Ultrafast Dynamics and Quantum Control Theory
About
The research conducted by the Ultrafast Dynamics and Quantum Control Theory group centers around theoretical explorations of the interaction between laser radiation and atoms or molecules. Our primary goal is to advance quantum control methods by integrating developments in quantum optics, molecular spectroscopy, and laser science. We are dedicated to pushing the boundaries of atomic, molecular, and optical sciences.
Our investigations span a diverse range of fundamental topics, including ultrafast Raman spectroscopy, the dynamics of ultracold gases, optical control of hybrid nanomaterials, and quantum many-body physics. The impact of our work extends into the realms of nanoscience and biomedicine, gaining ongoing significance as proposals for quantum-based technologies emerge. These technologies encompass quantum sensing, imaging, metrology, and quantum information.
Faculty
Publications
Books
1. Svetlana A. Malinovskaya, Irina Novikova, Edts., “From Atomic to Mesoscale: The Role of
Quantum Coherence in Systems of Various Complexities,” World Scientific Publishing Co. PTE.
LTD. Singapore. ISBN-13: 978-9814678698; ISBN-10: 9814678694 (2015).
Book chapters
2. Chathanathil, J.; Malinovskaya, S. Chirped pulse control of Raman coherence in atoms and
molecules. Adv. Quant. Chem. 89 (2023). Elsevier. http://dx.doi.org/10.1016/bs.aiq.2023.07.002.
3. Ramaswamy, A., Malinovskaya, S.A. Control with EIT: High Energy Charged Particle Detection.
In: ¨Unl¨u, H., Horing, N.J.M. (eds) Progress in Nanoscale and Low-Dimensional Materials and
Devices. Topics in Appl. Phys. 144, 363-392 (2022). Springer International Publishing
https://doi.org/10.1007/978-3-030-93460-6 12.
4. Gengyuan Liu, Svetlana A. Malinovskaya, “Adiabatic passage control methods for ultracold
alkali atoms and molecules using chirped laser pulses and optical frequency combs,” Adv. Quant.
Chem. 77, 241-294 (2018).
5. Ignacio R. Sola, Bo Y. Chang, Svetlana A. Malinovskaya, Vladimir S. Malinovsky, “Quantum
Control in Multilevel Systems,” Advances in At. Mol. Opt. Phys., 67, 151-256 (2018).
6. Svetlana A. Malinovskaya, Tom Collins, Vishesha Patel, “Ultrafast manipulation of Raman
transitions and prevention of decoherence using chirped pulses and optical frequency combs,”
Adv. Quantum Chem. 64, 211-258 (2012).
7. S. A. Malinovskaya. Observation and control of molecular motion using ultrafast laser pulses.
In: Trends in Chemical Physics Research”, Linke, A.N., ed., Nova Science Publishers, Inc. New
York, NY. ISBN: 1-59454-483-2. 257-280 (2005).
Peer Reviewed Journal Articles
8. Aneesh Ramaswamy, Jabir Chathanathil, Dimitra Kanta, Emmanuel Klinger, Aram Papoyan,
Svetlana Shmavonyan, Aleksandr Khanbekyan, Arne Wickenbrock, Dmitry Budker, Svetlana A
Malinovskaya, ”Mirrorless lasing: a theoretical perspective,” Opt. Memory and Neural Networks
32, S443-S466 (2023).
9. Sebastian C Carrasco, Michael H Goerz, Svetlana A Malinovskaya, Vladan Vuletic, Wolfgang
Schleich, Vladimir S Malinovsky, ”Dicke State Generation and Extreme Spin Squeezing via
Rapid Adiabatic Passage,” submitted (2023).
10. Jabir Chathanathil, Aneesh Ramaswamy, Vladimir S. Malinovsky, Dmitry Budker, Svetlana A.
Malinovskaya, ”Chirped fractional stimulated Raman adiabatic passage,” Phys. Rev. A 108,
043710 (2023).
11. Jabir Chathanathil, Dmitry Budker, Svetlana A. Malinovskaya, ”Quantum control via chirped
coherent anti-Stokes Raman spectroscopy,” Quantum Sci. Tech. 8, 045005 (2023).
12. I. R. Sola, B. Y. Chang, S. A. Malinovskaya, S. C. Carrasco, V. S. Malinovsky, ”Stimulated
Raman adiabatic passage with trains of weak pulses,” J. Phys. B: At. Mol. Opt. Phys. 55,
234002 (2022).
