Research Description and Publications

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1 Research Description and Publications Prof. A. Marjatta Lyyra August 29, 2011 Prof. Marjatta Lyyra s research in Atomic, Molecular and Optical Physics involves 1. Studies of Predissociation Dynamics 2. State-selected Photodissociation Dynamics Studies 3. Molecular Quantum Optics with applications of the Autler-Townes effect: A) to control angular momentum alignment B) to measure the absolute magnitude of the transition dipole matrix elements to probe the electronic transition dipole moment and its internuclear distance dependence C) to control the spin-orbit interaction and the mixing coefficients of a pair of singlet-triplet states D) to control predissociation dynamics 4. High Resolution Multiple Resonance Laser Spetroscopic Studies of the Structure of Small Molecules 1. Predissociation Dynamics Molecule formation through inverse predissociation in interstellar clouds and column densities of molecules were the focus of Prof. Lyyra s Ph.D. Thesis research in Stockholm, Sweden (Stockholm, 1979). Molecular lifetime measurements were used to determine predissociation rates and molecular oscillator strengths with this goal in mind. 2. State-selected Photodissociation Dynamics Studies During her postdoctoral research period Prof. Lyyra collaborated on applications of high resolution laser spectroscopy in photodissociation dynamics (Phys. Rev. Letters. 54, 2003 (1985), Phys. Rev. Lett. 61, 1485 (1988)) including state-selected photodissociation (J. Phys. Chem., 95, 8040 (1991). It was for the purpose of achieving a high level of state selectivity in these experiments that she co-pioneered high-resolution continuous wave triple resonance spectroscopy (Phys. Rev. Lett. 66, 2724 (1991)) in collaboration with the research group of Profs. William C. Stwalley and Paul D. Kleiber at the University of Iowa. 3. Molecular Quantum Optics with applications of the Autler-Townes effect: 1

2 More recently Prof. Lyyra s group at Temple University has used multi-level coherently driven double (three level), triple (four level: Phys. Rev. Lett. 66, (1991) and quadruple resonance (five level: Phys. Rev. A. 79, (2009)) laser excitation schemes to develop novel applications of coherence and quantum interference effects such as Electromagnetically Induced Transparency (EIT) and the Autler-Townes (AT) splitting in open molecular systems. Molecular systems offer opportunities for a rich variety of excitation schemes, but present also serious challenges. They are much more complex in terms of their energy level structure and relaxation mechanisms than atomic systems. Each molecular electronic state consists of a multitude of rovibrational levels. Because each excited rovibrational level is coupled to a number of lower lying rovibrational levels in other electronic states by spontaneous decay or other relaxation mechanisms, the system is unavoidably open. In contrast to an open system, a system is closed if the excitation and decay mechanisms do not involve energy levels beyond those that are needed for the observation of the coherence effect. In this sense, atoms are examples of closed systems. These differences between open and closed systems required also modifications in the closed system theoretical models in order to predict and simulate experimental results as shown in Prof. Lyyra s group s research. Molecular transition moments are also much smaller than atomic ones. Furthermore, due to their dense energy level structure, high spectral resolution is required in studies of molecular coherence effects. This further complicates the situation, since the cw lasers required for the high resolution, provide weaker electric field amplitudes. Thus the resulting Rabi frequencies Ω~ µe/ħ are smaller. Here µ is the electronic transition dipole moment matrix element and E the laser electric field amplitude. An additional difficulty has been also that molecular Rabi frequencies are small compared to the residual Doppler broadening. For all these reasons the emergence of applications of quantum optics in molecular systems was delayed compared to that of atoms. However, as the work of Prof. Lyyra s group has shown, multiple resonance excitation schemes enabled these experiments in Doppler broadened systems without the parasitic losses of population due to multi-photon ionization with pulsed lasers. In these experiments the velocity group selection by the first resonant laser excitation step results in sub-doppler resolution for the subsequent excitations (E. H. Ahmed et al. Physical Review A 76, , 2007). Therefore, modest Rabi frequencies in the range of a few hundred MHz with the correct laser excitation geometry are sufficient to overcome both the residual Doppler broadening and the inherent weakness of molecular transition dipole moment matrix elements in the molecular Rabi frequency. Using these techniques Prof. Lyyra s group, in collaboration with Prof. Lorenzo Narducci at Drexel University and Prof. Frank Spano at Temple University, has shown that the Autler- Townes effect can be used to control molecular angular momentum alignment (Phys. Rev. Lett. 83, 288 (1999)). In addition, the Autler-Townes effect was used to develop a frequency domain quantum control scheme to control quantum state singlet-triplet character. This work has been done in collaboration with Prof. F. C. Spano of the Chemistry Department at Temple University (T. Kirova and F. C. Spano, Phys. Rev. A, 71, , 2005). Prof. Lyyra s group has developed a frequency domain quantum control scheme to control spin-orbit interaction, i.e.to control the mixing coefficients of a pair of singlet and triplet rovibronic levels. This work has been submitted for publication. Their demonstration of frequency domain control of predissociation dynamics is in progress. 2

