- Open Access
High-intensity optical-field population transfer between eigenstates
APS Open Sci. 1, 000136 – Published 15 September, 2026
DOI: https://doi.org/10.1103/sy5j-g2cq
Abstract
Two types of coherent population transfer are developed using nonresonant intense ultrashort optical pulses. Transition-restricted wave-packet interference (WPI) achieves almost complete population transfer to the nearest state from the initial state. High-intensity optical-field population transfer between eigenstates (HOPE) also enables state-selective excitation of higher-lying states, exhibiting features of ac Stark-induced multiphoton Rabi oscillation and multipulse WPI. Experimentally, rotational excitation of nitric oxide from to via restricted WPI, and to , and via HOPE, was demonstrated with respective efficiencies of 90%, 85%, 70%, and 17%.
Physics Subject Headings (PhySH)
Article Text
Supplemental Material
References (54)
- C. P. Koch and M. Shapiro, Coherent control of ultracold photoassociation, Chem. Rev. 112, 4928 (2012).
- H. Pan, S. Mondal, C.-H. Yang, and K. Liu, Imaging characterization of the rapid adiabatic passage in a source-rotatable, crossed-beam scattering experiment, J. Chem. Phys. 147, 013928 (2017).
- H. Pan and K. Liu, Fermi-phase-induced interference in the reaction between Cl and vibrationally excited CH3D, Nat. Chem. 14, 545 (2022).
- W. E. Perreault, N. Mukherjee, and R. N. Zare, Quantum control of molecular collisions at 1 kelvin, Science 358, 356 (2017).
- W. E. Perreault, N. Mukherjee, and R. N. Zare, Cold quantum-controlled rotationally inelastic scattering of HD with and reveals collisional partner reorientation, Nat. Chem. 10, 561 (2018).
- R. Sussmann, R. Neuhauser, and H. J. Neusser, Stimulated Raman adiabatic passage with pulsed lasers: High resolution ion dip spectroscopy of polyatomic molecules, J. Chem. Phys. 100, 4784 (1994).
- I. I. Rabi, On the process of space quantization, Phys. Rev. 49, 324 (1936).
- S. Nandi, E. Olofsson, M. Bertolino, S. Carlström, F. Zapata, D. Busto, C. Callegari, M. Di Fraia, P. Eng-Johnsson, R. Feifel, et al., Observation of Rabi dynamics with a short-wavelength free-electron laser, Nature (London) 608, 488 (2022).
- A. de las Heras, C. Hernández-García, J. Serrano, A. Prodanov, D. Popmintchev, T. Popmintchev, and L. Plaja, Attosecond Rabi oscillations in high harmonic generation resonantly driven by extreme ultraviolet laser fields, Phys. Rev. Res. 7, 023268 (2025).
- A. F. Linskens, I. Holleman, N. Dam, and J. Reuss, Two-photon Rabi oscillations, Phys. Rev. A 54, 4854 (1996).
- M. Fushitani, C.-N. Liu, A. Matsuda, T. Endo, Y. Toida, M. Nagasono, T. Togashi, M. Yabashi, T. Ishikawa, Y. Hikosaka, T. Morishita, and A. Hishikawa, Femtosecond two-photon Rabi oscillations in excited He driven by ultrashort intense laser fields, Nat. Photon. 10, 102 (2016).
- R. Vijay, C. Macklin, D. H. Slichter, S. J. Weber, K. W. Murch, R. Naik, A. N. Korotkov, and I. Siddiqi, Stabilizing Rabi oscillations in a superconducting qubit using quantum feedback, Nature (London) 490, 77 (2012).
- K. Bergmann, H. Theuer, and B. W. Shore, Coherent population transfer among quantum states of atoms and molecules, Rev. Mod. Phys. 70, 1003 (1998).
- N. V. Vitanov, T. Halfmann, B. W. Shore, and K. Bergmann, Laser-induced population transfer by adiabatic passage techniques, Annu. Rev. Phys. Chem. 52, 763 (2001).
