High-resolution spectroscopy with and frequency stabilization of a cw dye laser

The hyperfine splittings of the Na D₁ and D₂ lines were investigated using a single mode cw dye laser. The light of the laser was scattered by the atoms of an atomic beam and the fluorescent light was observed as the frequency of the laser was tuned across the D lines. The Doppler width of the atomic beam was reduced to about 2.5 MHz so that the absorption width of the atoms of the beam was essentially determined by the natural width of the 3²P_1/2 and 3²P_3/2 levels, which is about 10 MHz. Since the linewidth observed for the hyperfine transitions was 30 MHz, most of the hyperfine components of the D₁ and D₂ lines could be resolved. In another experiment the frequency of the dye laser was locked to a hyperfine transition of the D₁ line. The observed variation of the output frequency of the dye laser was less than ±1.5 MHz. In addition, the intensity of the dye laser was controlled to about 10⁻³, using an electro-optically variable transmission filter.     

Characteristics of 20 year old iodine cell and compact iodine stabilized laser

Spectral quality and reliability of four kinds of¹²⁷ I ₂ cells for an wavelengtn standard were investigated. A 20 year old 10 cm long sealed off iodine cell has shown its long life and had sufficient absorption characteristics comparable to the newly made three cells in regard to spectral line width and signal-to-noise ratio of the absorption signal. A dispersion of absolute frequencies of the three cells including the 20 year old cell is in a range of 35 kHz, which is equivalent to a frequency reproducibility of 7.4X10^-11. A compact iodine stabilized 633 nm He-Ne laser with a 23 cm long resonator and 4 cm iodine cell has been developed. Its frequency stability has been estimated to be 9X10^-13 by the Allan deviation at integration time of 4000 s. The laser supplies 14 wavelength standards being locked at iodine absorption lines from a ton.     

Assignments of several groups of iodine (I2) lines in the B-X system

The spectra obtained by means of Fourier spectroscopy and the assignments of the B-X lines of I₂ in the vicinity of two argon ion laser lines (5145 and 5287 Å), three krypton ion laser lines (5208, 5308, and 5683 Å), and one HeNe laser line (6119 Å) are given. A detailed comparison, in the vicinity of the argon ion laser line (5145 Å), between the iodine wavenumbers calculated by means of the two sets of molecular constants previously published [Wei and Tellinghuisen, J. Mol. Spectrosc.50, 317–332 (1974); Barrow and Yee, J. C. S. Faraday II. 69, 684–700 (1973)] with those calculated from Fourier spectroscopy data, is presented.     

Theoretical assignment of the observed hyperfine structure in the saturated absorption spectra of I2129 and I127I129 vapors in the 633 nm wavelength region

The detailed structure observed in the saturated absorption spectrum of I₂¹²⁹ vapor in the 633 nm wavelength region in the spectral interval reported by Knox and Pao, has been interpreted to be the overlap between the hyperfine lines of the 8-4 P(54) line of I₂¹²⁹ and the 6-3 P(33) line of the I¹²⁷I¹²⁹ vapor. In this assignment, the nuclear electric quadrupole and nuclear magnetic terms in the Hamiltonian were diagonalized exactly and certain molecular parameters were varied to obtain the best fit with the observed spectrum. For I₂¹²⁹, the calculated distance (separation) of the center of the 8-4 P(54) line from the line center of the Ne²⁰ 633 nm laser transition is 0.04 cm^?1 and the RMS deviation between the theoretical and experimental hyperfine spectra is 0.3 MHz. Although the calculated frequency of R(60) transition in the 8-4 band is only 0.03 cm^?1 from the center of the laser line, we conclude on the basis of the larger RMS error (0.5 MHz) that this latter transition is less likely to be that responsible for the structure discussed in this paper.     

CW and pulsed Pb1–xSnxSe diode laser spectroscopy of 14NH3 and 15NH3 molecules

The absorption spectra of ¹⁴NH₃ and ¹⁵NH₃ molecules from 930 cm^-1 to 1220 cm^-1 have been obtained with CW and pulsed Pb_1–xSn_xSe diode lasers. The laser emission frequency has been tuned by varying crystal composition, diode temperature, hydrostatic pressure, or injection current. The registration of the absorption spectra with CW PbSe laser continuously tuned by varying hydrostatic pressure has been accomplished. The possibility of gas isotope abundancies measurements by diode lasers is considered.     

