Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Applications of quantum coherence in condensed matter nanostructures

Simon C. Benjamin

Published Jan 1, 2010• 0 citations
OpenAlex

Abstract

This thesis is concerned with studying the fascinating quantum properties of real-world nanostructures embedded in a noisy condensed matter environment. The interaction with light is used for controlling and manipulating the quantum state of the systems considered here. In some instances, laser pulses also provide a way of actively probing and controlling environmental interactions. The first two research chapters assess two different ways of performing all-optical spin qubit gates in self-assembled quantum dots. The principal conclusion is that an `adiabatic' control technique holds the promise of achieving a high fidelity when all primary sources of decoherence are taken into account. In the next chapter, it is shown that an optically driven quantum dot exciton interacting with the phonons of the surrounding lattice acts as a heat pump. Further, a model is developed which predicts the temperature-dependent damping of Rabi oscillations caused by bulk phonons, finding an excellent agreement with experimental data. A different system is studied in the following chapter: two electron spin qubits with no direct interaction, yet both exchange-coupled to an optically active mediator spin. The results of this study show that these general assumptions are sufficient for generating controlled electron spin entanglement over a wide range of parameters, even in the presence of noise. Finally, the Radical Pair model of the avian compass is investigated in the light of recent experimental results, leading to the surprising prediction that the electron spin coherence time in this molecular system seems to approach the millisecond timescale.

Related papers

Applications of quantum coherence in condensed matter nanostructures

Erik M. Gauger

This thesis is concerned with studying the fascinating quantum properties of real-world nanostructures embedded in a noisy condensed matter environment. The interaction with light is used for controlling and manipulating the quantum state of the systems considered here. In some instances, laser pulses also provide a way of actively probing and controlling environmental interactions. The first two research chapters assess two different ways of performing all-optical spin qubit gates in self-assembled quantum dots. The principal conclusion is that an `adiabatic' control technique holds the promise of achieving a high fidelity when all primary sources of decoherence are taken into account. In the next chapter, it is shown that an optically driven quantum dot exciton interacting with the phonons of the surrounding lattice acts as a heat pump. Further, a model is developed which predicts the temperature-dependent damping of Rabi oscillations caused by bulk phonons, finding an excellent agreement with experimental data. A different system is studied in the following chapter: two electron spin qubits with no direct interaction, yet both exchange-coupled to an optically active mediator spin. The results of this study show that these general assumptions are sufficient for generating controlled electron spin entanglement over a wide range of parameters, even in the presence of noise. Finally, the Radical Pair model of the avian compass is investigated in the light of recent experimental results, leading to the surprising prediction that the electron spin coherence time in this molecular system seems to approach the millisecond timescale.

arXiv:1001.4446•Jan 1, 2009•0 citations

Linking confined electron spins through coherent light-matter interaction.

Robert Stockill

Electron spins confined to self-assembled quantum dots are considered as nodes for a coherent optical network capable of supporting distributed quantum states. Through a series of experiments, the work contributing to this dissertation examines some of the key criteria for constructing such a network. First, the ability to optically extract a coherent spin state from the quantum dot without perturbing the nuclear environment is explored: nuclear feedback is an issue that has frustrated previous studies into electron spin coherence in these systems. With the novel techniques we develop, we identify and characterise the previously undetermined intrinsic mechanisms that govern the coherence of the central spin. We show how the coherence of the electron spin is intimately related to the growth of these strained nanostructures. Second, a model network is constructed in which two spins confined to separate quantum dots are projected into a highly entangled state. This is the first time electron spins in distant quantum dots have been entangled, and in doing so we demonstrate controllable entanglement generation at the highest rates recorded for optically accessible qubit definitions. We investigate the realisation of a hybrid quantum network by demonstrating the first interconnect between wholly different single quantum systems: a semiconductor quantum dot and a trapped ytterbium ion. In forming an optical link between these two complementary qubit definitions, we show that we can circumvent their intrinsic optical differences through coherent photon generation at the quantum dot. A network built from these diverse constituents could combine the ultrafast operations self-assembled quantum dots enable with the long coherence times states in trapped ions experience. Finally, in a step towards truly scalable entanglement generation between quantum dot spins, we design minimally invasive structures that will funnel large proportions of the optical dipole field from the optically dense material that surrounds the quantum dot. The techniques developed in this work and the knowledge gained from their operation should enable the demonstration the creation of high-order nonlocal states between quantum dot spins, single photons and trapped ions, as well as the development of new optically active systems that will benefit from enhanced spin coherence.