13. A. Ramaswamy, A.F. Latypov, S.A. Malinovskaya, ”Generation of the GHZ and the W state in
a series of Rydberg atoms trapped in optical lattices,” Adv. Theo. Comp. Phys. 5(3), 476-484
(2022).
14. J. Chathanathil, G. Lui, S. A. Malinovskaya, ”A semi-classical control theory of Coherent Anti-
Stokes Raman Scattering (CARS) maximizing vibrational coherence for remote detection,” Phys.
Rev. A, 104, 043701 (2021).
15. Elliot Pachniak, Svetlana A. Malinovskaya, ”Creation of quantum entangled states of Rydberg
atoms via chirped adiabatic passage,” Nature Sc. Rep. 11, 12980 (2021).
16. Svetlana A. Malinovskaya, ”Laser cooling using adiabatic rapid passage,” Frontiers of Phys. 16,
52601 (2021).
17. N. Pandya, G. Lui, F. A. Narducci, J. Chathanathil, S. A. Malinovskaya, ”Creation of the
maximum coherence via adiabatic passage in the four-wave mixing process of coherent anti-
Stokes Raman scattering,” Chem. Phys. Lett., 738, 136763 (2020).
18. Gengyuan Liu, Frank A. Narducci, Svetlana A. Malinovskaya, “Limits to remote molecular
detection via coherent anti-Stokes Raman spectroscopy using a maximal coherence control technique,”
J. Mod. Opt. 67, 21-25 (2020).
19. Svetlana A. Malinovskaya, Elliot Pachniak, “Generation of entanglement in spin states of Rydberg
atoms by chirped optical pulses,” Adv. Materials Lett. 10, 619-621 (2019).
20. Gengyuan Liu, Svetlana A. Malinovskaya, “Creation of ultracold molecules within the lifetime
scale by direct implementation of an optical frequency comb,” J. Mod. Opt. 65, 1309-1317
(2018).
21. Svetlana A. Malinovskaya, “Design of many-body spin states of Rydberg atoms excited to highly
tunable magnetic sublevels,” Opt. Lett. 42, 314-317 (2017).
22. Svetlana A. Malinovskaya, Gengyuan Liu, “Harmonic spectral modulation of an optical frequency
comb to control the ultracold molecules formation,” Chem. Phys. Lett., Frontiers
Article 664, 1-4 (2016).
23. Gengyuan Liu, Svetlana A. Malinovskaya, ”Two-photon adiabatic passage in ultracold Rb interacting
with a single nanosecond, chirped pulse,” J. Phys. B: At. Mol. Opt. Phys. 48, 194001
(2015).
24. Maxim Sukharev, Svetlana A. Malinovskaya, ”Collective effects in subwavelength hybrid systems:
a numerical analysis,” Mol. Phys. 113, 392-396 (2014).
25. Praveen Kumar, Svetlana A. Malinovskaya, Vladimir S. Malinovsky, ”Optimal control of multilevel
quantum systems in the field-interaction representation,” Phys. Rev. A 90, 033427
(2014).
26. G. Liu, V. Zakharov, T. Collins, P. Gould, S. A. Malinovskaya, “Population inversion in hyperfine
states of Rb with a single nanosecond chirped pulse in the framework of a four-level system, ”
Phys. Rev. A. 89, 041803(R) (2014).
27. E. Kusnetzova, G. Liu, S. A. Malinovskaya, “Adiabatic rapid passage two-photon excitation of
a Rydberg atom,” Phys. Scr. 160, 014024 (2014).
28. P. Kumar, S. A. Malinovskaya, I. Sola, and V. S. Malinovsky, “Selective creation of maximum
coherence in multi-level Λ system,” Mol. Phys. 112, 326-331 (2014).
29. S. A. Malinovskaya, S. L. Horton, “Rovibrational cooling using optical frequency combs in the
presence of decoherence,” J. Opt. Soc. Am. B 30, 482-488 (2013).
30. T. A. Collins, S. A. Malinovskaya, “Robust Control in Ultracold Alkali Metals Using A Single
Linearly Chirped Pulse,” J. Mod. Opt. 60, 28-35 (2013).
31. M. Sukharev, S. A. Malinovskaya, “Stimulated Raman adiabatic passage as a route to achieving
optical control in plasmonics,” Phys. Rev. A 86, 043406 (2012).
