This thesis addresses the problem of developing a quantum counter-part of the well established classical theory of control. We dwell on the fundamental fact that quantum states are generally not perfectly distinguishable, and quantum measurements typically introduce noise in the system being measured. Because of these, it is generally not clear whether the central concept of the classical control theory --- that of observing the system and then applying feedback --- is always useful in the quantum setting. We center our investigations around the problem of transforming the state of a quantum system into a given target state, when the system can be prepared in different ways, and the target state depends on the choice of preparation. We call this the "quantum tracking problem" and show how it can be formulated as an optimization problem that can be approached both numerically and analytically. This problem provides a simple route to the characterization of the quantum trade-off between information gain and disturbance, and is seen to have several applications in quantum information. In order to characterize the optimality of our tracking procedures, some figure-of-merit has to be specified. Naturally, distance measures for quantum states are the ideal candidates for this purpose. We investigated several possibilities, and found that there is usually a compromise between physically motivated and mathematically tractable measures. We also introduce an alternative to the Uhlmann-Jozsa fidelity for mixed quantum states, which besides reproducing a number of properties of the standard fidelity, is especially attractive because it is simpler to compute. We employ some ideas of convex analysis to construct optimal control schemes analytically. In particular, we obtain analytic forms of optimal controllers for stabilizing and tracking any pair of states of a single-qubit. In the case of stabilization, we find that feedback control is always useful, but because of the trade-off between information gain and disturbance, somewhat different from the type of feedback performed in classical systems. In the case of tracking, we find that feedback is not always useful, meaning that depending on the choice of states one wants to achieve, it may be better not to introduce any noise by the application of quantum measurements. We also demonstrate that our optimal controllers are immediately applicable in several quantum information applications such as state-dependent cloning, purification, stabilization, and discrimination. In all of these cases, we were able to recover and extend previously known optimal strategies and performances. Finally we show how optimal single-step control schemes can be concatenated to provide multi-step strategies that usually over-perform optimal control protocols based on a single interaction between the controller and the system.

This thesis addresses the problem of developing a quantum counter-part of the well established classical theory of control. We dwell on the fundamental fact that quantum states are generally not perfectly distinguishable, and quantum measurements typically introduce noise in the system being measured. Because of these, it is generally not clear whether the central concept of the classical control theory --- that of observing the system and then applying feedback --- is always useful in the quantum setting. We center our investigations around the problem of transforming the state of a quantum system into a given target state, when the system can be prepared in different ways, and the target state depends on the choice of preparation. We call this the "quantum tracking problem" and show how it can be formulated as an optimization problem that can be approached both numerically and analytically. This problem provides a simple route to the characterization of the quantum trade-off between information gain and disturbance, and is seen to have several applications in quantum information. In order to characterize the optimality of our tracking procedures, some figure-of-merit has to be specified. Naturally, distance measures for quantum states are the ideal candidates for this purpose. We investigated several possibilities, and found that there is usually a compromise between physically motivated and mathematically tractable measures. We also introduce an alternative to the Uhlmann-Jozsa fidelity for mixed quantum states, which besides reproducing a number of properties of the standard fidelity, is especially attractive because it is simpler to compute. We employ some ideas of convex analysis to construct optimal control schemes analytically. In particular, we obtain analytic forms of optimal controllers for stabilizing and tracking any pair of states of a single-qubit. In the case of stabilization, we find that feedback control is always useful, but because of the trade-off between information gain and disturbance, somewhat different from the type of feedback performed in classical systems. In the case of tracking, we find that feedback is not always useful, meaning that depending on the choice of states one wants to achieve, it may be better not to introduce any noise by the application of quantum measurements. We also demonstrate that our optimal controllers are immediately applicable in several quantum information applications such as state-dependent cloning, purification, stabilization, and discrimination. In all of these cases, we were able to recover and extend previously known optimal strategies and performances. Finally we show how optimal single-step control schemes can be concatenated to provide multi-step strategies that usually over-perform optimal control protocols based on a single interaction between the controller and the system.

