# Publications

## Operational advantage of basis-independent quantum coherence

EPL **125** (2019) ARTN 50005

## Mott polaritons in cavity-coupled quantum materials

New Journal of Physics IOP Publishing **21** (2019) 073066

We show that strong electron-electron interactions in quantum materials can give rise to electronic transitions that couple strongly to cavity fields, and collective enhancement of these interactions can result in ultrastrong effective coupling strengths. As a paradigmatic example we consider a Fermi-Hubbard model coupled to a single-mode cavity and find that resonant electron-cavity interactions result in the formation of a quasi-continuum of polariton branches. The vacuum Rabi splitting of the two outermost branches is collectively enhanced and scales with USD g_{\text{eff}}\propto\sqrt{2L} USD, where USD L USD is the number of electronic sites, and the maximal achievable value for USD g_{\text{eff}} USD is determined by the volume of the unit cell of the crystal. We find that USD g_{\text{eff}} USD for existing quantum materials can by far exceed the width of the first excited Hubbard band. This effect can be experimentally observed via measurements of the optical conductivity and does not require ultrastrong coupling on the single-electron level. Quantum correlations in the electronic ground state as well as the microscopic nature of the light-matter interaction enhance the collective light-matter interaction compared to an ensemble of independent two-level atoms interacting with a cavity mode.

## Emergence of correlated proton tunnelling in water ice.

Proceedings. Mathematical, Physical, and Engineering Sciences **475** (2019) 20180867-20180867

Several experimental and theoretical studies report instances of concerted or correlated multiple proton tunnelling in solid phases of water. Here, we construct a pseudo-spin model for the quantum motion of protons in a hexameric H2O ring and extend it to open system dynamics that takes environmental effects into account in the form of O-H stretch vibrations. We approach the problem of correlations in tunnelling using quantum information theory in a departure from previous studies. Our formalism enables us to quantify the coherent proton mobility around the hexagonal ring by one of the principal measures of coherence, the l 1 norm of coherence. The nature of the pairwise pseudo-spin correlations underlying the overall mobility is further investigated within this formalism. We show that the classical correlations of the individual quantum tunnelling events in long-time limit is sufficient to capture the behaviour of coherent proton mobility observed in low-temperature experiments. We conclude that long-range intra-ring interactions do not appear to be a necessary condition for correlated proton tunnelling in water ice.

## Theoretical description and experimental simulation of quantum entanglement near open time-like curves via pseudo-density operators.

Nature communications **10** (2019) 182-182

Closed timelike curves are striking predictions of general relativity allowing for time-travel. They are afflicted by notorious causality issues (e.g. grandfather's paradox). Quantum models where a qubit travels back in time solve these problems, at the cost of violating quantum theory's linearity-leading e.g. to universal quantum cloning. Interestingly, linearity is violated even by open timelike curves (OTCs), where the qubit does not interact with its past copy, but is initially entangled with another qubit. Non-linear dynamics is needed to avoid violating entanglement monogamy. Here we propose an alternative approach to OTCs, allowing for monogamy violations. Specifically, we describe the qubit in the OTC via a pseudo-density operator-a unified descriptor of both temporal and spatial correlations. We also simulate the monogamy violation with polarization-entangled photons, providing a pseudo-density operator quantum tomography. Remarkably, our proposal applies to any space-time correlations violating entanglement monogamy, such as those arising in black holes.

## Engineering statistical transmutation of identical quantum particles

PHYSICAL REVIEW B **99** (2019) ARTN 045430

## Coherent spin manipulation of individual atoms on a surface

Science American Association for the Advancement of Science **366** (2019) 509-512

Achieving time-domain control of quantum states with atomic-scale spatial resolution in nanostructures is a long-term goal in quantum nanoscience and spintronics. Here, we demonstrate coherent spin rotations of individual atoms on a surface at the nanosecond time scale, using an all-electric scheme in a scanning tunneling microscope (STM). By modulating the atomically confined magnetic interaction between the STM tip and surface atoms, we drive quantum Rabi oscillations between spin-up and spin-down states in as little as ~20 nanoseconds. Ramsey fringes and spin echo signals allow us to understand and improve quantum coherence. We further demonstrate coherent operations on engineered atomic dimers. The coherent control of spins arranged with atomic precision provides a solid-state platform for quantum-state engineering and simulation of many-body systems.

