li, W. Chen, and B. Yu, Appl. Spectrosc. Rev. 46, 440 (2011). [CrossRef]  

15. V. Koskinen, J. Fonsen, J. Kauppinen, and I. Kauppinen, Vib. Spectrosc. 42, 239 (2006). [CrossRef]  

16. V. Koskinen, J. Fonsen, K. Roth, and J. Kauppinen, Vib. Spectrosc. 48, 16 (2008). [CrossRef]  

17. C. Haisch, Meas. Sci. Technol. 23, 012001 (2011). [CrossRef]  

18. T. Tomberg, M. Vainio, T. Hieta, and L. Halonen, Sci. Rep. 8, 1848 (2018). [CrossRef]  

19. I. Galli, P. C. Pastor, G. D. Lonardo, L. Fusina, G. Giusfredi, D. Mazzotti, F. Tamassia, and P. D. Natale, Mol. Phys. 109, 2267 (2011). [CrossRef]  

20. D. Labrie and J. Reid, Appl. Phys. 24, 381 (1981). [CrossRef]  

21. M. Wahlen, R. S. Eng, and K. W. Nill, Appl. Opt. 16, 2350 (1977). [CrossRef]  

22. J. Westberg, J. Wang, and O. Axner, J. Quant. Spectrosc. Radiat. Transfer 113, 2049 (2012). [CrossRef]  

23. P. Kluczynski, J. Gustafsson, Å. M. Lindberg, and O. Axner, Spectrochim. Acta B Atom. Spectros. 56, 1277 (2001). [CrossRef]  

24. E. Zak, J. Tennyson, O. L. Polyansky, L. Lodi, N. F. Zobov, S. A. Tashkun, and V. I. Perevalov, J. Quant. Spectrosc. Radiat. Transfer 189, 267 (2017). [CrossRef]  

25. E. J. Zak, J. Tennyson, O. L. Polyansky, L. Lodi, N. F. Zobov, S. A. Tashkun, and V. I. Perevalov, J. Quant. Spectrosc. Radiat. Transfer 203, 265 (2017). [CrossRef]  

26. I. Gordon, L. S. Rothman, C. Hill, R. V. Kochanov, Y. Tan, P. Bernath, M. Birk, V. Boudon, A. Campargue, K. Chance, B. J. Drouin, J. Flaud, R. R. Gamache, J. Hodges, D. Jacquemart, V. I. Perevalov, A. Perrin, K. P. Shine, M. Smith, J. Tennyson, G. Toon, H. Tran, V. G. Tyuterev, A. Barbe, A. G. Császár, V. M. Devi, T. Furtenbacher, J. Harrison, J. Hartmann, A. Jolly, T. J. Johnson, T. Karman, I. Kleiner, A. A. Kyuberis, J. Loos, O. M. Lyulin, S. Massie, S. Mikhailenko, N. Moazzen-Ahmadi, H. S. P. Muller, O. V. Naumenko, A. V. Nikitin, O. L. Polyansky, M. Rey, M. Rotger, S. Sharpe, K. Sung, E. Starikova, S. Tashkun, J. Auwera, G. Wagner, J. Wilzewski, P. Wcisło, S. Yu, and E. J. Zak, J. Quant. Spectrosc. Radiat. Transfer 203, 3 (2017). [CrossRef]  

27. R. Lindley, A. M. Parkes, K. A. Keen, E. McNaghten, and A. J. Orr-Ewing, Appl. Phys. B 86, 707 (2007). [CrossRef]  

28. K. Stenström, B. Erlandsson, R. Hellborg, A. Wiebert, S. Skog, R. Vesanen, M. Alpsten, and B. Bjurman, J. Radiol. Nucl. Chem. 198, 203 (1995). [CrossRef]  

29. T. Tomberg, T. Hieta, M. Vainio, and L. Halonen, Analyst 144, 2291 (2019). [CrossRef]  

30. M. Oinonen, H. Hakanpää-Laitinen, K. Hämäläinen, A. Kaskela, and H. Jungner, Nucl. Instrum. Methods Phys. Res., Sect. B 268, 1117 (2010). [CrossRef]  

31. V. Sonnenschein, R. Terabayashi, H. Tomita, S. Kato, N. Hayashi, S. Takeda, L. Jin, M. Yamanaka, N. Nishizawa, A. Sato, K. Yoshida, and T. Iguchi, J. Appl. Phys. 124, 033101 (2018). [CrossRef]  

