Doppler-limited dye laser excitation spectroscopy of HCF

The cw dye laser excitation spectrum of the $\text{A}\text{?}{}^1\text{A″(000) ←}\text{X}\text{?}{}^1\text{A′(000)}$ vibronic band of HCF was observed between 17 188 and 17 391 cm^?1 with the Doppler-limited resolution, 0.04 cm^?1. The HCF molecule was produced by the reaction of discharged CF₄ with CH₃F, and 853 lines were observed, of which 516 transitions were assigned to K′_a ← K″_a = 3 ← 4, 2 ← 3, 1 ← 2, 0 ← 1, 1 ← 0, 2 ← 1, 0 ← 0, 1 ← 1, 2 ← 2, 3 ← 3, 2 ← 0, and 0 ← 2 subbands. A rotational analysis yielded the rotational constants and quartic and sextic centrifugal distortion constants for both the $\text{A}\text{?}$ and $\text{X}\text{?}$ states and the band origin, with good precision. The molecular constants determined reproduce the observed transition frequencies with an average deviation of 0.0038 cm^?1. Small rotational perturbations in the excited state were found at J = 5, 6 and J = 10, 11 of J_1,J and at J = 15, 16 of J_2,J?1 levels.     

Doppler-limited dye laser excitation spectroscopy of DCF

The dye laser excitation spectrum of the vibronic transition of DCF was observed between 17 200 and 17 400 cm⁻¹ with the Doppler-limited resolution. DCF was produced by the reaction of microwave-discharged CF₄ with CD₃F. The observed spectra, which were found to be nearly free of perturbations, were assigned to 858 transitions of the K′_a − K″_a = 4−5, 3−4, 2−3, 1−2, 0−1, 1−0, 2−1, 3−2, 3−3, 2−2, 1−1, 0−0, 2−0, and 0−2 subbands, and were analyzed to determine the rotational constants and centrifugal distortion constants for both the and à states. The rotational constants of DCF thus determined were combined with those of HCF to calculate the structural parameters for this molecule: r(C---H) = 1.138 Å, r(C---F) = 1.305 Å, and HCF = 104.1° for the ground state, and r(C---H) = 1.063 Å, r(C---F) = 1.308 Å, and HCF = 123.8° for the excited à state.     

Doppler-limited dye laser excitation spectroscopy of HCCl

The cw dye laser excitation spectrum of the $\text{A}\text{?}{}^1\text{A″(050) ←}\text{X}\text{?}{}^1\text{A′(000)}$ vibronic band of HCCl was observed between 16 539 and 16 656 cm^?1 with the Doppler-limited resolution, 0.03 cm^?1. The HCCl molecule was generated by the reaction of discharged CF₄ with CH₃Cl. The observed spectra were assigned to c-type transitions with ΔK_a = ±1 and also to axis-switching transitions with ΔK_a = 0 or ?2, but all with K′_a = 0, both for HC³⁵Cl and HC³⁷Cl. A rotational analysis yielded the rotational constants and quartic centrifugal distortion constants for the ground vibronic state and the band origin. A weak vibronic band, about one-third as intense as the main band, was found at about 57 cm^?1 to the violet of the main band for both isotopic species, and was ascribed to a transition from the ground vibronic state to a vibrational level, possibly (041), of the à state. The rotational levels of HC³⁵Cl in the à state showed a large perturbation; the J′ = 8, 9, and 10 levels were found to be split into two components. A normal coordinate analysis was carried out to calculate the centrifugal distortion constants and the inertia defect, which were in fair agreement with the observed values. The molecular structure of HCCl in the ground vibronic state was recalculated from the rotational constants of the two isotopic species combined with the 0.75B₀ + 0.25C₀ value previously reported for DC³⁵Cl.     

Doppler-limited dye laser excitation spectroscopy of the CCN radical

The cw dye laser excitation spectrum of the $\text{A}\text{?}{}^2\text{Δ}\text{(000) ←}\text{X}\text{?}{}^2\text{Π}\text{(000)}$ vibronic transition of the CCN radical was observed between 21 205 and 21 335 cm^?1 with the Doppler-limited resolution, 0.04 cm^?1. The CCN radical was produced by reaction of microwave discharged CF₄ with CH₃CN. The observed spectrum was analyzed to determine rotational and centrifugal constants and effective spin-orbit and spin-rotation coupling constants for both the $\text{A}\text{?}{}^2\text{Δ}\text{(000)}$ and the $\text{X}\text{?}{}^2\text{Π}\text{(000)}$ states, and also the Λ-type doubling constants for the $\text{X}\text{?}{}^2\text{Π}\text{(000)}$ state. The constants determined reproduce the observed spectrum with an average deviation of 0.0027 cm^?1, and are considered to be precise enough for predicting the ground-state microwave transition frequencies. No evidence was found for perturbation in either the $\text{A}\text{?}{}^2\text{Δ}\text{(000)}$ or the $\text{X}\text{?}{}^2\text{Π}\text{(000)}$ state.     

