A coherent mechanism of robust population inversion in atomic and molecular systems by a chirped field is presented. It is demonstrated that a field of sufficiently high chirp rate imposes a certain relative phase between a ground and excited state wavefunction of a two-level system. The value of the relative phase angle is thus restricted to be negative and close to 0 or $-\\pi$ for positive and negative chirp, respectively. This explains the unidirectionality of the population transfer from the ground to the excited state. In a molecular system composed of a ground and excited potential energy surface the symmetry between the action of a pulse with a large positive and negative chirp is broken. The same framwork of the coherent mechanism can explain the symmetry breaking and the population inversion due to a positive chirped field.
A coherent mechanism of robust population inversion in atomic and molecular systems by a chirped field is presented. It is demonstrated that a field of sufficiently high chirp rate imposes a certain relative phase between a ground and excited state wavefunction of a two-level system. The value of the relative phase angle is thus restricted to be negative and close to 0 or −pi for positive and negative chirp, respectively. This explains the unidirectionality of the population transfer from the ground to the excited state. In a molecular system composed of a ground and excited potential energy surface the symmetry between the action of a pulse with a large positive and negative chirp is broken. The same framwork of the coherent mechanism can explain the symmetry breaking and the population inversion due to a positive chirped field.
A coherent mechanism of robust population inversion in atomic and molecular systems by a chirped field is presented. It is demonstrated that a field of sufficiently high chirp rate imposes a certain relative phase between a ground and excited state wavefunction of a two-level system. The value of the relative phase angle is thus restricted to be negative and close to 0 or - pi for positive and negative chirp, respectively. This explains the unidirectionality of the population transfer from the ground to the excited state.In a molecular system composed of a ground and excited potential energy surface the symmetry between the action of a pulse with a large positive and negative chirp is broken. The same framwork of the coherent mechanism can explain the symmetry breaking and the population inversion due to a positive chirped field.
Detailed theoretical analysis and numerical simulation indicate that nearly complete electronic population inversion of molecular systems can be achieved with intense positively chirped broadband laser pulses. To provide a simple physical picture, a two-level model is used to examine the condition for the so-called π pulses and a four-level model is designed to demonstrate for molecular systems the correlation between the sign of the chirp and the excited state population. The proposed molecular π pulse is the combined result of vibrational coherence in the femtosecond regime and adiabatic inversion in the picosecond regime. Numerical results for a displaced oscillator, for LiH and for I2, show that the proposed molecular π pulse scheme is robust with respect to changes in field parameters such as the linear positive chirp rate, field intensity, bandwidth, and carrier frequency, and is stable with respect to thermal and condensed phase conditions including molecular rotation, rovibronic coupling, and electronic dephasing.
We discuss electronic population transfer in diatomic molecules. By analyzing time-dependent wave packets on electronic potential-energy surfaces, we investigate the efficiency and robustness of population transfer with intense, chirped laser pulses. Recently, the magnitude of the population transfer was observed to have a remarkable dependence on the sign of the chirp [J. Cao, C. J. Bardeen, and K. R. Wilson, Phys. Rev. Lett. 80, 1406 (1998)]. In this work we explain the reason for this asymmetry, and show how the frequency detuning, intensity, and chirp rate affect the results. In particular, we demonstrate efficient, robust population transfer for both positive and negative chirps. A Landau-Zener model of multiple avoided crossings is invoked to model the results.
Theoretical analysis leads us to the intriguing conclusion that nearly complete electronic population inversion of molecules can be achieved with intense positively chirped broadband laser pulses, as a combined result of vibrational coherence and adiabatic inversion. Strong field quantum calculations demonstrate inversion probabilities of up to 99%. The results are robust with respect to changes in light field parameters as well as to thermal and condensed phase conditions, are supported by experimental evidence, and have many potential applications in chemistry, biochemistry, biology, and physics.
A chirped laser pulse transfers population from one level to another level accessible by one photon dipole transition. We have used a pair of phase-locked chirped pulses of same frequency instead of a single chirped pulse to achieve phase control over the population transfer and thus creating coherent population distribution in hydrogen molecule. Simultaneous actions of the phase controlled interference and rapid adiabatic passages due to chirped pulses lead to the control in population transfer from the ground X(v = 0, j = 0) level to the C(v = 2, j = 1) level. We have extended this two-level system to a three-level 1 + 1 ladder system for population transfer from the X level to the J(v = 2, j = 2) level via the C intermediate level using two pairs of phase-locked laser chirped pulses and have achieved laudable control over the coherent population distribution.
Population inversion from an initial quantum state to a desired quantum state represents an exciting new frontier for quantum manipulation; that frontier is endowed with a strong interdisciplinary character and connections to other scientific fields, including atomic, molecular, and optical physics, as well as in solid-state devices, for fundamental studies, nuclear magnetic resonance and other spectroscopic techniques, metrology, interferometry, optical control of chemical reactions or quantum-information applications. Two-level systems are ubiquitous in these areas, and the driving of a population inversion is an important operation. So far various schemes for population transfer to a target state from an initial state have been proposed in theory and implemented in experiment. To be useful, such methods must, of course, be reliable, fast, and robust. Most literatures on two-level models investigated population inversion, which could be modelled by infinite-time processes. In this paper, by using a composite adiabatic passage (CAP) technique—in which the single pulse driving the quantum transition is replaced by a sequence of pulses with well-defined control phases, we investigate the population inversion problem of two-level quantum system with a finite duration. We take a sinusoidally varying pulse model that continuously vanishes at the beginning and the end of the finite duration as an example. The high-fidelity population inversion of the two-level system with finite duration is achieved. We discuss the effects of both coupling strength and detuning strength on the transition probability. It is found that this protocol could suppress the oscillations in the transition probability and reduce the admissible error bellow the 10 -4 quantum computation benchmark. The fidelity can arrive at 1, even with simple three- and five-composite pulse sequences. The protocol combines the advantages of adiabatic passage and composite pulses techniques. By choosing the composite phases appropriately, a high-fidelity, fast, stable and extremely robust complete population inversion is achieved for the finite-time two-level model. The values of the composite phases are universal for they do not depend on the pulse shapes and the chirp as long as the latter satisfy the symmetry property. Furthermore, the classical Hamiltonian is applied to describe the dynamic properties of the quantum system and further verify the effectiveness and feasibility of the proposed CAP technique. The results we present here are general and in principle apply to any two- and multi-level quantum systems. The accuracy of the CAP technique and its robustness against parameter variations make the protocol suitable for ultrahigh-fidelity quantum manipulation. We believe that the protocol can be widely used in many different areas of science, ranging from the quantum information, the quantum chemical, and the quantum optics to the ultracold atomic and molecular physics.