References

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  1. W. Kutschera, Int. J. Mass Spectrom. 349, 203 (2013).
    [Crossref]
  2. H. D. Graven, Proc. Natl. Acad. Sci. USA 112, 9542 (2015).
    [Crossref]
  3. J. Mohn, S. Szidat, K. Zeyer, and L. Emmenegger, Waste Manage. 32, 1516 (2012).
    [Crossref]
  4. G. Lappin and L. Stevens, Expert. Opin. Drug Metab. Toxicol. 4, 1021 (2008).
    [Crossref]
  5. M.-S. Yim and F. Caron, Prog. Nucl. Energy 48, 2 (2006).
    [Crossref]
  6. G. Genoud, M. Vainio, H. Phillips, J. Dean, and M. Merimaa, Opt. Lett. 40, 1342 (2015).
    [Crossref]
  7. J. M. Passmann, N. S. Radin, and J. A. D. Cooper, Anal. Chem. 28, 484 (1956).
    [Crossref]
  8. D. Romanini, A. Kachanov, N. Sadeghi, and F. Stoeckel, Chem. Phys. Lett. 264, 316 (1997).
    [Crossref]
  9. I. Galli, S. Bartalini, S. Borri, P. Cancio, D. Mazzotti, P. De Natale, and G. Giusfredi, Phys. Rev. Lett. 107, 270802 (2011).
    [Crossref]
  10. A. McCartt, T. Ognibene, G. Bench, and K. Turteltaub, Nucl. Instrum. Methods Phys. Res., Sect. B 361, 277 (2015).
    [Crossref]
  11. I. Galli, S. Bartalini, R. Ballerini, M. Barucci, P. Cancio, M. D. Pas, G. Giusfredi, D. Mazzotti, N. Akikusa, and P. D. Natale, Optica 3, 385 (2016).
    [Crossref]
  12. A. Fleisher, D. Long, Q. Liu, L. Gameson, and J. Hodges, J. Phys. Chem. Lett. 8, 4550 (2017).
    [Crossref]
  13. G. Genoud, J. Lehmuskoski, S. Bell, V. Palonen, M. Oinonen, M.-L. Koskinen-Soivi, and M. Reinikainen, Anal. Chem. 91, 12315 (2019).
    [Crossref]
  14. J. Li, W. Chen, and B. Yu, Appl. Spectrosc. Rev. 46, 440 (2011).
    [Crossref]
  15. V. Koskinen, J. Fonsen, J. Kauppinen, and I. Kauppinen, Vib. Spectrosc. 42, 239 (2006).
    [Crossref]
  16. V. Koskinen, J. Fonsen, K. Roth, and J. Kauppinen, Vib. Spectrosc. 48, 16 (2008).
    [Crossref]
  17. C. Haisch, Meas. Sci. Technol. 23, 012001 (2011).
    [Crossref]
  18. T. Tomberg, M. Vainio, T. Hieta, and L. Halonen, Sci. Rep. 8, 1848 (2018).
    [Crossref]
  19. I. Galli, P. C. Pastor, G. D. Lonardo, L. Fusina, G. Giusfredi, D. Mazzotti, F. Tamassia, and P. D. Natale, Mol. Phys. 109, 2267 (2011).
    [Crossref]
  20. D. Labrie and J. Reid, Appl. Phys. 24, 381 (1981).
    [Crossref]
  21. M. Wahlen, R. S. Eng, and K. W. Nill, Appl. Opt. 16, 2350 (1977).
    [Crossref]
  22. J. Westberg, J. Wang, and O. Axner, J. Quant. Spectrosc. Radiat. Transfer 113, 2049 (2012).
    [Crossref]
  23. P. Kluczynski, J. Gustafsson, Å. M. Lindberg, and O. Axner, Spectrochim. Acta B Atom. Spectros. 56, 1277 (2001).
    [Crossref]
  24. E. Zak, J. Tennyson, O. L. Polyansky, L. Lodi, N. F. Zobov, S. A. Tashkun, and V. I. Perevalov, J. Quant. Spectrosc. Radiat. Transfer 189, 267 (2017).
    [Crossref]
  25. E. J. Zak, J. Tennyson, O. L. Polyansky, L. Lodi, N. F. Zobov, S. A. Tashkun, and V. I. Perevalov, J. Quant. Spectrosc. Radiat. Transfer 203, 265 (2017).
    [Crossref]
  26. I. Gordon, L. S. Rothman, C. Hill, R. V. Kochanov, Y. Tan, P. Bernath, M. Birk, V. Boudon, A. Campargue, K. Chance, B. J. Drouin, J. Flaud, R. R. Gamache, J. Hodges, D. Jacquemart, V. I. Perevalov, A. Perrin, K. P. Shine, M. Smith, J. Tennyson, G. Toon, H. Tran, V. G. Tyuterev, A. Barbe, A. G. Császár, V. M. Devi, T. Furtenbacher, J. Harrison, J. Hartmann, A. Jolly, T. J. Johnson, T. Karman, I. Kleiner, A. A. Kyuberis, J. Loos, O. M. Lyulin, S. Massie, S. Mikhailenko, N. Moazzen-Ahmadi, H. S. P. Muller, O. V. Naumenko, A. V. Nikitin, O. L. Polyansky, M. Rey, M. Rotger, S. Sharpe, K. Sung, E. Starikova, S. Tashkun, J. Auwera, G. Wagner, J. Wilzewski, P. Wcisło, S. Yu, and E. J. Zak, J. Quant. Spectrosc. Radiat. Transfer 203, 3 (2017).
    [Crossref]
  27. R. Lindley, A. M. Parkes, K. A. Keen, E. McNaghten, and A. J. Orr-Ewing, Appl. Phys. B 86, 707 (2007).
    [Crossref]
  28. K. Stenström, B. Erlandsson, R. Hellborg, A. Wiebert, S. Skog, R. Vesanen, M. Alpsten, and B. Bjurman, J. Radiol. Nucl. Chem. 198, 203 (1995).
    [Crossref]
  29. T. Tomberg, T. Hieta, M. Vainio, and L. Halonen, Analyst 144, 2291 (2019).
    [Crossref]
  30. M. Oinonen, H. Hakanpää-Laitinen, K. Hämäläinen, A. Kaskela, and H. Jungner, Nucl. Instrum. Methods Phys. Res., Sect. B 268, 1117 (2010).
    [Crossref]
  31. V. Sonnenschein, R. Terabayashi, H. Tomita, S. Kato, N. Hayashi, S. Takeda, L. Jin, M. Yamanaka, N. Nishizawa, A. Sato, K. Yoshida, and T. Iguchi, J. Appl. Phys. 124, 033101 (2018).
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2019 (2)

