In the present work we analyze the dipole response of a diatomic heteronuclear molecule on the nonperturbative action of the external low-frequency laser field. Main results are obtained by numerical solution of the time-dependent Schrodinger equation for the nuclear subsystem of the molecule. We study the spectrum of polarization response and the influence of the coherent repopulation of the ro-vibrational states on it. Generally, we consider two cases: repopulation due to Raman-type transitions leading to the interference stabilization of the molecule and repopulation arising as a result of extremely short pulse action. We also study the transformation of a weak probe pulse propagating through the highly excited medium of the studied molecules.
In the present work we analyze the dipole response of a diatomic heteronuclear molecule on the nonperturbative action of the external low-frequency laser field. Main results are obtained by numerical solution of the time-dependent Schrodinger equation for the nuclear subsystem of the molecule. We study the spectrum of polarization response and the influence of the coherent repopulation of the ro-vibrational states on it. Generally, we consider two cases: repopulation due to Raman-type transitions leading to the interference stabilization of the molecule and repopulation arising as a result of extremely short pulse action. We also study the transformation of a weak probe pulse propagating through the highly excited medium of the studied molecules.
We propose a theoretical model used for dynamically manipulating an ultracold weakly bound heteronuclear alkali-metal diatomic molecule by a nonresonant single-cycle THz laser pulse. Taking the 6Li23Na molecule as an example, we first calculate the variation of the weakly bound state and quasibound state as a function of external electric field, and then reveal abundant interference patterns during and after the laser pulse due to the superpositions between states involving weakly bound state, scattering state, and quasibound state. Moreover, one can map out the nodes of the probability density of the weakly bound molecules by measuring the wavepacket dynamics.
Abstract We theoretically investigate molecular vibrational dynamics driven by intense and broadband terahertz (THz) pulses. The light–nuclei interaction is derived from a fully quantum-mechanical minimal coupling Hamiltonian to analyse the direct excitation of vibrational modes by the THz pulses. We show that for diatomic molecules a ‘vibrational moment’ can be defined in a manner similar to the dipole moment and that it has non-zero values only for heteronuclear diatomic molecules. Taking ultra-cold heteronuclear diatomic molecules as examples, we show that vibrational-mode excitation by THz pulse irradiation occurs in an almost stepwise manner, especially for low vibrational modes. A coherent control method using a frequency-controlled THz pulse sequence is also proposed.
The interaction is studied of a Gaussian pulsed or a continuous wave (CW) electric field with a molecule that has a nonzero difference d between the permanent dipoles of the ground and excited states involved in a transition. The unusual spectral effects associated with the transition with d ≠ 0, relative to the often studied case with d = 0, have been investigated previously in the two-level approximation and for continuous wave lasers. The observation of these effects, including markedly increased periods of excited state populations and negative Bloch-Siegart shifts, will often require the intense fields associated with pulsed rather than purely continuous wave electric fields. Transitions induced by continuous wave and pulsed laser-‘permanent dipole molecule’ interactions, for high field intensities and varying pulse durations, are investigated with model calculations carried out using exact Floquet and symmetry-adapted Riemann product integral methods. These calculations illustrate how the increased period of the excited state populations for dipolar molecules, and the associated molecule-field couplings, can be probed by sampling the time-dependent populations of the excited states using ultrashort to short pulses. The discussion illustrates the predictive and interpretive importance of the analytical expression for the molecule-EMF coupling provided by the rotating wave approximation (RWA) with d ≠ 0. The examples considered show, for example, temporal beating effects between the field and the RWA or Rabi frequencies and their dependence on d.
The absolute laser phase dependence of the time-dependent populations of the molecular states, including the steady-state (long time) populations of the states, associated with the interaction of a molecule with a pulsed laser is investigated using illustrative two-level examples. One-photon transitions, including the effects of permanent dipoles, are discussed as a function of the pulse duration, intensity, and (absolute) laser phase, for selected laser frequencies. The effects of laser phase can be large, depending on the values of the pulse duration for a given frequency and intensity. The effects of permanent dipoles, relative to no permanent dipoles, are significant for large laser field strengths ε0. When the laser-molecule coupling parameter b=μ12ε0/E21⩾0.2, where μ12 and E21 are the transition dipole and energy difference between the ground and excited states, respectively, the dynamics of the pulse-molecule interaction are (strongly) phase dependent, independent of pulse duration, whereas the corresponding steady-state populations of the molecular states may or may not be phase-dependent depending on the pulse duration. Analytical rotating wave approximations for pulsed laser-molecule interactions are useful for interpreting the dynamics and the steady-state results as a function of field strength and pulse duration, including the effects of permanent dipole moments. The results reported in this paper are based on molecular parameters associated with an S0→S1 electronic transition in a dipolar molecule. However, they are presented in reduced form and therefore can be scaled to other regions of the electromagnetic spectrum. Short, intense pulses at or beyond the limits of current laser technology will often be required for the types of absolute laser phase effects of this paper to be appreciable for electronic excitations. The discussion, in the UV-VIS, also suffers from the use of a two-level model and from the requirement of field intensities that can be beyond the Keldysh limit. For other spectral regions, these absolute laser phase effects will be much more readily applicable.
Excitation of multilevel Rydberg states (atoms and diatomic molecules) is studied under an intense time-periodic perturbation that is instantaneously turned on and off. For a one-quantum excitation from a lower lying state, general expressions for the Laplace images of the population amplitudes of Rydberg states are obtained with regard to their decay characteristics. It is shown that the problem considered is reduced to the determination of the positions and widths of the energy levels of a quantum system in the field of monochromatic laser radiation of the same frequency and intensity as that in a pulse mode. To determine these quantities, an integral formulation is proposed for the eigenvalue problem for energies that is relatively simply solved with regard to the effect of the ionic core and its complex vibration-rotation structure on diatomic molecules. The specific features of the excitation of Rydberg states and the behavior of Rydberg wave packets are studied depending on the intensity and duration of laser radiation. A quantum phenomenon of rotational orientation of electron-excited diatomic molecules is considered.
We model the response of a molecular medium to an intense pulse of light. We begin by reducing the Maxwell-Bloch equations for a multilevel molecular model system to a set of simplified propagation equations. We thereby obtain expressions for the frequency, temperature, and field intensity dependence of the ground and excited electronic state absorption cross sections, and the emission cross section, as well as the temperature dependence of the decay rate of the excited state. The phenomena of saturation, excited-state absorption, optically induced dichroism and birefringence, vibronic energy transfer, induced molecular alignment, decay of the matter-field interaction energy, and rotational diffusion are considered within the general formalism for describing the propagation of an intense pulse of light in the molecular medium. We find that the cross section for absorption (emission) of a photon is not identical to the cross section for molecular excitation (deexcitation) via the matter-field interaction. This is explained in terms of an energy balance between the matter, radiation, the matter-radiation interaction, and the bath responsible for the broadening of the molecular transitions. The inequality of these cross sections determines whether the system supplies or draws energy from the thermal bath. The rise in the vibrational temperature of molecules subjected to an intense short pulse is shown to significantly affect propagation of the pulse. The alignment of the molecular system resulting from saturation of the ground-state transition by a polarized laser pulse and the effects of the orientational dependence of the matter-field interaction including effects of rotational diffusion are determined. As an example of the formalism we consider pulse propagation in a Rhodamine 6G solution. We fit the parameters of the model to determine the frequency dependence of the ground- and excited-state absorption cross sections and the emission cross section and compare with experimentally determined cross sections. We describe the propagation of a pulse whose temporal width is comparable to the rotational diffusion time of the molecules in the dye solution and calculate polarization pulse probe signals.