arXiv subjects

Christiane P. Koch

Publications and source records attributed to Christiane P. Koch.

At least 55 records · Page 3Linked to original sources

arXiv2022

Rational pulse design for enantiomer-selective microwave three-wave mixing

Microwave three-wave mixing allows for enantiomer-selective excitation of randomly oriented chiral molecules into rotational states with different energy. The random orientation of molecules is reflected in the degeneracy of the rotational spectrum with respect to the orientational quantum number $M$ and reduces, if not accounted for, enantiomer-selectivity. Here, we show how to design pulse sequences with maximal enantiomer-selectivity from an analysis of the $M$-dependence of the Rabi frequencies associated with rotational transitions induced by resonant microwave drives. We compare different excitations schemes for rotational transitions and show that maximal enantiomer-selectivity at a given rotational temperature is achieved for synchronized three-wave mixing with circularly polarized fields.

quant-ph↗

arXiv2022

Quantum optimal control in quantum technologies. Strategic report on current status, visions and goals for research in Europe

Quantum optimal control, a toolbox for devising and implementing the shapes of external fields that accomplish given tasks in the operation of a quantum device in the best way possible, has evolved into one of the cornerstones for enabling quantum technologies. The last few years have seen a rapid evolution and expansion of the field. We review here recent progress in our understanding of the controllability of open quantum systems and in the development and application of quantum control techniques to quantum technologies. We also address key challenges and sketch a roadmap for future developments.

quant-ph↗

arXiv2022

Rydberg atom-enabled spectroscopy of polar molecules via Förster resonance energy transfer

Non-radiative energy transfer between a Rydberg atom and a polar molecule can be controlled by a DC electric field. Here we show how to exploit this control for state-resolved, non-destructive detection and spectroscopy of the molecules where the lineshape reflects the type of molecular transition. Using the example of ammonia, we identify the conditions for collision-mediated spectroscopy in terms of the required electric field strengths, relative velocities, and molecular densities. Rydberg atom-enabled spectroscopy is feasible with current experimental technology, providing a versatile detection method as basic building block for applications of polar molecules in quantum technologies and chemical reaction studies.

physics.atom-ph↗

arXiv2022

Engineering Strong Beamsplitter Interaction between Bosonic Modes via Quantum Optimal Control Theory

In continuous-variable quantum computing with qubits encoded in the infinite-dimensional Hilbert space of bosonic modes, it is a difficult task to realize strong and on-demand interactions between the qubits. One option is to engineer a beamsplitter interaction for photons in two superconducting cavities by driving an intermediate superconducting circuit with two continuous-wave drives, as demonstrated in a recent experiment. Here, we show how quantum optimal control theory (OCT) can be used in a systematic way to improve the beamsplitter interaction between the two cavities. We find that replacing the two-tone protocol by a three-tone protocol accelerates the effective beamsplitter rate between the two cavities. The third tone's amplitude and frequency are determined by gradient-free optimization and make use of cavity-transmon sideband couplings. We show how to further improve the three-tone protocol via gradient-based optimization while keeping the optimized drives experimentally feasible. Our work exemplifies how to use OCT to systematically improve practical protocols in quantum information applications.

quant-ph↗

arXiv2022

Reservoir-engineering shortcuts to adiabaticity

We propose a protocol that achieves fast adiabatic transfer between two orthogonal states of a qubit by coupling with an ancilla. The qubit undergoes Landau-Zener dynamics, whereas the coupling realizes a time-dependent Hamiltonian, which is diagonal in the spin's instantaneous Landau-Zener eigenstates. The ancilla (or meter), in turn, couples to a thermal bath, such that the overall dynamics is incoherent. We analyse the protocol's fidelity as a function of the strength of the coupling and of the relaxation rate of the meter. When the meter's decay rate is the largest frequency scale of the dynamics, the spin dynamics is encompassed by a master equation describing dephasing of the spin in the instantaneous eigenbasis. In this regime the fidelity of adiabatic transfer improves as the bath temperature is increased. Surprisingly, the adiabatic transfer is significantly more efficient in the opposite regime, where the time scale of the ancilla dynamics is comparable to the characteristic spin time scale. Here, for low temperatures the coupling with the ancilla tends to suppress diabatic transitions via effective cooling. The protocol can be efficiently implemented by means of a pulsed, stroboscopic coupling with the ancilla and is robust against moderate fluctuations of the experimental parameters.

quant-ph↗

arXiv2022

Increasing ion yield circular dichroism in femtosecond photoionisation using optimal control theory

