Arman Zaribafiyan

A tractable approach to solving the exact many-body electronic wavefunction has long remained an elusive goal in quantum chemistry. Accurate computation of the electronic structure and related properties of molecules would unlock a trove of precise information, but the exponential scaling of exact methods has impeded this possibility. In this work, we report that the combination of an incremental expansion of electronic correlation with effective utilization of modern cloud compute environments can overcome the long-standing barrier of intractability. As a demonstration of viability, we investigate the bond breaking of per- and polyfluoroalkyl substances (PFAS), a class of strongly correlated systems with pressing environmental relevance. Using the incremental Full Configuration Interaction (iFCI) method, we decompose the many-body wavefunction into independently computable units and distribute them across a record-breaking one million simultaneous cloud vCPUs. Calculations for perfluorooctanoic acid, the largest PFAS studied, involve correlating 150 electrons in 330 orbitals, corresponding to a wavefunction dimension of ∽10¹⁵¹ configurations and producing the most accurate correlation energies and electron densities to date. iFCI reveals an electron localization transition in the electronic state during bond dissociation, which standard quantum chemical methods (e.g., DFT) fail to capture due to insufficient treatment of correlation. The union of a highly parallel cloud-enabled infrastructure with a polynomial-scaling method that treats static and dynamical correlation on equal footing lays the foundation for further development of novel protocols for the degradation of PFAS, alongside potential for characterization and screening of advanced molecules and materials in a wide range of chemistries.

Quantum computers have the potential to advance material design and drug discovery by performing costly electronic structure calculations. A critical aspect of this application requires optimizing the limited resources of the quantum hardware. Here, we experimentally demonstrate an end-to-end pipeline that focuses on minimizing quantum resources while maintaining accuracy. Using density matrix embedding theory as a problem decomposition technique, and an ion-trap quantum computer, we simulate a ring of 10 hydrogen atoms without freezing any electrons. The originally 20-qubit system is decomposed into 10 two-qubit problems, making it amenable to currently available hardware. Combining this decomposition with a qubit coupled cluster circuit ansatz, circuit optimization, and density matrix purification, we accurately reproduce the potential energy curve in agreement with the full configuration interaction energy in the minimal basis set. Our experimental results are an early demonstration of the potential for problem decomposition to accurately simulate large molecules on quantum hardware.

The method of increments and frozen natural orbital (MI-FNO) framework is introduced to help expedite the application of noisy, intermediate-scale quantum (NISQ) devices for quantum chemistry simulations. The MI-FNO framework provides a systematic reduction of the occupied and virtual orbital spaces for quantum chemistry simulations. The correlation energies of the resulting increments from the MI-FNO reduction can then be solved by various algorithms, including quantum algorithms such as the phase estimation algorithm and the variational quantum eigensolver (VQE). The unitary coupled-cluster singles and doubles VQE framework is used to obtain correlation energies for the case of small molecules (i.e., BeH₂, CH₄, NH₃, H₂O, and HF) using the cc-pVDZ basis set. The quantum resource requirements are estimated for a constrained geometry complex catalyst that is utilized in industrial settings for the polymerization of α-olefins. We show that the MI-FNO approach provides a significant reduction in the quantum bit (qubit) requirements relative to the full system simulations. We propose that the MI-FNO framework can create scalable examples of quantum chemistry problems that are appropriate for assessing the progress of NISQ devices.

Eigenstate preparation is ubiquitous in quantum computing, and a standard approach for generating the lowest-energy states of a given system is by employing adiabatic state preparation (ASP). In the present work, we investigate a variational method for determining the optimal scheduling procedure within the context of ASP. In the absence of quantum error correction, running a quantum device for any meaningful amount of time causes a system to become susceptible to the loss of relevant information. Therefore, if accurate quantum states are to be successfully generated, it is crucial to find techniques that shorten the time of individual runs during iterations of annealing. We demonstrate our variational method toward this end by investigating the hydrogen and P4 molecules, as well as the Ising model problem on a two-dimensional triangular lattice. In both cases, the time required for one iteration to produce accurate results is reduced by several orders of magnitude in comparison to what is achievable via standard ASP. The significant shortening of the required time is achieved by using excited states partially during ASP. As a result, the required quantum coherence time to perform such a calculation on a quantum device becomes much less stringent with the implementation of this algorithm. In addition, our variational method is found to exhibit resilience against control errors, which are commonly encountered within the realm of quantum computing.

