Daniel M. Reich

Illuminating Molecular Symmetries with Bicircular High-Order-Harmonic Generation

We present a general theory of bicircular high-order-harmonic generation from N-fold rotationally symmetric molecules. Using a rotating frame of reference we predict the complete structure of the high-order-harmonic spectra for arbitrary driving frequency ratios and show how molecular symmetries can be directly identified from the harmonic signal. Our findings reveal that a characteristic fingerprint of rotational molecular symmetries can be universally observed in the ultrafast response of molecules to strong bicircular fields.

Optimal quantum control of Bose-Einstein condensates in magnetic microtraps: Comparison of gradient-ascent-pulse-engineering and Krotov optimization schemes

We study optimal quantum control of the dynamics of trapped Bose-Einstein condensates: The targets are to split a condensate, residing initially in a single well, into a double well, without inducing excitation, and to excite a condensate from the ground state to the first-excited state of a single well. The condensate is described in the mean-field approximation of the Gross-Pitaevskii equation. We compare two optimization approaches in terms of their performance and ease of use; namely, gradient-ascent pulse engineering (GRAPE) and Krotov’s method. Both approaches are derived from the variational principle but differ in the way the control is updated, additional costs are accounted for, and second-order-derivative information can be included. We find that GRAPE produces smoother control fields and works in a black-box manner, whereas Krotov with a suitably chosen step-size parameter converges faster but can produce sharp features in the control fields.

Cooling molecular vibrations with shaped laser pulses: optimal control theory exploiting the timescale separation between coherent excitation and spontaneous emission

Laser cooling of molecules employing broadband optical pumping involves a timescale separation between laser excitation and spontaneous emission. Here, we optimize the optical pumping step using shaped laser pulses. We derive two optimization functionals to drive population into those excited state levels that have the largest spontaneous emission rates to the target state. We show that, when using optimal control, laser cooling of molecules works even if the Franck–Condon map governing the transitions is preferential to heating rather than cooling. Our optimization functional is also applicable to the laser cooling of other degrees of freedom provided the cooling cycle consists of coherent excitation and dissipative de-excitation steps whose timescales are separated.

Optimal control theory for a unitary operation under dissipative evolution

We show that optimizing a quantum gate for an open quantum system requires the time evolution of only three states irrespective of the dimension of Hilbert space. This represents a significant reduction in computational resources compared to the complete basis of Liouville space that is commonly believed necessary for this task. The reduction is based on two observations: the target is not a general dynamical map but a unitary operation; and the time evolution of two properly chosen states is sufficient to distinguish any two unitaries. We illustrate gate optimization employing a reduced set of states for a controlled phasegate with trapped atoms as qubit carriers and a iW AP S gate with superconducting qubits.

Femtosecond two-photon photoassociation of hot magnesium atoms: A quantum dynamical study using thermal random phase wavefunctions

Two-photon photoassociation of hot magnesium atoms by femtosecond laser pulses, creating electronically excited magnesium dimer molecules, is studied from first principles, combining ab initio quantum chemistry and molecular quantum dynamics. This theoretical framework allows for rationalizing the generation of molecular rovibrational coherence from thermally hot atoms [L. Rybak, S. Amaran, L. Levin, M. Tomza, R. Moszynski, R. Kosloff, C. P. Koch, and Z. Amitay, Phys. Rev. Lett. 107, 273001 (2011)]. Random phase thermal wavefunctions are employed to model the thermal ensemble of hot colliding atoms. Comparing two different choices of basis functions, random phase wavefunctions built from eigenstates are found to have the fastest convergence for the photoassociation yield. The interaction of the colliding atoms with a femtosecond laser pulse is modeled non-perturbatively to account for strong-field effects.

Steering the optimization pathway in the control landscape using constraints

We show how additional constraints, restricting the spectrum of the optimized pulse or confining the system dynamics, can be used to steer optimization in quantum control towards distinct solutions. Our examples are multi-photon excitation in atoms and vibrational population transfer in molecules. We show that a spectral constraint is most effective in enforcing non-resonant two-photon absorption pathways in atoms and avoiding unnecessarily broad spectra in Raman transitions in molecules. While a constraint restricting the system to stay in an allowed subspace is also capable of identifying non-resonant excitation pathways, it does not avoid spurious peaks in the pulse spectrum. Both constraints are compatible with monotonic convergence but imply different additional numerical costs.

Exploiting non-Markovianity for quantum control

Quantum technology, exploiting entanglement and the wave nature of matter, relies on the ability to accurately control quantum systems. Quantum control is often compromised by the interaction of the system with its environment since this causes loss of amplitude and phase. However, when the dynamics of the open quantum system is non-Markovian, amplitude and phase flow not only from the system into the environment but also back. Interaction with the environment is then not necessarily detrimental. We show that the back-flow of amplitude and phase can be exploited to carry out quantum control tasks that could not be realized if the system was isolated. The control is facilitated by a few strongly coupled, sufficiently isolated environmental modes. Our paradigmatic example considers a weakly anharmonic ladder with resonant amplitude control only, restricting realizable operations to SO(N). The coupling to the environment, when harnessed with optimization techniques, allows for full SU(N) controllability.

Optimizing for an arbitrary perfect entangler. I. Functionals

Optimal control theory is a powerful tool for improving figures of merit in quantum information tasks. Finding the solution to any optimal control problem via numerical optimization depends crucially on the choice of the optimization functional. Here, we derive a functional that targets the full set of two-qubit perfect entanglers, gates capableofcreatingamaximallyentangledstateoutofsomeinitialproductstate.Thefunctionaldepends oneasily computable local invariants and unequivocally determines whether a gate is a perfect entangler. Optimization with our functional is most useful if the two-qubit dynamics allows for the implementation of more than one perfect entangler. We discuss the reachable set of perfect entanglers for a generic Hamiltonian that corresponds to several quantum information platforms of current interest.

Optimizing for an arbitrary perfect entangler. II. Application

Author(s): Goerz, MH; Gualdi, G; Reich, DM; Koch, CP; Motzoi, F; Whaley, KB; Vala, J; Muller, MM; Montangero, S; Calarco, T | Abstract:

Arbitrary quantum-state preparation of a harmonic oscillator via optimal control

The efficient initialization of a quantum system is a prerequisite for quantum technological applications. Here we show that several classes of quantum states of a harmonic oscillator can be efficiently prepared by means of a Jaynes-Cummings interaction with a single two-level system. This is achieved by suitably tailoring external fields which drive the dipole and/or the oscillator. The time-dependent dynamics that leads to the target state is identified by means of optimal control theory (OCT) based on Krotovs method. Infidelities below