Precision heterodyne measurements of ozone spectral lines near 9.5 μm

Precision measurements of 26 individual spectral lines of ozone near 9.5 μm were made using the GSFC infrared heterodyne spectrometer. The line profiles of 26 lines in near coincidence with the emission lines from a ¹²C¹⁶O₂ laser local oscillator were measured at resolving powers of 6 × 10⁶. The retrieved absolute line center frequencies, accurate to ±3 MHz, and the relative line intensities were compared to previous experimental results and theoretical calculations.     

New fir laser lines and frequency measurements from optically pumped13CD3OH3

We report the discovery of 57 new fir laser lines from¹³CD₃OH molecule optically pumped by a waveguide CO₂ laser of 300 MHz tunability. For all lines, precise frequency offset measurements between the CO₂ line center and the center of the absorbing¹³CD₃OH line were performed using the transferred Lamb-Dip technique. We have also measured directly the frequency of seven FIR laser lines by heterodyning with already known laser lines. We present a complete list of all known laser lines (134) and frequency measurements (24) for this molecule.Work supported by CNPq, FAPESP, FAEP-Brasil, and CNR-Italia     

CH<Subscript>3</Subscript>OH optically pumped by a <Superscript>13</Superscript>CO<Subscript>2</Subscript> laser: new laser lines and assignments

We report 12 new THz (far-infrared) laser lines from methanol (CH₃OH), ranging from 58.1 μm (5.2 THz) to 624.6 μm (0.5 THz). A ¹³CO₂ laser of wide tunability (110 MHz) has been used for optical pumping, allowing access to previously unexplored spectral regions. Optoacoustic absorption spectra were used as a guide to search for new THz laser lines, which have been characterized in wavelength, polarization, offset, relative intensity, and optimum operation pressure. For 20 laser lines previously observed, we have measured the absorption offset with respect to the ¹³CO₂ laser line center. PACS 33.20.Ea; 33.20.Vq; 33.80.-b     

Discovery and characterization of optically pumped far-infrared laser emissions using laser magnetic resonance spectroscopy

A laser magnetic resonance spectrometer has been used to discover and subsequently measure a far-infrared laser emission: the 166.6-micron line of CH₂F₂, optically pumped by the 9P24 CO₂ laser. By recording spectra for the NH radical, the frequency of this laser emission has been determined to be 1799950±13 MHz. Spectra for the NH radical were also recorded with two other far-infrared laser emissions: the 160.4-micron line of N₂H₄ (9P46 CO₂ pump) and the 328.6-micron line of ¹³CH₃OH (9P12 CO₂ pump). From the NH spectra, a discrepancy of 2.1 GHz with the previously measured laser frequency was identified for the 160.4-micron line. A three-laser heterodyne system was then used to remeasure the frequency to be 1868475.5±0.5 MHz. The NH spectra were also used to determine the frequency for the 328.6-micron line to be 912366±7 MHz, in agreement with the value previously calculated from the Rydberg–Ritz combination principle. PACS 07.57.Hm; 32.60.+i; 42.62.Eh     

基于高精细度光腔锁频激光的分子吸收光谱测量

利用高精细度光腔锁定激光频率,实现了对分子吸收光谱的高精度测量.光腔采用低热膨胀系数的殷钢结构设计和温度控制,实现了腔长度的稳定;通过将激光频率锁定在光腔纵模上,实现了高频率精度和高灵敏度的光腔衰荡光谱测量.利用该装置示范性地测量了二氧化碳分子在6470.42 cm~(-1)附近的光腔衰荡光谱和色散光谱,得到了高精度的谱线参数,并和数据库谱线参数进行了对比.     

