Abstract
The spectral resolution of all methods discussed in Chap.8 was in principle limited by the Doppler width of lines in the molecular absorption—or emission—spectra, although the laser linewidth might have been much smaller. In this chapter we present several techniques which overcome this resolution limit and which allow one to resolve the natural linewidth even in the presence of a much larger Doppler width. These techniques, which have been developed recently, have already stimulated experimental and theoretical atomic physics in an outstanding way. These various Doppler-free methods certainly represent an important step towards a more detailed knowledge of molecular structure and of deeper details regarding the interaction of E.M. radiation and matter.
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References
R. Abjean, M. Leriche: On the shapes of absorption lines in a divergent atomic beam. Opt. Commun. 15, 121 (1975)
R.W. Stanley: Gaseous atomic beam light source. J. Opt. Soc. Am. 56, 350 (1966)
G. Höning, M. Cjaikowski, W. Demtröder: High resolution laser spectroscopy of Cs2. J. Chem. Phys. 71, 2138 (1979)
W. Demtröder, F. Paech, R. Schmiedl: Hyperfine-structure in the visible spectrum of NO2 . Chem. Phys. Lett. 26, 381 (1974)
R. Schmiedl, I.R. Bonilla, F. Paech, W. Demtröder: Laser spectroscopy of NO2 under very high resolution. J. Mol. Spectrosc. 68, 236 (1977)
L.A. Hackel, K.H. Casleton, S.G. Kukolich, S. Ezekiel: Observation of magnetic octopole and scalar spin-spin interaction in I2 using laser spectroscopy. Phys. Rev. Lett. 35, 568 (1975);
L.A. Hackel, K.H. Casleton, S.G. Kukolich, S. Ezekiel: Observation of magnetic octopole and scalar spin-spin interaction in I2 using laser spectroscopy. J. Opt. Soc. Am. 64, 1387 (1974)
C. Duke, H. Fischer, H.J. Kluge, H. Kremmling, Th. Kühl, E.W. Otten: Determination of the isotope shift of Hg by on line laser-spectroscopy. Phys. Lett. 60A, 303 (1977)
Th. Kühl, P. Dabkiewicz, C. Duke, H. Fischer, H.J. Kluge, H. Kremmling: Nuclear shape staggering in very neutron-deficient Hg-isotopes detected by laser-spectroscopy. Phys. Rev. Lett. 39, 180 (1977)
G. Nowicki, K. Bekk, J. Göring, A. Hansen, H. Rebel, G. Schatz: Nuclear charge radii and nuclear moments of neutron deficient Ba-isotopes from high resolution laser spectroscopy. Phys. Rev. C18, 2369 (1978)
H.T. Duong, P. Jacquinot, P. Juncar, I. Lieberman, J. Pinard, J.L. Vialle: “High Resolution Laser Spectroscopy of the D-Lines of On-Line Produced Radioactive Sodium Isotopes”, in Laser Spectroscopy , ed. by I. Haroche, J.C. Pebay-Peyroula, T.W. Hänsch, S.E. Harris, Lecture Notes in Physics, Vol. 43 (Springer, Berlin, Heidelberg, New York 1975)
P. Jacquinot: “Atomic Beam Spectroscopy”, in High Resolution Laser Spectroscopy, ed. by K. Shimoda, Topics in Applied Physics, Vol. 13 (Springer, Berlin, Heidelberg, New York 1976)
W. Lange, J. Luther, A. Steudel: “Dyelasers in Atomic Spectroscopy”, in Advances in Atomic and Molecular Physics, Vol. 10, ed. by D.R. Bates, B. Bederson (Academic Press, New York 1974)
D.H. Levy, L. Wharton, R.E. Smalley: “Laser Spectroscopy in Supersonic Jets” , in Chemical and Biochemical Applications of Lasers, Vol. II, ed. by C.B. Moore (Academic Press, New York 1977)
