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The Journal of Chemical Physics

On readout of vibrational qubits using quantum beats

Dmytro Shyshlov, Eduardo Berrios, Martin Gruebele, Dmitri Babikov

Published Dec 9, 2014• 8 citations
Publisher

Abstract

Readout of the final states of qubits is a crucial step towards implementing quantum computation in experiment. Although not scalable to large numbers of qubits per molecule, computational studies show that molecular vibrations could provide a significant (factor 2-5 in the literature) increase in the number of qubits compared to two-level systems. In this theoretical work, we explore the process of readout from vibrational qubits in thiophosgene molecule, SCCl2, using quantum beat oscillations. The quantum beats are measured by first exciting the superposition of the qubit-encoding vibrational states to the electronically excited readout state with variable time-delay pulses. The resulting oscillation of population of the readout state is then detected as a function of time delay. In principle, fitting the quantum beat signal by an analytical expression should allow extracting the values of probability amplitudes and the relative phases of the vibrational qubit states. However, we found that if this procedure is implemented using the standard analytic expression for quantum beats, a non-negligible phase error is obtained. We discuss the origin and properties of this phase error, and propose a new analytical expression to correct the phase error. The corrected expression fits the quantum beat signal very accurately, which may permit reading out the final state of vibrational qubits in experiments by combining the analytic fitting expression with numerical modelling of the readout process. The new expression is also useful as a simple model for fitting any quantum beat experiments where more accurate phase information is desired.

DOI
10.1063/1.4903055

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Physical implementation of quantum gates acting on qubits does not achieve a perfect fidelity of 1. The actual output qubit may not match the targeted output of the desired gate. According to theoretical estimates, intrinsic gate fidelities >99.99% are necessary so that error correction codes can be used to achieve perfect fidelity. Here we test what fidelity can be accomplished for a CNOT gate executed by a shaped ultrafast laser pulse interacting with vibrational states of the molecule SCCl(2). This molecule has been used as a test system for low-fidelity calculations before. To make our test more stringent, we include vibrational levels that do not encode the desired qubits but are close enough in energy to interfere with population transfer by the laser pulse. We use two complementary approaches: optimal control theory determines what the best possible pulse can do; a more constrained physical model calculates what an experiment likely can do. Optimal control theory finds pulses with fidelity >0.9999, in excess of the quantum error correction threshold with 8 × 10(4) iterations. On the other hand, the physical model achieves only 0.9992 after 8 × 10(4) iterations. Both calculations converge as an inverse power law toward unit fidelity after >10(2) iterations/generations. In principle, the fidelities necessary for quantum error correction are reachable with qubits encoded by molecular vibrations. In practice, it will be challenging with current laboratory instrumentation because of slow convergence past fidelities of 0.99.

