arXiv subjects

Christiane P. Koch

Publications and source records attributed to Christiane P. Koch.

At least 127 records · Page 7Linked to original sources

arXiv2012

Monotonically convergent optimization in quantum control using Krotov's method

The non-linear optimization method developed by Konnov and Krotov [Automation and Remote Control 60, 1427 (1999)] has been used previously to extend the capabilities of optimal control theory from the linear to the non-linear Schrödinger equation [Sklarz and Tannor, Phys. Rev. A 66, 053619 (2002)]. Here we show that based on the Konnov-Krotov method, monotonically convergent algorithms are obtained for a large class of quantum control problems. It includes, in addition to non-linear equations of motion, control problems that are characterized by non-unitary time evolution, non-linear dependencies of the Hamiltonian on the control, time-dependent targets and optimization functionals that depend to higher than second order on the time-evolving states. We furthermore show that the non-linear (second order) contribution can be estimated either analytically or numerically, yielding readily applicable optimization algorithms. We demonstrate monotonic convergence for an optimization functional that is an eighth-degree polynomial in the states. For the 'standard' quantum control problem of a convex final-time functional, linear equations of motion and linear dependency of the Hamiltonian on the field, the second-order contribution is not required for monotonic convergence but can be used to speed up convergence. We demonstrate this by comparing the performance of first and second order algorithms for two examples.

quant-ph↗

arXiv2011

Generating Molecular Rovibrational Coherence by Two-Photon Femtosecond Photoassociation of Thermally Hot Atoms

The formation of diatomic molecules with rotational and vibrational coherence is demonstrated experimentally in free-to-bound two-photon femtosecond photoassociation of hot atoms. In a thermal gas at a temperature of 1000 K, pairs of magnesium atoms, colliding in their electronic ground state, are excited into coherent superpositions of bound rovibrational levels in an electronically excited state. The rovibrational coherence is probed by a time-delayed third photon, resulting in quantum beats in the UV fluorescence. A comprehensive theoretical model based on ab initio calculations rationalizes the generation of coherence by Franck-Condon filtering of collision energies and partial waves, quantifying it in terms of an increase in quantum purity of the thermal ensemble. Our results open the way to coherent control of a binary reaction.

quant-ph↗

arXiv2011

Controlling a diatomic shape resonance with non-resonant light

A (diatomic) shape resonance is a metastable state of a pair of colliding atoms quasi-bound by the centrifugal barrier imposed by the angular momentum involved in the collision. The temporary trapping of the atoms' scattering wavefunction corresponds to an enhanced atom pair density at low interatomic separations. This leads to larger overlap of the wavefunctions involved in a molecule formation process such as photoassociation, rendering the process more efficient. However, for an ensemble of atoms, the atom pair density will only be enhanced if the energy of the resonance comes close to the temperature of the atomic ensemble. Herein we explore the possibility of controlling the energy of a shape resonance by shifting it toward the temperature of atoms confined in a trap. The shifts are imparted by the interaction of non-resonant light with the anisotropic polarizability of the atom pair, which affects both the centrifugal barrier and the pair's rotational and vibrational levels. We find that at laser intensities of up to $5\times 10^{9}$ W/cm$^2$ the pair density is increased by one order of magnitude for $^{87}$Rb atoms at $100 μ$K and by two orders of magnitude for $^{88}$Sr atoms at $20 μ$K.

physics.atom-ph↗

arXiv2011

Formation of ultracold SrYb molecules in an optical lattice by photoassociation spectroscopy: theoretical prospects