G. Genoud, J. Lehmuskoski, S. Bell, V. Palonen, M. Oinonen, M.-L. Koskinen-Soivi, and M. Reinikainen, Anal. Chem. 91, 12315 (2019).
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T. Tomberg, T. Hieta, M. Vainio, and L. Halonen, Analyst 144, 2291 (2019).
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2018 (2)

V. Sonnenschein, R. Terabayashi, H. Tomita, S. Kato, N. Hayashi, S. Takeda, L. Jin, M. Yamanaka, N. Nishizawa, A. Sato, K. Yoshida, and T. Iguchi, J. Appl. Phys. 124, 033101 (2018).
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T. Tomberg, M. Vainio, T. Hieta, and L. Halonen, Sci. Rep. 8, 1848 (2018).
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2017 (4)

E. Zak, J. Tennyson, O. L. Polyansky, L. Lodi, N. F. Zobov, S. A. Tashkun, and V. I. Perevalov, J. Quant. Spectrosc. Radiat. Transfer 189, 267 (2017).
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E. J. Zak, J. Tennyson, O. L. Polyansky, L. Lodi, N. F. Zobov, S. A. Tashkun, and V. I. Perevalov, J. Quant. Spectrosc. Radiat. Transfer 203, 265 (2017).
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A. Fleisher, D. Long, Q. Liu, L. Gameson, and J. Hodges, J. Phys. Chem. Lett. 8, 4550 (2017).
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2016 (1)

2015 (3)

A. McCartt, T. Ognibene, G. Bench, and K. Turteltaub, Nucl. Instrum. Methods Phys. Res., Sect. B 361, 277 (2015).
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H. D. Graven, Proc. Natl. Acad. Sci. USA 112, 9542 (2015).
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G. Genoud, M. Vainio, H. Phillips, J. Dean, and M. Merimaa, Opt. Lett. 40, 1342 (2015).
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2013 (1)

W. Kutschera, Int. J. Mass Spectrom. 349, 203 (2013).
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2012 (2)

J. Mohn, S. Szidat, K. Zeyer, and L. Emmenegger, Waste Manage. 32, 1516 (2012).
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J. Westberg, J. Wang, and O. Axner, J. Quant. Spectrosc. Radiat. Transfer 113, 2049 (2012).
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2011 (4)

I. Galli, P. C. Pastor, G. D. Lonardo, L. Fusina, G. Giusfredi, D. Mazzotti, F. Tamassia, and P. D. Natale, Mol. Phys. 109, 2267 (2011).
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I. Galli, S. Bartalini, S. Borri, P. Cancio, D. Mazzotti, P. De Natale, and G. Giusfredi, Phys. Rev. Lett. 107, 270802 (2011).
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J. Li, W. Chen, and B. Yu, Appl. Spectrosc. Rev. 46, 440 (2011).
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C. Haisch, Meas. Sci. Technol. 23, 012001 (2011).
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2010 (1)