The Journal of Physical Chemistry A•Jul 18, 2012•15 citations
Readout of the final states of qubits is a crucial step towards implementing quantum computation in experiment. Although not scalable to large numbers of qubits per molecule, computational studies show that molecular vibrations could provide a significant (factor 2-5 in the literature) increase in the number of qubits compared to two-level systems. In this theoretical work, we explore the process of readout from vibrational qubits in thiophosgene molecule, SCCl2, using quantum beat oscillations. The quantum beats are measured by first exciting the superposition of the qubit-encoding vibrational states to the electronically excited readout state with variable time-delay pulses. The resulting oscillation of population of the readout state is then detected as a function of time delay. In principle, fitting the quantum beat signal by an analytical expression should allow extracting the values of probability amplitudes and the relative phases of the vibrational qubit states. However, we found that if this procedure is implemented using the standard analytic expression for quantum beats, a non-negligible phase error is obtained. We discuss the origin and properties of this phase error, and propose a new analytical expression to correct the phase error. The corrected expression fits the quantum beat signal very accurately, which may permit reading out the final state of vibrational qubits in experiments by combining the analytic fitting expression with numerical modelling of the readout process. The new expression is also useful as a simple model for fitting any quantum beat experiments where more accurate phase information is desired.
For practical realization of quantum information processing we need a quantum system that provides reliable preparation of the initial state, high-fidelity quantum gate operations, error tolerance, readout of the result of quantum computation and scalability of the system to increase the number of qubits. In this dissertation we show how these requirements can be addressed for molecular quantum computer. For computational study of quantum information processing with molecules we employ thiophosgene (SCCl2) molecule that has been used as a test system for quantum control experiments [Mol. Phys. 105, 1999 (2007)]. We investigate the gateway scheme of control in which transitions between the vibrational states that encode qubits are only allowed through the intermediate “gateway” state in the B electronic state. This scheme of control provides reliable preparation of the initial qubit state and allows using UV/vis laser pulses. We demonstrate that high-fidelity quantum gates are possible to achieve in molecular quantum computer. The optimal control theory is employed to obtain a shape of laser pulse that performs CNOT gate with ~0.9999 fidelity. Analysis of frequency profile of the optimal pulse shows that preparation of the high-fidelity computational pulse requires only 64 frequency channels. Error tolerance of the computational pulse is studied by modifying amplitudes and phases of frequency components. It is shown that gate fidelity remains high after small modifications are introduced to the optimal pulse. The scheme of readout of quantum information using quantum beat spectroscopy is proposed. The quantum beat signal is obtained from excitation of the final superposition of the qubit states to a readout state in the B electronic state with a time-delayed pulse. We find that fitting the quantum beat signal with a standard fitting expression produces a phase error and propose a new accurate expression that includes phase correction term. The system of two atomic ions trapped in a double-well potential is also studied as a first step towards scalable quantum computation with trapped molecular ions. The rigorous computational treatment of the system provides explanation of the vibrational energy transfer between the ions in terms of wave packet dynamics in the accurate asymmetric potential.
Within the scope of molecular quantum computing with vibrational qubits, we analyse the impact of phases that are present during the quantum computation processes. While the phase relation in superposition states and its temporal evolution are crucial to any implementation of quantum computing, we elucidate the special challenge that emerges for phase control of qubits encoded in molecular vibrational eigenstates. Phase correctly prepared superposition states in general exist only for a finite time and with the inherent entanglement in molecular vibrational qubit systems their development displays a complex pattern. We show that the free relative phase evolution in such qubit systems can be utilized for the implementation of quantum phase gates. Moreover, a practical experimental realization of phase correct quantum gates acting on molecular vibrational qubits could be accomplished by a decomposition into laser-induced population transfer and free evolution phase gates. This concept adds to the flexibility in the implementation of quantum gate sequences and algorithms. A modification, where only a reduced number of selected relative phases needs to be adjusted, will make this scheme more robust and versatile. Finally, we also disclose and discuss another key feature for the implementation of phase correct quantum gates, i.e. the dependence of the quantum gate fidelity on the absolute or carrier-envelope phase of the driving femtosecond laserfield.
Accurate rotation–vibration energy levels and transition dipoles of the molecule thiophosgene are used to model the execution of quantum gates with shaped laser pulses. Qubits are encoded in 2 n vibrational computing states on the ground electronic surface of the molecule. Computations are carried out by cycling amplitude between these computing states and a gateway state with a shaped laser pulse. The shaped pulse that performs the computation is represented by a physical model of a 128–1024 channel pulse shaper. Pulse shapes are optimized with a standard genetic algorithm, yielding experimentally realizable computing pulses. The robustness of optimization is studied as a function of the vibrational states selected, rotational level structure, additional vibrational levels not assigned to the computation, and compensation for laser power variation across a molecular ensemble.
In the context of molecular quantum computation the optimal control theory (OCT) is used to obtain shaped laser pulses for high-fidelity control of vibrational qubits. Optimization is done in time domain and the OCT algorithm varies values of electric field in each time step independently, tuning hundreds of thousands of parameters to find one optimal solution. Such flexibility is not available in experiments, where pulse shaping is done in frequency domain and the number of "tuning knobs" is much smaller. The question of possible experimental interpretations of theoretically found OCT solutions arises. In this work we analyze very accurate optimal pulse that we obtained for implementing quantum gate CNOT for the two-qubit system encoded into the exited vibrational states of thiophosgene molecule. Next, we try to alter this pulse by reducing the number of available frequency channels and intentionally introducing systematic and random errors (in frequency domain, by modifying the values of amplitudes and phases of different frequency components). We conclude that a very limited number of frequency components (only 32 in the model of thiophosgene) are really necessary for accurate control of the vibrational two-qubit system, and such pulses can be readily constructed using OCT. If the amplitude and phase errors of different frequency components do not exceed ±3% of the optimal values, one can still achieve accurate transformations of the vibrational two-qubit system, with gate fidelity of CNOT exceeding 0.99.
My thesis focuses on theoretical studies in the molecular quantum computing with vibrational qubits. We studied how the molecular vibrational properties affect the fidelity of the logic gates. Our approach is to encode states of the quantum information register into the vibrational eigenstates of a molecule and use the shaped laser pulse (femtosecond, infrared) to control the vibrational state-to-state transition. By using the Optimal Control Theory to shape a femtosecond laser and numerical propagation of laser-driven vibrational wave packets, we analyzed how the vibrational properties of a two-qubit system affect the accuracy of the quantum gates and how to effectively control the vibrational state-to-state transitions. From these studies, we found the anharmonicities are very important for the control of the vibrational state-to-state transitions and an intricate interplay between the frequencies and anharmonicities in the two-qubit system leads to the occurrence of resonances between different transitions in the vibrational manifold. Such resonances cause "leakage" of population into other vibrational states and hinder the control. From theoretical analysis of resonances, we formulate several criteria for selection of molecule for implementation of the vibrational two-qubit system. These criteria can help experimentalists to choose the best molecules to achieve accurate qubit transformations in the experiment.
Physical implementation of quantum gates acting on qubits does not achieve a perfect fidelity of 1. The actual output qubit may not match the targeted output of the desired gate. According to theoretical estimates, intrinsic gate fidelities >99.99% are necessary so that error correction codes can be used to achieve perfect fidelity. Here we test what fidelity can be accomplished for a CNOT gate executed by a shaped ultrafast laser pulse interacting with vibrational states of the molecule SCCl(2). This molecule has been used as a test system for low-fidelity calculations before. To make our test more stringent, we include vibrational levels that do not encode the desired qubits but are close enough in energy to interfere with population transfer by the laser pulse. We use two complementary approaches: optimal control theory determines what the best possible pulse can do; a more constrained physical model calculates what an experiment likely can do. Optimal control theory finds pulses with fidelity >0.9999, in excess of the quantum error correction threshold with 8 × 10(4) iterations. On the other hand, the physical model achieves only 0.9992 after 8 × 10(4) iterations. Both calculations converge as an inverse power law toward unit fidelity after >10(2) iterations/generations. In principle, the fidelities necessary for quantum error correction are reachable with qubits encoded by molecular vibrations. In practice, it will be challenging with current laboratory instrumentation because of slow convergence past fidelities of 0.99.