32. V. Patel, S. A. Malinovskaya, “Realization of population inversion under the nonadiabatic conditions
induced by the coupling between vibrational modes,” Int. J.Quant. Chem. 112, 3739-3743
(2012).
33. T. A. Collins, S. A. Malinovskaya, “Manipulation of ultracold rubidium atoms using a single
linearly chirped laser pulse,” Opt. Lett. 37, 2298-2300 (2012).
34. P.E. Hawkins, S.A. Malinovskaya, V.S. Malinovsky, “Ultrafast geometric control of a single qubit
using chirped pulses,” Phys. Scr. 147, 014013 (2012).
35. P. Kumar, S.A. Malinovskaya, V.S. Malinovsky, “Optimal control of population and coherence
in three-level -systems,” J. Phys. B: At. Mol. Opt. Phys., 44, 154010 (2011).
36. Vishesha Patel, Svetlana Malinovskaya, “Nonadiabatic effects induced by the coupling between
vibrational modes via Raman fields”, Phys. Rev. A 83, 013413 (2011).
37. S. Malinovskaya, W. Shi, “Feshbach-to-ultracold molecular state Raman transitions via a femtosecond
optical frequency comb”, J. Mod. Opt. 57, 1871-1876 (2010).
38. S. Malinovskaya, V. Patel, T. Collins, “Internal state cooling with a femtosecond optical frequency
comb”, Int. J. Quant. Chem. 110, 3080-3085 (2010).
39. W. Shi, S. Malinovskaya, “Implementation of a single femtosecond optical frequency comb for
molecular cooling”, Phys. Rev. A 82, 013407 (2010).
40. Praveen Kumar, Svetlana A. Malinovskaya, “Quantum dynamics manipulation using optimal
control theory in the presence of laser field noise”, J.Mod. Opt. 57, 1243-1250 (2010).
41. Vishesha Patel, Vladimir Malinovsky, Svetlana Malinovskaya, “Effects of phase and coupling
between the vibrational modes on selective excitation in CARS microscopy”, Phys. Rev. A 81,
063404 (2010).
42. S. A. Malinovskaya, “Optimal Coherence via Adiabatic Following”, Optics Communications
282, 3527-3529 (2009).
43. B. Corn, S. A. Malinovskaya, “An ab initio analysis of charge redistribution upon isomerization
of retinal in rhodopsin and bacteriorhodopsin”, Int. J. Quant. Chem. 109, 3131-3141 (2009).
44. S. A. Malinovskaya, “Robust control by two chirped pulse trains in the presence of decoherence”,
J. Mod. Opt. 56, 784-789 (2009).
45. Svetlana A. Malinovskaya, Vladimir S. Malinovsky, “Optimal coherence via chirped pulse adiabatic
passage in the presence of dephasing”, J. Mod. Opt. 55, 3101-3108 (2008).
46. S. A. Malinovskaya, “Prevention of decoherence by two femtosecond chirped pulse trains”, Optics
Lett. 33, 2245-2247 (2008).
47. S. A. Malinovskaya, V. S. Malinovsky, “Chirped Pulse Adiabatic Control in CARS for Imaging
of Biological Structure and Dynamics”, Optics Lett. 32, 707-709 (2007).
48. S. A. Malinovskaya, “Chirped Pulse Control Methods for Imaging of Biological Structure and
Dynamics”, Int. J. Quant. Chem. 107, 3151-3158 (2007).
49. S. A. Malinovskaya, “Mode selective excitation using ultrafast chirped laser pulses”, Phys. Rev.
A. 73, 033416 (4pp) (2006).
50. S. Malinovskaya, “Pulse function for control of the coherent excitation in stimulated Raman
spectroscopy”, Int. J. Quant. Chem. 102, 313-317 (2005).
51. S. Malinovskaya, P. Bucksbaum, P. Berman, “On the role of coupling in mode selective excitation
using ultrafast pulse shaping in stimulated Raman spectroscopy”, J. Chem. Phys. 121, 3434-
3437 (2004).
52. S. Malinovskaya, P. Bucksbaum, P. Berman, “Theory of selective excitation in Stimulated Raman Scattering”, Phys. Rev. A 69, 013801 (2004).
53. S. Malinovskaya, R. Cabrera-Trujillo, J.R. Sabin, E. Deumens and Y. Ohrn, “Dynamics of proton-acetylene collisions at 30 eV”, J. Chem. Phys. 117, 1103-1108 (2002).