M. Oinonen, H. Hakanpää-Laitinen, K. Hämäläinen, A. Kaskela, and H. Jungner, Nucl. Instrum. Methods Phys. Res., Sect. B 268, 1117 (2010).
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2008 (2)

V. Koskinen, J. Fonsen, K. Roth, and J. Kauppinen, Vib. Spectrosc. 48, 16 (2008).
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G. Lappin and L. Stevens, Expert. Opin. Drug Metab. Toxicol. 4, 1021 (2008).
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2007 (1)

R. Lindley, A. M. Parkes, K. A. Keen, E. McNaghten, and A. J. Orr-Ewing, Appl. Phys. B 86, 707 (2007).
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2006 (2)

M.-S. Yim and F. Caron, Prog. Nucl. Energy 48, 2 (2006).
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V. Koskinen, J. Fonsen, J. Kauppinen, and I. Kauppinen, Vib. Spectrosc. 42, 239 (2006).
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2001 (1)

P. Kluczynski, J. Gustafsson, Å. M. Lindberg, and O. Axner, Spectrochim. Acta B Atom. Spectros. 56, 1277 (2001).
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1997 (1)

D. Romanini, A. Kachanov, N. Sadeghi, and F. Stoeckel, Chem. Phys. Lett. 264, 316 (1997).
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1995 (1)

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1981 (1)

D. Labrie and J. Reid, Appl. Phys. 24, 381 (1981).
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1977 (1)

1956 (1)

J. M. Passmann, N. S. Radin, and J. A. D. Cooper, Anal. Chem. 28, 484 (1956).
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Akikusa, N.

Alpsten, M.

K. Stenström, B. Erlandsson, R. Hellborg, A. Wiebert, S. Skog, R. Vesanen, M. Alpsten, and B. Bjurman, J. Radiol. Nucl. Chem. 198, 203 (1995).
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Auwera, J.

I. Gordon, L. S. Rothman, C. Hill, R. V. Kochanov, Y. Tan, P. Bernath, M. Birk, V. Boudon, A. Campargue, K. Chance, B. J. Drouin, J. Flaud, R. R. Gamache, J. Hodges, D. Jacquemart, V. I. Perevalov, A. Perrin, K. P. Shine, M. Smith, J. Tennyson, G. Toon, H. Tran, V. G. Tyuterev, A. Barbe, A. G. Császár, V. M. Devi, T. Furtenbacher, J. Harrison, J. Hartmann, A. Jolly, T. J. Johnson, T. Karman, I. Kleiner, A. A. Kyuberis, J. Loos, O. M. Lyulin, S. Massie, S. Mikhailenko, N. Moazzen-Ahmadi, H. S. P. Muller, O. V. Naumenko, A. V. Nikitin, O. L. Polyansky, M. Rey, M. Rotger, S. Sharpe, K. Sung, E. Starikova, S. Tashkun, J. Auwera, G. Wagner, J. Wilzewski, P. Wcisło, S. Yu, and E. J. Zak, J. Quant. Spectrosc. Radiat. Transfer 203, 3 (2017).
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Axner, O.

J. Westberg, J. Wang, and O. Axner, J. Quant. Spectrosc. Radiat. Transfer 113, 2049 (2012).
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P. Kluczynski, J. Gustafsson, Å. M. Lindberg, and O. Axner, Spectrochim. Acta B Atom. Spectros. 56, 1277 (2001).
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Ballerini, R.

Barbe, A.

I. Gordon, L. S. Rothman, C. Hill, R. V. Kochanov, Y. Tan, P. Bernath, M. Birk, V. Boudon, A. Campargue, K. Chance, B. J. Drouin, J. Flaud, R. R. Gamache, J. Hodges, D. Jacquemart, V. I. Perevalov, A. Perrin, K. P. Shine, M. Smith, J. Tennyson, G. Toon, H. Tran, V. G. Tyuterev, A. Barbe, A. G. Császár, V. M. Devi, T. Furtenbacher, J. Harrison, J. Hartmann, A. Jolly, T. J. Johnson, T. Karman, I. Kleiner, A. A. Kyuberis, J. Loos, O. M. Lyulin, S. Massie, S. Mikhailenko, N. Moazzen-Ahmadi, H. S. P. Muller, O. V. Naumenko, A. V. Nikitin, O. L. Polyansky, M. Rey, M. Rotger, S. Sharpe, K. Sung, E. Starikova, S. Tashkun, J. Auwera, G. Wagner, J. Wilzewski, P. Wcisło, S. Yu, and E. J. Zak, J. Quant. Spectrosc. Radiat. Transfer 203, 3 (2017).
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Bartalini, S.

