Entanglement is one of the most technologically important quantum phenomena and its con-trolled creation brings us a step closer to the realisation of a quantum computer. Hybrid electron and nuclear spin systems which combine long nuclear decoherence times with the high polarisation and rapid processing times of electron spins are considered reliable candidates for the representation of the fundamental building block of a quantum computer, the qubit. In the literature electron spins quite often play the role of a mediator which can access, manipulate and couple states with long coherence times, beneficial for storing quantum information. Despite the fact that an electron spin can be a useful resource for nuclear spin systems, its permanent presence can be a source of decoherence. The use of transient photoexcited electron spins provide an additional advantage and once the operations which involve the electron spin are completed, the electron spin can decay and not interfere further with the evolution of the system. In this thesis we report magnetic resonance experiments and density functional theory calculations for the demonstration of nuclear - nuclear entanglement using photoexcited triplet states. We study homonuclear and heteronuclear fullerene derivatives and we identify in each case the relevant parameters that can lead to high fidelity entangling operations. The hyperfine interaction in a homonuclear system is the key parameter which determines the degree of entanglement between the nucelar spins according to a recent theoretical proposal. We measure and calculate the hyperfine interaction in homonuclear systems with 13C nuclear spins in order to prove the feasibility of this scheme. Further experiments on a fullerene system with two nuclear spins a 31P and a 1H show that entangling operations of high fidelity which involve the demonstration of CNOT gates, are possible within the lifetime of the triplet state.
Entanglement is one of the most technologically important quantum phenomena and its con-trolled creation brings us a step closer to the realisation of a quantum computer. Hybrid electron and nuclear spin systems which combine long nuclear decoherence times with the high polarisation and rapid processing times of electron spins are considered reliable candidates for the representation of the fundamental building block of a quantum computer, the qubit. In the literature electron spins quite often play the role of a mediator which can access, manipulate and couple states with long coherence times, beneficial for storing quantum information. Despite the fact that an electron spin can be a useful resource for nuclear spin systems, its permanent presence can be a source of decoherence. The use of transient photoexcited electron spins provide an additional advantage and once the operations which involve the electron spin are completed, the electron spin can decay and not interfere further with the evolution of the system. In this thesis we report magnetic resonance experiments and density functional theory calculations for the demonstration of nuclear - nuclear entanglement using photoexcited triplet states. We study homonuclear and heteronuclear fullerene derivatives and we identify in each case the relevant parameters that can lead to high fidelity entangling operations. The hyperfine interaction in a homonuclear system is the key parameter which determines the degree of entanglement between the nucelar spins according to a recent theoretical proposal. We measure and calculate the hyperfine interaction in homonuclear systems with 13C nuclear spins in order to prove the feasibility of this scheme. Further experiments on a fullerene system with two nuclear spins a 31P and a 1H show that entangling operations of high fidelity which involve the demonstration of CNOT gates, are possible within the lifetime of the triplet state.
Electron spin resonance (ESR) experiments are used to assess the possibilities for processing quantum information in the electronic and nuclear spins of endohedral fullerenes. It is shown that ¹⁵N@C₆₀ can be used for universal two-qubit quantum computing. The first step in this scheme is to initialize the nuclear and electron spins that each store one qubit. This was achieved with a magnetic field of 8.6 T at 3 K, by applying resonant RF and microwave radiation. This dynamic nuclear polarization technique made it possible to show that the nuclear T₁ time of ¹⁵N@C����� is on the order of twelve hours at 4.2 K. The electronic T₂ is the limiting decoherence time for the system. At 3.7 K, this can be extended to 215 μs by using amorphous sulphur as the solvent. Pulse sequences are described that could perform all single-qubit gates to the two qubits independently, as well as CNOT gates. After these manipulations, the value of the qubits should be measured. Two techniques are demonstrated for this, by measuring the nuclear spin. Sc@C₈₂ could also be useful for quantum computation. By comparing ESR measurements with density functional theory calculations, it is shown how the orientation of a Sc@C₈₂ molecule in an applied magnetic field affects the molecule's Zeeman and hyperfine coupling. Hence the g- and A-tensors are written in the coordinate frame of the molecule. Pulsed ESR measurements show that the decoherence time at 20 K is 13 μs, which is 20 times longer than had been previously reported. Carbon nanotubes have been filled with endohedral fullerenes, forming 1D arrays that could lead to a scalable quantum computer. N@C₆₀ and Sc@C₈₂ have been used for this filling in various concentrations. ESR measurements of these samples are consistent with simulations of the dipolar coupling.