54. M. Kollmar, H. Steinhagen, J. Janssen, B. Goldfuss, S. Malinovskaya, J. Vazquez, F. Rominger and G. Helmchen, “(h3 - Phenylallyl) ( phosphanyloxazoline ) palladium Complexes: X-Ray Crystallographic Studies, NMR Investigations and Ab initio/DFT Calculations”, Chem. Eur. J. 8, 3103-3114 (2002).
55. S. A. Malinovskaya, L. S. Cederbaum, “The role of coherence and time in the mechanism of dynamical symmetry braking and localization ”, Int. J. Quant. Chem. 80, 950-957 (2000).
56. S. A. Malinovskaya, L. S. Cederbaum, “Violation of electronic optical selection rules in X-ray emission by nuclear dynamics: time-dependent formulation”, Phys. Rev. A 61, 42706 (2000).
57. S.A. Malinovskaya, P.V. Schastnev, V.N. Ikorskii, “Magnetic susceptibility and parameters of exchange interactions between octahedral Co (II) complexes and nitroxyl imidazoline radical,” Chemical Physics Reports 15, 1171-1179 (1996).
58. S.A. Malinovskaya, P.V. Schastnev, V.N. Ikorskii, “Magnetic susceptibility and parameters of exchange interaction of Co(II) octahedral complex compounds with nitroxyl imidazoline radical”, Khimicheskaya Fizika 15, 63-70 (1996).
59. S.A. Malinovskaya, R.N. Musin, P.V. Schastnev, “Analytical approximation of conformational dependence of exchange interaction parameters in axially-coordinated complexes of Cu(II) with nitroxyl radicals”, J. Struct. Chem. 36, 23-28 (1995).
60. S.A. Malinovskaya, P.V. Schastnev, R.N. Musin, V.N. Ikorskii, “Exchange parameters of five-spin clusters of Cu(II) coordination compounds with imidazoline nitroxide radicals”, J. Struct. Chem. 34, 398-401 (1993).
61. S.A. Malinovskaya, P.V. Schastnev, “Method and program for magnetic susceptibility calculation of a system of clusters composed of exchange-interacting paramagnetic species including the anisotropy of g-factor and zero-field splitting”, J. Struct. Chem. 34, 394-397 (1993).
62. R.N. Musin, P.V. Schastnev, S.A. Malinovskaya, “Delocalization mechanism of ferromagnetic exchange interaction in the complexes of Copper(II) with nitroxyl radicals,” Trends Applied Theoretical Chemistry 9, 167-173 (1992).
63. R.N. Musin, P.V. Schastnev, S.A. Malinovskaya, “Delocalization mechanism of ferromagnetic exchange interaction in the complexes of Copper(II) with nitroxyl radicals,” Inorg. Chem. 31, 4118-4121 (1992).
64. S.A. Malinovskaya, P.V. Schastnev, R.N. Musin, S.A. Mustafaev, I.A. Grigor’ev, “Influence of structural factors on delocalization of spin density in nitroxyl radicals of the imidazoline series,” J. Struct. Chem. 32, 42-46 (1991).
Peer Reviewed Conference Papers and Other Works
65. Aneesh Ramaswamy and Svetlana Malinovskaya, “Atom-photon entanglement transfer using a 3-D multimode cavity with a single uniformly moving mirror,” In: 54th Annual Meeting of the APS Division of Atomic, Molecular and Optical Physics (Spokane, Washington, U.S.A). Abstract: U10.00006 (2023).
66. J Chathanathil, A Ramaswamy, S Malinovskaya, ”Selective excitation for imaging via chirped fractional stimulated Raman adiabatic passage,” In: Biophotonics Congress: Optics in the Life Sciences 2023. Optica Publishing Group NTu3C.3 (2023). doi: 10.1364/NTM.2023.NTu3C.3.
67. Nicolas DeStefano, Saeed Pegahan, Irina Novikova, Eugeniy Mikhailov, Seth Aubin, Todd Averett, Shukui Zhang, Alexandre Camsonne, Gunn Park, Aneesh Ramaswamy, Svetlana Malinovskaya, ”Electron Beam Profiling Using Coherent Atomic Magnetometry,” Bulletin of the American Physical Society, G01.00005 (2023).
68. A Ramaswamy, S Malinovskaya, ”Atom-photon entanglement transfer using a 3-D multimode cavity with a single uniformly moving mirror,” Bulletin of the American Physical Society, U10.00006 (2023).