•Oct 14, 2016•1 citation

Quantum information processing in mesoscopic systems

Jose Garcia Coello

This thesis discusses various schemes and protocols for quantum information processing in mesoscopic systems with particular focus on using the spin of a particle as the bearer of information. The first chapter introduce various aspects of the field of quantum information used in this thesis such as qubits, entanglement, its quantification, quantum logic gates and entanglement swapping. In this chapter concepts such as AKLT states, decoherence and adiabatic elimination are introduced as they will be relevant in the thesis. In chapter 2 we introduce the Quantum Dots as the solid state system that will primarily be used as the hardware for the development of Quantum Information Processing (QIP). The different properties of quantum dots depending on their size are discussed. The exchange interaction between tunnel coupled quantum dots and the background of quantum computation in quantum dots is described. The principal sources of decoherence and the measurement techniques for spin qubits are presented. In chapter 3, carbon nanowires filled with N@C60 dimers are studied to analyse the entanglement between nuclear spins. The dimer is modelled as a two coupled nuclear spin- electron spin pair with a Heisenberg interaction. The entanglement have been studied depending on the temperature and the intensity of an external magnetic field. Witnessing the entanglement, and particularly bound entanglement are discussed. In chapter 4, the way to extract a singlet from a quantum dot is explored. The system that we model will be consisting of a triple dot and analyse the best way to get the singlet out, with each electron in a separate dot. The chief motivation is to create a singlet between separate dots in a time-scale much faster than that given by spinspin exchange interactions. In chapter 5, quantum logic gates in a triple dot system has been studied. Such gates have been widely studied in double and single quantum dots. Motivated by the advent of experimental set ups of triple dots, we have studied the natural quantum gates that came out of a triple dot system. There are still two spin quantum bits in the three dots and there is an empty intervening dot, which imparts the scheme some advantages, as well as a substantial difference from the class of schemes studied so far. In chapter 6, we model a large square dot. As we describe in chapter 2, the properties of the large dots make them behave with some interesting properties such as hosting Wigner molecules of electrons inside. We explore the application of these structures for quantum information processing. We show here how to get singlet/triplet measurement, entanglement swapping, and how to prepare a 1D AKLT state, using the square dot as a construction block of the system. Finally in chapter 7 conclusions and further work. Here we indicate the further work that could be done with the knowledge present in this thesis and motivated by future advances in the technology.

•Nov 28, 2012•0 citations

Quantum information processing in nanostructures

Reina Estupiñán, John-Henry

Since information has been regarded as a physical entity, the field of quantum information theory has blossomed. This brings novel applications, such as quantum computation. This field has attracted the attention of numerous researchers with backgrounds ranging from computer science, mathematics and engineering, to the physical sciences. Thus, we now have an interdisciplinary field where great efforts are being made in order to build devices that should allow for the processing of information at a quantum level, and also in the understanding of the complex structure of some physical processes at a more basic level. This thesis is devoted to the theoretical study of structures at the nanometer-scale, "nanostructures," through physical processes that mainly involve the solid-state and quantum optics, in order to propose reliable schemes for the processing of quantum information. Initially, the main results of quantum information theory and quantum computation are briefly reviewed. Next, the state-of-the-art of quantum dots technology is described. In so doing, the theoretical background and the practicalities required for this thesis are introduced. A discussion of the current quantum hardware used for quantum information processing is given. In particular, the solid-state proposals to date are emphasised. A detailed prescription is given, using an optically-driven coupled quantum dot system, to reliably prepare and manipulate exciton maximally entangled Bell and Greenberger-Horne-Zeilinger (GHZ) states. Manipulation of the strength and duration of selective light-pulses needed for producing these highly entangled states provides us with crucial elements for the processing of solid-state based quantum information. The all-optical generation of states of the so-called Bell basis for a system of two quantum dots (QDs) is exploited for performing the quantum teleportation of the excitonic state of a dot in an array of three coupled QDs. Theoretical predictions suggest that several hundred single quantum bit rotations and controlled-NOT gates could be performed before decoherence of the excitonic states takes place. In addition, the exciton coherent dynamics of a coupled QD system confined within a semiconductor single mode microcavity is reported. It is shown that this system enables the control of exciton entanglement by varying the coupling strength between the optically-driven dot system and the microcavity. The exciton entanglement shows collapses and revivals for suitable amplitudes of the incident radiation field and dot-cavity coupling strengths. The results given here could offer a new approach for the control of decoherence mechanisms arising from entangled "artificial molecules." In addition to these ultrafast coherent optical control proposals, an approach for reliable implementation of quantum logic gates and long decoherence times in a QD system based on nuclear magnetic resonance (NMR) is given, where the nuclear resonance is controlled by the ground state "magic number" transitions of few-electron QDs in an external magnetic field. The dynamical evolution of quantum registers of arbitrary length in the presence of environmentally-induced decoherence effects is studied in detail. The cases of quantum bits (qubits) coupling individually to different environments ("independent decoherence"), and qubits interacting collectively with the same reservoir ("collective decoherence") are analysed in order to find explicit decoherence functions for any number of qubits. The decay of the coherences of the register is shown to strongly depend on the input states: this sensitivity is a characteristic of both types of coupling (collective and independent) and not only of the collective coupling, as has been reported previously. A non-trivial behaviour - "recoherence" - is found in the decay of the off-diagonal elements of the reduced density matrix in the specific situation of independent decoherence. The results lead to the identification of decoherence-free states in the collective decoherence limit. These states belong to subspaces of the system's Hilbert space that do not become entangled with the environment, making them ideal elements for the engineering of "noiseless" quantum codes. The relations between decoherence of the quantum register and computational complexity based on the new dynamical results obtained for the register density matrix are also discussed. This thesis concludes by summarising and pointing out future directions, and in particular, by discussing some biological resonant energy transfer processes that may be useful for the processing of information at a quantum level.