We investigate how optimal control theory can be used to improve Circular Dichroism (CD) signals for A--band of fenchone measured via the photoionization yield upon further excitation. These transitions are electric dipole forbidden to first order, which translates into low population transfer to the excited state (~8%) but also allows for a clearer interplay between electric and magnetic transition dipole moments, which are of the same order of magnitude. Using a model including the electronic ground and excited A state as well as all permanent and transition multipole moments up to the electric quadrupole, we find that the absolute CD signal of randomly oriented molecules can be increased by a factor 3.5 when using shaped laser pulses, with the anisotropy parameter g increasing from 0.06 to 1. Our insights provide additional evidence on how optimal control can assist in amplifying chiral signatures via interactions of permanent and transition multipole moments.

physics.chem-ph↗

arXiv2021

Fano interference in quantum resonances from angle-resolved elastic scattering

Asymmetric spectral line shapes are a hallmark of interference of a quasi-bound state with a continuum of states. Such line shapes are well known for multichannel systems, for example, in photoionization or Feshbach resonances in molecular scattering. On the other hand, in resonant single channel scattering, the signature of such interference may disappear due to the orthogonality of partial waves. Here, we show that probing the angular dependence of the cross section allows us to unveil asymmetric Fano profiles also in a single channel shape resonance. We observe a shift in the peak of the resonance profile in the elastic collisions between metastable helium and deuterium molecules with detection angle, in excellent agreement with theoretical predictions from full quantum scattering calculations. Using a model description for the partial wave interference, we can disentangle the resonant and background contributions and extract the relative phase responsible for the characteristic Fano-like profiles from our experimental measurements.

quant-ph↗

arXiv2021

Lie algebra for rotational subsystems of a driven asymmetric top

We present an analytical approach to construct the Lie algebra of finite-dimensional subsystems of the driven asymmetric top rotor. Each rotational level is degenerate due to the isotropy of space, and the degeneracy increases with rotational excitation. For a given rotational excitation, we determine the nested commutators between drift and drive Hamiltonians using a graph representation. We then generate the Lie algebra for subsystems with arbitrary rotational excitation using an inductive argument.

quant-ph↗

arXiv2021

Resource-efficient dissipative entanglement of two trapped-ion qubits

We demonstrate a simplified method for dissipative generation of an entangled state of two trapped-ion qubits. Our implementation produces its target state faster and with higher fidelity than previous demonstrations of dissipative entanglement generation and eliminates the need for auxiliary ions. The entangled singlet state is generated in $\sim$7 ms with a fidelity of 0.949(4). The dominant source of infidelity is photon scattering. We discuss this error source and strategies for its mitigation.

quant-ph↗

arXiv2021

Coherent Control of Ultrafast Bond Making and Subsequent Molecular Dynamics: Demonstration of Final-State Branching Ratio Control

Quantum coherent control of ultrafast bond making and the subsequent molecular dynamics is crucial for the realization of a new photochemistry, where a shaped laser field is actively driving the chemical system in a coherent way from the thermal initial state of the reactants to the final state of the desired products. We demonstrate here coherent control over the relative yields of Mg$_2$ molecules that are generated via photoassociation and subsequently photodriven into different groups of final states. The strong-field process involves non-resonant multiphoton femtosecond photoassociation of a pair of thermally hot magnesium atoms into a bound Mg$_{2}$ molecule and subsequent molecular dynamics on electronically excited states. The branching-ratio control is achieved with linearly chirped laser pulses, utilizing the different chirp dependence that various groups of final molecular states display for their post-pulse population. Our study establishes the feasibility of high degree coherent control over quantum molecular dynamics that is initiated by femtosecond photoassociation of thermal atoms.

physics.atom-ph↗

arXiv2021

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 $\sqrt{i\text{SWAP}}$ gate with superconducting qubits.

quant-ph↗

arXiv2020

Determining the nature of quantum resonances by probing elastic and reactive scattering in cold collisions

Scattering resonances play a central role in collision processes in physics and chemistry. They help building an intuitive understanding of the collision dynamics due to the spatial localization of the scattering wavefunctions. For resonances that are localized in the reaction region, located at short separation behind the centrifugal barrier, sharp peaks in the reaction rates are the characteristic signature, observed recently with state-of-the-art experiments in low energy collisions. If, however, the localization occurs outside of the reaction region, mostly the elastic scattering is modified. This may occur due to above barrier resonances, the quantum analogue of classical orbiting. By probing both elastic and inelastic scattering of metastable helium with deuterium molecules in merged beam experiments, we differentiate between the nature of quantum resonances -- tunneling vs above barrier -- and corroborate our findings by calculating the corresponding scattering wavefunctions.

physics.chem-ph↗

arXiv2020

Complete Controllability Despite Degeneracy: Quantum Control of Enantiomer-Specific State Transfer in Chiral Molecules