This thesis addresses the problem of developing a quantum counter-part of the well established classical theory of control. We dwell on the fundamental fact that quantum states are generally not perfectly distinguishable, and quantum measurements typically introduce noise in the system being measured. Because of these, it is generally not clear whether the central concept of the classical control theory --- that of observing the system and then applying feedback --- is always useful in the quantum setting. We center our investigations around the problem of transforming the state of a quantum system into a given target state, when the system can be prepared in different ways, and the target state depends on the choice of preparation. We call this the "quantum tracking problem" and show how it can be formulated as an optimization problem that can be approached both numerically and analytically. This problem provides a simple route to the characterization of the quantum trade-off between information gain and disturbance, and is seen to have several applications in quantum information. In order to characterize the optimality of our tracking procedures, some figure-of-merit has to be specified. Naturally, distance measures for quantum states are the ideal candidates for this purpose. We investigated several possibilities, and found that there is usually a compromise between physically motivated and mathematically tractable measures. We also introduce an alternative to the Uhlmann-Jozsa fidelity for mixed quantum states, which besides reproducing a number of properties of the standard fidelity, is especially attractive because it is simpler to compute. We employ some ideas of convex analysis to construct optimal control schemes analytically. In particular, we obtain analytic forms of optimal controllers for stabilizing and tracking any pair of states of a single-qubit. In the case of stabilization, we find that feedback control is always useful, but because of the trade-off between information gain and disturbance, somewhat different from the type of feedback performed in classical systems. In the case of tracking, we find that feedback is not always useful, meaning that depending on the choice of states one wants to achieve, it may be better not to introduce any noise by the application of quantum measurements. We also demonstrate that our optimal controllers are immediately applicable in several quantum information applications such as state-dependent cloning, purification, stabilization, and discrimination. In all of these cases, we were able to recover and extend previously known optimal strategies and performances. Finally we show how optimal single-step control schemes can be concatenated to provide multi-step strategies that usually over-perform optimal control protocols based on a single interaction between the controller and the system.

Quantum control of many body atomic spins is often pursued in the context of an atom-light quantum interface, where a quantized light field acts as a "quantum bus" that can be used to entangle distant atoms. One key challenge is to improve the coherence of the atom-light interface and the amount of atom-light entanglement it can generate, given the constraints of working with multilevel atoms and optical fields in a 3D geometry. We have explored new ways to achieve this, through rigorous optimization of the spatial geometry, and through control of the internal atomic state. Our basic setup consists of a quantized probe beam passing through an atom cloud held in a dipole trap, first generating spin-probe entanglement through the Faraday interaction, and then using backaction from a measurement of the probe polarization to squeeze the collective atomic spin. The relevant figure of merit is the metrologically useful spin squeezing determined by the enhancement in the resolution of rotations of the collective spin, relative to the commonly used spin coherent state. With an optimized free-space geometry, and by using a 2-color probe scheme to suppress tensor light shifts, we achieve 3(2) dB of metrologically useful spin squeezing. We can further increase atom-light coupling by implementing internal state control to prepare spin states with larger initial projection noise relative to the spin coherent state. Under the right conditions this increase in projection noise can lead to stronger measurement backaction and increased atom-atom entanglement. With further internal state control the increased atom-atom entanglement can then be mapped to a basis where it corresponds to improved squeezing of, e.g., the physical spin-angular momentum or the collective atomic clock pseudospin. In practice, controlling the collective spin of N ~ 10⁶ atoms in this fashion is an extraordinarily difficult challenge because errors in the control of individual atoms tend to be highly correlated. By employing precise internal state control, we have prepared and detected projection noise limited "cat" states (which have initial projection noise that is larger by a factor of 2f = 8 for Cs relative to the spin coherent state) and estimate that we can generate up to 6.0(5) dB of metrologically useful spin squeezing, demonstrating the advantage of using the internal atomic structure as a resource for ensemble control.

Quantum computers have seen rapid development over the last two decades. Despite this, they are not yet scalable or fault-tolerant (i.e. we cannot address arbitrarily many error-corrected qubits). Therefore, improvements that include consideration of the underlying physics are paramount. To do this, we must reduce existing errors and understand how algorithms perform without error correction. In this dissertation, we provide contributions toward these goals. We organize these efforts into three groups. Firstly, we focus on quantum control. We introduce a novel scheme for performing entangling gates on superconducting qubits. We create fast, high-fidelity entangling operations and single-qubit gates to implement arbitrary quantum operations. Then, we implement entangling gates on real transmon qubits. Finally, we develop new techniques for entangling gates on spin qubits. In total, we improve low-level device performance with high-fidelity entangling operations. Secondly, we focus on quantum simulation algorithms. First, we apply error mitigation techniques to a quantum simulation algorithm while simultaneously performing device characterization. Then we take advantage of known symmetries of the input Hamiltonian to improve the same algorithm. Then, we demonstrate that this reduces resources compared to other approaches in the presence of noise. Then we compare this technique with state-of-the-art approaches. Then, we improve this algorithm with approaches from quantum control. Finally, we develop a novel algorithm to simulate spin chains on a quantum processor with improved resources compared to other techniques. In total, we improve quantum simulation algorithms, with the aim of better utilizing current devices. Thirdly, we consider the ADAPT-VQE algorithm, which is used to construct quantum circuits for preparing trial states in quantum simulation. In total, we improve gate counts for the algorithm, improve a separate algorithm by utilizing the gradient criterion, and leverage the repeating structure of an input Hamiltonian to improve performance. Finally, we provide a deeper understanding of ADAPT-VQE and demonstrate its robustness to scaling issues of competing algorithms. In total, we improve the algorithm and its applicability. Thus, we improve quantum simulation algorithms that can be run in the near term. / Doctor of Philosophy / The computers that we interact with every day rely on the processing of bits, represented as 1's or 0's. The rules that govern how they operate mostly rely on classical physics (i.e. discovered before quantum physics), which does not include any quantum effects. If we instead allow for quantum rules and quantum bits ("qubits"'), new types of algorithms are possible. That is to say, quantum computers can do some things more efficiently than classical computers. As such, there is a massive effort to build these devices. Because these devices are so delicate and in their early stages, this requires an understanding of the algorithm and the physical device performing it. Therefore, improving the overall performance requires taking high and low-level aspects of this design into consideration. In this dissertation, we provide three groups of contributions to achieving this goal. In the first group, we improve the device performance by considering how operations are performed on qubits, primarily in terms of producing quantum operations that have no classical analog. In the second group, we improve the simulation of quantum systems on quantum devices with a focus on how existing imperfections in the device impact the results. In the third group, we make improvements to an algorithm used to simulate quantum systems like molecules, while also developing a deeper understanding of how the algorithm functions. In each of these parts, we develop novel techniques to improve device and algorithm performance, contributing to the applicability and utility of current and future quantum devices.