3 Prof. Lyyra s group has also demonstrated that the Autler-Townes effect can be used as a precision probe of the molecular electronic transition dipole moment (Phys. Rev. Lett, 88, (2002), J.Chem. Phys 124, , (2006)) and its internuclear distance dependence (Na 2 A 1 Σ u - X 1 Σ g system: Phys. Rev. A 77, , 2008, and Li 2 A 1 Σ u - X 1 Σ g system J. Chem. Phys., 129, , 2008). In this case an accurate measurement of the coupling laser E field amplitude together with the simulation of the Autler-Townes split line shape play a key role. Such accurate measurements of the electronic transition dipole moment matrix element, a key parameter in the Einstein A coefficient, will be of broad interest in a multitude of applications. One of the reasons for this is that these measurements avoid some of the systematic problems associated with lifetime and calibrated intensity measurements, which have been traditionally used to extract information about the electronic transition dipole moment experimentally. The lifetime measurements suffer from the contributions of multiple electronic transition moments in the radiative decay of any molecular excited rovibronic level to a number of similar levels of several lower lying electronic states. On the other hand, the calibrated intensity measurements of a number of spectral lines of an electronic transition avoids this complication, but yields only a relative transition dipole moment. In collaboration with Prof. J. Huennekens (Lehigh University), Prof. Lyyra s group has demonstrated that by combining the Autler-Townes splitting based measurements with calibrated intensity measurements; a relative transition dipole moment can be normalized to an absolute scale (the 3 1 П 1(X) 1 Σ and 3 1 П 2(A) 1 Σ Transitions of NaK: J. Chem. Phys. 129, Article No , 2008). Thus, the combination of these two methods extends the range of the Autler-Townes splitting based measurements to much weaker transitions. In an ongoing collaboration with theorists engaged in state-of the-art ab initio calculations (Profs. Svetlana Kotochigova, Temple University, and Sylvie Magnier, Rennes, France, Gwang-Hi Jeung, France), Prof. Lyyra s group has shown very good agreement between experimental data and theoretical calculations for the lightest molecule with a core, the Lithium dimer, as expected. Thus, we expect that experiment will provide a critical test for ab initio calculations also in the future. 4. High Resolution Multiple Resonance Laser Spetroscopic Studies of the Structure of Small Molecules Prof. Lyyra s group s ongoing work on alkali dimer molecular structure includes a global deperturbation analysis of the A 1 Σ u and b 3 Π u states coupled by the spin-orbit interaction. This work has resulted in a full characterization of the rovibrational levels in terms of their percentage of singlet and triplet character as well as their experimentally determined term values in these perturbed states. This work has been done in collaboration with Prof. Tom Bergeman (Stony Brook), Prof. Li Li and Dr. Feng Xie (Tsinghua University), Prof. Svetlana Kotochigova (Temple University), Prof. Sylvie Magnier (Lille, France), Prof. V.B. Sovkov and Prof. V. S. Ivanov (St. Petersburg), Prof.John Huennekens (Lehigh University) and Dr. Amanda Ross (Lyon) among others. This research is of special relevance to research on cold molecule formation and diagnostics. The results of this collaboration have been published: 1. for K 2 J. Chem. Phys., 117 (20): , (2002) 2. for Na 2 J. Chem. Phys., 127, Article No ,pp. 1-17, (2007) 3. for Rb 2, Phys. Rev. A 80, , (2009), and 4. for Cs 2, Phys. Rev. A 83, (2011). 3

4 Publications by Prof. Marjatta Lyyra [Citations as of June indicated in brackets after the year of publication. An overview is available at the end of the publication list] INVITED REVIEW ARTICLES AND BOOK CHAPTERS: 1. A. M. Lyyra, P. D. Kleiber and W. C. Stwalley, "All-Optical Triple Resonance: Spectroscopy and State-Selected Photodissociation Dynamics", in Molecular Dynamics and Spectroscopy by Stimulated Emission Pumping, H. -L. Dai and R. W. Field eds., Advances in Physical Chemistry (World Scientific Publishing), pp , (1995)[7]. 2 L. Li and A. M. Lyyra, "Triplet States of Na 2 and Li 2 : Perturbation Facilitated Optical- Optical Double Resonance Spectroscopy", Spectrochimica Acta Part A 55, (1999) [46]. 3. A. M. Lyyra, F. C. Spano, J. Qi and T. Kirova,"Prospects for All-Optical Alignment and Quantum State Control of Nonpolar Molecules", ACS Symposium Series Volume 821 on Laser Control and Manipulation of Molecules, pp , June REFEREED PAPERS: 1. J. Brzozowski, N. Elander, P. Erman and M. Lyyra, "On the Interstellar Abundance of the CH Radical", Astrophys. J 193, (1974). [30] 2. J. Brzozowski, N. Elander, P. Erman and M. Lyyra, "Lifetimes of the Excited Levels in Some Important Ion-Molecules", Physics Scripta 10, (1974). [30] 3. P. Erman, M. Lyyra and I. Martinson, "High Resolution Measurements of the z 5 F 0 and y 5 F 0 Lifetimes in Neutral Iron", Phys. Lett., 49A, (1974). [13] 4. M. Lyyra, J. Rasanen and F. Stenman, "Raman Scattering from Pyrene", Physica Fennica 10, (1975). [4] 5. J. Brzozowski, P. Erman, M. Lyyra and W. M. Hayden-Smith, "Radiative Lifetimes of Resonance Levels in FeI and FeII", Physica Scripta 14, (1976). [19] 6. J. Brzozowski, P. Erman and M. Lyyra, "Predissociation Rates and Perturbations of the A, B, B', C, D and F States in NO Studied Using Time Resolved Spectroscopy", Physics Scripta 14, (1976). [66] 7. J. Brzozowski, P. Erman and M. Lyyra, "Precision Estimates of the Predissociation Rates of the OH A 2 Σ State (v 2)", Physics Scripta 17, (1978). [102] 8. O. Appelblad, A. Lagerqvist and M. Lyyra, "The Spectrum of Cu0: Rotational Analysis of a 4 Σ 1/2 2 Π 1/2 Transition", Physics Scripta 18, (1978). [11] 9. O. Appelblad, A. Lagerqvist and M. Lyyra, "The Spectrum of Cu0: Rotational Analysis of a band at 4182 Å", Physica Scripta 20, (1979). [6] 4

