arXiv subjects

Christiane P. Koch

Publications and source records attributed to Christiane P. Koch.

At least 91 records · Page 5Linked to original sources

arXiv2016

Maximizing Hole Coherence in Ultrafast Photoionization of Argon with SPA-Optimization

Photoionization with attosecond pulses populates hole states in the photoion. Superpositions of hole states represent ideal candidates for time-dependent spectroscopy, for example via pump-probe studies. The challenge consists in identifying pulses that create coherent superpositions of hole states while satisfying practical constraints. Here, we employ quantum optimal control to maximize the degree of coherence between these hole states. To this end, we introduce a derivative-free optimization method with Sequential PArametrization update (SPA-optimization). We demonstrate the versatility and computational efficiency of SPA-optimization for photoionization in argon by maximizing the coherence between the $3s$ and $3p_0$ hole states using shaped attosecond pulses. We show that it is possible to maximize the hole coherence while simultaneously prescribing the ratio of the final hole state populations.

quant-ph↗

arXiv2016

Hybrid benchmarking of arbitrary quantum gates

We present a protocol for Interleaved Randomized Benchmarking of arbitrary quantum gates using Monte Carlo sampling of quantum states. It is generally applicable, including non-Clifford gates while preserving key advantages of Randomized Benchmarking such as error amplification as well as independence from state preparation and measurement errors. This property is crucial for implementations in many contemporary systems. Although the protocol scales exponentially in the number of qubits, it is superior to direct Monte Carlo sampling of the average gate fidelity in both the total number of experiments by orders of magnitude and savings in classical preprocessing, that are exponential.

quant-ph↗

arXiv2016

Direct probe of anisotropy in atom-molecule collisions via quantum scattering resonances

Anisotropy is a fundamental property of particle interactions. It occupies a central role in cold and ultra-cold molecular processes, where long range forces have been found to significantly depend on orientation in ultra-cold polar molecule collisions. Recent experiments have demonstrated the emergence of quantum phenomena such as scattering resonances in the cold collisions regime due to quantization of the intermolecular degrees of freedom. Although these states have been shown to be sensitive to interaction details, the effect of anisotropy on quantum resonances has eluded experimental observation so far. Here, we directly measure the anisotropy in atom-molecule interactions via quantum resonances by changing the quantum state of the internal molecular rotor. We observe that a quantum scattering resonance at a collision energy of $k_B$ x 270 mK appears in the Penning ionization of molecular hydrogen with metastable helium only if the molecule is rotationally excited. We use state of the art ab initio and multichannel quantum molecular dynamics calculations to show that the anisotropy contributes to the effective interaction only for $H_2$ molecules in the first excited rotational state, whereas rotationally ground state $H_2$ interacts purely isotropically with metastable helium. Control over the quantum state of the internal molecular rotation allows us to switch the anisotropy on or off and thus disentangle the isotropic and anisotropic parts of the interaction. These quantum phenomena provide a challenging benchmark for even the most advanced theoretical descriptions, highlighting the advantage of using cold collisions to advance the microscopic understanding of particle interactions.

physics.chem-ph↗

arXiv2016

Controlling open quantum systems: Tools, achievements, and limitations

The advent of quantum devices, which exploit the two essential elements of quantum physics, coherence and entanglement, has sparked renewed interest in the control of open quantum systems. Successful implementations face the challenge to preserve the relevant nonclassical features at the level of device operation. A major obstacle is decoherence which is caused by interaction with the environment. Optimal control theory is a tool that can be used to identify control strategies in the presence of decoherence. We review here recent advances in optimal control methodology that allow for tackling typical tasks in device operation for open quantum systems and discuss examples of relaxation-optimized dynamics. Optimal control theory is also a useful tool to exploit the environment for control. We discuss examples and point out possible future extensions.

quant-ph↗

arXiv2016

Photoassociation spectroscopy in Penning ionization reactions at sub-Kelvin temperatures

Penning ionization reactions in merged beams with precisely controlled collision energies have been shown to accurately probe quantum mechanical effects in reactive collisions. A complete microscopic understanding of the reaction is, however, faced with two major challenges---the highly excited character of the reaction's entrance channel and the limited precision of even the best state-of-the-art ab initio potential energy surfaces. Here, we suggest photoassociation spectroscopy as a tool to identify the character of orbiting resonances in the entrance channel and probe the ionization width as a function of inter-particle separation. We introduce the basic concept and discuss the general conditions under which this type of spectroscopy will be successful.

physics.atom-ph↗

arXiv2015

Quantum optimal control of photoelectron spectra and angular distributions

Photoelectron spectra and photoelectron angular distributions obtained in photoionization reveal important information on e.g. charge transfer or hole coherence in the parent ion. Here we show that optimal control of the underlying quantum dynamics can be used to enhance desired features in the photoelectron spectra and angular distributions. To this end, we combine Krotov's method for optimal control theory with the time-dependent configuration interaction singles formalism and a splitting approach to calculate photoelectron spectra and angular distributions. The optimization target can account for specific desired properties in the photoelectron angular distribution alone, in the photoelectron spectrum, or in both. We demonstrate the method for hydrogen and then apply it to argon under strong XUV radiation, maximizing the difference of emission into the upper and lower hemispheres, in order to realize directed electron emission in the XUV regime.