Quantum Computation and Information requires high accuracy in gate control despite noises and imperfections from the environment and physical implementation. Here we introduce an SCQC Formalism based on dynamical decoupling and reverse engineering. Space Curve Quantum Control Formalism discovers the tight connections between quantum, geometric, and classical systems. We are able to use such connections to build noise-canceling, precise control, and time-optimal arbitrary gates. / Doctor of Philosophy / Quantum Computation and Information is a fast-developing technology and its application is within reach. But errors due to noises in the environment and imperfections from physical implementation are roadblocks to the practical application. In this thesis, we will introduce the Space Curve Quantum Control Formalism, which builds connections between Geometric, Quantum, and Classical pictures. We utilize these connections to build noise-robust quantum gates and time-optimal gates.

Methods of controlling molecular rotations using linearly polarized femtosecond and picosecond pulses are considered and analyzed theoretically. These laser pulses, typically in the infrared, are highly non-resonant with respect to the electronic degrees of freedom of the molecules and have intensities of &sim; 10^13 to 10^14 W/cm&sup2;. It is shown how these laser pulses can force small linear molecules to align with the direction of the electric field vector of the laser both in the presence of the laser field as well as after the application of a short laser pulse. Recent experiments on laser-induced molecular alignment are modeled and excellent agreement between experiment and theory is found. Additional methods of controlling molecular rotational dynamics are outlined. The first method considers the forced rotational acceleration of diatomic molecules, called the <i>optical centrifuge</i>. Here, the direction of polarization of a linearly polarized laser field is made to smoothly rotate faster and faster. The molecules, which tend to align with the polarization vector of the laser field, follow the rotation of the laser polarization and are accelerated to high angular momentum. The second method considers the control of field-free rotational dynamics by applying phase shifts to the molecular wave function at select times called <i>fractional revivals</i>. At these select moments, an initially localized wave function splits into several copies of the initial state. Adding phase shifts to the copies then induces interference effects which can be used to control the subsequent evolution of the rotational wave function. This same control scheme has a close link to quantum information and this connection is outlined. Finally, a recently proposed method of controlling the quantum dynamics of the classically chaotic kicked rotor system [J. Gong and P. Brumer, Phys. Rev. Lett. 86, 1741 (2001)] is analyzed from a phase space perspective. It is shown that the proposed quantum control can be linked to small islands of stability in the classical phase space. An experimentally feasible variant of this control scenario using wave packets of molecular alignment is proposed. Two applications of molecular alignment are discussed. The first application uses field-free aligned molecules as a non-linear medium for compression of a laser pulse to the 1 fs regime at optical wavelengths. At such durations, these laser pulses contain nearly a single oscillation of the electric field and represent the shortest laser pulses physically achievable for such frequencies. The second application uses molecular alignment to create a sort of gas phase "molecular crystal" which forms a basis for laser-induced electron diffraction and imaging of the aligned molecules. Here, a first laser pulse aligns the molecules in space. A second laser pulse is then used to ionize outer-shell electrons, accelerate them in the laser field, and steer them back to collide with the parent ion creating a diffraction image with sub-femtosecond and sub-Angstrom resolution.