•Jan 1, 2002•0 citations

Creation and manipulation of quantum states in nanostructures

Brendon W. Lovett

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.

•Jan 1, 2011•0 citations

Nanoscale Coherent Control. Ultrafast dynamics of single molecules, individual light harvesting complexes and discrete nanoantennas at room temperature.

Daan Brinks

Ultrafast pulses allow observation of molecular dynamics with femtosecond time resolution through pump probe experiments. However, averaging over an ensemble of molecules tends to wash out phase sensitive information, necessary to probe quantum effects, due to the intrinsic inhomogeneity in molecular conformations, orientations and interactions that lead to unique potential energy landscapes for each molecule. It is therefore important to go beyond the ensemble average when looking at quantum dynamics of organic systems at room temperature, and resolve the behaviour of specific molecules on an individual basis. In this thesis, we show the creation, manipulation and observation of ultrafast coherent effects in single molecules at room temperature, and resolve a certain measure of environmental influence on the specific dynamics of each molecule. Moreover, we apply this insight to investigate a functional light harvesting biosystem, and lay the basis for a technique that has the time and space resolution required to observe these systems in vivo. In chapter 1, we introduce the concepts and techniques the research in this thesis is built on. In chapter 2, we treat the possibility of controlling ultrafast pulses at the high-NA diffraction limit, and come to conclusions about the procedure to follow there that hold for all pulse-shaping experiments. We show in proof of principle experiments that we can control the ultrafast characteristics of optical pulses in nanometric excitation volumes. In chapters 3 and 4 we report the creation, detection and control of ultrafast quantum dynamics in single organic molecules at room temperature. We show that manipulation of superposition states is possible in these systems within a coherence dephasing time of ~50 fs. This leads to the first observation of rabi-oscillations in room temperature single molecules, to ultrafast operation of an organic qubit, and to the creation of non-stationary superposition states (vibrational wavepackets). We probe the influence of the local environment on the composition and dynamics of these wavepackets and show we can optimize the state preparation protocol for each individual molecule in its own nanoenvironment, leading to high fidelity coherent control. In these chapters we lay out the proof of principle work of detecting the quantumdynamics of a complex system in interaction with its environment at room temperature. In chapter 5 we discuss application of these techniques to the investigation of long lived coherence in photosynthetic systems. We show that electronic coherence between different rings of the LH2 system persists to time scales of 100s of femtoseconds at room temperature. Moreover we show that the energy transfer pathways in LH2 adapt to environmentally induced changes in the molecule and that the nature of the transfer remains coherent for each pathway, providing strong evidence that coherent energy transfer is the optimum process for energy transfer in photosynthesis. Finally, in chapter 6 we take the technical development one step further and report on the creation of a framework based on plasmonic antennas that allows for control of the amplitude-phase characteristics in nanometric sized hotspot fields. We show for the first time that the ultrafast characteristics of plasmonic hotspots can directly be engineered through design of the plasmonic system and experimentally demonstrate two much-anticipated examples: a sub-diffraction resolution phase shaper and an ultrafast plasmonic switch for pump probe experiments. The results presented in this thesis form the first creation and observation of ultrafast coherent dynamics in individual molecular systems at room temperature. This is a necessary step to be able to do true quantum tomography in complex systems, resolve the influence of the environment on molecular dynamics, and investigate the physics that determines evolutionary optimization and functionality in biomolecules.