5 10. M. Lyyra and P. R. Bunker, "The Potential Energy Curve of the B 1 Π u State of Na 2 ", Chem.Phys Lett. 61, (1979). [9]. 11. T. A. Carlson, J. Copley, N. Duric, N. Elander, P. Erman, M. Larson and M. Lyyra, "The Oscillator Strengths and the Dissociation Energy of SiH as Determined from Time Resolved Precision Spectroscopy", Astronomy and Astrophysics 83, (1980). [36] 12. A. S.-C. Cheung, R. C. Hansen, A. M. Lyyra and A. J. Merer, "A Novel Electronic- Hyperfine Perturbation in the C 4 Σ - State of VO", J. Mol. Spectrosc. 86, (1981). [12] 13. A. S.-C. Cheung, N. Lee, A. M. Lyyra, A. J. Merer and A. W. Taylor, "Spectroscopic Properties of the 5 i Ground State of Fe0", J. Mol. Spectrosc. 95, (1982). [52] 14. A. S.-C. Cheung, A. M. Lyyra, A. J. Merer and A. W. Taylor, "Laser Spectroscopy of FeO: Rotational Analysis of Some Sub-Bands of the Orange System", J. Mol. Spectrosc, 102, (1983). [38] 15. P. D. Kleiber, A. M. Lyyra, S. P. Heneghan and W. C. Stwalley, "Stimulated Emission in Laser Pumped Magnesium Vapor", J. Opt. Soc. Am. B 2, (1985). [7] 16. P. D. Kleiber, A. M. Lyyra, K. M. Sando, S. P. Heneghan and W. C. Stwalley, "Far Wing Absorption Profiles of a Reactive Collision Mg H 2 ", Phys. Rev. Letters. 54, (1985). [73] 17. P. D. Kleiber, A. M. Lyyra, K. M. Sando, V. Zafiropulos and W. C. Stwalley, "Reactive Collision Dynamics by Far Wing Laser Scattering: Mg H 2 ", J. Chem. Phys. 85, (1986). [93] 18. A. M. Lyyra, K. M. Sando and P. D. Kleiber, "Comparison of the Collisional Redistribution Profiles for MgHe and MgH 2, ys. Rev. A. 35, (1987). [3] 19. W. T. Luh, K. M. Sando, A. M. Lyyra and W. C. Stwalley, "Free-Bound-Free Resonance Fluorescence in the K 2 Yellow Diffuse Band: Theory and Experiment", Chem. Phys. Lett. 144, (1988). [15] 20. W. T. Luh, J. T. Bahns, A. M. Lyyra, K. M. Sando, P. D. Kleiber and W. C. Stwalley, "Direct Excitation Studies of the Diffuse Bands of Alkali Metal Dimers", J. Chem. Phys. 88, (1988). [29] 21. W. T. Luh, P. D. Kleiber, A. M. Lyyra, W. C. Stwalley and K. C. Lin, "Laser-Induced Fluorescence of the B 1 Π - X 1 Σ Band System of the Isotopic Lithium Hydrides", J. Mol. Spectrosc., 129, (1988)[8]. 22. V. Zafiropulos, P. D. Kleiber, K. M. Sando, X. Zeng, A. M. Lyyra and W. C. Stwalley, "Energy Dependent Photodissociation Dynamics Probed by Fluorescence Polarization", Phys. Rev. Lett. 61, (1988)[22] 5

6 23. L. Li, A. M. Lyyra and W. C. Stwalley, "Absolute Vibrational Numbering and Molecular Constants for the Na g State", J. Mol. Spectrosc. 134, (1989). [15] 24. X. Xie, R. W. Field, L. Li, A. M. Lyyra, J. T. Bahns and W. C. Stwalley, "The Absolute Vibrational Numbering and Molecular Constants of the Na Π g State", J. Mol. Spectrosc. 134, (1989). [21] 25. G. Pichler, A. M. Lyyra, P. D. Kleiber, W. C. Stwalley, R. Hammer, K. M. Sando and H. H. Michels, "Laser-Induced Chemiluminescence of the LiMg Excimer", Chem. Phys. Lett. 156, (1989)[11]. 26. H. Wang, L. Li, A. M. Lyyra and W. C. Stwalley, "CW Optical-Optical Double Resonance Excitations of 39 K 2 Rydberg States", J. Mol. Spectrosc, 137, (1989). [20] 27. A. M. Lyyra, W. T. Luh, L. Li, H. Wang and W. C. Stwalley, "The A 1 Σ u State of the Potassium Dimer", J. Chem. Phys., 92, (1990). [25] 28. M. Masters, J. Huennekens, W. T. Luh, L. Li, A. M. Lyyra, K. Sando, V. Zafiropulos, W. C. Stwalley, "Bound-Free 1 3 Π 1 3 Σ Emission from the NaK Molecule: Determination of the 1 3 Σ Repulsive Wall Above the Dissociation Limit", J. Chem. Phys. 92, (1990). [24] 29. L. Li, A. M. Lyyra, W. T. Luh and W. C. Stwalley, "Observation of the 39 K 2 a 3 Σ u State by Perturbation Facilitated Optical-Optical Double Resonance (PFOODR) Resolved Fluorescence Spectroscopy", J. Chem. Phys. 93, (1990)[71]. 30. W. C. Stwalley, P. D. Kleiber, K. M. Sando, A. M. Lyyra, L. Li, S. Ananthamurthy, S. Bililign, H. Wang, J. Wang, and V. Zafiropulos, "Metal-Metal, Metal-Rare Gas and Metal-Hydrogen Reactive Transition States", Faraday Discussions of the Chemical Society No. 91, (1991). [2] 31. T.-J. Whang, H. Wang, A. M. Lyyra, L. Li and W. C. Stwalley, "Optical-Optical Double Resonance Spectroscopy of the Na Π g State", J. Mol. Spectrosc. 145, (1991). [32] 32. L. Li, A. M. Lyyra, W. C. Stwalley, M. Li and R. W. Field, "The Na Σ g ~ 2 3 Π g ~ 1 3 g Triple Perturbation: Deperturbation of the (v Σ, v Π, v ) = (6, 2, 7) and (7, 3, 8) Interactions", J. Mol. Spectrosc. 147, (1991). [14] 33. L. Li, A. M. Lyyra, H. Wang and W. C. Stwalley, "Highly State-Selective Collisional Energy Transfer Between 1 g and 1 Σ g Rydberg States in K 2 ", Chem. Phys. Lett. 179, (1991). [10] 34. H. Wang, T. J. Wang, A. M. Lyyra and W. C. Stwalley, "Study of the 4 1 Σ g State of Na 2 by Optical-Optical Double Resonance Spectroscopy", J. Chem. Phys. 94, (1991). [32] 35. A. M. Lyyra, H. Wang, T.-J. Whang, L. Li and W. C. Stwalley, "CW All-Optical Triple Resonance (AOTR) Spectroscopy", Phys. Rev. Lett. 66, (1991). [47] 6