Spins in a solid-state environment and photons are both promising physical systems regarding the implementation of qubits. Whereas electron and nuclear spins act very well as localized qubits that are able to store and process quantum information, photons are the primary candidates to transmit quantum information between distant locations. Entanglement, on the other hand, is a fundamental resource of quantum information processing enabling, e.g., secure communication over long distances. The generation and manipulation of entanglement are thus fundamental steps in order to leverage the benefits of quantum information processing. The aim of this dissertation is therefore to theoretically investigate entangling mechanisms for various physical systems. A functioning source of entangled photons is a basic hardware component required for quantum communication. To this end, we study a system composed of semiconductor quantum wells inside a microcavity, known as intersubband cavity system, in which the interaction of the electronic system with the cavity field can reach the ultrastrong coupling regime. The ground state contains a finite number of photons, and we find that these photons are entangled. The amount of entanglement is quantified analytically, and maximal entanglement is found to be possible. The technique of entanglement purification allows to restore maximal entanglement that has decreased, e.g. due to decoherence. Purification requires quantum memory, a role for which electron spins in electrically-defined quantum dots are well suited. However, existing purification protocols are rather unpractical in this case. Here, the concept of asymmetric bilateral two-qubit operations is introduced to purify spin entanglement by harnessing the typical interaction between electrons in neighboring quantum dots. As it turns out, this concept can be applied to a variety of qubit systems, e.g. superconducting qubits or spins in nitrogen-vacancy centers in diamond. The latter example offers several possibilities to implement a qubit, of which the intrinsic nitro- gen nuclear spin has proven its viability in many ways. We develop a scheme to deterministically couple two nuclear spin qubits, in which the interaction is mediated by an optical cavity. It is found that an entangling two-qubit gate, also required for universal quantum computation, can be implemented with operation times below 100 nanoseconds, i.e. several orders of magnitude faster compared to the decoherence time of the nuclear spin. The verification of entanglement, which is required e.g. in entanglement-based quantum com- munication to detect an eavesdropping attack, typically involves a measurement of qubit states. Using the input-output formalism, we derive a fully quantum-mechanical model of an optical readout scheme to measure the spin state of an electron in a self-assembled quantum dot.
Coupled electron-nuclear spins are promising physical systems for quantum in-formation processing: By combining the long coherence times of the nuclear spins with the ability to initialize, control, and measure the electron spin state, the favor-able properties of each spin species are utilized. This thesis discusses a procedure to initialize these nuclear spin qubits, and presents a vision of how these systems could be used as the fundamental processing unit of a quantum computer. The fo-cus of this thesis is on control of a system in which a single electron spin is coupled to N nuclear spins via resolvable anisotropic hyperfine (AHF) interactions. High-fidelity universal control of this le-Nn system is possible using only excitations on a single electron spin transition. This electron spin actuator control is implemented by using optimal control theory to find the modulation sequences that generate the desired unitary operations. Decoherence and the challenge of making useful qubits from these systems are also discussed. Experimental evidence of control using an electron spin actuator was acquired with a custom-built pulsed electron spin resonance spectrometer. Complex mod-
Molecular nanostructures are promising building blocks for future quantum technologies, provided methods of harnessing their multiple degrees of freedom can be identified and implemented. Due to low decoherence rates, nuclear spins are considered ideal candidates for storing quantum information, while optical excitations can give rise to fast and controllable interactions for information processing. A recent paper [M. Schaffry et al., Phys. Rev. Lett. 104, 200501 (2010)] proposed a method for entangling two nuclear spins through their mutual coupling to a transient optically excited electron spin. Building on the same idea, we present here an extended and much more detailed theoretical framework, showing that this method is in fact applicable to a much wider class of molecular structures than previously discussed in the original proposal.