I. Galli, S. Bartalini, R. Ballerini, M. Barucci, P. Cancio, M. D. Pas, G. Giusfredi, D. Mazzotti, N. Akikusa, and P. D. Natale, Optica 3, 385 (2016).
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I. Galli, S. Bartalini, S. Borri, P. Cancio, D. Mazzotti, P. De Natale, and G. Giusfredi, Phys. Rev. Lett. 107, 270802 (2011).
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Barucci, M.

Bell, S.

G. Genoud, J. Lehmuskoski, S. Bell, V. Palonen, M. Oinonen, M.-L. Koskinen-Soivi, and M. Reinikainen, Anal. Chem. 91, 12315 (2019).
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Bench, G.

A. McCartt, T. Ognibene, G. Bench, and K. Turteltaub, Nucl. Instrum. Methods Phys. Res., Sect. B 361, 277 (2015).
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Bernath, P.

I. Gordon, L. S. Rothman, C. Hill, R. V. Kochanov, Y. Tan, P. Bernath, M. Birk, V. Boudon, A. Campargue, K. Chance, B. J. Drouin, J. Flaud, R. R. Gamache, J. Hodges, D. Jacquemart, V. I. Perevalov, A. Perrin, K. P. Shine, M. Smith, J. Tennyson, G. Toon, H. Tran, V. G. Tyuterev, A. Barbe, A. G. Császár, V. M. Devi, T. Furtenbacher, J. Harrison, J. Hartmann, A. Jolly, T. J. Johnson, T. Karman, I. Kleiner, A. A. Kyuberis, J. Loos, O. M. Lyulin, S. Massie, S. Mikhailenko, N. Moazzen-Ahmadi, H. S. P. Muller, O. V. Naumenko, A. V. Nikitin, O. L. Polyansky, M. Rey, M. Rotger, S. Sharpe, K. Sung, E. Starikova, S. Tashkun, J. Auwera, G. Wagner, J. Wilzewski, P. Wcisło, S. Yu, and E. J. Zak, J. Quant. Spectrosc. Radiat. Transfer 203, 3 (2017).
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Birk, M.

I. Gordon, L. S. Rothman, C. Hill, R. V. Kochanov, Y. Tan, P. Bernath, M. Birk, V. Boudon, A. Campargue, K. Chance, B. J. Drouin, J. Flaud, R. R. Gamache, J. Hodges, D. Jacquemart, V. I. Perevalov, A. Perrin, K. P. Shine, M. Smith, J. Tennyson, G. Toon, H. Tran, V. G. Tyuterev, A. Barbe, A. G. Császár, V. M. Devi, T. Furtenbacher, J. Harrison, J. Hartmann, A. Jolly, T. J. Johnson, T. Karman, I. Kleiner, A. A. Kyuberis, J. Loos, O. M. Lyulin, S. Massie, S. Mikhailenko, N. Moazzen-Ahmadi, H. S. P. Muller, O. V. Naumenko, A. V. Nikitin, O. L. Polyansky, M. Rey, M. Rotger, S. Sharpe, K. Sung, E. Starikova, S. Tashkun, J. Auwera, G. Wagner, J. Wilzewski, P. Wcisło, S. Yu, and E. J. Zak, J. Quant. Spectrosc. Radiat. Transfer 203, 3 (2017).
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Bjurman, B.

K. Stenström, B. Erlandsson, R. Hellborg, A. Wiebert, S. Skog, R. Vesanen, M. Alpsten, and B. Bjurman, J. Radiol. Nucl. Chem. 198, 203 (1995).
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Borri, S.

I. Galli, S. Bartalini, S. Borri, P. Cancio, D. Mazzotti, P. De Natale, and G. Giusfredi, Phys. Rev. Lett. 107, 270802 (2011).
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Boudon, V.

I. Gordon, L. S. Rothman, C. Hill, R. V. Kochanov, Y. Tan, P. Bernath, M. Birk, V. Boudon, A. Campargue, K. Chance, B. J. Drouin, J. Flaud, R. R. Gamache, J. Hodges, D. Jacquemart, V. I. Perevalov, A. Perrin, K. P. Shine, M. Smith, J. Tennyson, G. Toon, H. Tran, V. G. Tyuterev, A. Barbe, A. G. Császár, V. M. Devi, T. Furtenbacher, J. Harrison, J. Hartmann, A. Jolly, T. J. Johnson, T. Karman, I. Kleiner, A. A. Kyuberis, J. Loos, O. M. Lyulin, S. Massie, S. Mikhailenko, N. Moazzen-Ahmadi, H. S. P. Muller, O. V. Naumenko, A. V. Nikitin, O. L. Polyansky, M. Rey, M. Rotger, S. Sharpe, K. Sung, E. Starikova, S. Tashkun, J. Auwera, G. Wagner, J. Wilzewski, P. Wcisło, S. Yu, and E. J. Zak, J. Quant. Spectrosc. Radiat. Transfer 203, 3 (2017).
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Campargue, A.