69. A Ramaswamy, S Malinovskaya, ”Transparency in two level systems using an optical frequency comb with sinusoidal phase modulation,” Bulletin of the American Physical Society, N01.00043 (2023).
70. J Chathanathil, A Ramaswamy, S Malinovskaya, ”Control of Quantum Coherence via Chirped Fractional Stimulated Raman Adiabatic Passage,” Bulletin of the American Physical Society, M11.00006 (2023).
71. Jabir Chathanathil, Gengyuan Liu, and Svetlana Malinovskaya, ”Remote detection using maximal coherence control technique in coherent anti-Stokes Raman spectroscopy,” Optical Sensors and Sensing Congress 2022 (AIS, LACSEA, Sensors, ES), Technical Digest Series (Optica Publishing Group, 2022), LM3B.5 (2022), https://doi.org/10.1364/LACSEA.2022.LM3B.5.
72. Svetlana A. Malinovskaya and Aneesh Ramaswamy, “Transparency in a two-level system using state phase control”, In: Frontiers in Optics + Laser Science 2022. Optica Publishing Group, https://doi.org/10.1364/FIO.2022.JTu4B.72 (2022).
73. Jabir Chathanathil, Francesco Narducci, Svetlana Malinovskaya, ”The detuning controlled maximum coherence via C-CARS,” Bulletin of the American Physical Society, S07.00007 (2022).
74. Aneesh Ramaswamy, Irina Novikova, Svetlana Malinovskaya, ”Controlling optical response to charged particles in EIT media,” Bulletin of the American Physical Society, M06.00007 (2022).
75. Svetlana Malinovskaya, ”Many-body physics with spin states of trapped Rydberg atoms,” Bulletin of the American Physical Society, H03.00008 (2021).
76. Aneesh Ramaswamy, Svetlana Malinovskaya, and Irina Novikova, “Developing a quantum control scheme for the detection of high energy charged particles using the strong non-linear optical response of atomic media in EIT states,” In: 52nd Annual Meeting of the APS Division of Atomic, Molecular and Optical Physics. Abstract: Z10.00004 (2021).
77. Aneesh Ramaswamy and Svetlana Malinovskaya. “Femtosecond optical frequency combs and applications to quantum control of three-level atomic systems”. In: 51st Annual Meeting of the APS Division of Atomic, Molecular and Optical Physics (Portland, Oregon, U.S.A). Abstract: Q01.00156. (2020).
78. Aneesh Ramaswamy, Svetlana Malinovskaya, and Irina Novikova, “A model of electromagnetically induced transparency and high energy charged particles in atomic media,” In: 51st Annual Meeting of the APS Division of Atomic, Molecular and Optical Physics (Portland, Oregon, U.S.A). Abstract: Q01.00155 (2020).
79. E. Pachniak, Y.V. Rostovtsev, S.A. Malinovskaya, ”Quantum control of entanglement using spin states in Rydberg atoms,” OSA Conference on Coherence and Quantum Optics, Th1A.3 (2019).
80. S. A. Malinovskaya, E. Pachniak, ”Many-Body Physics with Spin States of Rydberg Atoms,” 2018 IEEE Photonics Society Summer Topical Meeting Series (SUM), 221 (2018).
81. V. S. Malinovsky, S. A. Malinovskaya, B. Y.Chang, I. R. Sola, B. M. Garraway, ”From Rabi oscillations to adiabatic passage in multi-level quantum systems with a train of weak pulses.,” Latin America Optics and Photonics Conference, Optical Society of America (OSA), W4A (2018).
82. Svetlana A. Malinovskaya ”Enhanced contrast CARS for biochemical and environmental analysis,” Imaging and Applied Optics 2016, Optical Society of America, paper LM4G.3. https://doi.org/10.1364/LACSEA.2016.LM4G.3 (2016).
83. S. A. Malinovskaya, ”Theory of molecular cooling using optical frequency combs in the presence of decoherence,” Frontiers in Optics, San Jose, CA, USA. ISBN: 978-1-55752-917-6 Frequency Combs-II-Applications (FThH) (2011).
84. S. A. Malinovskaya, “Optimal Coherence Using Chirped Pulse Trains for Enhanced Imaging,” Frontiers in Optics 2008/Laser Science, Optical Society of America, paper FTuY4. https://doi.org/10.1364/FIO.2008.FTuY4 (2008).
