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Physical Review A

Simulation of stimulated Raman adiabatic passage from the 1 S to the 2 S states of the hydrogen and antihydrogen atoms

AbdAlGhaffar K. Amer, A. Capra, Tim Friesen, M. C. Fujiwara, Takamasa Momose, Chukman So, F. Robicheaux

Published Sep 16, 2025• 0 citations
Publisher

Abstract

Achieving a high population of antihydrogen and hydrogen atoms in the $2S$ level is essential for spectroscopy measurements testing similarities between matter and antimatter. We propose and examine the efficiency of applying the STIRAP (stimulated Raman adiabatic passage) process in achieving high population transfer from the 1$S$ to the $2S$ levels. We utilized a circularly polarized Lyman alpha $(\mathrm{Ly}\text{\ensuremath{-}}\ensuremath{\alpha})$ pulse to couple the $1S$ state to the $2P$ state and a microwave pulse to couple the $2P$ state and the $2S$ state. We calculate the efficiency of the STIRAP process for transferring the population between the stretched states $(1{S}_{d},2{S}_{d})$ as a function of experimental parameters such as Rabi frequencies and pulse durations. We find that a $\mathrm{Ly}\text{\ensuremath{-}}\ensuremath{\alpha}$ pulse with an energy of a few nanojoules could produce nearly perfect transfer at zero detunings for atoms on the laser beam axis. We extended the analysis to a thermal ensemble of atoms, where Doppler detuning affects the velocity distribution of the hydrogen atoms produced in the $2S$ level. We found that the width of such velocity distribution is controlled by the Rabi frequency. We show that the peak velocity of the hydrogen atoms in the $2S$ level after STIRAP can be controlled by the $\mathrm{Ly}\text{\ensuremath{-}}\ensuremath{\alpha}$ pulse detuning. The efficiency of STIRAP in transferring population increases at low temperature $(T\ensuremath{\sim}1\phantom{\rule{0.16em}{0ex}}\mathrm{mK})$. Finally, we show that a background magnetic field improves the transfer rates between the other trappable states $(1{S}_{c},2{S}_{c})$.