I. Gordon, L. S. Rothman, C. Hill, R. V. Kochanov, Y. Tan, P. Bernath, M. Birk, V. Boudon, A. Campargue, K. Chance, B. J. Drouin, J. Flaud, R. R. Gamache, J. Hodges, D. Jacquemart, V. I. Perevalov, A. Perrin, K. P. Shine, M. Smith, J. Tennyson, G. Toon, H. Tran, V. G. Tyuterev, A. Barbe, A. G. Császár, V. M. Devi, T. Furtenbacher, J. Harrison, J. Hartmann, A. Jolly, T. J. Johnson, T. Karman, I. Kleiner, A. A. Kyuberis, J. Loos, O. M. Lyulin, S. Massie, S. Mikhailenko, N. Moazzen-Ahmadi, H. S. P. Muller, O. V. Naumenko, A. V. Nikitin, O. L. Polyansky, M. Rey, M. Rotger, S. Sharpe, K. Sung, E. Starikova, S. Tashkun, J. Auwera, G. Wagner, J. Wilzewski, P. Wcisło, S. Yu, and E. J. Zak, J. Quant. Spectrosc. Radiat. Transfer 203, 3 (2017).
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Cancio, P.

I. Galli, S. Bartalini, R. Ballerini, M. Barucci, P. Cancio, M. D. Pas, G. Giusfredi, D. Mazzotti, N. Akikusa, and P. D. Natale, Optica 3, 385 (2016).
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I. Galli, S. Bartalini, S. Borri, P. Cancio, D. Mazzotti, P. De Natale, and G. Giusfredi, Phys. Rev. Lett. 107, 270802 (2011).
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Caron, F.

M.-S. Yim and F. Caron, Prog. Nucl. Energy 48, 2 (2006).
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Chance, K.

I. Gordon, L. S. Rothman, C. Hill, R. V. Kochanov, Y. Tan, P. Bernath, M. Birk, V. Boudon, A. Campargue, K. Chance, B. J. Drouin, J. Flaud, R. R. Gamache, J. Hodges, D. Jacquemart, V. I. Perevalov, A. Perrin, K. P. Shine, M. Smith, J. Tennyson, G. Toon, H. Tran, V. G. Tyuterev, A. Barbe, A. G. Császár, V. M. Devi, T. Furtenbacher, J. Harrison, J. Hartmann, A. Jolly, T. J. Johnson, T. Karman, I. Kleiner, A. A. Kyuberis, J. Loos, O. M. Lyulin, S. Massie, S. Mikhailenko, N. Moazzen-Ahmadi, H. S. P. Muller, O. V. Naumenko, A. V. Nikitin, O. L. Polyansky, M. Rey, M. Rotger, S. Sharpe, K. Sung, E. Starikova, S. Tashkun, J. Auwera, G. Wagner, J. Wilzewski, P. Wcisło, S. Yu, and E. J. Zak, J. Quant. Spectrosc. Radiat. Transfer 203, 3 (2017).
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Chen, W.

J. Li, W. Chen, and B. Yu, Appl. Spectrosc. Rev. 46, 440 (2011).
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Cooper, J. A. D.

J. M. Passmann, N. S. Radin, and J. A. D. Cooper, Anal. Chem. 28, 484 (1956).
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Császár, A. G.

I. Gordon, L. S. Rothman, C. Hill, R. V. Kochanov, Y. Tan, P. Bernath, M. Birk, V. Boudon, A. Campargue, K. Chance, B. J. Drouin, J. Flaud, R. R. Gamache, J. Hodges, D. Jacquemart, V. I. Perevalov, A. Perrin, K. P. Shine, M. Smith, J. Tennyson, G. Toon, H. Tran, V. G. Tyuterev, A. Barbe, A. G. Császár, V. M. Devi, T. Furtenbacher, J. Harrison, J. Hartmann, A. Jolly, T. J. Johnson, T. Karman, I. Kleiner, A. A. Kyuberis, J. Loos, O. M. Lyulin, S. Massie, S. Mikhailenko, N. Moazzen-Ahmadi, H. S. P. Muller, O. V. Naumenko, A. V. Nikitin, O. L. Polyansky, M. Rey, M. Rotger, S. Sharpe, K. Sung, E. Starikova, S. Tashkun, J. Auwera, G. Wagner, J. Wilzewski, P. Wcisło, S. Yu, and E. J. Zak, J. Quant. Spectrosc. Radiat. Transfer 203, 3 (2017).
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I. Galli, S. Bartalini, S. Borri, P. Cancio, D. Mazzotti, P. De Natale, and G. Giusfredi, Phys. Rev. Lett. 107, 270802 (2011).
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Dean, J.