Doppler-limited dye laser excitation spectroscopy of the DSO radical

The $\text{A}\text{?}{}^2\text{A′(003) ←}\text{X}\text{?}{}^2\text{A″(000)}$ vibronic transition (16 370 to 16 425 cm^?1) of the DSO radical in studied by Doppler-limited dye laser excitation spectroscopy. DSO is produced in a flow system by reacting the products of a microwave discharge in O₂ with D₂S. About 637 observed lines are assigned to 987 transitions of the 19 subbands: K′_a ← K″_a = 6 ← 5, 5 ← 4, 4 ← 3, 3 ← 2, 2 ← 1, 1 ← 0, 0 ← 1, 1 ← 2, 2 ← 3, 3 ← 4, 0 ← 0, 1 ← 1, 2 ← 2, 3 ← 3, 4 ← 4, 3 ← 1, 2 ← 0, 0 ← 2, and 1 ← 3. They are analyzed to determine rotational constants, centrifugal distortion constants, and spin-rotation constants for both the ground and the excited electronic states. The band origin obtained is 16 413.874 (2.5σ = 0.002) cm^?1. The rotational constants determined are combined with the previous result on HSO (M. Kakimoto et al., J. Mol. Spectrosc.80, 334–350 (1980)) to calculate the structural parameters for this radical in both the states: $\text{r(}\text{SO}\text{) = 1.494(5)}\text{A}\text{?}$, $\text{r(}\text{SH}\text{) = 1.389(5)}\text{A}\text{?}$, and ∠HSO = 106.6(5)° for the $\text{X}\text{?}{}^2\text{A″}$ state, and $\text{r(}\text{SO}\text{) = 1.661(10)}\text{A}\text{?}$, $\text{r(}\text{SH}\text{) = 1.342(8)}\text{A}\text{?}$, and ∠HSO = 95.7(21)° for the $\text{A}\text{?}{}^2\text{A′(003)}$ state, where values in parentheses denote 2.5σ.     

Doppler-limited dye laser excitation spectroscopy of the HSO radical

The cw dye laser excitation spectrum of the vibronic transition of the HSO radical was observed between 16 420 and 16 520 cm⁻¹ with Doppler-limited resolution, 0.03 cm⁻¹. The HSO radical was produced by reaction of discharged oxygen with H₂S or CH₃SH. The observed spectra were assigned to 751 transitions of the K′_a ← K″_a = 2 ← 3, 1 ← 2, 0 ← 1, 1 ← 0, 2 ← 1, and 3 ← 2 subbands, and were analyzed to determine rotational constants, centrifugal distortion constants, and spin-rotation interaction constants with good precision. The signs of the spin-rotation interaction constants were determined for both the upper and the lower state from the observed spectra. The band origin obtained is 16 483.0252 (2.5σ = 0.0013) cm⁻¹. The molecular constants which were determined reproduce the observed transitions with an average deviation of 0.0045 cm⁻¹.     

Photo-stability of laser dye solutions under Copper-vapour-laser excitation

The photo-stability of laser dyes, Rhodamine-6G, Rhodamine-B, and Kiton-Red, under high repetition rate (6.3 kHz) Copper-vapour-laser (CVL) irradiation has been investigated. Exhaustive photo-bleaching of these dyes in different solvents has been carried out to study the extent to which the dye photo-degraded products would interfere with the lasing process in high-power CVL-pumped dye lasers. Our results indicate that the photo-degradation of dyes occurs predominantly through excited-state intermolecular reactions, involving the singlet state, rather than the process of nonlinear optical absorption in individual molecules. Received: 13 March 2000 / Revised version: 2 August 2000 / Published online: 21 March 2001     

Stark quantum beats under pulsed dye laser excitation

The method of quantum beat spectroscopy is extended to the study of pure electric field splittings. As an example Stark splittings of the 6s6p ¹P₁ term of Ba I are investigated by observing quantum beats after excitation by a short resonant dye-laser pulse. The derived value for the tensorial polarizability is in good agreement with previous work. Occurence and shapes of Stark quantum beat signals under different experimental conditions are discussed.     

Design of a dye laser for nonlinear spectroscopy

Special requirements should be met by a pulsed dye laser in order to provide reproducible data in a nonlinear experiment. The cavity and pumping laser are chosen to minimize effects due to detailed dye characteristics. A suitable ruby pumping laser is described.     

High resolution laser excitation spectroscopy of barium monosulfide

High-resolution spectra of BaS were recorded using laser excitation spectroscopy. BaS molecules were synthesized in a Broida-type oven. The observed rotationally-resolved spectrum of BaS in the 12 100–12 765 cm^?1 spectral range contains the 2-1, 3-1, 3-2, 4-2, 5-2, 5-3 vibrational bands of the A′¹Π–X¹Σ⁺ transition and the 4-1, 5-1, 5-2 vibrational bands of the a³Π₁–X¹Σ⁺ transition. Approximately 1000 lines of the A′¹Π–X¹Σ⁺ transition and 600 lines of the a³Π₁–X¹Σ⁺ transition for the main isotopologue ¹³⁸Ba³²S (67.5% natural abundance) were measured. Rotational and vibrational parameters were derived for the A′¹Π and a³Π₁ states.     