- B. W. Shore, Coherent manipulations of atoms using laser light, Acta Phys. Slov. 58, 243 (2008).
- N. V. Vitanov, A. A. Rangelov, B. W. Shore, and K. Bergmann, Stimulated Raman adiabatic passage in physics, chemistry, and beyond, Rev. Mod. Phys. 89, 015006 (2017).
- B. W. Shore, Picturing stimulated Raman adiabatic passage: A STIRAP tutorial, Adv. Opt. Photon. 9, 563 (2017).
- N. Mukherjee and R. N. Zare, Stark-induced adiabatic Raman passage for preparing polarized molecules, J. Chem. Phys. 135, 024201 (2011).
- N. Mukherjee, W. E. Perreault, and R. N. Zare, Stark-induced adiabatic passage processes to selectively prepare vibrationally excited single and superposition of quantum states, in Frontiers and Advances in Molecular Spectroscopy, edited by J. Laane (Elsevier, Amsterdam, The Netherlands, 2018), Chap. 1, pp. 1–46.
- N. Mukherjee, Quantum-controlled collisions of molecules, J. Phys. Chem. A 127, 418 (2023).
- H. Chadwick, P. M. Hundt, M. E. van Reijzen, B. L. Yoder, and R. D. Beck, Quantum state specific reactant preparation in a molecular beam by rapid adiabatic passage, J. Chem. Phys. 140, 034321 (2014).
- K. K. W. Ma and C. K. Law, Three-photon resonance and adiabatic passage in the large-detuning Rabi model, Phys. Rev. A 92, 023842 (2015).
- K.-X. Yan, Y. Qiu, Y. Xiao, Y.-H. Chen, and Y. Xia, Generating three-photon Rabi oscillations without a large-detuning condition, Phys. Rev. A 110, 043711 (2024).
- P. Li, W. Yang, X. Li, S. Xue, J. Li, and H. Du, Three-photon Rabi oscillations in lasing at 391 nm, Phys. Rev. A 111, 063501 (2025).
- L. Sirko, A. Buchleitner, and H. Walther, Rabi-nutations of four- and six-photon transitions between Rydberg states, Opt. Commun. 78, 403 (1990).
- J. He, B. Pasquiou, R. G. Escudero, S. Zhou, M. Borkowski, and F. Schreck, Coherent three-photon excitation of the strontium clock transition, Phys. Rev. Res. 7, L012050 (2025).
- R. E. Carley, E. Heesel, and H. H. Fielding, Femtosecond lasers in gas phase chemistry, Chem. Soc. Rev. 34, 949 (2005).
- M. Gühr, Ultrafast molecular spectroscopy in the gas phase, in Structural Dynamics with X-ray and Electron Scattering, edited by K. Amini, A. Rouzée, M. J. J. Vrakking (Royal Society of Chemistry, Cambridge, UK, 2023), Chap. 1, pp. 1–53.
- J. Karczmarek, J. Wright, P. Corkum, and M. Ivanov, Optical centrifuge for molecules, Phys. Rev. Lett. 82, 3420 (1999).
- D. M. Villeneuve, S. A. Aseyev, P. Dietrich, M. Spanner, M. Y. Ivanov, and P. B. Corkum, Forced molecular rotation in an optical centrifuge, Phys. Rev. Lett. 85, 542 (2000).
- C. Wu, G. Zeng, Y. Gao, N. Xu, L.-Y. Peng, H. Jiang, and Q. Gong, Controlling molecular rotational population by wave-packet interference, J. Chem. Phys. 130, 231102 (2009).
- K. Ohmori, Wave-packet and coherent control dynamics, Annu. Rev. Phys. Chem. 60, 487 (2009).
- Y. Ohshima and H. Hasegawa, Coherent rotational excitation by intense nonresonant laser fields, Int. Rev. Phys. Chem. 29, 619 (2010).
- S. Shi and H. Rabitz, Quantum mechanical optimal control of physical observables in microsystems, J. Chem. Phys. 92, 364 (1990).