Quantum computers have the potential to perform accurate and efficient electronic structure calculations, enabling the simulation of properties of materials. However, today’s noisy, intermediate-scale quantum (NISQ) devices have a limited number of qubits and gate operations due to the presence of errors. Here, we propose a systematically improvable end-to-end pipeline to alleviate these limitations. Our proposed resource-efficient pipeline combines problem decomposition techniques for compact molecular representations, circuit optimization methods for compilation, solving the eigenvalue problem on advanced quantum hardware, and error-mitigation techniques in post-processing the results. Using the density matrix embedding theory for compact representation, and an ion-trap quantum computer, we simulate a ring of 10 hydrogen atoms taking into account all electrons equally and explicitly in the electronic structure calculation. In our experiment, we simulated the largest molecular system on a quantum computer within chemical accuracy with respect to total molecular energy calculated by the full CI method. Our methods reduce the number of qubits required for high-accuracy quantum simulations by an order of magnitude in the present work, enabling the simulation of larger, more industrially relevant molecules using NISQ devices. They are further systematically improvable as devices’ computational capacity continues to grow.

With the aim of establishing a framework to efficiently perform the practical application of quantum chemistry simulation on near-term quantum devices, we envision a hybrid quantum--classical framework for leveraging problem decomposition (PD) techniques in quantum chemistry. Specifically, we use PD techniques to decompose a target molecular system into smaller subsystems requiring fewer computational resources. In our framework, there are two levels of hybridization. At the first level, we use a classical algorithm to decompose a target molecule into subsystems, and utilize a quantum algorithm to simulate the quantum nature of the subsystems. The second level is in the quantum algorithm. We consider the quantum--classical variational algorithm that iterates between an expectation estimation using a quantum device and a parameter optimization using a classical device. We investigate three popular PD techniques for our hybrid approach: the fragment molecular-orbital (FMO) method, the divide-and-conquer (DC) technique, and the density matrix embedding theory (DMET). We examine the efficacy of these techniques in correctly differentiating conformations of simple alkane molecules. In particular, we consider the ratio between the number of qubits for PD and that of the full system; the mean absolute deviation; and the Pearson correlation coefficient and Spearman's rank correlation coefficient. Sampling error is introduced when expectation values are measured on the quantum device. Therefore, we study how this error affects the predictive performance of PD techniques. The present study is our first step to opening up the possibility of using quantum chemistry simulations at a scale close to the size of molecules relevant to industry on near-term quantum hardware.

The advent of new special-purpose hardware such as FPGA or ASIC-based annealers and quantum processors has shown potential in solving certain families of complex combinatorial optimization problems more efficiently than conventional CPUs. We show that to address an industrial optimization problem, a hybrid architecture of CPUs and non-CPU devices is inevitable. In this paper, we propose problem decomposition as an effective method for designing a hybrid CPU--non-CPU optimization solver. We introduce the required algorithmic elements for making problem decomposition a viable approach in meeting the real-world constraints such as communication time and the potential higher cost of using non-CPU hardware. We then turn to the well-known maximum clique problem, and propose a new method of decomposition for this problem. Our method enables us to solve the maximum clique problem on very large graphs using non-CPU hardware that is considerably smaller than the size of the graph. As an example, we show that the maximum clique problem on the com-Amazon graph, with 334,863 vertices and 925,872 edges, can be solved with a single call to a device that can embed a fully connected graph of size at least 21 nodes, such as the D-Wave 2000Q. We also show that our proposed problem decomposition approach can improve the runtime of two of the best-known classical algorithms for large, sparse graphs, namely PMC and BBMCSP, by orders of magnitude. In the light of our study, we believe that new non-CPU hardware that is small in size could become competitive with CPUs if it could be either mass produced and highly parallelized, or able to provide high-quality solutions to specific, small-sized problems significantly faster than CPUs.

The limited connectivity of current and next-generation quantum annealers motivates the need for efficient graph-minor embedding methods. These methods allow non-native problems to be adapted to the target annealer's architecture. The overhead of the widely used heuristic techniques is quickly proving to be a significant bottleneck for solving real-world applications. To alleviate this difficulty, we propose a systematic and deterministic embedding method, exploiting the structures of both the input graph of the specific problem and the quantum annealer. We focus on the specific case of the Cartesian product of two complete graphs, a regular structure that occurs in many problems. We divide the embedding problem by first embedding one of the factors of the Cartesian product in a repeatable pattern. The resulting simplified problem consists of the placement and connecting together of these copies to reach a valid solution. Aside from the obvious advantage of a systematic and deterministic approach with respect to speed and efficiency, the embeddings produced are easily scaled for larger processors and show desirable properties for the number of qubits used and the chain length distribution. To conclude, we briefly address the problem of circumventing inoperable qubits by presenting possible extensions of the method.