7 36. Jiaxiang Wang, He Wang, P. D. Kleiber, A. M. Lyyra and W. C. Stwalley, "State- Selected Photodissociation of the B 1 Π u State of K 2 by All-Optical Triple Resonance Spectroscopy", Journal of Physical Chemistry, 95, (1991). [9] 37. T. -J. Whang, A. M. Lyyra, W. C. Stwalley and L. Li, "The Na g State: CW Perturbation Facilitated Optical-Optical Double Resonance Spectroscopy", J. Mol. Spectrosc., 149, (1991). [18] 38. L. Li, T. An. T. -J. Whang, A. M. Lyyra, W. C. Stwalley, R. W. Field and R. A. Bernheim, "Hyperfine Splitting of the 1 3 g Triplet Rydber State of Li 2 ", J.Chem. Phys. 96, (1992). [31] 39. H. Wang, W. C. Stwalley and A. M. Lyyra, "Assignment of Diabatic and Adiabatic Atomic Asymptotic Limits of K 2 Rydberg States J. Chem. Phys. 96, (1992). [15] 40. G. Jong, H. Wang, C-C. Tsai, W. C. Stwalley and A. M. Lyyra "The Study of the 39 K 2 Rydberg 1 g States by CW Optical-Optical Double Resonance Spectroscopy", J. Mol. Spectrosc., 154, (1992). [14] 41. T.-J. Whang, W. C. Stwalley, L. Li and A. M. Lyyra, "Observations of the 3(3d) 3 Σ g State of Na 2 ", J. Mol. Spectrosc. 155, (1992). [26] 42. G. Jong, L. Li, T. J. Whang, W. C. Stwalley, A. M. Lyyra, M. Li and J. A. Coxon, "CW All-Optical Triple Resonance Spectroscopy of K 2 : Deperturbation analysis of the A 1 Σ u (v 12) and b 3 Π u (13 v 24) States, Mol. Spectrosc. 155, (1992). [43] 43. T.-J. Whang, A. M. Lyyra, W. C. Stwalley and L. Li, " CW Perturbation-Facilitated Triple Resonance Spectroscopy of the Na 2 b 3 Π u State",J. Chem. Phys., 97, (1992). [32] 44. Li, Q. Zhu, A. M. Lyyra, T. -J. Whang, W. C. Stwalley, R. W. Field and M. H. Alexander, "Collision-Induced Transitions between A 1 Σ u and b 3 Π u States of Na 2 : The `Gateway' effect of Perturbed Levels", J. Chem. Phys., 97, (1992). [28] 45. T.-J. Whang, W. C. Stwalley, L. Li and A. M. Lyyra, "Na Σ g State", J. Mol. pectrosc. 157, (1993). [14] 46. L. N. Ding, M. A. Young, P. D. Kleiber, W. C. Stwalley and A. M. Lyyra, "Photofragmentation Spectroscopy of MgD 2, Phys. Chem, 97, (1993). [61] 47. L. Li, Q. Zhu, A. M. Lyyra, T. -J. Whang, W. C. Stwalley, R. W. Field and M. H. Alexander, "Rotational Energy Transfer in the Na 2 b 3 Π u State: Propensity Rules for Transitions between Hyperfine Components",J. Chem. Phys., 98, (1993). [13] 48. L. Li, Q. Zhu, A. M. Lyyra, T. -J. Whang, W. C. Stwalley, R. W. Field and M. H. Alexander, "Rotational Energy Transfer in the Na 2 b 3 Π u State: Propensity Rules for Rotation, Spin-Orbit Component, and e/f Parity Changing Collisions",J. Chem. Phys., 7