State-of-the-art {\em ab initio} techniques have been applied to compute the potential energy curves for the SrYb molecule in the Born-Oppenheimer approximation for the ground state and first fifteen excited singlet and triplet states within the coupled-cluster framework. The leading long-range coefficients describing the dispersion interactions at large interatomic distances are also reported. The electric transition dipole moments have been obtained as the first residue of the polarization propagator computed with the linear response coupled-cluster method restricted to single and double excitations. Spin-orbit coupling matrix elements have been evaluated using the multireference configuration interaction method restricted to single and double excitations with a large active space. The electronic structure data was employed to investigate the possibility of forming deeply bound ultracold SrYb molecules in an optical lattice in a photoassociation experiment using continuous-wave lasers. Photoassociation near the intercombination line transition of atomic strontium into the vibrational levels of the strongly spin-orbit mixed $b^3Σ^+$, $a^3Π$, $A^1Π$, and $C^1Π$ states with subsequent efficient stabilization into the $v^{\prime\prime}=1$ vibrational level of the electronic ground state is proposed. Ground state SrYb molecules can be accumulated by making use of collisional decay from $v^{\prime\prime}=1$ to $v^{\prime\prime}=0$. Alternatively, photoassociation and stabilization to $v^{\prime\prime}=0$ can proceed via stimulated Raman adiabatic passage provided that the trapping frequency of the optical lattice is large enough and phase coherence between the pulses can be maintained over at least tens of microseconds.

physics.atom-ph↗

arXiv2011

Prospects for fast Rydberg gates on an atom chip

Atom chips are a promising candidate for a scalable architecture for quantum information processing provided a universal set of gates can be implemented with high fidelity. The difficult part in achieving universality is the entangling two-qubit gate. We consider a Rydberg phase gate for two atoms trapped on a chip and employ optimal control theory to find the shortest gate that still yields a reasonable gate error. Our parameters correspond to a situation where the Rydberg blockade regime is not yet reached. We discuss the role of spontaneous emission and the effect of noise from the chip surface on the atoms in the Rydberg state.

quant-ph↗

arXiv2011

The Quantum Speed Limit of Optimal Controlled Phasegates for Trapped Neutral Atoms

We study controlled phasegates for ultracold atoms in an optical potential. A shaped laser pulse drives transitions between the ground and electronically excited states where the atoms are subject to a long-range 1/R^3 interaction. We fully account for this interaction and use optimal control theory to calculate the pulse shapes. This allows us to determine the minimum pulse duration, respectively, gate time T that is required to obtain high fidelity. We accurately analyze the speed limiting factors, and we find the gate time to be limited either by the interaction strength in the excited state or by the ground state vibrational motion in the trap. The latter needs to be resolved by the pulses in order to fully restore the motional state of the atoms at the end of the gate.

quant-ph↗

arXiv2010

Vibrational stabilization of ultracold KRb molecules. A comparative study

The transfer of weakly bound KRb molecules from levels just below the dissociation threshold into the vibrational ground state with shaped laser pulses is studied. Optimal control theory is employed to calculate the pulses. The complexity of modelling the molecular structure is successively increased in order to study the effects of the long-range behavior of the excited state potential, resonant spin-orbit coupling and singlet-triplet mixing.

physics.atom-ph↗

arXiv2010

Correlation dynamics after short-pulse photoassociation

Two atoms in an ultracold gas are correlated at short inter-atomic distances due to threshold effects where the potential energy of their interaction dominates the kinetic energy. The correlations manifest themselves in a distinct nodal structure of the density matrix at short inter-atomic distances. Pump-probe spectroscopy has recently been suggested [Phys. Rev. Lett. 103, 260401 (2009)] to probe these pair correlations: A suitably chosen, short photoassociation laser pulse depletes the ground state pair density within the photoassociation window, creating a non-stationary wave packet in the electronic ground state. The dynamics of this non-stationary wave packet is monitored by time-delayed probe and ionization pulses. Here, we discuss how the choice of the pulse parameters affects experimental feasibility of this pump-probe spectroscopy of two-body correlations.

physics.atom-ph↗

arXiv2009

A Chebychev propagator with iterative time ordering for explicitly time-dependent Hamiltonians

A propagation method for time-dependent Schrödinger equations with an explicitly time-dependent Hamiltonian is developed where time ordering is achieved iteratively. The explicit time-dependence of the time-dependent Schrödinger equation is rewritten as an inhomogeneous term. At each step of the iteration, the resulting inhomogeneous Schrödinger equation is solved with the Chebychev propagation scheme presented in J. Chem. Phys. 130, 124108 (2009). The iteratively time-ordering Chebychev propagator is shown to be robust, efficient and accurate and compares very favorably to all other available propagation schemes.

