Accuracy and Resource Estimations for Quantum Chemistry on a Near-Term Quantum Computer.

One of the most important application areas of molecular quantum chemistry is the study and prediction of chemical reactivity. Large-scale, fully error-tolerant quantum computers could provide exact or near-exact solutions to the underlying electronic structure problem with exponentially less effort than a classical computer thus enabling highly accurate predictions for comparably large molecular systems. In the nearer future, however, only "noisy" devices with a limited number of qubits that are subject to decoherence will be available. For such near-term quantum computers the hybrid quantum-classical variational quantum eigensolver algorithm in combination with the unitary coupled-cluster ansatz (UCCSD-VQE) [ Peruzzo et al. Nat. Commun. 2014 , 5 , 4213 and McClean et al. New J. Phys. 2016 , 18 , 023023 ] has become an intensively discussed approach that could provide accurate results before the dawn of error-tolerant quantum computing. In this work we present an implementation of UCCSD-VQE that allows for the first time to treat both open- and closed-shell molecules. We study the accuracy of the obtained energies for nine small molecular systems as well as for four exemplary chemical reactions by comparing to well-established electronic structure methods like (nonunitary) coupled-cluster and density functional theory. Finally, we roughly estimate the required quantum hardware resources to obtain "useful" results for practical purposes.

Estimating the Error of an Analog Quantum Simulator by Additional Measurements.

We study an analog quantum simulator coupled to a reservoir with a known spectral density. The reservoir perturbs the quantum simulation by causing decoherence. The simulator is used to measure an operator average, which cannot be calculated using any classical means. Since we cannot predict the result, it is difficult to estimate the effect of the environment. Especially, it is difficult to resolve whether the perturbation is small or if the actual result of the simulation is in fact very different from the ideal system we intend to study. Here, we show that in specific systems a measurement of additional correlators can be used to verify the reliability of the quantum simulation. The procedure only requires additional measurements on the quantum simulator itself. We demonstrate the method theoretically in the case of a single spin connected to a bosonic environment.

Decoherence spectroscopy with individual two-level tunneling defects.

Recent progress with microfabricated quantum devices has revealed that an ubiquitous source of noise originates in tunneling material defects that give rise to a sparse bath of parasitic two-level systems (TLSs). For superconducting qubits, TLSs residing on electrode surfaces and in tunnel junctions account for a major part of decoherence and thus pose a serious roadblock to the realization of solid-state quantum processors. Here, we utilize a superconducting qubit to explore the quantum state evolution of coherently operated TLSs in order to shed new light on their individual properties and environmental interactions. We identify a frequency-dependence of TLS energy relaxation rates that can be explained by a coupling to phononic modes rather than by anticipated mutual TLS interactions. Most investigated TLSs are found to be free of pure dephasing at their energy degeneracy points, around which their Ramsey and spin-echo dephasing rates scale linearly and quadratically with asymmetry energy, respectively. We provide an explanation based on the standard tunneling model, and identify interaction with incoherent low-frequency (thermal) TLSs as the major mechanism of the pure dephasing in coherent high-frequency TLS.