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APS Open Science

High-intensity optical-field population transfer between eigenstates

Anonymous, Yasuhiro Ohshima

Published Sep 8, 2026• 0 citations
Publisher

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 J = 1 / 2 to J = 3 / 2 via restricted WPI, and to J = 5 / 2 , 7 / 2 , and 9 / 2 via HOPE, was demonstrated with respective efficiencies of 90%, 85%, 70%, and 17%.

DOI
10.1103/sy5j-g2cq

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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 J = 1 / 2 to J = 3 / 2 via restricted WPI, and to J = 5 / 2 , 7 / 2 , and 9 / 2 via HOPE, was demonstrated with respective efficiencies of 90%, 85%, 70%, and 17%.
We present the experimental demonstration of a novel, efficient, and selective technique to prepare population inversion. The technique is an extension of Stark-chirped rapid adiabatic passage (SCRAP), i.e., SCRAP among three states. In this process a Lambda-type quantum system is driven by two laser pulses, the pump and Stokes pulses, which are appropriately detuned from transition frequencies. A third laser pulse induces a dynamic Stark shift in the upper energy level, and the timing of all three pulses is controlled in order to prepare population inversion between the two lower states in the Lambda-type level scheme. Our data on population transfer in nitric oxide (NO) molecules clearly show that SCRAP among three states provides an advantageous alternative to such techniques as stimulated Raman adiabatic passage.
Ultrafast pulse shapes are used to control simultaneously the optimal population transfer coefficients and rotational wave-packet quantum interferences in the $E{}^{1}{\ensuremath{\Sigma}}_{g}^{+}$ state of Li2{\mathrm{Li}}_{2}Li2​ $({\ensuremath{\nu}}_{E}=9,$ JE=27{J}_{E}=27JE​=27 and 29). By dividing the spectral bandwidth of the ultrafast pulses into multiple ``control domains'' centered on each resonant wavelength, the population transfer coefficients can be manipulated independently of the wave-packet interferences to maximize the Li2{\mathrm{Li}}_{2}Li2​ photoionization yield at arbitrary short pump-probe time delays. To investigate the population transfer coefficients with and without wave-packet interferences, respectively, the pump polarization is set to be either parallel to or at the magic angle (\ensuremath{\sim}55\ifmmode^\circ\else\textdegree\fi{}) relative to the probe polarization. A comparison is made between phases that are symmetric and antisymmetric about the resonances. The effects of resonant and nonresonant frequencies are separately established and quantified. It is estimated that up to 90% of the possible nonresonant Rabi oscillations can be brought into phase simultaneously for each rovibrational state in the wave packet, while at the same time a constant phase offset added to one of the control domains establishes the phase of the wave-packet interference.
Coherent light-matter interaction drives a variety of interesting processes in a quantum system. Rabi oscillation is one such process offering a periodic population transfer between quantum states in an ultrashort time scale. Here we demonstrate a robust and simple scheme to achieve femtosecond twophoton Rabi oscillations by intense NIR laser pulses, using excited He atoms prepared by EUV-FEL. The extension to multiphoton regime will expand the applicability to highly excited or dipole-forbidden states.
The main goal of this PhD work is an experimental study of coherent excitation of atomic and molecular wavepackets, i.e. superpositions of many quantum eigenstates, by shaped femtosecond pulses. Approaches allowing nearly complete population transfer between quantum eigenstates were well studied in the past within the two level approximation. In this work we focus on adiabatic and non-adiabatic methods of population transfer beyond the two-level approximation. Excitation of multi-level target states is possible due to broad spectrum of an ultrashort pulse which contains frequencies needed for multiple transitions to different states in the final superposition. At the same time, the spectrum of an ultrashort pulse can be modified, or ``shaped'', in order to affect the excitation process and control the amplitudes in the final superposition. Both non-adiabatic and quasi-adiabatic methods were first implemented and studied in electronic wavepackets in alkali atoms. The non-adiabatic approach revealed features linked to the strong-field perturbations of the energy level structure of the quantum system. An adiabatic method was implemented for the first time on a femtosecond time scale, and was thoroughly characterized. The control over complex amplitudes in the target superposition was demonstrated as well as completeness of the population transfer. In the second part of this work, we focused on coherent control of rotational wavepackets in diatomic molecules. Rotational excitation by a periodic train of femtosecond pulses was investigated in the context of ``delta-kicked'' rotor - a paradigm system for studying quantum chaos, and the effect of quantum resonance was demonstrated for the first time in a system of true quantum rotors. Control of uni-directional molecular rotation was proposed and demonstrated with a novel ``chiral pulse train'' - a sequence of femtosecond pulses with polarization rotating from pulse to pulse by a predefined angle. All the developed techniques offer new tools in coherent control of atomic and molecular wavepackets on an ultrashort time scale.
We present extended experimental investigations and numerical studies on coherently driven population inversion in a three-state molecular quantum system by sequential double-Stark-chirped rapid adiabatic passage (SCRAP) (D-SCRAP) and three-state-SCRAP (T-SCRAP). D-SCRAP and T-SCRAP are alternative extensions of SCRAP. In D-SCRAP and T-SCRAP, a $\ensuremath{\Lambda}$-type quantum system is coherently driven by two laser pulses, the pump and Stokes pulses, which are slightly detuned from transition frequencies. A third strong laser pulse induces dynamic Stark shifts of the relevant transitions. If the timing of the three pulses is appropriately chosen, the quantum system is prepared to almost complete population inversion between the two lower states in the $\ensuremath{\Lambda}$-type level scheme. The transfer process is robust with regard to fluctuations of experimental parameters, provided some limitations are met. The paper presents convincing experimental data on D-SCRAP and T-SCRAP, driving efficient and selective population transfer to a highly excited vibrational level in nitrous oxide (NO) molecules. T-SCRAP yields transfer efficiencies of up to 95%. The efficiency of T-SCRAP is almost uneffected by the limited lifetime of the intermediate state in the $\ensuremath{\Lambda}$ system. The paper also presents data on the accurate experimental determination of Rabi frequencies and Stark shifts. This involves measurements of power broadening, Autler-Townes splittings, and Stark-shifted spectral lines in NO molecules. Moreover, we discuss the calibration of absolute transfer efficiences by comparison with stimulated emission pumping. The experimental data are confirmed by extended numerical simulations. The simulations also serve to intensively study the properties and dynamics of D-SCRAP and T-SCRAP.