J.B. Anderson: “Molecular Beams from Nozzle Sources”, in Molecular Beams and Low Density Gas Dynamics, ed. by P.P. Wegener (Dekker, New York 1974)
D.E. Pritchard, R. Ahmed-Bitar, W.P. Lapatovich: “Laser Spectroscopy of Bound Na Ne and Related Atomic Physics”, in Ref.1.11a, p.355
A. Hermann, S. Leutwyler, E. Schuhmacher, L. Wöste: On metal atom clusters IV: Photoionization thresholds and multiphoton ionization spectra of alkali-metal molecules. Helv. Chim. Acta 61, 453 (1978)
K. Bergmann, W. Demtröder, P. Hering: Laser diagnostics in molecular beams. Appl. Phys. 8, 65 (1975)
M.P. Sinha, A. Schultz, R.N. Zare: Internal state distribution of alkali dimers in supersonic nozzle beams. J. Chem. Phys. 58, 549 (1973)
S.L. Kaufman: High resolution laser spectroscopy in fast beams. Opt. Commun. 17, 309 (1976)
W.H. Wing, G.A. Ruff, W.E. Lamb, J.J. Spezeski: Observation of the infrared spectrum of the hydrogen molecular ion HD+. Phys. Rev. Lett. 36, 1488 (1976)
T. Meier, H. Hühnermann, W. Wagner: High-resolution spectroscopy on a fast beam of metastable xenon ions. Opt. Commun. 20, 397 (1977)
E.W. Otten: “Hyperfine and Isotope Shift Measurements”, in Atomic Physics, Vol. 5, ed. by R. Marrus, M. Prior, H. Shugart (Plenum Press, New York 1977) p. 239
B.A. Huber, T.M. Miller, P.C. Cosby, H.D. Zeman, R.L. Leon, J.T. Moseley, J.R. Peterson: Laser-ion-coaxial beams spectrometer. Rev. Sci. Instrum. 48, 1306 (1977)
M. Dufay, M.L. Gaillard: “High Resolution Studies in Fast Ion Beams”, in Ref .1.11a , p.231
R. Neugart, S.L. Kaufman, W. Klempt, G. Moruzzi: “High Resolution Spectroscopy in Fast Atomic Beams”, in Ref.1.11a, p.446
K. Bergmann, U. Hefter, P. Hering: Molecular beam diagnostics with internal state selection. Chem. Phys. 32, 329 (1978);
K. Bergmann, U. Hefter, P. Hering: Molecular beam diagnostics with internal state selection. J. Chem. Phys. 65, 488 (1976)
K. Bergmann, U. Hefter, P. Hering: Molecular beam diagnostics with internal state selection: Velocity distribution and dimer formation in a supersonic Na/Na2-beam. Chem. Phys. 32, 329 (1978)
K. Bergmann, R. Engelhardt, U. Hefter, P. Hering: Molecular beam diagnostics with internal state selection II: Intensity distribution of a Na/Na2 supersonic beam. Chem. Phys. 44. 23 (1979)
M.E. Kaminsky, R.T. Hawkins, F.V. Kowalski, L.A. Schawlow: Identification of absorption lines by modulated lower level population: Spectrum of Na2. Phys. Rev. Lett. 36, 671 (1976)
W. Demtröder, D. Eisel, H.J. Foth, G. Höning, M. Raab, H.J. Vedder, D. Zevgolis: Sub-doppler laser spectroscopy of small molecules. J. Mol. Structure 59, 291 (1980)
N.F. Ramsay: Molecular Beams (Oxford Univ. Press, New York 1956)
J.C. Zorn, T.C. English: Molecular beam electric resonance spectroscopy. Adv.At. Mol. Phys. 9, 243 (1973)
W. Ertmer, B Hofer: . hyperfine structure measurements of the metastable states 3d2 4s 4 F 3/2 9/2of 45Sc using laser-fluorescenceatomic beam magnetic resonance echnique. Z. Phys. A 276, 9 (1976)