8 98, (1993). [10] 49. C. -C. Tsai, J. T. Bahns, T. -J. Whang, H. Wang, W. C. Stwalley and A. M. Lyyra, Optical-Optical Double Resonance Spectroscopy of the 1 Σ g Shelf States and 1 Π g States of Na 2 Using an Ultrasensitive Ionization Detector, Phys. Rev. Letters 71, (1993). [22] 50. T. -J. Whang, C. -C. Tsai, W. C. Stwalley, A. M. Lyyra and L. Li, "Spectroscopic Study of the Na Σ g State by CW Perturbation-Facilitated Optical-Optical Double Resonance Spectroscopy", J. Mol. Spectrosc., 160, (1993). [19] 51. L. N. Ding, P. D. Kleiber, M. A. Young, W. C. Stwalley and A. M. Lyyra, "Photodissociation Spectroscopy of Mg 2 (X 2 Σ u A 2 Σ g ),Phys. Rev. A., 48, (1993). [22] 52. B. Ji, A. Yiannopoulou, P. D. Kleiber, A. M. Lyyra and W. C. Stwalley, "Final State Alignment from the Quantum State-Selected Photodissociation of K 2 by All-Optical Triple Resonance Spectroscopy", Phys. Rev. A. 49, R1535-R1538 (1994). [4] 53. A. Yiannopoulou, B. Ji, L. Li, M. Li, K. Urbanski, A. M. Lyyra, W. C. Stwalley and G. - H. Jeung, "The Doubly Excited 1 3 Σ g - State of 7 Li 2 ",J. Chem. Phys. 101, (1994). [33] 54. A. Yiannopoulou, K. Urbanski, A. M. Lyyra, L. Li, B. Ji, J. T. Bahns and W. C. Stwalley, "Perturbation Facilitated Optical-Optical Double Resonance Spectroscopy of the 2 3 Σ g, 3 3 Σ g and 4 3 Σ g Rydberg states of 7 Li 2 ", J. Chem. Phys. 102, (1995). [36] 55. A. Yiannopoulou, T. Leininger, A. M. Lyyra and G. -H. Jeung, "Theoretically Synthesized Rovibronic Transition Spectra of KRb, International Journal of Quant. Chem., 57, (1996). [11] 56. B. Ji, P. D. Kleiber, W. C. Stwalley, A. Yiannopoulou, A. M. Lyyra and P. S. Julienne, "Quantum State Selected Photodissociation of K 2 (B 1 Π u X 1 Σ g ): A Case Study of Final Alignment in All-Optical Multiple Resonance Photodissociation",J. Chem. Phys., 102, (1995). [10] 57. J. T. Kim, H. Wang, C. C. Tsai, J. T. Bahns and W. C. Stwalley, G. Jong and A. M. Lyyra, "Observation of the 4 3 Σ g, 3 3 Π g, 2 3 g and b 3 Π u states of 39 K 2 by PFOODR Spectroscopy", J. Chem. Phys., 102, (1995). [28] and 103, 9891 (1995) [10] 58. A. Yiannopoulou, K. Urbanski, S. Antonova, A. M. Lyyra, L. Li, T. An, T. -J. Whang, B. Ji, X. T. Wang, W. C. Stwalley, T. Leininger and G. -H. Jeung, " The 2 3 Π g and 3 3 Π g States of 7 Li 2 : Optical-Optical Double Resonance Spectroscopy and ab initio Calculations J. Chem. Phys. 103, , (1995). [26] 59. B. Ji, C. -C. Tsai, Li Li, T. -J. Whang, A. M. Lyyra, H. Wang, J. T. Bahns, W. C. Stwalley and R. J. LeRoy, Phys. "Determination of the Long Range Potential and Dissociation Energy of the 1 3 g State of Na 2 ", J. Chem. Phys. 103, (1995). [24] 8

9 60. A. Yiannopoulou, K. Urbanski, A. M. Lyyra, Li Li, T. An, B. Ji, and W. C. Stwalley",The 1 3 g state of 7 Li 2,"J. Mol. Spectrosc. 172, (1995). [16] 61. K. Urbanski, S. Antonova, A. Yiannopoulou, A. M. Lyyra, L. Li and W. C. Stwalley, "All-Optical Triple Resonance Spectroscopy of the A 1 Σ u State of 7 Li 2 ", J. Chem. Phys. 104, (1996). [33]. See also Errata J. Chem. Phys., 116, (2002). 62. L. Li, A. Yiannopoulou, K. Urbanski, A. M. Lyyra, B. Ji, W. C. Stwalley and T. An, "Hyperfine Structures of the 7 Li 2 b 3 Π u, 2 3 Π g and 3 3 Π g States: CW PFOODR Spectroscopy", J. Chem. Phys. 105, , 1996 [27]), see also J. Chem. Phys. 106, 8626 (1997 [8]). 63. L. Li, S. Antonova, A.Yiannopoulou, K. Urbanski and A. M. Lyyra, "State-to-State Collision Energy Transfer in 7 Li 2 within high-lying Triplet States: Gateway Effect of Mixed Levels in Energy Transfer between Singlet and Triplet States", J. Chem. Phys. 105, (1996). [10] 64. G. Zhao, W. T. Zemke, J.T. Kim, B. Ji, H. Wang, J. T. Bahns, W. C. Stwalley, L. Li, A. M. Lyyra and C. Amiot, "New Measurements of the a 3 Σ u State of K 2 and Improved Analysis of Long-Range Dispersion and Exchange Interactions between two K Atoms", J. Chem. Phys. 105, (1996). [41] 65. S. Antonova, K. Urbanski, A. M. Lyyra and L. Li, "State to State Collisional Energy Transfer in Singlet States of Li 2 for Symmetry Forbidden Transitions", Chem. Phys. Letters., 267, (1997).[4] 66. K. Urbanski, S. Antonova, L. Li, A.M. Lyyra, L. Li and B. Ji, " The G 1 Π g State of 7 Li 2 Revisited: Observation and Analysis of High Vibrational Levels, J. Chem. Phys., 109, (1998). [7] 67. Y. Liu, J. Li, H. Gao, D. Chen, L. Li, R. W. Field and A. M. Lyyra, " Predissociation of the Na Π g and Other Triplet States", J. Chem. Phys. 108, (1998). [27] 68. X.J. Wang, J. Yang, J.B. Qi and A. M. Lyyra, Precise Molecular Constants for the 6 Li 2 A 1 Σ u -X 1 Σ g System by Sub Doppler Polarization Spectroscopy, J. Mol. Spectrosc., 191, (1998). [8] 69. V. S. Ivanov, V. B. Sovkov, L. Li, A. M. Lyyra, G. Lazarov and J. Huennekens, New Vibrational Numbering and Potential Energy Curve for the 3 3 Π g Electronic State of the Li 2 Molecule, J. Mol. Spectrosc. 194, (1999). [23] 70. S. Antonova, G. Lazarov, K. Urbanski, A. M. Lyyra, L. Li, G. -H. Jeung and W. C. Stwalley, "Predissociation of the F(4) 1 Σ g State of 7 Li 2 ", J. Chem. Phys 112, (2000). [22] 71. L. Li, G. Lazarov and A. M. Lyyra, Predissociation of the 7 Li Σ g State, J. Mol. Spectrosc. 191, (1998). [7] 72. H. Chen, L. Li, G. Lazarov, X. Wang, A. M. Lyyra, J. Huennekens and R. W. Field, Rotational Pattern Difference in Resolved Fluorescence Spectra with Different 9