85. S. A. Malinovskaya, “Chirped Pulse Adiabatic Passage in CARS,” Frontiers in Optics 2007/Laser Science XXIII, Optical Society of America 2007, paper JWC9. https://doi.org/10.1364/FIO.2007.JWC9 (2007).
86. S.A. Malinovskaya, “Chirped Pulse Adiabatic Passage in CARS for Imaging of Biological Structure and Dynamics”, AIP Conference Proceedings 963 (2), 216-218 (2007).
87. P.V. Schastnev, S.A. Malinovskaya, V.N. Ikorskii, “Method for spin magnetic susceptibility calculation of clusters of transition metals with paramagnetic ligands including anisotropic effects. Magnetic susceptibility and exchange parameters of coordinational compounds Cu(II) and Ni(II) with nitroxyl radicals”, Proceedings of VI International School-Symposium on Chemical Physics, “Burevestnik”, 79-87 (1994) (in Russian).
88. S.A. Malinovskaya, “Structure and Magnetic Properties of Nitroxyl Radicals of Imidazoline Series and of Their Complexes with Transition Metals. Theoretical Analysis.”, Thesis for Ph.D. degree in Physics and Mathematics, Novosibirsk State University and the Institute of Chemical Kinetics and Combustion, Siberian Branch of Russian Academy of Science, Novosibirsk (1993) (in Russian).
89. S.A. Malinovskaya, “Structure and Magnetic Properties of Nitroxyl Radicals of Imidazoline Series and of Their Complexes with Transition Metals. Theoretical Analysis.”, Author’s Abstract Book of Thesis for Ph.D. degree in Physics and Mathematics, Novosibirsk State University and the Institute of Chemical Kinetics and Combustion, Siberian Branch of Russian Academy of Science, Novosibirsk (1993) (in Russian).
Patents
90. S. A. Malinovskaya, V. S. Malinovsky, “CARS microscopy and spectroscopy using ultrafast chirped pulses,” USP 7847933 (2010).
Research Areas
View research projects below.
Atoms in their highly excited electronic states, referred to as Rydberg atoms, have terrific nonlinear optical properties. They are highly polarizable and, when trapped, interact with each other via the dipole-dipole or the van-der-Waals interactions depending on interatomic distance. They possess condensed matter-like collective behavior as serve as a platform to study quantum many-body physics. Collective spin states of such atoms carry rich properties including novel quantum magnetism, quantum phases and entanglement. It is very important to be able to design coherent superposition states of different kinds because they underlie every quantum information task. We develop strategies to generate superposition states of different classes from the dressed state Hamiltonian. Understanding of the inherent evolution of many-body states depending on laser properties suggests the control schemes for manipulation of dynamics steering the system to a desired coherent superposition spin state. We apply our methods to generation of the W and the Greenberger-Horne-Zeilinger (GHZ) states. We use the multipartite entangled states of Rydberg atoms to create the multiphoton entangled radiation states in a cavity and in free space. Our methodology exploits chirped adiabatic passage and provides a key step toward the resolution of a general problem of creating entanglement in high-dimensional quantum entities.
Bibliography:
S. A. Malinovskaya, "Design of many-body spin states of Rydberg atoms excited to highly tunable magnetic sublevels," Opt. Lett. 42, 314 (2017).
E. Pachniak, S. A. Malinovskaya, "Creation of quantum entangled states of Rydberg atoms via chirped adiabatic passage", Nature Sc. Rep. 11, 12980 (2021).
E. Pachniak, Y. V. Rostovtsev, S. A. Malinovskaya, "Quantum control of entanglement using spin states in Rydberg atoms", OSA Conference on Coherence and Quantum Optics, Th1A.3 (2019).
Stimulated Raman Adiabatic Passage (STIRAP) is a widely used method for adiabatic population transfer in a multilevel system. In this work, we study STIRAP under novel conditions and focus on the fractional STIRAP, which is known to create a superposition state with the maximum coherence. In both configurations, STIRAP and F-STIRAP, we implement pulse chirping aiming at a higher contrast, a broader range of parameters for adiabaticity, and a higher spectral selectivity.
Such goals target improvement of quantum imaging, sensing and metrology, and broaden the range of applications of quantum control techniques and protocols. In conventional STIRAP and F-STIRAP the two-photon resonance is required conceptually to satisfy the adiabaticity condition for dynamics within the dark state. Here, we account for a non-zero two-photon detuning and present control schemes to achieve the adiabatic conditions in STIRAP and F-STIRAP by pulse chirping. We show that the chirped configuration – C-STIRAP – permits adiabatic passage to a predetermined final state among two nearly degenerate, when conventional STIRAP fails to resolve them. We demonstrate this selectivity across a broad range of two-photon detuning values and pulse chirp rates.