Devi, V. M.

I. Gordon, L. S. Rothman, C. Hill, R. V. Kochanov, Y. Tan, P. Bernath, M. Birk, V. Boudon, A. Campargue, K. Chance, B. J. Drouin, J. Flaud, R. R. Gamache, J. Hodges, D. Jacquemart, V. I. Perevalov, A. Perrin, K. P. Shine, M. Smith, J. Tennyson, G. Toon, H. Tran, V. G. Tyuterev, A. Barbe, A. G. Császár, V. M. Devi, T. Furtenbacher, J. Harrison, J. Hartmann, A. Jolly, T. J. Johnson, T. Karman, I. Kleiner, A. A. Kyuberis, J. Loos, O. M. Lyulin, S. Massie, S. Mikhailenko, N. Moazzen-Ahmadi, H. S. P. Muller, O. V. Naumenko, A. V. Nikitin, O. L. Polyansky, M. Rey, M. Rotger, S. Sharpe, K. Sung, E. Starikova, S. Tashkun, J. Auwera, G. Wagner, J. Wilzewski, P. Wcisło, S. Yu, and E. J. Zak, J. Quant. Spectrosc. Radiat. Transfer 203, 3 (2017).
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Drouin, B. J.

I. Gordon, L. S. Rothman, C. Hill, R. V. Kochanov, Y. Tan, P. Bernath, M. Birk, V. Boudon, A. Campargue, K. Chance, B. J. Drouin, J. Flaud, R. R. Gamache, J. Hodges, D. Jacquemart, V. I. Perevalov, A. Perrin, K. P. Shine, M. Smith, J. Tennyson, G. Toon, H. Tran, V. G. Tyuterev, A. Barbe, A. G. Császár, V. M. Devi, T. Furtenbacher, J. Harrison, J. Hartmann, A. Jolly, T. J. Johnson, T. Karman, I. Kleiner, A. A. Kyuberis, J. Loos, O. M. Lyulin, S. Massie, S. Mikhailenko, N. Moazzen-Ahmadi, H. S. P. Muller, O. V. Naumenko, A. V. Nikitin, O. L. Polyansky, M. Rey, M. Rotger, S. Sharpe, K. Sung, E. Starikova, S. Tashkun, J. Auwera, G. Wagner, J. Wilzewski, P. Wcisło, S. Yu, and E. J. Zak, J. Quant. Spectrosc. Radiat. Transfer 203, 3 (2017).
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Emmenegger, L.

J. Mohn, S. Szidat, K. Zeyer, and L. Emmenegger, Waste Manage. 32, 1516 (2012).
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Eng, R. S.

Erlandsson, B.

K. Stenström, B. Erlandsson, R. Hellborg, A. Wiebert, S. Skog, R. Vesanen, M. Alpsten, and B. Bjurman, J. Radiol. Nucl. Chem. 198, 203 (1995).
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Flaud, J.

I. Gordon, L. S. Rothman, C. Hill, R. V. Kochanov, Y. Tan, P. Bernath, M. Birk, V. Boudon, A. Campargue, K. Chance, B. J. Drouin, J. Flaud, R. R. Gamache, J. Hodges, D. Jacquemart, V. I. Perevalov, A. Perrin, K. P. Shine, M. Smith, J. Tennyson, G. Toon, H. Tran, V. G. Tyuterev, A. Barbe, A. G. Császár, V. M. Devi, T. Furtenbacher, J. Harrison, J. Hartmann, A. Jolly, T. J. Johnson, T. Karman, I. Kleiner, A. A. Kyuberis, J. Loos, O. M. Lyulin, S. Massie, S. Mikhailenko, N. Moazzen-Ahmadi, H. S. P. Muller, O. V. Naumenko, A. V. Nikitin, O. L. Polyansky, M. Rey, M. Rotger, S. Sharpe, K. Sung, E. Starikova, S. Tashkun, J. Auwera, G. Wagner, J. Wilzewski, P. Wcisło, S. Yu, and E. J. Zak, J. Quant. Spectrosc. Radiat. Transfer 203, 3 (2017).
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Fleisher, A.

A. Fleisher, D. Long, Q. Liu, L. Gameson, and J. Hodges, J. Phys. Chem. Lett. 8, 4550 (2017).
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Fonsen, J.