•Oct 19, 2012•0 citations
This thesis is concerned with studying the fascinating quantum properties of real-world nanostructures embedded in a noisy condensed matter environment. The interaction with light is used for controlling and manipulating the quantum state of the systems considered here. In some instances, laser pulses also provide a way of actively probing and controlling environmental interactions.
The first two research chapters assess two different ways of performing all-optical spin qubit gates in self-assembled quantum dots. The principal conclusion is that an `adiabatic' control technique holds the promise of achieving a high fidelity when all primary sources of decoherence are taken into account.
In the next chapter, it is shown that an optically driven quantum dot exciton interacting with the phonons of the surrounding lattice acts as a heat pump. Further, a model is developed which predicts the temperature-dependent damping of Rabi oscillations caused by bulk phonons, finding an excellent agreement with experimental data.
A different system is studied in the following chapter: two electron spin qubits with no direct interaction, yet both exchange-coupled to an optically active mediator spin. The results of this study show that these general assumptions are sufficient for generating controlled electron spin entanglement over a wide range of parameters, even in the presence of noise.
Finally, the Radical Pair model of the avian compass is investigated in the light of recent experimental results, leading to the surprising prediction that the electron spin coherence time in this molecular system seems to approach the millisecond timescale.
This thesis is concerned with studying the fascinating quantum properties of real-world nanostructures embedded in a noisy condensed matter environment. The interaction with light is used for controlling and manipulating the quantum state of the systems considered here. In some instances, laser pulses also provide a way of actively probing and controlling environmental interactions. The first two research chapters assess two different ways of performing all-optical spin qubit gates in self-assembled quantum dots. The principal conclusion is that an `adiabatic' control technique holds the promise of achieving a high fidelity when all primary sources of decoherence are taken into account. In the next chapter, it is shown that an optically driven quantum dot exciton interacting with the phonons of the surrounding lattice acts as a heat pump. Further, a model is developed which predicts the temperature-dependent damping of Rabi oscillations caused by bulk phonons, finding an excellent agreement with experimental data. A different system is studied in the following chapter: two electron spin qubits with no direct interaction, yet both exchange-coupled to an optically active mediator spin. The results of this study show that these general assumptions are sufficient for generating controlled electron spin entanglement over a wide range of parameters, even in the presence of noise. Finally, the Radical Pair model of the avian compass is investigated in the light of recent experimental results, leading to the surprising prediction that the electron spin coherence time in this molecular system seems to approach the millisecond timescale.
Electron spins confined to self-assembled quantum dots are considered as nodes for a coherent optical network capable of supporting distributed quantum states. Through a series of experiments, the work contributing to this dissertation examines some of the key criteria for constructing such a network. First, the ability to optically extract a coherent spin state from the quantum dot without perturbing the nuclear environment is explored: nuclear feedback is an issue that has frustrated previous studies into electron spin coherence in these systems. With the novel techniques we develop, we identify and characterise the previously undetermined intrinsic mechanisms that govern the coherence of the central spin. We show how the coherence of the electron spin is intimately related to the growth of these strained nanostructures. Second, a model network is constructed in which two spins confined to separate quantum dots are projected into a highly entangled state. This is the first time electron spins in distant quantum dots have been entangled, and in doing so we demonstrate controllable entanglement generation at the highest rates recorded for optically accessible qubit definitions. We investigate the realisation of a hybrid quantum network by demonstrating the first interconnect between wholly different single quantum systems: a semiconductor quantum dot and a trapped ytterbium ion. In forming an optical link between these two complementary qubit definitions, we show that we can circumvent their intrinsic optical differences through coherent photon generation at the quantum dot. A network built from these diverse constituents could combine the ultrafast operations self-assembled quantum dots enable with the long coherence times states in trapped ions experience. Finally, in a step towards truly scalable entanglement generation between quantum dot spins, we design minimally invasive structures that will funnel large proportions of the optical dipole field from the optically dense material that surrounds the quantum dot. The techniques developed in this work and the knowledge gained from their operation should enable the demonstration the creation of high-order nonlocal states between quantum dot spins, single photons and trapped ions, as well as the development of new optically active systems that will benefit from enhanced spin coherence.
