Composite pulses for high fidelity population transfer in three-level systems

In this work, we propose a composite pulses scheme by modulating phases to achieve high fidelity population transfer in three-level systems. To circumvent the obstacle that not enough variables are exploited to eliminate the systematic errors in the transition probability, we put forward a cost function to find the optimal value. The cost function is independently constructed either in ensuring an accurate population of the target state, or in suppressing the population of the leakage state, or both of them. The results demonstrate that population transfer is implemented with high fidelity even when existing the deviations in the coupling coefficients. Furthermore, our composite pulses scheme can be extensible to arbitrarily long pulse sequences. As an example, we employ the composite pulses sequence for achieving the three-atom singlet state in an atom-cavity system with ultrahigh fidelity. The final singlet state shows robustness against deviations and is not seriously affected by waveform distortions. Also, the singlet state maintains a high fidelity under the decoherence environment.

On the optimality of optical pumping for a closed Λ-system with large decay rates of the intermediate excited state

We use optimal control theory to show that for a closed Λ-system where the excited intermediate level decays to the lower levels with a common large rate, the optimal scheme for population transfer between the lower levels is actually optical pumping. In order to obtain this result we exploit the large decay rate to eliminate adiabatically the weakly coupled excited state, then perform a transformation to the basis comprised of the dark and bright states, and finally apply optimal control to this transformed system. Subsequently, we confirm the optimality of the optical pumping scheme for the original closed Λ-system using numerical optimal control. We also demonstrate numerically that optical pumping remains optimal when the decay rate to the target state is larger than that to the initial state or the two rates are not very different from each other. The present work is expected to find application in various tasks of quantum information processing, where such systems are encountered

Superposition of nuclear states in multi-lambda systems using x-ray laser pulses

Nuclear-state population transfer in the multi-lambda systems with N = 5 that interact with four X-ray laser pulses are investigated theoretically. By using the coincident pulses and stimulated Raman adiabatic passage (STIRAP) techniques, the population transfer from one initially populated ground state to an arbitrary coherent superposition of other ground states. Since the frequency of currently available X-ray lasers is lower than the gamma rays, in this method, X-ray laser pulses with different frequencies are interacting with the accelerated nuclei. We employ the Morris-Shore (MS) transformation to reduce the five-states system to two separate three-state and two-state linkage. The required laser intensities were calculated, which satisfy the conditions of coincident pulses and multi-lambda STIRAP techniques. Considering the spontaneous emission from excited states, the master equation has to be used for numerical study, and it is shown that an arbitrary superposition of final ground states can be obtained. Also, it is observed that by increasing the number of coincident pulses, the population of ground states gets closer to the ideal situation.

Dynamic signature of electronically nonadiabatic coupling in sodium hydride: a rigorous test for the symmetric quasi-classical model applied to realistic, ab initio electronic states.

Sodium hydride (NaH) in the gas phase presents a seemingly simple electronic structure making it a potentially tractable system for the detailed investigation of nonadiabatic molecular dynamics from both computational and experimental standpoints. The single vibrational degree of freedom, as well as the strong nonadiabatic coupling that arises from the excited electronic states taking on considerable ionic character, provides a realistic chemical system to test the accuracy of quasi-classical methods to model population dynamics where the results are directly comparable against quantum mechanical benchmarks. Using a simulated pump-probe experiment, this work presents computational predictions of population transfer through the avoided crossings of NaH via symmetric quasi-classical Meyer-Miller (SQC/MM), Ehrenfest, and exact quantum dynamics on realistic, ab initio potential energy surfaces. The main driving force for population transfer arises from a sharply localized avoided crossing between the C and D singlet sigma potential energy surfaces which causes most of the population to transfer between t=15 and t=30 fs depending on the initially excited vibronic wavepacket. While quantum mechanical effects are expected due to the reduced mass of NaH, predictions of the population dynamics from both the SQC/MM and Ehrenfest models perform remarkably well against the quantum dynamics benchmark. Additionally, an analysis of the vibronic structure in the nonadiabatically coupled regime and predicted transient absorption signatures are presented using a variational eigensolver methodology. The prospects for complementary experimental measurements are also assessed.