S.D. Rosner, R.A. Holt, T.D. Gaily: Measurement of the zero field by perfine structure of a single vibrational-rotational level of Na2 by a laser-fluorescence molecular beam resonance technique. Phys. Rev. Lett. 35, 785 (1975)
J. Pembczynski, W. Ertmer, U. Johann, S. Penselin, P. Stinner : Measurement of the hyperfine structure of metastable atomic states of Mn using the ABMR-LIRF method. Z. Physik A291, 207 (1979) ;
J. Pembczynski, W. Ertmer, U. Johann, S. Penselin, P. Stinner : Measurement of the hyperfine structure of metastable atomic states of Mn using the ABMR-LIRF method. Z. Physik A294, 313 (1980)
M. Dubke, W. Jitschin, G. Meisel’, W.J. Childs: Laser-RF-double resonance measurement of the quadrupole moments of 95Mo and 97Mo. Phys. Lett. 65A, 109 (1978)
W. Zeiske, G. Meisel, H. Gebauer, B. Hofer, W. Ertmer: Hyperfine structure of cw dye laser populated high lying levels of 45Sc by atomicbeam magnetic-resonance. Phys. Lett. 55A, 405 (1976)
P. Grundevik, M. Gustayson, I. Lindgren, G. Olson, L. Robertsson, A. Rosén, S. Svanberg: Precision method for hyperfine-structure studies in low-abundance isotopes. Phys. Rev. Lett. 42, 1528 (1979)
W.R Bennet, Jr.: Hole-burning effects in a He-Ne-optical maser. Phys. Rev. 126, 580 (1962)
W.E. Lamb: Theory of an optical maser. Phys. Rev. 134A, 1429 (1964)
A. Szöke, A. Javan: Isotope shift and saturation behavior of the 1.15 — μ transition of Ne. Phys. Rev. Lett. 10, 521 (1963)
T.W. Hänsch, M.H. Nayfeh, S.A. Lee, S.M. Curry, I.S. Shahin: Precision measurement of the Rydberg constant by laser saturation spectroscopy of the Balmer α-line in hydrogen and deuterium. Phys. Rev. Lett. 32, 1336 (1974)
T.W. Hänsch, A.L. Schawlow, G.W. Series: The spectrum of atomic hydrogen. Scient. Am. 240, 94 (March 1979)
H. Gerhardt, E. Matthias, F. Schneider, A. Timmermann: Isotope shifts and hyperfine structure of the 6s–7p-transitions in the cesium isotopes 133, 135 and 137. Z. Phys. A 288, 327 (1978)
M.S. Sorem, A.L. Schawlow: Saturation spectroscopy in molecular iodine by intermodulated fluorescence. Opt. Commun. 5, 148 (1972)
H.J. Foth: “Sättigungsspektroskopie an Molekülen”; Diplomthesis, Kaiserslautern (1976)
M.D. Levenson, A.L. Schawlow: Hyperfine interactions in molecular iodine. Phys. Rev. A6, 10 (1972)
R.S. Lowe, H. Gerhardt, W. Dillenschneider, R.F. Curl, Jr., F.K. Tittel: Intermodulated fluorescence spectroscopy of B02 using a stabilized dye laser. J. Chem. Phys. 70, 42 (1979)
H.J. Foth, F. Spieweck: Hyperfine structure of the R(98), (58–1)-line of I2 at λ=514.5 nm. Chem. Phys. Lett. 65, 347 (1979)
10.37b M. Broyer, J. Vigué, J.C. Lehmann: Effective hyperfine Hamiltonian in homonuclear diatomic molecules. J. Phys. 39, 591 (1978)
J.L. Hall: “Sub-Doppler Spectroscopy, Methane Hyperfine Spectroscopy and the Ultimate Resolution Limits”, in Ref. 1.7, p. 105
S.N. Bagayev, E.V. Baklanov, E. Titov, V.P. Chebotayev: Reproducibility of the frequency of an He-Ne-laser with a methane absorbing cell. JETP Lett. 20, 130 (1974)
J.C. Hall, J.A. Magyar: “High Resolution Saturated Absorption Studies of Methane and Some Methyl-Halides”, in Ref. 1.13, p. 173
W.G. Schweitzer, E.G. Kessler, R.D. Deslattes, H.P. Layer, J.R. Whetstone: Description, performance and wavelength of iodine stabilised lasers. Appl. Opt. 12, 2927 (1973)