In the C-F-STIRAP, chirping of the pump and the Stokes pulses with different time delays permits a complete compensation of the two-photon detuning and results in a selective maximum coherence of the target state with higher spectral resolution than for conventional F-STIRAP. Applications of C-F-STIRAP to the NV center in diamond and the sensitivity enhancement of NV-based Ramsey spectroscopy are analyzed.
References
[1] J. Chathanathil, A. Ramaswamy, V. Malinovsky, D. Budker, S. A. Malinovskaya, ”Chirped fractional stimulated Raman adiabatic passage,” Phys. Rev. A. 108, 043710 (2023).
The CSRS and CARS techniques serve as an efficient tool to observe and coherently control vibrational dynamics in complex molecular systems. Generally, solvent environment increases complexity of the energy distribution and decreases coherence time owing to the coupling between the solute and solvent molecules. It significantly complicates light-matter interactions and makes it more difficult to find mechanisms of energy transfer, which requires high precision control.
Theoretical studies address (a) control of excitation of molecular vibrations taking into consideration phenomena originated in condensed phase, and (b) manifestation of dynamical changes in CSRS and CARS spectroscopy. We develop quantum theory of coherent stimulated Raman scattering (CSRS) and coherent anti-Stokes Raman scattering (CARS) spectroscopy and microscopy in application to investigation of ultrafast dynamics of polyatomic molecular systems on real time scale and to advance noninvasive imaging techniques.
A semiclassical theory is developed describing a multimode molecular system involved in the CSRS dynamics. A model system consists of a set of quantum, two-level systems describing normal vibrational modes in a molecule. External electromagnetic fields are treated classically. The theory is developed for an impulsive and non-impulsive stimulated Raman scattering, determined by the pulse duration with respect to a typical period of vibrational motion. Maxwell-Bloch equations are developed to determine evolution of Raman fields as a function of the induced polarization [NSP05]. Femtosecond pulse shaping is analyzed in terms of pulse amplitude and phase modulation as control parameters for selective excitation of two-level systems. In [JCP04, JQC05] pulse shapes for the amplitude modulation are proposed to be used in impulsive Raman scattering. In [PRA06] a method for coherent control in non-impulsive regime is developed implementing a transform-limited pump pulse and a linearly-chirped Stokes pulse.
We analyzed a possibility to create a maximum coherence in a predetermined vibrational mode and optimize CARS signals at a given pulse intensity. We developed two new methods for adiabatic population transfer that maximizes state coherence by implementation of two linearly chirped pulses in the Raman configuration. One of the methods is particularly robust in experimental realization and led to a patent. We revealed the effects of relative phase and coupling between the vibrational modes on selective excitation in CARS microscopy. V. Patel, S.A. Malinovskaya, Phys. Rev. A 83, 013413 (2011); V. Patel, V. Malinovsky, S. Malinovskaya, Phys. Rev. A 81, 063404 (2010); S. Malinovskaya, Opt. Comm. 282, 3527 (2009); S.A. Malinovskaya, V.S. Malinovsky, J. Mod. Opt. 55, 3101 (2008); S.A. Malinovskaya, Int. J. Quant. Chem. 107, 3151 (2007); S.A. Malinovskaya, V.S. Malinovsky, Opt. Lett. 32, 707 (2007); S.A. Malinovskaya, Phys. Rev. A 73, 033416 (2006).
Mirrorless lasing has been a topic of particular interest for about a decade due to promising new horizons for quantum science and applications. In this project, we review first-principles theory that describes this phenomenon, and study degenerate mirrorless lasing in a vapor of Rb atoms, the mechanisms of amplification of light generated in the medium with population inversion between magnetic sublevels within the line, and challenges associated with experimental realization.
Keywords: quantum optics, stimulated emission processes, mirrorless lasing, amplified spontaneous emission, alkali vapors
DOI: 10.3103/S1060992X23070172
Based on the dressed state analysis originated from the Liouville von Neumann equation with relaxation, we developed a method to sustain high level of coherence in the selected vibrational mode in the presence of fast vibrational energy relaxation. The method implements two chirped pulse trains with the repetition rate close to the relaxation rate. S.A. Malinovskaya, J. Mod. Opt. 56, 784 (2009); S.A. Malinovskaya, Opt. Lett. 33, 2245 (2008).