Calculation of improved12C16O molecular constants and rotational-vibrational transition frequencies

We report the calculation of¹²C¹⁶O molecular constants and rotational-vibrational transition frequencies of the electronic ground state with improved accuracy. It is based on a recent paper containing results of accurate frequency measurements of a few CO lines. By using these data new rotational constants have been determined, they are then utilized to calculate band center frequencies of four bands. Futhermore, four vibrational constants were computed by means of the calculated band center frequencies. Tables of band center frequencies, andP andR branch transition frequencies are given for the bands 1–0 to 20–19. It was not possible to obtain standard deviations of line frequencies. It is shown, however, that the best molecular constants published lead to line frequencies with deviations of a few hundred MHz. Line frequencies calculated with the new molecular constants coincide exactly with frequencies measured. Finally, it is shown that there are pairs of transitions whose frequencies are close together. By measuring frequency differences of a number of such pairs it should be possible to further improve CO molecular constants.     

Linewidth and intensity measurements of SO2 lines at 94 GHz with self-broadening and broadening by H2O and N2

In the frequency range between 91.5 and 95.5 GHz, three rotational lines of the ³²S¹⁶O₂ and two rotational lines of the ³⁴S¹⁶O₂ molecules in the fundamental vibrational state, and also two lines of the ³²S¹⁶O₂ molecule in the v₂ vibrational state, have been investigated. Center frequencies and absolute absorptions have been measured and compared with theoretical values. Furthermore, the self-broadening and broadening by H₂O and N₂ of the transition 23(6,18)–24(5,19) with the line center at 94.064 GHz have been investigated. The following linewidth parameters were found: SO₂-SO₂, 18.2±0.3 MHz/torr; SO₂-N₂, 3.8±0.1 MHz/torr; SO₂-H₂O, 15.2±0.2 MHz/torr. The bridge spectrometer and the measuring method used are also described.     

Resonance fluorescence of gaseous chlorine excited with a single longitudinal mode argon ion laser

Resonance fluorescence spectra of gaseous chlorine, excited with a high power single longitudinal mode argon ion laser which was tuned through the lasing profiles of the 4880-, 4965-, 5017-, and 5145-Å lines, were studied. Five progressions of fluorescence lines were found and assigned as the fluorescence of ³⁵Cl³⁵Cl and ³⁷Cl³⁷Cl isotopic molecules resonantly excited from v = 0 and 1 levels of the X¹Σ state to the B³Π state. The fluorescence line positions agreed with those of the theoretical calculation within 0.2 cm^?1. The fluorescence intensities were very weak due to the extremely small transition probability between the B³Π and the X¹Σ states.     

IR absorption measurements and new FIR emission lines in CH3OH by use of a frequency-tunable CW waveguide CO2 laser

The IR absorption in CH₃OH in the vicinity of CO₂ laser lines has been measured quantitatively by use of a 300 MHz tunable waveguide CO₂ laser with output powers of about 3 W. Information on frequency offsets from the CO₂ line centers, small signal and saturated absorption coefficients of FIR laser pump transitions is obtained. Some stronger pump transitions with frequency offsets larger than 50 MHz gave rise to the observation of 8 new FIR emission lines with wavelengths from 43 to 125 μm.     

Pressure broadening by argon in the hyperfine resolved P(10) and P(70) (17,1) transitions of I2 XΣ(0g)→BΠ(0u) using sub-Doppler laser saturation spectroscopy

The dependence of pressure broadening upon hyperfine component in the P(10) and P(70) lines of the (17,1) band of the I₂ X¹Σ(0_g⁺)→B³Π(0_u⁺) has been studied using laser saturation spectroscopy. By limiting absorption to the zero velocity group, Doppler broadening is removed, lineshapes with widths (FWHM) <9 MHz are detectable, and collision-induced broadening is measured at pressures of 0.2-1.2 Torr. The rates for broadening by argon are 8.3±0.3 and 10.7±0.4 MHz/Torr for the P(70) and P(10) lines, respectively. No significant variation in broadening rates is observed for the 15 hyperfine components of these even rotational lines. The effects of velocity cross-relaxation introduce a broad baseline into the spectra, which is strongly dependent on rotational state, pressure, and laser modulation frequency. The observed broadening rates correlate well with prior measurements and the polarizability of the collision partner.     