Neutral atom systems are an appealing platform for the development and testing of quantum control and measurement techniques. This dissertation presents experimental investigations of control and measurement tools using as a testbed the 16-dimensional hyperfine manifold associated with the electronic ground state of cesium atoms. On the control side, we present an experimental realization of a protocol to implement robust unitary transformations in the presence of static and dynamic perturbations. We also present an experimental realization of inhomogeneous quantum control. Specifically, we demonstrate our ability to perform two different unitary transformations on atoms that see different light shifts from an optical addressing field. On the measurement side, we present experimental realizations of quantum state and process tomography. The state tomography project encompasses a comprehensive evaluation of several measurement strategies and state estimation algorithms. Our experimental results show that in the presence of experimental imperfections, there is a clear tradeoff between accuracy, efficiency and robustness in the reconstruction. The process tomography project involves an experimental demonstration of efficient reconstruction by using a set of intelligent probe states. Experimental results show that we are able to reconstruct unitary maps in Hilbert spaces with dimension ranging from d=4 to d=16. To the best of our knowledge, this is the first time that a unitary process in d=16 is successfully reconstructed in the laboratory.

Quantum information processing has been the subject of countless discoveries since the early 1990's. It is believed to be the way of the future for computation: using quantum systems permits one to perform computation exponentially faster than on a regular classical computer. Unfortunately, quantum systems that not isolated do not behave well. They tend to lose their quantum nature due to the presence of the environment. If key information is known about the noise present in the system, methods such as quantum error correction have been developed in order to reduce the errors introduced by the environment during a given quantum computation. In order to harness the quantum world and implement the theoretical ideas of quantum information processing and quantum error correction, it is imperative to understand and quantify the noise present in the quantum processor and benchmark the quality of the control over the qubits. Usual techniques to estimate the noise or the control are based on quantum process tomography (QPT), which, unfortunately, demands an exponential amount of resources. This thesis presents work towards the characterization of noisy processes in an efficient manner. The protocols are developed from a purely abstract setting with no system-dependent variables. To circumvent the exponential nature of quantum process tomography, three different efficient protocols are proposed and experimentally verified. The first protocol uses the idea of quantum error correction to extract relevant parameters about a given noise model, namely the correlation between the dephasing of two qubits. Following that is a protocol using randomization and symmetrization to extract the probability that a given number of qubits are simultaneously corrupted in a quantum memory, regardless of the specifics of the error and which qubits are affected. Finally, a last protocol, still using randomization ideas, is developed to estimate the average fidelity per computational gates for single and multi qubit systems. Even though liquid state NMR is argued to be unsuitable for scalable quantum information processing, it remains the best test-bed system to experimentally implement, verify and develop protocols aimed at increasing the control over general quantum information processors. For this reason, all the protocols described in this thesis have been implemented in liquid state NMR, which then led to further development of control and analysis techniques.

Methods of controlling molecular rotations using linearly polarized femtosecond and picosecond pulses are considered and analyzed theoretically. These laser pulses, typically in the infrared, are highly non-resonant with respect to the electronic degrees of freedom of the molecules and have intensities of &sim; 10^13 to 10^14 W/cm&sup2;. It is shown how these laser pulses can force small linear molecules to align with the direction of the electric field vector of the laser both in the presence of the laser field as well as after the application of a short laser pulse. Recent experiments on laser-induced molecular alignment are modeled and excellent agreement between experiment and theory is found. Additional methods of controlling molecular rotational dynamics are outlined. The first method considers the forced rotational acceleration of diatomic molecules, called the <i>optical centrifuge</i>. Here, the direction of polarization of a linearly polarized laser field is made to smoothly rotate faster and faster. The molecules, which tend to align with the polarization vector of the laser field, follow the rotation of the laser polarization and are accelerated to high angular momentum. The second method considers the control of field-free rotational dynamics by applying phase shifts to the molecular wave function at select times called <i>fractional revivals</i>. At these select moments, an initially localized wave function splits into several copies of the initial state. Adding phase shifts to the copies then induces interference effects which can be used to control the subsequent evolution of the rotational wave function. This same control scheme has a close link to quantum information and this connection is outlined. Finally, a recently proposed method of controlling the quantum dynamics of the classically chaotic kicked rotor system [J. Gong and P. Brumer, Phys. Rev. Lett. 86, 1741 (2001)] is analyzed from a phase space perspective. It is shown that the proposed quantum control can be linked to small islands of stability in the classical phase space. An experimentally feasible variant of this control scenario using wave packets of molecular alignment is proposed. Two applications of molecular alignment are discussed. The first application uses field-free aligned molecules as a non-linear medium for compression of a laser pulse to the 1 fs regime at optical wavelengths. At such durations, these laser pulses contain nearly a single oscillation of the electric field and represent the shortest laser pulses physically achievable for such frequencies. The second application uses molecular alignment to create a sort of gas phase "molecular crystal" which forms a basis for laser-induced electron diffraction and imaging of the aligned molecules. Here, a first laser pulse aligns the molecules in space. A second laser pulse is then used to ionize outer-shell electrons, accelerate them in the laser field, and steer them back to collide with the parent ion creating a diffraction image with sub-femtosecond and sub-Angstrom resolution.