quant-ph↗

arXiv2009

Pump-probe spectroscopy of two-body correlations in ultracold gases

We suggest pump-probe spectroscopy to study pair correlations that determine the many-body dynamics in weakly interacting, dilute ultracold gases. A suitably chosen, short laser pulse depletes the pair density locally, creating a 'hole' in the electronic ground state. The dynamics of this non-stationary pair density is monitored by a time-delayed probe pulse. The resulting transient signal allows to spectrally decompose the 'hole' and to map out the pair correlation functions.

quant-ph↗

arXiv2009

Photoassociation and coherent transient dynamics in the interaction of ultracold rubidium atoms with shaped femtosecond pulses - II. Theory

Photoassociation of ultracold rubidium atoms with femtosecond laser pulses is studied theoretically. The spectrum of the pulses is cut off in order to suppress pulse amplitude at and close to the atomic resonance frequency. This leads to long tails of the laser pulse as a function of time giving rise to coherent transients in the photoassociation dynamics. They are studied as a function of cutoff position and chirp of the pulse. Molecule formation in the electronically excited state is attributed to off-resonant excitation in the strong-field regime.

physics.atom-ph↗

arXiv2009

A Chebychev propagator for inhomogeneous Schrödinger equations

We present a propagation scheme for time-dependent inhomogeneous Schrödinger equations which occur for example in optimal control theory or in reactive scattering calculations. A formal solution based on a polynomial expansion of the inhomogeneous term is derived. It is subjected to an approximation in terms of Chebychev polynomials. Different variants for the inhomogeneous propagator are demonstrated and applied to two examples from optimal control theory. Convergence behavior and numerical efficiency are analyzed.

quant-ph↗

arXiv2009

Stimulating the production of deeply bound RbCs molecules with laser pulses: the role of spin-orbit coupling in forming ultracold molecules

We investigate the possibility of forming deeply bound ultracold RbCs molecules by a two-color photoassociation experiment. We compare the results with those for Rb_2 in order to understand the characteristic differences between heteronuclear and homonuclear molecules. The major differences arise from the different long-range potential for excited states. Ultracold 85Rb and 133Cs atoms colliding on the X^1Sigma+ potential curve are initially photoassociated to form excited RbCs molecules in the region below the Rb(5S) + Cs(6P_1/2) asymptote. We explore the nature of the Omega=0^+ levels in this region, which have mixed A^1Sigma^+ and b^3Pi character. We then study the quantum dynamics of RbCs by a time-dependent wavepacket (TDWP) approach. A wavepacket is formed by exciting a few vibronic levels and is allowed to propagate on the coupled electronic potential energy curves. For a detuning of 7.5 cm-1, the wavepacket for RbCs reaches the short-range region in about 13 ps, which is significantly faster than for the homonuclear Rb_2 system; this is mostly because of the absence of an R^-3 long-range tail in the excited-state potential curves for heteronuclear systems. We give a simple semiclassical formula that relates the time taken to the long-range potential parameters. For RbCs, in contrast to Rb_2, the excited-state wavepacket shows a substantial peak in singlet density near the inner turning point, and this produces a significant probability of deexcitation to form ground-state molecules bound by up to 1500 cm-1. Our analysis of the role of spin-orbit coupling concerns the character of the mixed states in general and is important for both photoassociation and stimulated Raman deexcitation.