physics.atom-ph↗

arXiv2015

Hybrid Optimization Schemes for Quantum Control

Optimal control theory is a powerful tool for solving control problems in quantum mechanics, ranging from the control of chemical reactions to the implementation of gates in a quantum computer. Gradient-based optimization methods are able to find high fidelity controls, but require considerable numerical effort and often yield highly complex solutions. We propose here to employ a two-stage optimization scheme to significantly speed up convergence and achieve simpler controls. The control is initially parametrized using only a few free parameters, such that optimization in this pruned search space can be performed with a simplex method. The result, considered now simply as an arbitrary function on a time grid, is the starting point for further optimization with a gradient-based method that can quickly converge to high fidelities. We illustrate the success of this hybrid technique by optimizing a holonomic phasegate for two superconducting transmon qubits coupled with a shared transmission line resonator, showing that a combination of Nelder-Mead simplex and Krotov's method yields considerably better results than either one of the two methods alone.

quant-ph↗

arXiv2015

Training Schrödinger's cat: quantum optimal control

It is control that turns scientific knowledge into useful technology: in physics and engineering it provides a systematic way for driving a system from a given initial state into a desired target state with minimized expenditure of energy and resources -- as famously applied in the Apollo programme. As one of the cornerstones for enabling quantum technologies, optimal quantum control keeps evolving and expanding into areas as diverse as quantum-enhanced sensing, manipulation of single spins, photons, or atoms, optical spectroscopy, photochemistry, magnetic resonance (spectroscopy as well as medical imaging), quantum information processing and quantum simulation. --- Here state-of-the-art quantum control techniques are reviewed and put into perspective by a consortium uniting expertise in optimal control theory and applications to spectroscopy, imaging, quantum dynamics of closed and open systems. We address key challenges and sketch a roadmap to future developments.

quant-ph↗

arXiv2015

Coherent control of bond making: The performance of rationally phase-shaped femtosecond laser pulses

The first step in the coherent control of a photoinduced binary reaction is bond making or photoassociation. We have recently demonstrated coherent control of bond making in multi-photon femtosecond photoassociation of hot magnesium atoms, using linearly chirped pulses [Levin et al., arXiv:1411.1542]. The detected yield of photoassociated magnesium dimers was enhanced by positively chirped pulses which is explained theoretically by a combination of purification and chirp-dependent Raman transitions. The yield could be further enhanced by pulse optimization resulting in pulses with an effective linear chirp and a sub-pulse structure, where the latter allows for exploiting vibrational coherences. Here, we systematically explore the efficiency of phase-shaped pulses for the coherent control of bond making, employing a parametrization of the spectral phases in the form of cosine functions. We find up to an order of magnitude enhancement of the yield compared to the unshaped transform-limited pulse. The highly performing pulses all display an overall temporally increasing instantaneous frequency and are composed of several overlapping sub-pulses. The time delay between the first two sub-pulses almost perfectly fits the vibrational frequency of the generated intermediate wavepacket.These findings are in agreement with chirp-dependent Raman transitions and exploitation of vibrational dynamics as underlying control mechanisms.

physics.atom-ph↗

arXiv2015

Cold interactions between an Yb$^+$ ion and a Li atom: Prospects for sympathetic cooling, radiative association, and Feshbach resonances

The electronic structure of the (LiYb)$^+$ molecular ion is investigated with two variants of the coupled cluster method restricted to single, double, and noniterative or linear triple excitations. Potential energy curves for the ground and excited states, permanent and transition electric dipole movements, and long-range interaction coefficients $C_4$ and $C_6$ are reported. The data is subsequently employed in scattering calculations and photoassociation studies. Feshbach resonances are shown to be measurable despite the ion's micromotion in the Paul trap. Molecular ions can be formed in their singlet electronic ground state by one-photon photoassociation and in triplet states by two-photon photoassociation; and control of cold atom-ion chemistry based on Feshbach resonances should be feasible. Conditions for sympathetic cooling of an Yb$^+$ ion by an ultracold gas of Li atoms are found to be favorable in the temperature range of 10$\,$mK to 10$\,$nK; and further improvements using Feshbach resonances should be possible. Overall, these results suggest excellent prospects for building a quantum simulator with ultracold Yb$^+$ ions and Li atoms.

physics.atom-ph↗

arXiv2014

Asymptotic model for shape resonance control of diatomics by intense non-resonant light: Universality in the single-channel approximation