10 Detection Schemes, J. Mol. Spectrosc., 196, (1999). [7] 73. L.Li, A. Yiannopoulou, K. Urbanski, A. M. Lyyra, B. Ji, W. C. Stwalley and T. An, Hyperfine Structures of the Triplet States of 7 Li 2, Continuous Wave Perturbation Facilitated Double Resonance Spectroscopy, Journal of the Korean Physical Society 32 (3), (1998). [5] 74. C. Linton, F. Martin, A. J. Ross, I. Russier, P. Crozet, A. Yiannopoulou, L. Li and A. M. Lyyra, The High Lying Vibrational Levels and the Dissociation Energy of the a 3 Σ u State of 7 Li 2, J. Mol. Spectrosc. 196, (1999). [27] 75. G. Larazov, A. M. Lyyra, L. Li and J. Huennekens, The 4 3 Π g State of Na 2 : Vibrational Numbering and the Hyperfine Structure, J. Mol. Spectrosc., 196, (1999). [17] 76. L. Li, Y. Liu, J. Li, D. Chen, A. M. Lyyra, S. Antonova and G. Lazarov, Predissociation of Na 2 and Li 2, Ch. J. Chem. Phys, 11, (1998). 77. J. Qi, G. Lazarov, X. Wang, L. Li, L. M. Narducci, A. M. Lyyra, and F. C. Spano, Autler-Townes Splitting in Molecular Lithium: Prospects for All-Optical Alignment of Nonpolar Molecules, Phys. Rev. Letters 83, (1999). [52] 78. R. Cote, A. Dalgarno, A. M. Lyyra and L. Li, Observation of a Shape Resonance in the a 3 Σ u State of 7 Li 2, Phys. Rev. A 60, (1999). [9] 79. L. Li, X. J. Wang, J. Yang, G. Lazarov, J. Qi and A. M. Lyyra, Comment on Experimental Observation of Spontaneous Emission Cancellation in the Na 2 Molecular System, Phys. Rev. Lett. 84, 4016 (2000). [40] 80. V. S. Ivanov, V. B. Sovkov, L. Li, A. M. Lyyra and T. -J. Whang, Analysis of the Na Σ g (v=15, N=27 and v=5, N=39) a 3 Σ u Continua: Potentials and Transition Moment Function, J. Chem. Phys. 114, (2001). [12] 81. G. Lazarov, A. M. Lyyra, and L. Li, Enhanced Access to the Dark Triplet States of 7 Li 2 Through New Singlet-Triplet A 1 Σ u -b 3 Π u Perturbation Window Levels; PerturbationFacilitated Optical-Optical Double Resonance Study of the 2 3 Σ g State, J. Mol. Spectroscopy, 205, (2001). [17] 82. J. Shang, J. Qi, L. Li and A. M. Lyyra, The perturbation between the G 1 Π g and 2 1 g States of 7 Li 2, J. Mol. Spectroscopy 203, (2000). [5] 83. A. M. Lyyra, J. Qi and F. C. Spano, Autler-Townes Splitting and ac Stark Shift: Prospects for All-Optical Alignment of Nonpolar Molecules, invited paper, Herzberg Memorial Issue of the Canadian Journal of Physics 79, (2001) 84. L. Li., X. Dai, Y. Liu, J. O. Clevenger, R. W. Field, G. H. Jeung, N. Geum and A. M. Lyyra, The Predissociation of the 1 3 Σ g - State of 7 Li 2 ", J. Mol. Spectroscopy 205, (2001). [6] 85. L. Li, Y. Liu and A. M. Lyyra, "Rydberg and Doubly Excited States of Na 2 and Li 2 ", J. Chin. Chem. Soc. (invited paper) 48, (2001). [3] 10