J.L. Hall: “Saturated Absorption Spectroscopy”, in Atomic Physics, Vol. 3, ed. by St. Smith, G.K. Walters (Plenum Press, New York 1973) p. 615 ff
V.S. Letokhov, V.P. Chebotayer: Quantum optical frequency standards. Sov. Phys. J. Quantum Electron. 4, 137 (1974)
J.L. Hall: The laser absolute wavelength standard problem. IEEE J. QE-4, 638 (1968)
R.L. Barger, J.B. West, T.C. English: Frequency stabilization of a cw dye laser. Appl. Phys. Lett. 27, 31 (1975)
J.C. Bergquist, R.L. Barger, D.J. Glaze: “High Resolution Spectroscopy of Calcium Atoms”, in Ref. 1.11b, p. 120
R.G. Brewer: Precision determination of CH3F-dipole moment by nonlinear infrared spectroscopy. Phys. Rev. Lett. 25, 1639 (1970)
G. Hermann, A. Scharman: Resonance effects in the output of a He-Nelaser with an axial magnetic field. Phys. Lett. 24A, 606 (1967);
G. Hermann, A. Scharman: Resonance effects in the output of a He-Nelaser with an axial magnetic field. Z. Phys. 254, 46 (1972)
M.S. Feld: “Laser Saturated Spectroscopy in Coupled Doppler-Broadened Transitions”, in Ref. 1.6, pp. 369–420
P. Toschek: “General Survey of Laser Saturated Spectroscopy”, in Ref. 1.7, pp. 13–28
A. Schabert, R. Keil, P.E. Toschek: Dynamic Stark effect of an optical line observed by cross-saturated absorption. Appl. Phys. 6, 181 (1975)
I.M. Beterov, V.P. Chebotayev: “Three Level Systems and Their Interaction with Radiation”, in Progress in Quantum Electronics, Vol. 3 (Pergamon Press 1974)
M. Sargent, III, P. Toschek, H.G. Danielsmeyer: Unidirectional saturation spectroscopy. Appl. Phys. 11, 55 (1976)
V.S. Letokhov, V.P. Chebotayev: Nonlinear Laser Spectroscopy, Springer Series in Optical Sciences, Vol. 4, ed. by D.L. MacAdam (Springer, Berlin, Heidelberg, New York 1977)
N. Bloembergen (ed.): Nonlinear Spectroscopy, Proc. Intern. School Enrico Fermi, Course LXIV, Varenna 1977 (North-Holland, Amsterdam 1977)
J.L. Hall: “The Lineshape Problem in Laser-Saturated Molecular Absorption”, in Lectures on Theoretical Physics, Boulder Summer School (Gordon and Breach, New York 1975)
R. Balian, S. Haroche, S. Liebermann (eds.): Frontiers in Laser Spec— troscopy (North-Holland, Amsterdam 1977)
C. Wieman, Th.W. Hänsch: Doppler-free laser polarization spectroscopy. Phys. Rev. Lett. 36, 1170 (1976)
V. Stert, R. Fischer: Doppler-free polarization spectroscopy using linear polarized light. Appl. Phys. 17, 151 (1978)
H. Gerhardt, T. Huhle, J. Neukammer, P.J. West: High resolution polarization spectroscopy of the 557 nm transition of Kr I. Opt. Commun. 26, 58 (1978)
M. Raab, G. Höning, R. Castell, W. Demtröder: Doppl r-free polarization spectroscopy of the Cs molecule at x = 6270 Å . Chem. Phys. p py 2 Lett. 66, 307 (1979)
R.E. Teets, F.V. Kowalski, W.T. Hill, N. Carlson, T.W. Hänsch: “Laser Polarization Spectroscopy”, in Advances in Laser Spectroscopy, Proc. Soc. Phot. Opt. Instr. Eng., Vol. 113, San Diego (1977) p. 80
M.E. Rose: Elementary Theory of Angular Momentum (Wiley, New York 1957)
B. Judd: Angular Momentum Theory for Diatomic Molecules (Academic Press, New York 1975)
M. Raab, G. Höning, W. Demtröder, C.R. Vidal: High resolution studies of the Cs2-molecule. Chem. Phys. (in preparation)