We prove complete controllability for rotational states of an asymmetric top molecule belonging to degenerate values of the orientational quantum number M. Based on this insight, we construct a pulse sequence that energetically separates population initially distributed over degenerate M-states, as a precursor for orientational purification. Introducing the concept of enantio-selective controllability, we determine the conditions for complete enantiomer-specific population transfer in chiral molecules and construct pulse sequences realizing this transfer for population initially distributed over degenerate M-states. This degeneracy presently limits enantiomer-selectivity for any initial state except the rotational ground state. Our work thus shows how to overcome an important obstacle towards separating, with electric fields only, left-handed from right-handed molecules in a racemic mixture.

quant-ph↗

arXiv2020

Fundamental Bounds on Qubit Reset

Qubit reset is a basic prerequisite for operating quantum devices, requiring the export of entropy. The fastest and most accurate way to reset a qubit is obtained by coupling the qubit to an ancilla on demand. Here, we derive fundamental bounds on qubit reset in terms of maximum fidelity and minimum time, assuming control over the qubit and no control over the ancilla. Using the Cartan decomposition of the Lie algebra of qubit plus two-level ancilla, we identify the types of interaction and controls for which the qubit can be purified. For these configurations, we show that a time-optimal protocol consists of purity exchange between qubit and ancilla brought into resonance, where the maximum fidelity is identical for all cases but the minimum time depends on the type of interaction and control. Furthermore, we find the maximally achievable fidelity to increase with the size of the ancilla Hilbert space, whereas the reset time remains constant.

quant-ph↗

arXiv2020

Optimally controlled quantum discrimination and estimation

Quantum discrimination and estimation are pivotal for many quantum technologies, and their performance depends on the optimal choice of probe state and measurement. Here we show that their performance can be further improved by suitably tailoring the pulses that make up the interferometer. Developing an optimal control framework and applying it to the discrimination and estimation of a magnetic field in the presence of noise, we find an increase in the overall achievable state distinguishability. Moreover, the maximum distinguishability can be stabilized for times that are more than an order of magnitude longer than the decoherence time.

quant-ph↗

arXiv2019

Krotov: A Python implementation of Krotov's method for quantum optimal control

We present a new open-source Python package, krotov, implementing the quantum optimal control method of that name. It allows to determine time-dependent external fields for a wide range of quantum control problems, including state-to-state transfer, quantum gate implementation and optimization towards an arbitrary perfect entangler. Krotov's method compares to other gradient-based optimization methods such as gradient-ascent and guarantees monotonic convergence for approximately time-continuous control fields. The user-friendly interface allows for combination with other Python packages, and thus high-level customization. The package is being developed at https://github.com/qucontrol/krotov

quant-ph↗

arXiv2019

Optimized Sampling of Mixed-State Observables

Quantum dynamical simulations of statistical ensembles pose a significant computational challenge due to the fact that mixed states need to be represented. If the underlying dynamics is fully unitary, for example in ultrafast coherent control at finite temperatures, one approach to approximate time-dependent observables is to sample the density operator by solving the Schrödinger equation for a set of wave functions with randomized phases. We show that, on average, random-phase wave functions perform well for ensembles with high mixedness, whereas at higher purities a deterministic sampling of the energetically lowest-lying eigenstates becomes superior. We prove that minimization of the worst-case error for computing arbitrary observables is uniquely attained by eigenstate-based sampling. We show that this error can be used to form a qualitative estimate of the set of ensemble purities for which the sampling performance of the eigenstate-based approach is superior to random-phase wave functions. Furthermore we present refinements to both schemes which remove redundant information from the sampling procedure to accelerate their convergence. Finally, we point out how the structure of low-rank observables can be exploited to further improve eigenstate-based sampling schemes.

quant-ph↗

arXiv2019

Quantum control of molecular rotation

The angular momentum of molecules, or, equivalently, their rotation in three-dimensional space, is ideally suited for quantum control. Molecular angular momentum is naturally quantized, time evolution is governed by a well-known Hamiltonian with only a few accurately known parameters, and transitions between rotational levels can be driven by external fields from various parts of the electromagnetic spectrum. Control over the rotational motion can be exerted in one-, two- and many-body scenarios, thereby allowing to probe Anderson localization, target stereoselectivity of bimolecular reactions, or encode quantum information, to name just a few examples. The corresponding approaches to quantum control are pursued within separate, and typically disjoint, subfields of physics, including ultrafast science, cold collisions, ultracold gases, quantum information science, and condensed matter physics. It is the purpose of this review to present the various control phenomena, which all rely on the same underlying physics, within a unified framework. To this end, we recall the Hamiltonian for free rotations, assuming the rigid rotor approximation to be valid, and summarize the different ways for a rotor to interact with external electromagnetic fields. These interactions can be exploited for control --- from achieving alignment, orientation, or laser cooling in a one-body framework, steering bimolecular collisions, or realizing a quantum computer or quantum simulator in the many-body setting.

quant-ph↗