11 86. Y. Liu, B. Ji, A. S. -C. Cheung, W. C. Stwalley, R. W. Field, A. M. Lyyra, and Li Li, " The Hyperfine Structure of the 1 3 g state of Na 2 ", J. Chem. Phys., 115, (2001). [8] 87. P. Yi, M. Song, Y. Liu, A. M. Lyyra and L. Li, "New Pair of A 1 Σ u -b 3 Π u. Mixed Levels in 6 Li 7 Li", Chem. Phys. Lett, 349, , (2001). [8] 88. V. S. Ivanov, V. B. Sovkov, N. Gallice, L. Li, Y. Liu, A. M. Lyyra and S. Magnier, "Use of Bound-Free Structured Spectra in Determining RKR Potentials: The 4 3 Π g State of Na 2 ", J. Mol. Spectrosc. 209, , (2001). [8] 89. J. Qi, F. C. Spano, T. Kirova, A. Lazoudis, J. Magnes, L. Li, L. M. Narducci, R. W. Field and A. M. Lyyra, Measurement of Transition Dipole Moments in Molecular Lithium using Electromagnetically Induced Transparency, Physical Review Letters, 88, to (2002). [39] 90. L. Li, A. Lazoudis, P. Yi, Y. Liu, J. Huennekens, R. W. Field and A. M. Lyyra," Hyperfine Structures of the 1 3 g, 2 3 Π g and 3 3 Σ g States of 6 Li 7 Li", J. Chem. Phys., 116, , (2002). [8] 91. X. J. Wang, J. Magnes, A. M. Lyyra, A. J. Ross, F. Martin, P. M. Dove and R. J. Le Roy, "Born-Oppenheimer Breakdown in a Combined Isotopomer Analysis of the A 1 Σ u - X 1 Σ g System of Li 2 ", J. Chem. Phys., 117 (20): , (2002). [16] 92. M. R. Manaa, A. J. Ross, F. Martin, P. Crozet, A. M. Lyyra, L. Li, C. Amiot and T. Bergeman," Spin-Orbit Interactions, New Spectral data, and Deperturbation of the Coupled b 3 Π u and A 1 Σ u States of K 2 ", J. Chem. Phys., 117 (24): , (2002). [32] 93. J. Magnes, E. Ahmed, C. Goldberg, A. M. Lyyra, S. Magnier, M. Aubert-Frécon, Y. Liu and L. Li, Observation of the K g State by cw Perturbation-Facilitated Optical- Optical Double Resonance Spectroscopy, J. Mol. Spectroscopy, 221, 72-79, (2003). [9] 94. Y. Liu, L. Li, G. Lazarov, A. Lazoudis, A. M. Lyyra and R.W. Field, Hyperfine structures of the 2 3 Σ g, 3 3 Σ g and 4 3 Σ g States of the Na 2 Dimer, J. Chem. Phys.,121, , (2004). [5] 95. P. Yi, M. Song, Y. Liu, R. W. Field, L. Li and A. M. Lyyra, "Experimental Observation of Autler-Townes Splitting of the Na 2 A 1 Σ u -b 3 Π u Mixed Levels, Optics Communications, 233 (1-3): , (2004). [4] 96. E. Ahmed, A. M. Lyyra, L. Li, V. S. Ivanov, V. B. Sovkov and S. Magnier, Revision of the K Πg and 4 3 Σ g States: New Vibrational Numberings and New Potential Energy Functions, Journal of Molecular Spectroscopy, 229, (2005). [8] 97. Y. Chu, F. Xie, D. Li, L. Li, V. B. Sovkov, V. S. Ivanov and A. M. Lyyra, Experimental Study of the 39 K Π g State by Perturbation Facilitated Infrared-Infrared Double Resonance and Two-Photon Excitation Spectroscopy, J. Chem. Phys., 122, to , (2005).[11] 11

12 98. L. Li, P. Qi, A. Lazoudis, E. Ahmed and A. M. Lyyra, Observation of Electromagnetically Induced Transparency in Two-Photon Transitions of K 2,Chem. Phys. Lett. 403, , (2005) [7]. 99. E. Ahmed, A. M. Lyyra, F. Xie, D. Li, Y. Chu, L. Li, V. S. Ivanov, V. B. Sovkov and S. Magnier, New Experimental Data on the K 2 _a 3 Σ u State Analyzed with the Multiparameter Approach, J. Mol. Spectrosc, 234, (2005).[9] 100. E. Ahmed, A. Hansson, P. Qi, L. Li, T. Kirova, J. Qi, A. Lazoudis, S. Magnier, S. Kotochigova and A. M. Lyyra, Measurement of the Electronic Transition Dipole Moment by Autler Townes Splitting: Comparison of Three and Four Level Excitation Schemes for the Na 2 A 1 Σ u X 1 Σ g System, J. Chem. Phys. 124, to 13 (2006). [17] 101. P. Qi, A. M. Lyyra, Y. Liu, C. Cui, L. Li and G. H. Jeung, The Na Π g State: New Observations and Hyperfine Structure, J. Chem. Phys. 124, (2006).[2] 102. Jianbing Qi and A. Marjatta Lyyra, Electromagnetically Induced Transparency and Dark Fluorescence in a Cascade Three-Level Diatomic Lithium System, Phys. Rev. A 73, (2006). [6] 103. D. Li, F. Xie, L. Li, V. B, Sovkov, V. S. Ivanov, E. Ahmed, A. M. Lyyra, J. Huennekens and S. Magnier, The K 2 3 Σ g State: Observation and Analysis, J. Chem. Phys., 126, , (2007).[6] 104. P. Qi, J. Bai, E. Ahmed, A. M. Lyyra, S. Kotochigova, A. J. Ross, C. Effantin, P. Zalicki, J. Vigue, G. Chawla, R. W. Field, T. J. Whang, W. C. Stwalley, L. Li and T. Bergeman, New Spectroscopic Data and Global Analysis of Data on the A and b States of Na 2, J. Chem. Phys., 127, ,pp. 1-17, (2007).[13] 105. D. Li, F. Xie, L. Li, A. Lazoudis and A. M. Lyyra, New Observation of the 3 Σ g, 1 3 g, and 2 3 П g States and Molecular Constants will all 6 Li 2, 7 Li 2 and 6 Li 7 Li Data, J. Mol. Spectrosc., 246, , (2007).[3] 106. E. Ahmed and A. M. Lyyra, The Effect of Doppler Broadening on Autler-Townes Splitting in the Molecular Cascade Excitation Scheme, Physical Review A 76, , (2007).[4] 107. Peng Qi, Guenadiy Lazarov and A. Marjatta Lyyra, Improved Molecular constants for the low Vibrational Levels of the F(4) 1 Σ g state of 7 Li 2, J. Mol. Spectrosc., 247, , (2008). [1] 108. Feng Xie, Dan Li, Luke Tyree, Li Li, Vladimir B. Sovkov, Valery S. Ivanov, Sylvie Magnier and A. Marjatta Lyyra, Observation and Calculation of the Cs g and b 3 П 0u States, J. Chem. Phys. 128, , (2008).[5] 109. E. Ahmed, Peng Qi, B. Beser, J. Bai, R. W. Field, J. P. Huennekens and A. M. Lyyra, Experimental Mapping of the Absolute Magnitude of the Transition Dipole Moment Function, μ e (R), of the Na 2 A 1 Σ u X 1 Σ g, Phys. Rev. A 77, , (2008).[4] 12