Fast, low-noise, mode-by-mode, cavity-enhanced absorption spectroscopy by diode-laser self-locking

A new technique of cavity enhanced absorption spectroscopy is described. Molecular absorption spectra are obtained by recording the transmission maxima of the successive TEM_oo resonances of a high-finesse optical cavity when a Distributed Feedback Diode Laser is tuned across them. A noisy cavity output is usually observed in such a measurement since the resonances are spectrally narrower than the laser. We show that a folded (V-shaped) cavity can be used to obtain selective optical feedback from the intracavity field which builds up at resonance. This induces laser linewidth reduction and frequency locking. The linewidth narrowing eliminates the noisy cavity output, and allows measuring the maximum mode transmissions accurately. The frequency locking permits the laser to scan stepwise through the successive cavity modes. Frequency tuning is thus tightly optimized for cavity mode injection. Our setup for this technique of Optical-Feedback Cavity-Enhanced Absorption Spectroscopy (OF-CEAS) includes a 50 cm folded cavity with finesse ∼20 000 (ringdown time ∼20 μs) and allows recording spectra of up to 200 cavity modes (2 cm⁻¹) using 100 ms laser scans. We obtain a noise equivalent absorption coefficient of ∼5×10⁻¹⁰ cm⁻¹ for 1 s averaging over scans, with a dynamic range of four orders of magnitude.     

Opto-mechanical estimation of micro-trap with cold atoms via nonlinear stimulated Raman scattering spectrum

In this paper a method for identifying the wavelength range of a tunable vertical cavity surface-emitting laser (VCSEL) is introduced. The measuring technology is wavelength modulation spectroscopy (WMS). The laser is tuned over its wavelength by applying a temperature ramp using the onboard Peltier element. During this ramp the 2f absorption lines are recorded. After finishing the temperature ramp and collecting the lines, a ratio-compare algorithm calculates the theoretical amplitudes of selected predefined lines. Then it compares the measured 2f line amplitudes iteratively with the theoretical ones. If the error of the ratios of the calculated and the measured lines is below a predefined limit, the searched lines and hence the emission wavelength are identified.     

Intracavity Laser Spectroscopy of NiCl System G: Identification of a [13.0] Π3/2 State

The (0,0) vibronic band of NiCl system G with a bandhead near 12 961 cm⁻¹ was recorded at high resolution in absorption using intracavity laser spectroscopy (ILS). For the ILS absorption spectra, the NiCl molecules were produced in a nickel hollow cathode, operated with a small amount of CCl₄, and line positions were referenced to iodine spectra. Fourier transform (FT) emission spectroscopy was used to record an extensive region of the spectrum used in a vibronic analysis of system G. For the FT spectra, excited NiCl molecules were produced in a high-temperature King-type carbon tube furnace. We show that this transition is the (0,0) vibronic band associated with a newly identified ²Π_3/2 excited state and the X²Π_3/2 ground state. The molecular constants for the new ²Π_3/2 electronic state are derived from the rotational analysis. Improved vibronic constants for the band are obtained from analysis of the FT spectra.     

Effects of neon matrix environment on three vibronic emission systems of PbS

Laser sources have been used to explore three emission band systems of the PbS molecule in solid neon matrices. The D → X emission (origin near 29 630 cm^?1), excited biphotonically, consists of broad bands originating from V′ = 0. With laser excitation tuned into the region of the band system origin near 21 860 cm^?1, the B → X system shows emission narrowing of inhomogeneously broadened absorption. Hot luminescence from the B state is also reported. In the a → X system near 14 625 cm^?1 the intensities of phonon sidebands on the high-frequency side of the zero-phonon lines are found to be very sensitive to laser power. Lifetimes of the a, A, and B states of PbS in solid argon have been measured as 260, 0.95, and 1.8 μsec.     

A high-resolution cw dye laser spectrometer

The construction and utilization of a high-resolution cw dye laser spectrometer is described. The laser incorporates pressure tuned intra-cavity etalons enabling the single mode output laser frequency to be tuned more than one nm in a continuous scan. In the scan the laser jumps from one cavity mode to the next in ～ 50 MHz steps. In comparison to molecular Doppler widths this mode jumping is negligible. As an example of the use of the instrument, a high-resolution absorption spectrum of molecular iodine between the sodium D lines is presented. A unique frequency counter provides the calibration of the absorption spectrum.