## Development and characterization of a flux-pumped lumped element Josephson parametric amplifier

EPJ Web of Conferences EDP Sciences **198** (2019)

Josephson parametric amplification is a tool of paramount importance in circuit-QED especially for the quantum-noise-limited single-shot readout of superconducting qubits. We developed a Josephson parametric amplifier (JPA) based on a lumped-element LC resonator, in which the inductance L is composed by a geometric inductance and an array of 4 superconducting quantum interference devices (SQUIDs). We characterized the main figures of merit of the device, obtaining a −3 dB bandwidth BW = 15 MHz for a gain G = 21 dB and a 1 dB compression point P1dB = −115 dBm. The obtained results are promising for the future use of such JPA as the first stage of amplification for single-shot readout of superconducting qubits.

## Uncertainty equality with quantum memory and its experimental verification

NPJ QUANTUM INFORMATION **5** (2019) ARTN 39

## Unconventional field-induced spin gap in an S=1/2 Chiral staggered chain

Physical Review Letters American Physical Society **122** (2019) 057207-

We investigate the low-temperature magnetic properties of the molecule-based chiral spin chain ½CuðpymÞðH2OÞ4SiF6 · H2O (pym ¼ pyrimidine). Electron-spin resonance, magnetometry and heat capacity measurements reveal the presence of staggered g tensors, a rich low-temperature excitation spectrum, a staggered susceptibility, and a spin gap that opens on the application of a magnetic field. These phenomena are reminiscent of those previously observed in nonchiral staggered chains, which are explicable within the sine-Gordon quantum-field theory. In the present case, however, although the sineGordon model accounts well for the form of the temperature dependence of the heat capacity, the size of the gap and its measured linear field dependence do not fit with the sine-Gordon theory as it stands. We propose that the differences arise due to additional terms in the Hamiltonian resulting from the chiral structure of ½CuðpymÞðH2OÞ4SiF6 · H2O, particularly a uniform Dzyaloshinskii-Moriya coupling and a fourfold periodic staggered field.

## Manipulating quantum materials with quantum light (vol 99, 085116, 2019)

Physical Review B (2019)

© 2019 American Physical Society. The interaction Hamiltonian (Formula Presented) Eq. (14) describing the interaction between the cavity and the electronic system was obtained by expanding the Peierls Hamiltonian in Eq. (A4) up to first order in the small parameter (Formula Presented) All results presented in the paper are consistent with this appro imate interaction Hamiltonian, leading to an effective Hamiltonian that depends quadratically on. However, it turns out that a straightforward improvement of the parameters entering the effective Hamiltonian in Eq. (26) can be obtained by including the second-order term in the Peierls Hamiltonian in Eq. (A4). This term gives rise to modifications of our results that are also of order through a renormalization of the nearest-neighbor hopping amplitude (Formula Presented) The authors would like to thank M. A. Sentef for bringing the importance of the second-order term in Eq. (A4) to our attention.

## Manipulating quantum materials with quantum light

Physical Review B American Physical Society **99** (2019) 085116-

We show that the macroscopic magnetic and electronic properties of strongly correlated electron systems can be manipulated by coupling them to a cavity mode. As a paradigmatic example we consider the Fermi-Hubbard model and find that the electron-cavity coupling enhances the magnetic interaction between the electron spins in the ground-state manifold. At half filling this effect can be observed by a change in the magnetic susceptibility. At less than half filling, the cavity introduces a next-nearest-neighbor hopping and mediates a long-range electron-electron interaction between distant sites. We study the ground-state properties with tensor network methods and find that the cavity coupling can induce a phase characterized by a momentum-space pairing effect for electrons.

## Hyperfine interaction of individual atoms on a surface

Science American Association for the Advancement of Science **362** (2018) 336-339

Taking advantage of nuclear spins for electronic structure analysis, magnetic resonance imaging, and quantum devices hinges on knowledge and control of the surrounding atomic-scale environment. We measured and manipulated the hyperfine interaction of individual iron and titanium atoms placed on a magnesium oxide surface by using spin-polarized scanning tunneling microscopy in combination with single-atom electron spin resonance. Using atom manipulation to move single atoms, we found that the hyperfine interaction strongly depended on the binding configuration of the atom. We could extract atom- and position-dependent information about the electronic ground state, the state mixing with neighboring atoms, and properties of the nuclear spin. Thus, the hyperfine spectrum becomes a powerful probe of the chemical environment of individual atoms and nanostructures.