R. Castell, K. Wickert, W. Demtröder: Polarization spectroscopy of I2 with accurate absolute wavelength measurements using a wavemeter. Opt. Commun. (in preparation)
R. Teets, R. Feinberg, T.W. Hänsch, A.L. Schawlow: Simplification of spectra by polarization labeling. Phys. Rev. Lett. 37, 683 (1976)
N.W. Carlson, A.J. Taylor, A.L. Schawlow: Identification of Rydberg states in Na2 by two-step polarization labeling. Phys. Rev. Lett. 45, 18 (1980)
C. Delsart, J.C. Keller: “Doppler-Free Laser Induced Dichroism and Birefringence”, in Ref. 1.11, p. 154
F.V. Kowalski, W.T. Hill, A.L. Schawlow: Saturated-interference spectroscopy. Opt. Lett. 2, 112 (1978)
R. Schieder: Interferometric nonlinear spectroscopy. Opt. Commun. 26, 113 (1978)
T.J. Bridge, T.K. Chang: Accurate rotational constants of CO2 from measurements of cw beats in bulk GaAs between CO2 vibrational-rotational laser lines. Phys. Rev. Lett. 22, 811 (1969)
F.R. Petersen, D.G. McDonald, F.D. Cupp, B.L. Danielson: Rotational 1 constants for 12C1602 from beats between Lamb-dip stabilized laser lines. Phys. Rev. Lett. 31, 573 (1973); in Ref. 1.8, p. 555 C. Freed, D.L. Spears, R.G. O’Donnell: “Precision Heterodyne Calibration”, in Ref. 1.8, p. 171
L.A. Hackel, K.H. Casleton, S.G. Kukolich, S. Ezekiel: Observation of magnetic octupole and scalar spin-spin interactions in I2 using laser spectroscopy. Phys. Rev. Lett. 35, 568 (1975)
F. Spiewek: “Wavelength Stabilisation of the Ar+-Laser line at λ = 515 nm for length Measurements of Highest Precision”, in Laser 77 OptoElectronics, ed. by W. Waidelich (ipc, science and technology press, Guildford, England 1977)
A.L. Betz, E.C. Sutton, R.A. McLaren: “Infrared Heterodyne Spectroscopy in Astronomy”, in Ref. 1.11, p. 31
Y.R. Shen (ed.): Nonlinear Infrared Generation, Topics in Applied Physics, Vol. 16 (Springer, Berlin, Heidelberg, New York 1977)
N. Bloembergen, M.D. Levenson: “Doppler-Free Two Photon Absorption Spectroscopy”, in Ref. 1.13, p. 315
J.M. Worlock: “Two Photon Spectroscopy”, in Laser Handbook, ed. by F.T. Arrecchi, E.O. Schulz-Dubois (North-Holland, Amsterdam 1972)
B. Cagnac, G. Grynberg, F. Biraben: Spectroscopie d’absorption multiphotonique sans effet Doppler. J. Phys. 34, 845 (1973)
G. Grynberg, B. Cagnac: Doppler-free multiphoton spectroscopy. Rep. Prog. Phys. 40, 791–841 (1977)
F. Biraben, B. Cagnac, G. Grynberg: Experimental evidence of two photon transition without Doppler broadening. Phys. Rev. Lett. 32, 643 (1974)
G. Grynberg, B. Cagnac, F. Biraben: “Multiphoton Resonant Processes in Atoms”, in Coherent Nonlinear Optics, ed. by M.S. Feld , V.S. Letokhov (Springer, Berlin, Heidelberg, New York 1980)
T.W. Hänsch, K. Harvey, G. Meisel, A.L. Schawlow: Two photon spectroscopy of Na 3s -4d without Doppler-broadening using cw dye laser. Opt. Commun. 11, 50 (1974)
M.D. Levenson, N. Bloembergen: Observation of two-photon absorption without Doppler-broadening on the 3s -5s transition in sodium vapor. Phys. Rev. Lett. 32, 645 (1974)
S.A. Lee, J. Helmcke, J.L. Hall, P. Stoicheff: Doppler-free two photon transitions to Rydberg levels. Opt. Lett. 3, 141 (1978)