The highly parallel nature of the fundamental principles of quantum mechanics means that certain key resource-intensive tasks --- including searching, code decryption and medical, chemical and material simulations --- can be computed polynomially or even exponentially faster with a quantum computer. In spite of its remarkably fast development, the field of quantum computing is still young, and a large-scale prototype using any one of the candidate quantum bits (or 'qubits') under investigation has yet to be developed. Spin-based qubits in condensed matter systems are excellent candidates. Spins controlled using magnetic resonance have provided the first, most advanced, and highest fidelity experimental demonstrations of quantum algorithms to date. Despite having highly promising control characteristics, most physical ensembles investigated using magnetic resonance are unable to produce entanglement, a critical missing ingredient for a pure-state quantum computer. Quantum objects are said to be entangled if they cannot be described individually: they remain fundamentally linked regardless of their physical separation. Such highly non-classical states can be exploited for a host of quantum technologies including teleportation, metrology, and quantum computation. Here I describe how to experimentally create, control and characterise entangled quantum ensembles using magnetic resonance. I first explore the relationship between entanglement and quantum metrology and demonstrate a sensitivity enhancement over classical resources using molecular sensors controlled with liquid-state nuclear magnetic resonance. I then examine the computational potential of irreversible relaxation processes in combination with traditional reversible magnetic resonance control techniques. I show how irreversible processes can polarise both nuclear and electronic spins, which improves the quality of qubit initialisation. I discuss the process of quantum state tomography, where an arbitrary quantum state can be accurately measured and characterised, including components which go undetected using traditional magnetic resonance techniques. Lastly, I combine the above findings to initialise, create and characterise entanglement between an ensemble of electron and nuclear spin defects in silicon. I further this by generating pseudo-entanglement between an ensemble of nuclear spins mediated by a transient electron spin in a molecular system. These findings help pave the way towards a particular architecture for a scalable, spin-based quantum computer.
Quantum networks promise to be the future architecture for secure communication and distributed quantum computation. This thesis describes experiments on nitrogenvacancy (NV) centres that lead towards a versatile multi-node quantum network consisting ofmulti-qubit nodes. The NV centre in diamond is a spinful optically-active crystal defect. NVs are a prime network-node candidate due to demonstrated coherence times beyond 100ms and longitudinal relaxation times exceeding 1s and their spin-selective optical interface which facilitates the generation of spin-photon entanglement. Entangling links between nodes are therefore readily created by overlapping the emission of two NVs on a beam splitter. Besides NVs, we further address individual 13C nuclear spins in the vicinity and use these spins as a quantum resource. Our goal is to propel these nuclear spins to constitute robust quantummemories which store and manipulate quantum information in an NV-based quantum network. The experiments described in this thesis are thematically separated into three groups. First, we explore the NV-nuclear interplay. We demonstrate nuclear-spin control by observing the Zeno effect on up to two logical qubits within the state space of three nuclear spins (Chapter 3). We further realize that the always-on magnetic hyperfine interaction between NV and nuclear spins will limit the nuclear spin coherence when entangling distant NV centres (Chapter 4). A systematic experimental study probes our theoretical prediction and we additionally demonstrate improved robustness for logical states within decoherence-protected state spaces (Chapter 5) and finally for individual nuclear spins (Chapter 6). Second,we use remoteNV-NV entangled states to demonstrate experimental milestones in quantumnetworks. The realization of a high-fidelity entangled link over a distance of 1.3km permits the loophole-free violation of Bell’s inequality (Chapter 7). We further increase the entangling rate by three orders of magnitude such that it exceeds the decoherence rate of an entangled state on our network. This allows us to convert our probabilistic entanglement generation into a deterministic process which delivers entangled states at prespecifiedmoments in time (Chapter 8). Third, we finally combine the concepts of nuclear-spin quantum memories and remote entanglement generation to demonstrate entanglement distillation in a network setting (Chapter 9). We subsequently generate two raw entangled input states between two remote NV centres. The first state is stored on nuclear spins to liberate both NVs for the second round of state generation. Finally, a higher-fidelity entangled state is distilled via local operations. This constitutes the first quantum-network demonstration that relies on the control of multiple fully-coherent quantum systems per network node.