This thesis discusses various schemes and protocols for quantum information processing in mesoscopic systems with particular focus on using the spin of a particle as the bearer of information. The first chapter introduce various aspects of the field of quantum information used in this thesis such as qubits, entanglement, its quantification, quantum logic gates and entanglement swapping. In this chapter concepts such as AKLT states, decoherence and adiabatic elimination are introduced as they will be relevant in the thesis. In chapter 2 we introduce the Quantum Dots as the solid state system that will primarily be used as the hardware for the development of Quantum Information Processing (QIP). The different properties of quantum dots depending on their size are discussed. The exchange interaction between tunnel coupled quantum dots and the background of quantum computation in quantum dots is described. The principal sources of decoherence and the measurement techniques for spin qubits are presented. In chapter 3, carbon nanowires filled with N@C60 dimers are studied to analyse the entanglement between nuclear spins. The dimer is modelled as a two coupled nuclear spin- electron spin pair with a Heisenberg interaction. The entanglement have been studied depending on the temperature and the intensity of an external magnetic field. Witnessing the entanglement, and particularly bound entanglement are discussed. In chapter 4, the way to extract a singlet from a quantum dot is explored. The system that we model will be consisting of a triple dot and analyse the best way to get the singlet out, with each electron in a separate dot. The chief motivation is to create a singlet between separate dots in a time-scale much faster than that given by spinspin exchange interactions. In chapter 5, quantum logic gates in a triple dot system has been studied. Such gates have been widely studied in double and single quantum dots. Motivated by the advent of experimental set ups of triple dots, we have studied the natural quantum gates that came out of a triple dot system. There are still two spin quantum bits in the three dots and there is an empty intervening dot, which imparts the scheme some advantages, as well as a substantial difference from the class of schemes studied so far. In chapter 6, we model a large square dot. As we describe in chapter 2, the properties of the large dots make them behave with some interesting properties such as hosting Wigner molecules of electrons inside. We explore the application of these structures for quantum information processing. We show here how to get singlet/triplet measurement, entanglement swapping, and how to prepare a 1D AKLT state, using the square dot as a construction block of the system. Finally in chapter 7 conclusions and further work. Here we indicate the further work that could be done with the knowledge present in this thesis and motivated by future advances in the technology.
Since information has been regarded as a physical entity, the field of quantum information theory has blossomed. This brings novel applications, such as quantum computation. This field has attracted the attention of numerous researchers with backgrounds ranging from computer science, mathematics and engineering, to the physical sciences. Thus, we now have an interdisciplinary field where great efforts are being made in order to build devices that should allow for the processing of information at a quantum level, and also in the understanding of the complex structure of some physical processes at a more basic level. This thesis is devoted to the theoretical study of structures at the nanometer-scale, "nanostructures," through physical processes that mainly involve the solid-state and quantum optics, in order to propose reliable schemes for the processing of quantum information. Initially, the main results of quantum information theory and quantum computation are briefly reviewed. Next, the state-of-the-art of quantum dots technology is described. In so doing, the theoretical background and the practicalities required for this thesis are introduced. A discussion of the current quantum hardware used for quantum information processing is given. In particular, the solid-state proposals to date are emphasised. A detailed prescription is given, using an optically-driven coupled quantum dot system, to reliably prepare and manipulate exciton maximally entangled Bell and Greenberger-Horne-Zeilinger (GHZ) states. Manipulation of the strength and duration of selective light-pulses needed for producing these highly entangled states provides us with crucial elements for the processing of solid-state based quantum information. The all-optical generation of states of the so-called Bell basis for a system of two quantum dots (QDs) is exploited for performing the quantum teleportation of the excitonic state of a dot in an array of three coupled QDs. Theoretical predictions suggest that several hundred single quantum bit rotations and controlled-NOT gates could be performed before decoherence of the excitonic states takes place. In addition, the exciton coherent dynamics of a coupled QD system confined within a semiconductor single mode microcavity is reported. It is shown that this system enables the control of exciton entanglement by varying the coupling strength between the optically-driven dot system and the microcavity. The exciton entanglement shows collapses and revivals for suitable amplitudes of the incident radiation field and dot-cavity coupling strengths. The results given here could offer a new approach for the control of decoherence mechanisms arising from entangled "artificial molecules." In addition to these ultrafast coherent optical control proposals, an approach for reliable implementation of quantum logic gates and long decoherence times in a QD system based on