T.W. Hänsch, S.A. Lee, R. Wallenstein, C. Wieman: Doppler-free twophoton spectroscopy of hydrogen 1S -2S. Phys. Rev. Lett. 34, 307 (1975)
A.I. Ferguson, J.E.M. Goldsmith, T.W. Hänsch, E.W. Weber: “High Resolution Spectroscopy of Atomic Hydrogen”, in Ref .1.13b, p.31
F.H.M. Faisal, R. Wallenstein, H. Zacharias: Three-photon excitation of xenon and carbon-monoxide. Phys. Rev. Lett. 39, 1138 (1977)
P. Bräunlich: “Multiphoton Spectroscopy”, in Progress in Atomic Spectroscopy; Part B, ed. by W. Hanle, H. Kleinpoppen (Plenum Press, New York 1978) p. 777
J.H. Eberly (ed.): Multiphoton Processes (Wiley, New York 1978)
P. Franken: Interference effects in the resonance fluorescence of “crossed” excited states. Phys. Rev. 121, 508 (1961)
R.W. Field, T.H. Bergeman: Radio-frequency spectroscopy and perturbation analysis in CS Al (v =0). J. Chem. Phys. 54, 2936 (1971)
W. Hanle: Über magnetische Beeinflussung der Polarisation der Resonanzfluoreszenz. Z. Phys. 30, 93 (1924)
M. McClintock, W. Demtröder, R.N. Zare: Level crossing studies of Na2 using laser induced fluorescence. J. Chem. Phys. 51, 5509 (1969)
R.N. Zare: Molecular level crossing spectroscopy. J. Chem. Phys. 45, 4510 (1966)
R.N. Zare: Interference effects in molecular fluorescence. Acc. Chem. Res. 4, 361 (1971)
F.W. Dalby, M. Broyer, J.C. Lehmann: “Electric Field Level Crossing in Molecular Iodine”, in Ref. 1.7, p. 226
J.C. Lehmann: “Probing Small Molecular with Lasers”, in Frontiers in Laser Spectroscopy, Vol. I, ed. by R. Balian, S. Haroche, S. Liberman (North-Holland, Amsterdam 1977)
M. Broyer, J.C. Lehmann, J. Vigue: g-factors and lifetimes in the B-state of molecular iodine. J. Phys. 36, 235 (1975)
H. Figger, D.L. Monts, R.N. Zare: Anomalous magnetic depolarization of fluorescence from the NO2 B2-state. J. Mol. Spectrosc. 68, 388 (1977);
J.R. Bonilla, W. Demtröder: Level crossing spectroscopy of NO2 using Doppler reduced laser excitation in molecular beams. Chem. Phys. Lett. 53, 223 (1978)
S. Svanberg: “Measurement and Calculation of Excited Alkali Hyperfine and Stark Parameters”, in Ref .1.11a , p.183
H. Figger, H. Walther: Optical resolution beyond the natural linewidth: A level crossing experiment on the 3 2P3/2-level of sodium using a tunable dye laser. Z. Phys. 267, 1 (1974)
M.S. Feld, A. Sanchez, A. Javan: “Theory of Stimulated Level Crossing”, in Ref. 1.7, p. 87
A.C. Luntz, R.G. Brewer: Zeeman-tuned level crossing in 1Σ CH4. J. Chem. Phys. 53, 3380 (1970)
A.C. Luntz, R.G. Brewer, K.L. Foster, J.D. Swalen: Level crossing in CH observed by nonlinear absorption. Phys. Rev. Lett. 23, 951 (1969)
J.S. Levine, P. Boncyk, A. Javan: Observation of hyperfine level crossing in stimulated emission. Phys. Rev. Lett. 22, 267 (1969)
G. Hermann, A. Scharmann: Untersuchungen zur Zeeman-Spektroskopie mit Hilfe nichtlinearer Resonanzen eines Multimoden Lasers. Z. Phys. 254, 46 (1972)
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Demtröder, W. (1981). High-Resolution Sub-Doppler Laser Spectroscopy. In: Laser Spectroscopy. Springer Series in Chemical Physics, vol 5. Springer, Berlin, Heidelberg. https://doi.org/10.1007/978-3-662-08257-7_10
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