## Molecular electronic spin qubits from a spin-frustrated trinuclear copper complex

Chemical Communications Royal Society of Chemistry **54** (2018) 12934-12937

The trinuclear copper(II) complex [Cu3(saltag)(py)6]ClO4 (H5saltag = tris(2-hydroxybenzylidene)triaminoguanidine) was synthesized and characterized by experimental as well as theoretical methods. This complex exhibits a strong antiferromagnetic coupling (J = −298 cm−1) between the copper(II) ions, mediated by the N–N diazine bridges of the tritopic ligand, leading to a spin-frustrated system. This compound shows a T2 coherence time of 340 ns in frozen pyridine solution, which extends to 591 ns by changing the solvent to pyridine-d5. Hence, the presented compound is a promising candidate as a building block for molecular spintronics.

## Geometry of quantum correlations in space-time

PHYSICAL REVIEW A **98** (2018) ARTN 052312

## Proton tunnelling in hydrogen bonds and its implications in an induced-fit model of enzyme catalysis

PROCEEDINGS OF THE ROYAL SOCIETY A-MATHEMATICAL PHYSICAL AND ENGINEERING SCIENCES **474** (2018) ARTN 20180037

## Experimental test of the relation between coherence and path information

Communications Physics **1** (2018)

© 2018, The Author(s). Quantum coherence stemming from the superposition behaviour of a particle beyond the classical realm, serves as one of the most fundamental features in quantum mechanics. The wave-particle duality phenomenon, which shares the same origin, has a strong relationship with quantum coherence. Recently, an elegant relation between quantum coherence and path information has been theoretically derived. Here, we experimentally test such new duality by l1-norm measure and the minimum-error state discrimination. We prepare three classes of two-photon states encoded in polarisation degree of freedom, with one photon serving as the target and the other photon as the detector. We observe that wave-particle-like complementarity and Bagan’s equality, defined by the duality relation between coherence and path information, is well satisfied. Our results may shed new light on the original nature of wave-particle duality and on the applications of quantum coherence as a fundamental resource in quantum technologies.

## Probing quantum features of photosynthetic organisms

NPJ QUANTUM INFORMATION **4** (2018) ARTN 60

## Measuring quantumness: from theory to observability in interferometric setups

EUROPEAN PHYSICAL JOURNAL D **72** (2018) ARTN 219

## Publisher Correction: Magnetic edge states and coherent manipulation of graphene nanoribbons.

Nature (2018)

In Fig. 1 of this Letter, there should have been two nitrogen (N) atoms at the 1,3-positions of all the blue chemical structures (next to the oxygen atoms), rather than one at the 2-position. The figure has been corrected online, and the original incorrect figure is shown as Supplementary Information to the accompanying Amendment.

## Electrically controlled nuclear polarization of individual atoms

Nature Nanotechnology Nature Publishing Group **13** (2018) 1120–1125-

Nuclear spins serve as sensitive probes in chemistry1 and materials science2 and are promising candidates for quantum information processing3,4,5,6. NMR, the resonant control of nuclear spins, is a powerful tool for probing local magnetic environments in condensed matter systems, which range from magnetic ordering in high-temperature superconductors7,8 and spin liquids9 to quantum magnetism in nanomagnets10,11. Increasing the sensitivity of NMR to the single-atom scale is challenging as it requires a strong polarization of nuclear spins, well in excess of the low polarizations obtained at thermal equilibrium, as well as driving and detecting them individually4,5,12. Strong nuclear spin polarization, known as hyperpolarization, can be achieved through hyperfine coupling with electron spins2. The fundamental mechanism is the conservation of angular momentum: an electron spin flips and a nuclear spin flops. The nuclear hyperpolarization enables applications such as in vivo magnetic resonance imaging using nanoparticles13, and is harnessed for spin-based quantum information processing in quantum dots14 and doped silicon15,16,17. Here we polarize the nuclear spins of individual copper atoms on a surface using a spin-polarized current in a scanning tunnelling microscope. By employing the electron–nuclear flip-flop hyperfine interaction, the spin angular momentum is transferred from tunnelling electrons to the nucleus of individual Cu atoms. The direction and magnitude of the nuclear polarization is controlled by the direction and amplitude of the current. The nuclear polarization permits the detection of the NMR of individual Cu atoms, which is used to sense the local magnetic environment of the Cu electron spin.