DOI
10.1103/wx74-xg4j

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Achieving a high population of antihydrogen and hydrogen atoms in the 2S2S2S level is essential for spectroscopy measurements testing similarities between matter and antimatter. We propose and examine the efficiency of applying the STIRAP (stimulated Raman adiabatic passage) process in achieving high population transfer from the 1SSS to the 2S2S2S levels. We utilized a circularly polarized Lyman alpha (Ly\ensuremath-\ensuremathα)(\mathrm{Ly}\text{\ensuremath{-}}\ensuremath{\alpha})(Ly\ensuremath-\ensuremathα) pulse to couple the 1S1S1S state to the 2P2P2P state and a microwave pulse to couple the 2P2P2P state and the 2S2S2S state. We calculate the efficiency of the STIRAP process for transferring the population between the stretched states (1Sd,2Sd)(1{S}_{d},2{S}_{d})(1Sd​,2Sd​) as a function of experimental parameters such as Rabi frequencies and pulse durations. We find that a Ly\ensuremath-\ensuremathα\mathrm{Ly}\text{\ensuremath{-}}\ensuremath{\alpha}Ly\ensuremath-\ensuremathα pulse with an energy of a few nanojoules could produce nearly perfect transfer at zero detunings for atoms on the laser beam axis. We extended the analysis to a thermal ensemble of atoms, where Doppler detuning affects the velocity distribution of the hydrogen atoms produced in the 2S2S2S level. We found that the width of such velocity distribution is controlled by the Rabi frequency. We show that the peak velocity of the hydrogen atoms in the 2S2S2S level after STIRAP can be controlled by the Ly\ensuremath-\ensuremathα\mathrm{Ly}\text{\ensuremath{-}}\ensuremath{\alpha}Ly\ensuremath-\ensuremathα pulse detuning. The efficiency of STIRAP in transferring population increases at low temperature (T\ensuremath∼1mK)(T\ensuremath{\sim}1\phantom{\rule{0.16em}{0ex}}\mathrm{mK})(T\ensuremath∼1mK). Finally, we show that a background magnetic field improves the transfer rates between the other trappable states (1Sc,2Sc)(1{S}_{c},2{S}_{c})(1Sc​,2Sc​).
Achieving a high population of antihydrogen/hydrogen atoms in the 2S level is essential for spectroscopy measurements testing similarities between matter and antimatter. We propose and examine the efficiency of applying the STIRAP (Stimulated Raman Adiabatic Passage) process in achieving high population transfer from the 1S to the 2S levels. We utilized a circularly polarized Lyman alpha, Ly-ααα, pulse to couple the 1S state to the 2P state and a microwave pulse to couple the 2P state and the 2S state. We calculate the efficiency of the STIRAP process for transferring the population between the stretched states (1Sd,2Sd)(1S_d, 2S_d)(1Sd​,2Sd​) as a function of experimental parameters such as Rabi frequencies and pulse durations. We find that a Ly-ααα pulse with an energy of a few nanojoules could produce nearly perfect transfer at zero detunings for atoms on the laser beam axis. We extended the analysis to a thermal ensemble of atoms, where Doppler detuning affects the velocity distribution of the hydrogen atoms produced in the 2S level. We found that the width of such velocity distribution is controlled by the Rabi frequency. We show that the peak velocity of the hydrogen atoms in the 2S level after STIRAP can be controlled by the Ly-ααα pulse detuning. The efficiency of STIRAP in transferring population increases at low temperature (T$\sim$1~mK). Finally, we show that a background magnetic field improves the transfer rates between the other trappable states (1Sc,2Sc)(1S_c, 2S_c)(1Sc​,2Sc​).
We investigate the coherent population transfer and associated effects for a three level atomic system, with the third level being a Rydberg state. The scheme adopted here is the stimulated Raman adiabatic passage (STIRAP). An atomic beam of metastable helium is orthogonally crossing two laser beams in a tunable dc electric field. The ir laser of 790 - 830 nm connects the triplet 3P state to the Rydberg states (n = 12 - 50) and the uv laser of 389 nm connects the metastable triplet 2S state to the triplet 3P state. A third laser of 1083 nm driving 2S-2P transition is applied downstream, providing a strong bichromatic force on the atoms remaining in the 2S state to deflect them, establishing the absolute count of Rydberg atoms. Rydberg atoms can be ionized by background thermal radiations at room temperature and it is observed in this experiment. This fact actually enables precise measurement, especially spectroscopy, of Rydberg atoms by simply looking at the ions, which are easy to detect. It is also confirmed that background thermal radiation could significantly redistribute the population between neighboring Rydberg states. The 2S, 3P and the final Rydberg states all have magnetic sub-levels, hence the linkage pattern of the excitation has non-trivial crossings, if the polarizations of the two lasers are not parallel to each other. Those phase differences in different excitation paths induced by the laser polarizations can lead to interference which would determine the excitation probability and the polarization of the excited atom. Theoretical calculations predict interesting interference patterns as a function of laser polarizations and Rabi frequencies. Those interference structures have been experimentally observed. Transverse velocity distribution in the atomic beam turns out to be a limiting factor in the efficiency of production of Rydberg atoms. The transverse velocity of an atom can not only induce one-photon detuning but also two-photon detuning, which could effectively reduce the STIRAP process efficiency. By adding a laser to make Doppler molasses in the transverse direction, we can heat or cool the atomic beam transversely and verify this effect. | 190 pages
