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.
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.
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.
Nanostructures are promising building blocks for quantum technologies due to their reproducible nature and ability to self-assemble into complex structures. However, the need to control these nanostructures represents a key challenge. Hence, this thesis investigates the manipulation and creation of quantum states in certain nanostructures. The results of this thesis can be applied to quantum information processing and to extremely sensitive magnetic-field measurements.In the first research chapter, we propose and examine methods for entangling two (remote) nuclear spins through their mutual coupling to a transient optically excited electron spin. From our calculations we identify the specific molecular properties that permit high entangling power gates for different protocols.In the next research chapter, we investigate another method to create entanglement; this time between two remote electronic spins. This method uses a very sensitive magnetic-field sensor based on a crystal defect that allows the detection of single magnetic moments. The act of sensing the local field constitutes a two-qubit projective measurement. This entangling operation is remarkably robust to imperfections occurring in an experiment.The third research chapter presents an augmented sensor consisting of a nitrogen-vacancy centre for readout and an `amplifier' spin system that directly senses tiny local magnetic fields. Our calculations show that this hybrid structure has the potential to detect magnetic moments with a sensitivity and spatial resolution far beyond that of a sensor based on only a nitrogen-vacancy centre, and indeed this may be the physical limit for sensors of this class.Finally, the last research chapter investigates measurements of magnetic-field strength using an ensemble of spin-active molecules. Here, we describe a quantum strategy that can beat the common standard strategy. We identify the conditions for which this is possible and find that this crucially depends on the decoherence present in the system.
Nanostructures are promising building blocks for quantum technologies due to their reproducible nature and ability to self-assemble into complex structures. However, the need to control these nanostructures represents a key challenge. Hence, this thesis investigates the manipulation and creation of quantum states in certain nanostructures. The results of this thesis can be applied to quantum information processing and to extremely sensitive magnetic-field measurements.In the first research chapter, we propose and examine methods for entangling two (remote) nuclear spins through their mutual coupling to a transient optically excited electron spin. From our calculations we identify the specific molecular properties that permit high entangling power gates for different protocols.In the next research chapter, we investigate another method to create entanglement; this time between two remote electronic spins. This method uses a very sensitive magnetic-field sensor based on a crystal defect that allows the detection of single magnetic moments. The act of sensing the local field constitutes a two-qubit projective measurement. This entangling operation is remarkably robust to imperfections occurring in an experiment.The third research chapter presents an augmented sensor consisting of a nitrogen-vacancy centre for readout and an `amplifier' spin system that directly senses tiny local magnetic fields. Our calculations show that this hybrid structure has the potential to detect magnetic moments with a sensitivity and spatial resolution far beyond that of a sensor based on only a nitrogen-vacancy centre, and indeed this may be the physical limit for sensors of this class.Finally, the last research chapter investigates measurements of magnetic-field strength using an ensemble of spin-active molecules. Here, we describe a quantum strategy that can beat the common standard strategy. We identify the conditions for which this is possible and find that this crucially depends on the decoherence present in the system.
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.
Molecular spins offer promise in emerging quantum technologies such as quantum sensing and computing. At low temperatures, nuclear spin-spin interactions affect electron spin coherence lifetimes through pure dephasing. Nuclear-spin noise can originate from spin pairs within a molecule itself, pairs in a surrounding environment system, or pairs in which one spin is on the molecule and the other in the environment. Improving coherence times requires detailed knowledge of the dominant sources of dephasing. Here, we analyze the decoherence behavior of two molecular qubit candidates with various ligands and in different nuclear-spin containing solvents. We apply an electronic-structure enhanced, non-Markovian perturbative theoretical method to connect experimentally comparable dephasing times to individual spin pairs. This analysis allows the development of a computational workflow to strategically improve coherence lifetimes in spin systems where decoherence is dominated by spin-spin dephasing.
Abstract Controlling molecular spin quantum bits optically offers the potential to effectively reduce decoherence and raise the working temperature of quantum computers. Here, exchange interactions and spin dynamics, as mediated by an optically driven triplet state, are calculated for a molecule that consists of a pair of radicals and represents a potential quantum-circuit building block. Consistent with the previous experimental observation of spin coherence induced by the triplet state, our work demonstrates an optically driven quantum gate operation scheme in a molecule. A technological blueprint combining a two-dimensional molecular network and programmable nanophotonics, both of which are sufficiently developed, is proposed. We thus realize computational exploration of chemical databases to identify suitable candidates for molecular spin quantum bits and couplers to be hybridized with nanophotonic devices. The work presented here is proposed to realize a new approach for exploring molecular excited states and click chemistry, toward advancing molecular quantum technology.