- D. Goswami, Optical pulse shaping approaches to coherent control, Phys. Rep. 374, 385 (2003).
- A. Rouzée, O. Ghafur, K. Vidma, A. Gijsbertsen, O. M. Shir, T. Bäck, A. Meijer, W. J. van der Zande, D. Parker, and M. J. J. Vrakking, Evolutionary optimization of rotational population transfer, Phys. Rev. A 84, 033415 (2011).
- T. Hellerer, A. M. Enejder, and A. Zumbusch, Spectral focusing: High spectral resolution spectroscopy with broad-bandwidth laser pulses, Appl. Phys. Lett. 85, 25 (2004).
- K. Wang, A. Hardikar, A. A. Milner, and V. Milner, Optical centrifuge with zero rotational acceleration, Phys. Rev. A 112, 053102 (2025).
- See Supplemental Material at http://link.aps.org/supplemental/10.1103/sy5j-g2cq for details of the TDSE calculations, pulse characterization, and instantaneous Raman-Floquet analysis, which includes Refs. [53, 54].
- J. H. Shirley, Solution of the Schrödinger equation with a Hamiltonian periodic in time, Phys. Rev. 138, B979 (1965).
- H. Hasegawa and Y. Ohshima, Decoding the state distribution in a nonadiabatic rotational excitation by a nonresonant intense laser field, Phys. Rev. A 74, 061401(R) (2006).
- N. C. Geib, M. Zilk, T. Pertsch, and F. Eilenberger, Common pulse retrieval algorithm: A fast and universal method to retrieve ultrashort pulses, Optica 6, 495 (2019).
- R. Engleman, P. Rouse, H. Peek, and V. Baiamonte, Beta and gamma band systems of nitric oxide, Technical Report, Division of Technical Information Extension, U.S. Atomic Energy Commission, 1969.
- D. X. Wang, C. Haridass, and S. Reddy, The gamma system of the nitric oxide isotopomers, J. Mol. Spectrosc. 175, 73 (1996).
- R. N. Zare, Angular Momentum: Understanding Spatial Aspects in Chemistry and Physics (John Wiley and Sons, Inc., New York, 1991).
- C. Deng, F. Shen, S. Ashhab, and A. Lupascu, Dynamics of a two-level system under strong driving: Quantum-gate optimization based on Floquet theory, Phys. Rev. A 94, 032323 (2016).
- R. Merlin, Rabi oscillations, Floquet states, Fermi's golden rule, and all that: Insights from an exactly solvable two-level model, Am. J. Phys. 89, 26 (2021).
- H. Sambe, Steady states and quasienergies of a quantum-mechanical system in an oscillating field, Phys. Rev. A 7, 2203 (1973).
- K. Drese and M. Holthaus, Floquet theory for short laser pulses, Eur. Phys. J. D 5, 119 (1999).
- T. N. Ikeda, S. Tanaka, and Y. Kayanuma, Floquet-Landau-Zener interferometry: Usefulness of the Floquet theory in pulse-laser-driven systems, Phys. Rev. Res. 4, 033075 (2022).
- A. Kuhn, S. Steuerwald, and K. Bergmann, Coherent population transfer in NO with pulsed lasers: The consequences of hyperfine structure, Doppler broadening and electromagnetically induced absorption, Eur. Phys. J. D 1, 57 (1998).
- D. Ikeda, K. Mizuse, and Y. Ohshima, Direct imaging of the hyperfine depolarization in electronically excited NO molecules, Phys. Rev. A 107, 043116 (2023).
- S. A. McDowell and W. J. Meath, Average energy approximations for anisotropic triple-dipole dispersion energy coefficients using three-body interactions involving, Can. J. Chem. 76, 483 (1998).
- J. Danielak, U. Domin, R. Ke, M. Rytel, and M. Zachwieja, Reinvestigation of the emission band system of the NO molecule, J. Mol. Spectrosc. 181, 394 (1997).