13 110. S. J. Sweeney, E. Ahmed, P. Qi, T. Kirova, A. M. Lyyra and J. Huennekens, Measurement of Absolute Dipole Moment Functions of the 3 1 П 1(X) 1 Σ and 3 1 П 2(A) 1 Σ Transitions in NaK using Autler-Townes Spectroscopy and Calibrated Fluorescence, J. Chem. Phys. 129 Article No , (2008).[3] 111. A. Lazoudis, E. H. Ahmed, L. Li, T. Kirova, P. Qi, A. Hansson, J. Magnes, and A. M. Lyyra, Experimental Observation of the Dependence of Autler-Townes Splitting on the Probe and Coupling Laser Wavenumber Ratio in Doppler Broadened Open Molecular Cascade Systems, Phys. Rev. A, 78, (2008). [2] 112. O. Salihoglu, P. Qi, E. Ahmed, S, Kotochigova, S. Magnier and A. M. Lyyra, Comparison of Autler-Townes Splitting Based Absolute Measurements of the 7 Li 2 A 1 Σ u - X 1 Σ g Electronic Transition Dipole Moment with ab initio Theory, J. Chem. Phys., 129, Article No , (2008). [2] 113. E. H. Ahmed, Peng Qi and A. M. Lyyra, cw All-Optical Quadruple Resonance Spectroscopy: a Five Level Coherently Driven Molecular System, Phys. Rev. A. 79, (2009). [1] 114. F. Xie, V. B. Sovkov, A. M. Lyyra, D. Li, S. Ingram, V. S. Ivanov, S. Magnier and L. Li, Experimental Observation of the Cs 2 a 3 Σ u Triplet Ground State: Multiparameter Morse Long Range Potential Analysis and Molecular Constants, J. Chem. Phys., 130, (2009). [8] 115. H. Salami, T. Bergeman, B. Beser, J. Bai, S. Kotochigova, A. M. Lyyra, J. Huennekens, C. Lisdat, A. V. Stolyarov, O. Dulieu, P. Crozet and A. J. Ross, Spectroscopic observations, spin-orbit functions and coupled channel deperturbation of the A 1 Σ u and b 3 П 0u states of Rb 2, Phys. Rev. A, 80, (2009). [7] 116. B. Beser, V. B.Sovkov, J.Bai, E. H. Ahmed, C. C. Tsai, F. Xie, L. Li, V. S. Ivanov, and A. M. Lyyra, Experimental investigation of the 85Rb2 a3σu triplet ground state: Multiparameter MLR potential analysis, J. Chem. Phys. 131, (2009). [2] 117. A. Lazoudis, P. Qi, T. V. Kirova, E. H. Ahmed, and A. M. Lyyra, Electromagnetically Induced Transparency in an open Λ- type molecular system, to be submitted to Phys. Rev. A, (2010) A. Lazoudis, T. V. Kirova, E. H. Ahmed,, P. Qi, J. Huennekens, and A. M. Lyyra Electromagnetically Induced Transparency in an open V-type Molecular System accepted, Phys. Rev. A (2011) Jianmei Bai, E. H. Ahmed, B. Beser, Y. Guan, S. Kotochigova, A. M. Lyyra, S. Ashman, C. M. Wolfe, J. Huennekens, Feng Xie, Dan Li, Li Li, M. Tamanis, R. Ferber, A. Drozdova, E. Pazyuk, A. V. Stolyarov, J. G. Danzl, H.-C. N agerl, N. Bouloufa, O. Dulieu, C. Amiot, H. Salami, T. Bergeman, Global analysis of data on the spin-orbitcoupled A 1 Σ u and b 3 Π u states of Cs 2, Phys. Rev. A 83, (2011). [1] 13

14 120. C. M. Wolfe, S. Ashman J. Bai, B. Beser, E. H. Ahmed, A. M. Lyyra, and J. Huennekens, Collisional Transfer of Population and Orientation in NaK, J. Chem. Phys., 134, , (2011) F. Xie, L. Li, D. Li, V. Sovkov, K. Minaev, V. Ivanov, S. Magnier, and A. M. Lyyra, Joint Analysis of the Cs 2 a 3 Σ u and 3 3 Π 1g (1g(?)) States, accepted, J. Chem. Phys. (2011) E. H. Ahmed, S. Ingram, T. Kirova, O. Salihoglu, J. Huennekens, J. Qi, Yafei Guan, and A. M. Lyyra, Quantum Control of Spin-Orbit Interaction Using the Autler-Townes Effect, accepted, Physical Review Letters (2011). Web of Science, August 25, 2011: Publications and citations Results found: 132 Sum of the Times Cited: 2304 Sum of Times Cited without self-citations: 1777 Citing Articles: 1224 Average Citations per Item: h-index : 28 Publications each year: 14

15 Citations each year: 15

[Citations as of indicated in brackets after the year of publication]

[Citations as of indicated in brackets after the year of publication] SCIENTIFIC SYNOPSIS Prof. Marjatta Lyyra co-pioneered high- resolution continuous wave triple resonance spectroscopy with initial applications in the areas of large internuclear distance spectroscopy and

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