Some characteristics of dye lasers with nitrogen laser pulse excitation

Results from experiments in which the ultraviolet pulses from a nitrogen laser are used to obtain laser action from organic dyes are described. The dyes include three in the xanthene group (rhodamine 6G, B, and sodium fluorescein) and two coumarins, 7-diethylamino-4-methylcoumarin and 7-N-dimethylamino-4, 6-dimethylcoumarin) in ethanol solvent. With these dyes, laser power is available over the entire visible range from 4200 to 6300 Å when used with a rotatabie diffraction grating. The range of tunability of one of the dyes was extended to 1000 Å by appropriate acidification. The spectral halfwidth of the light varied between 7 and 15 Å over the range of tunability. Maximum repetition rates of 100 pps were obtained. Maximum power efficiency of 25% was found for rhodamine 6G. Overall output pulse shapes were found to be in agreement with the theory of Sorokinet al. Output pulse widths varied from 1 to 7 nsec. Other dyes which we have found to lase by this method of excitation include acridone, chloro-aluminium pthalocyanine and 4-methylumbelliferone. However, these dyes will not be discussed further in the text.Partially supported by US Army Research Office, Durham, North Carolina.     

Opto-acoustic spectroscopy with a visible CW dye laser

The first use of a tunable visible laser in conjunction with an opto-acoustic cell is described. By using a longitudinal resonance of the gas cell NO₂ can be detected around 10 p.p.b., the same order of detectivity as in the infrared. The use of the technique for studying photodissociation in the visible and u.v. is discussed.     

Coherent spectroscopy with a distributed feedback dye laser

A simple and flexible distributed feedback dye laser source pumped by the harmonic of a mode-locked YAG laser is described. Measurements of dephasing times of isotopic and hot bands in CS₂ liquid exploiting both the frequency and time-resolution of this source are reported.     

High-resolution (Doppler-limited) spectroscopy using quantum-cascade distributed-feedback lasers

Lasing characteristics were evaluated for distributed-feedback quantum-cascade (QC) lasers operating in a continuous mode at cryogenic temperatures. These tests were performed to determine the QC lasers' suitability for use in high-resolution spectroscopic applications, including Doppler-limited molecular absorption and pressure-limited lidar applications. By use of a rapid-scan technique, direct absorbance measurements of nitric oxide (NO) and ammonia (NH>(3)) were performed with several QC lasers, operating at either 5.2 or 8.5 microm. Results include time-averaged linewidths of better than 40 MHz and long-term laser frequency reproducibility, even after numerous temperature cycles, of 80 MHz or better. Tuning rates of 2.5 cm(-1) in 0.6 ms can be easily achieved. Noise-equivalent absorbance of 3 x 10(-6) was also obtained without optimizing the optical arrangement.     

Electron beam excitation studies of potential dye vapor phase laser systems

Excitation processes of selected dye vapor-rare gas mixtures pumped by an electron beam have been studied. These experiments revealed the importance of effective collisional electron energy transfer pumping via a dense rare gas rather than a radiative energy transfer from an excimer laser gas mixture to achieve population inversion in an organic dye vapor. Work supported in part by the Energy Research and Development Adinistration, the Robert A. Welch Foundation and the National Science Foundation.     

NaK分子激发态的预离解和碰撞激发转移

用Ar+激光器固定频率488.0nm线激发Na-K混合蒸汽,NaK分子激发态通过自发辐射、预离解和与基态原子的碰撞激发转移而去布居,测量在不同K原子密度下原子荧光对分子荧光的强度比,结合NaK(E)态寿命,得到了预离解率和碰撞激发转移率.     

Doppler-limited dye laser excitation spectrum of the C2 Swan band (v′ − v″ = 1 − 0)

The dye laser excitation spectrum of the Swan band (v′ ? v″ = 1 ? 0) has been observed with Doppler-limited resolution. The C₂ molecule was generated by the reaction of microwave discharge products of CF₄ with CH₄. The high sensitivity of laser excitation spectroscopy has enabled us to observe not only $\text{ΔΩ}\text{= 0}$ transitions, but also $\text{ΔΩ}\text{= ± 1}$ transitions and to determine molecular constants including the spin-orbit coupling constant for both the d³Π_g and a³Π_u states. The parameters thus obtained for a³Π_u were favorably compared with those previously obtained from the Ballik-Ramsay band. The present results on the d³Π_gv = 1 state were combined with those of an earlier Fourier spectroscopic study on the Swan band (v′ ? v″ = 0 ? 0) to derive equilibrium molecular constants for the d³Π_g state. The contributions of the spin-rotation interaction and the centrifugal correction for the spin-orbit coupling to the energy levels in a ³Π state have been discussed in detail.