physics.atom-ph↗

arXiv2008

Two-photon coherent control of femtosecond photoassociation

Photoassociation with short laser pulses has been proposed as a technique to create ultracold ground state molecules. A broad-band excitation seems the natural choice to drive the series of excitation and deexcitation steps required to form a molecule in its vibronic ground state from two scattering atoms. First attempts at femtosecond photoassociation were, however, hampered by the requirement to eliminate the atomic excitation leading to trap depletion. On the other hand, molecular levels very close to the atomic transition are to be excited. The broad bandwidth of a femtosecond laser then appears to be rather an obstacle. To overcome the ostensible conflict of driving a narrow transition by a broad-band laser, we suggest a two-photon photoassociation scheme. In the weak-field regime, a spectral phase pattern can be employed to eliminate the atomic line. When the excitation is carried out by more than one photon, different pathways in the field can be interfered constructively or destructively. In the strong-field regime, a temporal phase can be applied to control dynamic Stark shifts. The atomic transition is suppressed by choosing a phase which keeps the levels out of resonance. We derive analytical solutions for atomic two-photon dark states in both the weak-field and strong-field regime. Two-photon excitation may thus pave the way toward coherent control of photoassociation. Ultimately, the success of such a scheme will depend on the details of the excited electronic states and transition dipole moments. We explore the possibility of two-photon femtosecond photoassociation for alkali and alkaline-earth metal dimers and present a detailed study for the example of calcium.

physics.atom-ph↗

arXiv2008

Perspectives for coherent optical formation of strontium molecules in their electronic ground state

Optical Feshbach resonances [Phys. Rev. Lett. 94, 193001 (2005)] and pump-dump photoassociation with short laser pulses [Phys. Rev. A 73, 033408 (2006)] have been proposed as means to coherently form stable ultracold alkali dimer molecules. In an optical Feshbach resonance, the intensity and possibly frequency of a cw laser are ramped up linearly followed by a sudden switch-off of the laser. This is applicable to tightly trapped atom pairs. In short-pulse photoassociation, the pump pulse forms a wave-packet in an electronically excited state. The ensuing dynamics carry the wave-packet to shorter internuclear distances where, after half a vibrational period, it can be deexcited to the electronic ground state by the dump pulse. Short-pulse photoassociation is suited for both shallow and tight traps. The applicability of these two means to produce ultracold molecules is investigated here for $^{88}$Sr. Dipole-allowed transitions proceeding via the $B^1Σ_u^+$ excited state as well as transitions near the intercombination line are studied.

physics.atom-ph↗

arXiv2008

Engineering an all-optical route to ultracold molecules in their vibronic ground state

We propose an improved photoassociation scheme to produce ultracold molecules in their vibronic ground state for the generic case where non-adiabatic effects facilitating transfer to deeply bound levels are absent. Formation of molecules is achieved by short laser pulses in a Raman-like pump-dump process where an additional near-infrared laser field couples the excited state to an auxiliary state. The coupling due to the additional field effectively changes the shape of the excited state potential and allows for efficient population transfer to low-lying vibrational levels of the electronic ground state. Repetition of many pump-dump sequences together with collisional relaxation allows for accumulation of molecules in v=0.

physics.atom-ph↗

arXiv2008

Protecting coherence in Optimal Control Theory: State dependent constraint approach

Optimal control theory is developed for the task of obtaining a primary objective in a subspace of the Hilbert space while avoiding other subspaces of the Hilbert space. The primary objective can be a state-to-state transition or a unitary transformation. A new optimization functional is introduced which leads to monotonic convergence of the algorithm. This approach becomes necessary for molecular systems subject to processes implying loss of coherence such as predissociation or ionization. In these subspaces controllability is hampered or even completely lost. Avoiding the lossy channels is achieved via a functional constraint which depends on the state of the system at each instant in time. We outline the resulting new algorithm, discuss its convergence properties and demonstrate its functionality for the example of a state-to-state transition and of a unitary transformation for a model of cold Rb2.

quant-ph↗

arXiv2006

Theoretical model for ultracold molecule formation via adaptive feedback control

We investigate pump-dump photoassociation of ultracold molecules with amplitude- and phase-modulated femtosecond laser pulses. For this purpose a perturbative model for the light-matter interaction is developed and combined with a genetic algorithm for adaptive feedback control of the laser pulse shapes. The model is applied to the formation of 85Rb2 molecules in a magneto-optical trap. We find for optimized pulse shapes an improvement for the formation of ground state molecules by more than a factor of 10 compared to unshaped pulses at the same pump-dump delay time, and by 40% compared to unshaped pulses at the respective optimal pump-dump delay time. Since our model yields directly the spectral amplitudes and phases of the optimized pulses, the results are directly applicable in pulse shaping experiments.

physics.atom-ph↗