Non-resonant light interacting with diatomics via the polarizability anisotropy couples different rotational states and may lead to strong hybridization of the motion. The modification of shape resonances and low-energy scattering states due to this interaction can be fully captured by an asymptotic model, based on the long-range properties of the scattering [Crubellier et al. arXiv:1412.0569]. Remarkably, the properties of the field-dressed shape resonances in this asymptotic multi-channel description are found to be approximately linear in the field intensity up to fairly large intensity. This suggests a perturbative single-channel approach to be sufficient to study the control of such resonances by the non-resonant field. The multi-channel results furthermore indicate the dependence on field intensity to present, at least approximately, universal characteristics. Here we combine the nodal line technique to solve the asymptotic Schrödinger equation with perturbation theory. Comparing our single channel results to those obtained with the full interaction potential, we find nodal lines depending only on the field-free scattering length of the diatom to yield an approximate but universal description of the field-dressed molecule, confirming universal behavior.

physics.atom-ph↗

arXiv2014

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 capable of creating a maximally-entangled state out of some initial product state. The functional depends on easily-computable local invariants and uniquely determines when a gate evolves into 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.

quant-ph↗

arXiv2014

Optimizing for an arbitrary perfect entangler. II. Application

The difficulty of an optimization task in quantum information science depends on the proper mathematical expression of the physical target. Here we demonstrate the power of optimization functionals targeting an arbitrary perfect two-qubit entangler, creating a maximally-entangled state out of some initial product state. For two quantum information platforms of current interest, nitrogen vacancy centers in diamond and superconducting Josephson junctions, we show that an arbitrary perfect entangler can be reached faster and with higher fidelity than specific two-qubit gates or local equivalence classes of two-qubit gates. Our results are obtained with two independent optimization approaches, underlining the crucial role of the optimization target.

quant-ph↗

arXiv2014

Asymptotic model for shape resonance control of diatomics by intense non-resonant light

We derive a universal model for atom pairs interacting with non-resonant light via the polarizability anisotropy, based on the long range properties of the scattering. The corresponding dynamics can be obtained using a nodal line technique to solve the asymptotic Schrödinger equation. It consists in imposing physical boundary conditions at long range and vanishing of the wavefunction at a position separating inner zone and asymptotic region. We show that nodal lines which depend on the intensity of the non-resonant light can satisfactorily account for the effect of the polarizability at short range. The approach allows to determine the resonance structure, energy, width, channel mixing and hybridization even for narrow resonances.

physics.atom-ph↗

arXiv2014

Femtosecond wavepacket interferometry using the rotational dynamics of a trapped cold molecular ion

A Ramsey-type interferometer is suggested, employing a cold trapped ion and two time-delayed off-resonant femtosecond laser pulses. The laser light couples to the molecular polarization anisotropy, inducing rotational wavepacket dynamics. An interferogram is obtained from the delay dependent populations of the final field-free rotational states. Current experimental capabilities for cooling and preparation of the initial state are found to yield an interferogram visibility of more than 80\%. The interferograms can be used to determine the polarizability anisotropy with an accuracy of about $\pm 2\%$, respectively $\pm 5\%$, provided the uncertainty in the initial populations and measurement errors are confined to within the same limits.

quant-ph↗

arXiv2014

Coherent Control of Bond Making

We demonstrate for the first time coherent control of bond making, a milestone on the way to coherent control of photo-induced bimolecular chemical reactions. In strong-field multiphoton femtosecond photoassociation experiments, we find the yield of detected magnesium dimer molecules to be enhanced for positively chirped pulses and suppressed for negatively chirped pulses. Our ab initio model shows that control is achieved by purification via Franck-Condon filtering combined with chirp-dependent Raman transitions. Experimental closed-loop phase optimization using a learning algorithm yields an improved pulse that utilizes vibrational coherent dynamics in addition to chirp-dependent Raman transitions. Our results show that coherent control of binary photo-reactions is feasible even under thermal conditions.

physics.atom-ph↗

arXiv2014

Laser pulses for coherent xuv Raman excitation

We combine multi-channel electronic structure theory with quantum optimal control to derive Raman pulse sequences that coherently populate a valence excited state. For a neon atom, Raman target populations of up to 13% are obtained. Superpositions of the ground and valence Raman states with a controllable relative phase are found to be reachable with up to 4.5% population and phase control facilitated by the pump pulse carrier envelope phase. Our results open a route to creating core-hole excitations in molecules and aggregates that locally address specific atoms and represent the first step towards realization of multidimensional spectroscopy in the xuv and x-ray regimes.

quant-ph↗

arXiv2014

Exploiting Non-Markovianity of the Environment for Quantum Control

When the environment of an open quantum system is non-Markovian, amplitude and phase flow not only from the system into the environment but also back. Here we show that this feature can be exploited to carry out quantum control tasks that could not be realized if the system was isolated. Inspired by recent experiments on superconducting phase circuits, we consider an anharmonic ladder with resonant amplitude control only. This restricts realizable operations to SO(N). The ladder is immersed in an environment of two-level systems. Strongly coupled two-level systems lead to non-Markovian effects, whereas the weakly coupled ones result in single-exponential decay. Presence of the environment allows for implementing diagonal unitaries that, together with SO(N), yield the full group SU(N). Using optimal control theory, we obtain errors that are solely $T_1$-limited.

quant-ph↗