Retinal proteins, often called rhodopsins, are involved in a variety of responses of living cells to light, e.g., vision in higher organisms. All rhodopsins contain the molecule retinal as their chromophore. The activation of the rhodopsins is initiated by a photoinduced isomerization of retinal, which represents one of the fastest chemical reactions. Understanding the mechanism of the isomerization of the retinal in the visual pigment rhodopsin and development of the methods for control of the isomerization yield is the objective of our research . We develop a theory and perform numerical calculations of ultrafast dynamics in the rhodopsin molecule subject to interaction with external ultrafast electromagnetic fields.
In the framework of quantum-chemical methods (Restricted Hartree-Fock, Moller-Plesset perturbation theory and Density Functional Theory) we analyzed the charge transfer in the rhodopsin and the bacteriorhodopsin as a mechanism for photoinduced isomerization reaction. We demonstrated that the isomerization reaction is accompanied by the substantial charge transfer within the isomerization region. Understanding the mechanism of the retinal in the visual pigment rhodopsin provides vital information for the development of methods for control of the isomerization yield. B. Corn, S.A. Malinovskaya, Int. J. Quant. Chem. 109, 3131 (2009).
The project is devoted to theoretical studies of the optical frequency comb interaction with molecules. The excitation of two-photon Raman transitions is investigated induced by two pulse trains with the locked phase and also by crafted femtosecond pulse trains. Possibilities of selective excitation of predetermined Raman transitions are investigated taking into account effects of decoherence. The objectives of the project are to gain insight into the mechanisms of pulse train interactions with matter, to learn about factors that govern molecular states time evolution, and to develop new control methods of molecular dynamics in the presence of fast decoherence.
The optical frequency combs were implemented for rovibrational cooling of molecules from the Feshbach states. We developed a semiclassical theory of an optical frequency comb interaction with a three-level system and taking into account decoherence. We proposed a novel method for cooling of internal degrees of freedom in molecules from Feshbach states using a single, phase modulated optical frequency comb. The mechanism is based on the adiabatic, coherent accumulation of the population in the target, ultracold molecular state. S. Malinovskaya, W. Shi, J. Mod. Opt. 57, 1871 (2010); S. Malinovskaya, V. Patel, T. Collins, Int. J. Quant. Chem. 110, 3080 (2010); W. Shi, S. Malinovskaya, Phys. Rev. A 82, 013407 (2010); S.A. Malinovskaya, T. Collins, V. Patel, Adv. Quant. Chem. (2012).
In light of newest advancements in x-ray pulsed radiation, theoretical investigations of electron and nuclear dynamics in molecules following core-electron excitation or ionization have become of particular interest. In this project we study molecular dynamics following core-shell interaction with x-ray pulses and focus on the development of time-dependent picture of the resonant x-ray emission, Auger emission and resonant x-ray stimulated Raman scattering. We develop coherent control methods applicable to x-ray pulsed radiation to govern core-excitation and the induced dynamics. The objectives of investigations include time-dependent formulation of dynamical symmetry breaking and core-hole localization in highly symmetrical molecules, control of dynamical distortions caused by vibronic coupling, and the study of dissociation dynamics of the core-excited molecules. Work on this project helps us in understanding of the nature of the x-ray pulse interaction with matter, explains many features present in the x-ray and Auger spectra originated from the vibronic coupling of the core-excited state manifold, and will result in new methods of quantum control of molecular dynamics.
This project is devoted to the implementation of OCT to study dynamics and to develop methods to control coherence in multilevel systems. We implement the Krotov method to find the control fields to maximize coherence between predetermined states for the resonance and off-resonance case. P. Kumar, S.A. Malinovskaya, V.S. Malinovsky, J. Phys. B: At. Mol. Opt. Phys. 44, 154010 (2011).
We performed studies of the quantum dynamics using OCT in the presence of laser field noise. We investigated the dynamics in the HF molecule and the OH radical induced by noisy control fields and learned the extent to which noise is tolerable without a loss of controllability. Robust noisy control fields are obtained for the field-to-noise ratio ranging from 1 to 10. We demonstrated that in the presence of small amplitudes of noise, noise cooperates with the field following the stochastic resonance mechanism. P. Kumar, S. A. Malinovskaya, J. Mod. Opt. 57, 1243 (2010).