V. Koskinen, J. Fonsen, K. Roth, and J. Kauppinen, Vib. Spectrosc. 48, 16 (2008).
[Crossref]

V. Koskinen, J. Fonsen, J. Kauppinen, and I. Kauppinen, Vib. Spectrosc. 42, 239 (2006).
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Furtenbacher, T.

I. Gordon, L. S. Rothman, C. Hill, R. V. Kochanov, Y. Tan, P. Bernath, M. Birk, V. Boudon, A. Campargue, K. Chance, B. J. Drouin, J. Flaud, R. R. Gamache, J. Hodges, D. Jacquemart, V. I. Perevalov, A. Perrin, K. P. Shine, M. Smith, J. Tennyson, G. Toon, H. Tran, V. G. Tyuterev, A. Barbe, A. G. Császár, V. M. Devi, T. Furtenbacher, J. Harrison, J. Hartmann, A. Jolly, T. J. Johnson, T. Karman, I. Kleiner, A. A. Kyuberis, J. Loos, O. M. Lyulin, S. Massie, S. Mikhailenko, N. Moazzen-Ahmadi, H. S. P. Muller, O. V. Naumenko, A. V. Nikitin, O. L. Polyansky, M. Rey, M. Rotger, S. Sharpe, K. Sung, E. Starikova, S. Tashkun, J. Auwera, G. Wagner, J. Wilzewski, P. Wcisło, S. Yu, and E. J. Zak, J. Quant. Spectrosc. Radiat. Transfer 203, 3 (2017).
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Fusina, L.

I. Galli, P. C. Pastor, G. D. Lonardo, L. Fusina, G. Giusfredi, D. Mazzotti, F. Tamassia, and P. D. Natale, Mol. Phys. 109, 2267 (2011).
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Galli, I.

I. Galli, S. Bartalini, R. Ballerini, M. Barucci, P. Cancio, M. D. Pas, G. Giusfredi, D. Mazzotti, N. Akikusa, and P. D. Natale, Optica 3, 385 (2016).
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I. Galli, S. Bartalini, S. Borri, P. Cancio, D. Mazzotti, P. De Natale, and G. Giusfredi, Phys. Rev. Lett. 107, 270802 (2011).
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I. Galli, P. C. Pastor, G. D. Lonardo, L. Fusina, G. Giusfredi, D. Mazzotti, F. Tamassia, and P. D. Natale, Mol. Phys. 109, 2267 (2011).
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Gamache, R. R.

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Supplementary Material (1)

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Data Availability

Data underlying the results presented in this paper are not publicly available at this time but may be obtained from the authors upon reasonable request.

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Figures (5)

Fig. 1.
Fig. 1. Simulated absorption spectra for 1 ppb of $^{14}{{\rm CO}_2}$ at a pressure of 20 mbar and 70 mbar are shown in orange and blue, respectively, in (a). $\alpha$ denotes the normalized absorption coefficient. A simulation of ${2}f$ wavelength-modulated spectrum at 70 mbar and a modulation amplitude of $0.01\;{{\rm cm}^{- 1}}$ are presented in (b).
Fig. 2.
Fig. 2. Experimental setup comprises a quantum cascade laser, a photoacoustic cell, a lock-in amplifier, and a data acquisition card. The photoacoustic signal is recorded at the second harmonic of the modulation frequency.
Fig. 3.
Fig. 3. Experimental spectra for different pressures with a constant modulation amplitude of $0.009\;{{\rm cm}^{- 1}}$ are presented in (a). The spectra for different modulation amplitudes at a constant pressure of 60 mbar are shown in (b). The solid lines act as a guide to the eye. All the spectra are averaged over 30 scans for an acquisition time of 33 min.
Fig. 4.
Fig. 4. Experimental spectra for 1000, 500, 100, and 0 ppt of a $^{14}{{\rm CO}_2}$ sample are presented in blue, orange, yellow, and purple, respectively, in (a). The corresponding fit through these points are depicted by a solid line. The fit residuals are shown in (b). The $^{14}{\rm C/C}$ ratio determined by computing the ratio of absorption line areas from the experimental data as a function of mixing ratio are plotted in (c), with the black line depicting the expected linear behavior.
Fig. 5.
Fig. 5. Allan deviation plot for 1 ppb and 500 ppt of $^{14}{{\rm CO}_2}$ . The sample gas pressure at the start of the measurement is 40 mbar. The noise equivalent concentration (NEC) for 1 ppb of $^{14}{{\rm CO}_2}$ is 30 ppt at an averaging time of 9 min. The expected $1/\sqrt t$ behavior for a white-noise-dominated system is depicted by the grey dashed line.

Equations (2)

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S = S m P C c e l l N t o t c m σ ,
N N E A = α m i n P t ,