We report studies of state-to-state vibrational energy transfer in an isolated polyatomic molecule driven by combined stimulated Raman adiabatic passage (STIRAP) and counter-diabatic fields (CDFs). The goal of these studies is development of a method for improving the efficiency of level-to-level population transfer under conditions that degrade the efficiency of conventional STIRAP-generated population transfer. The vehicles for our studies are selective population of one of a pair of near-degenerate states in nonrotating SCCl 2 and enhancing the yield of nonrotating HNC in the HCN → HNC isomerization reaction. The efficiency of the population transfer within a subset of states embedded in a manifold of states is examined for the cases in which the transition dipole moments between the initial and target states are much smaller than and comparable to the transition dipole moments between background states and for the case in which the subset states have large transition dipole moments with the background states. We show that, in a subset of states that is coupled to background states, a combination of STIRAP fields and CDFs that do not individually generate processes that are competitive with the desired population transfer can generate population transfer efficiency greater than can ordinary STIRAP with field strength and/or pulse duration similarly restricted and that the exact CDF for an isolated three-level system is a useful approximation to the exact CDF for three- and five-state systems embedded in background states. We report a study of the stability of the STIRAP and approximate CDF control protocol to variation of the CDF intensity, the relative phase between the STIRAP and CDFs, and the pulse duration.
The technique of stimulated Raman adiabatic passage (STIRAP) has become an established procedure for producing complete population inversion in atoms or molecules via application of Stokes and pump pulses in a counterintuitive sequence. Previously we reported on numerical and analytical investigations showing some of the additional and important phenomena that arise when some of the levels involved have nonzero angular momentum, the field polarization directions have no simplifying symmetries, and Zeeman splitting lifts the magnetic sublevel degeneracy. Here we verify our theoretical findings using the metastable neon system: 3^{3}3P0{\mathit{P}}_{0}P0​?3{\mathrm{?}}^{3}?3P1{\mathit{P}}_{1}P1​?3{\mathrm{?}}^{3}?3P2{\mathit{P}}_{2}P2​ with the corresponding angular momentum sequence J=0?J=1?J=2. In particular, we demonstrate that it is possible to transfer all population from the single initial state to any single selectable final magnetic sublevel M. Selectivity can be achieved either by choosing special laser polarization angles or, for fixed polarizations, by tuning the two lasers into two-photon resonance between the initial and desired final state. The complete control of magnetic sublevel population enabled by this procedure extends the customary experimental methods for producing oriented or aligned beams of atoms. In addition, we demonstrate very clearly the previous prediction that population transfer may fail for certain sets of parameters (detunings, Rabi frequencies, and polarization angles). \textcopyright{} 1996 The American Physical Society.
Stimulated Raman scattering involving adiabatic passage (STIRAP) is a proven technique for population transfer in three-level systems with strong oscillator strengths. We show that the STIRAP process should also yield high transfer efficiencies when the densities of states near the intermediate and final levels are high, provided certain criteria for the experimentally controllable parameters are met. We also show that high transfer efficiencies may even be possible when the pump and Stokes lasers can access levels outside of the three-level system. The criteria are derived with an approach that emphasizes the adiabatic nature of the transfer process in an eigenvector of the interaction Hamiltonian that resembles a trapped state. The results are compared to density matrix calculations.
Previous studies have demonstrated that when experimental conditions generate non-adiabatic dynamics that prevents highly efficient population transfer between states of an isolated system by stimulated Raman adiabatic passage (STIRAP), the addition of an auxiliary counter-diabatic field (CDF) can restore most or all of that efficiency. This paper examines whether that strategy is also successful in a non-isolated system in which the energies of the states fluctuate, e.g., when a solute is subject to collisions with solvent. We study population transfer in two model systems: (i) the three-state system used by Demirplak and Rice [J. Chem. Phys. 116, 8028 (2002)] and (ii) a four-state system, derived from the simulation studies of Demirplak and Rice [J. Chem. Phys. 125, 194517 (2006)], that mimics HCl in liquid Ar. Simulation studies of the vibrational manifold of HCl in dense fluid Ar show that the collision induced vibrational energy level fluctuations have asymmetric distributions. Representations of these asymmetric energy level fluctuation distributions are used in both models (i) and (ii). We identify three sources of degradation of the efficiency of STIRAP generated selective population transfer in model (ii): too small pulse areas of the laser fields, unwanted interference arising from use of strong fields, and the vibrational detuning. For both models (i) and (ii), our examination of the efficiency of STIRAP + CDF population transfer under the influence of the asymmetric distribution of the vibrational energy fluctuations shows that there is a range of field strengths and pulse durations under which STIRAP + CDF control of population transfer has greater efficiency than does STIRAP generated population transfer.