nuclear magnetic resonance (NMR) is given, where the nuclear resonance is controlled by the ground state "magic number" transitions of few-electron QDs in an external magnetic field. The dynamical evolution of quantum registers of arbitrary length in the presence of environmentally-induced decoherence effects is studied in detail. The cases of quantum bits (qubits) coupling individually to different environments ("independent decoherence"), and qubits interacting collectively with the same reservoir ("collective decoherence") are analysed in order to find explicit decoherence functions for any number of qubits. The decay of the coherences of the register is shown to strongly depend on the input states: this sensitivity is a characteristic of both types of coupling (collective and independent) and not only of the collective coupling, as has been reported previously. A non-trivial behaviour - "recoherence" - is found in the decay of the off-diagonal elements of the reduced density matrix in the specific situation of independent decoherence. The results lead to the identification of decoherence-free states in the collective decoherence limit. These states belong to subspaces of the system's Hilbert space that do not become entangled with the environment, making them ideal elements for the engineering of "noiseless" quantum codes. The relations between decoherence of the quantum register and computational complexity based on the new dynamical results obtained for the register density matrix are also discussed. This thesis concludes by summarising and pointing out future directions, and in particular, by discussing some biological resonant energy transfer processes that may be useful for the processing of information at a quantum level.
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.
Ultrafast pulses allow observation of molecular dynamics with femtosecond time resolution through pump probe experiments. However, averaging over an ensemble of molecules tends to wash out phase sensitive information, necessary to probe quantum effects, due to the intrinsic inhomogeneity in molecular conformations, orientations and interactions that lead to unique potential energy landscapes for each molecule. It is therefore important to go beyond the ensemble average when looking at quantum dynamics of organic systems at room temperature, and resolve the behaviour of specific molecules on an individual basis. In this thesis, we show the creation, manipulation and observation of ultrafast coherent effects in single molecules at room temperature, and resolve a certain measure of environmental influence on the specific dynamics of each molecule. Moreover, we apply this insight to investigate a functional light harvesting biosystem, and lay the basis for a technique that has the time and space resolution required to observe these systems in vivo. In chapter 1, we introduce the concepts and techniques the research in this thesis is built on. In chapter 2, we treat the possibility of controlling ultrafast pulses at the high-NA diffraction limit, and come to conclusions about the procedure to follow there that hold for all pulse-shaping experiments. We show in proof of principle experiments that we can control the ultrafast characteristics of optical pulses in nanometric excitation volumes. In chapters 3 and 4 we report the creation, detection and control of ultrafast quantum dynamics in single organic molecules at room temperature. We show that manipulation of superposition states is possible in these systems within a coherence dephasing time of ~50 fs. This leads to the first observation of rabi-oscillations in room temperature single molecules, to ultrafast operation of an organic qubit, and to the creation of non-stationary superposition states (vibrational wavepackets). We probe the influence of the local environment on the composition and dynamics of these wavepackets and show we can optimize the state preparation protocol for each individual molecule in its own nanoenvironment, leading to high fidelity coherent control. In these chapters we lay out the proof of principle work of detecting the quantumdynamics of a complex system in interaction with its environment at room temperature. In chapter 5 we discuss application of these techniques to the investigation of long lived coherence in photosynthetic systems. We show that electronic coherence between different rings of the LH2 system persists to time scales of 100s of femtoseconds at room temperature. Moreover we show that the energy transfer pathways in LH2 adapt to environmentally induced changes in the molecule and that the nature of the transfer remains coherent for each pathway, providing strong evidence that coherent energy transfer is the optimum process for energy transfer in photosynthesis. Finally, in chapter 6 we take the technical development one step further and report on the creation of a framework based on plasmonic antennas that allows for control of the amplitude-phase characteristics in nanometric sized hotspot fields. We show for the first time that the ultrafast characteristics of plasmonic hotspots can directly be engineered through design of the plasmonic system and experimentally demonstrate two much-anticipated examples: a sub-diffraction resolution phase shaper and an ultrafast plasmonic switch for pump probe experiments. The results presented in this thesis form the first creation and observation of ultrafast coherent dynamics in individual molecular systems at room temperature. This is a necessary step to be able to do true quantum tomography in complex systems, resolve the influence of the environment on molecular dynamics, and investigate the physics that determines evolutionary optimization and functionality in biomolecules.