Quantum computing has emerged as a transformative approach for tackling complex problems in quantum chemistry, particularly in simulating multielectron systems and electron-phonon interactions. However, the current noisy intermediate-scale quantum (NISQ) devices face significant challenges in implementing practical quantum algorithms due to error accumulation caused by increased circuit depth, qubit counts, and gate operations. To address these challenges, we present TenCirChem, an open-source Python package specifically designed for implementing variational quantum algorithms in quantum computational chemistry. TenCirChem demonstrates exceptional performance in simulating unitary coupled-cluster circuits through its innovative use of compact representations for quantum states and excitation operators. This package supports noisy circuit simulation and provides advanced algorithms for variational quantum dynamics, enabling researchers to explore complex chemical phenomena. Its capabilities are exemplified in various applications, including the calculation of potential energy curves and the investigation of quantum gate error impacts on molecular systems. Moreover, TenCirChem’s seamless integration with real quantum hardware makes it a versatile tool for both simulation and experimentation. A key innovation developed within the TenCirChem framework is the Clifford-based Hamiltonian engineering approach for molecules (CHEM). This algorithm addresses the critical challenge of achieving chemical accuracy with shallow quantum circuits, a fundamental requirement for practical applications on NISQ devices. CHEM employs a sophisticated Clifford-based Hamiltonian transformation that operates within the variational quantum eigensolver (VQE) framework using hardware-efficient ansatz. The method ensures four crucial advantages: (1) generation of initial circuit parameters corresponding to Hartree-Fock energy, (2) maximization of initial energy gradients with respect to circuit parameters, (3) minimal classical processing overhead without additional quantum resource requirements, and (4) compatibility with any circuit topology. Through quantum hardware emulator demonstrations, CHEM has achieved chemical accuracy for systems up to 12 qubits with fewer than 30 two-qubit gates, representing a significant advancement in practical quantum computational chemistry. To enhance the efficiency of variational quantum algorithms, we developed the sequential optimization with approximate parabola (SOAP) method, specifically designed for parameter optimization in unitary coupled-cluster ansatz. SOAP addresses the critical bottleneck of measurement requirements in VQE by implementing an innovative optimization strategy that approximates the energy landscape as quadratic functions. This approach minimizes the number of energy evaluations while incorporating parameter correlations through the integration of average directions from previous iterations. Benchmark studies demonstrate SOAP’s superior performance, showing faster convergence and enhanced noise robustness compared to traditional optimization methods. The method’s scalability has been validated through numerical simulations of up to 20 qubits, and its practical efficacy has been confirmed through experiments on superconducting quantum computers. For simulating electron-phonon systems, we introduce a variational basis state encoding algorithm that significantly reduces resource requirements compared to conventional unary and binary encoding schemes. Our approach achieves smaller scaling than traditional methods for qubits and gates for systems obeying the area law of entanglement entropy, this remarkable reduction in resource requirements comes at the cost of a constant amount of additional measurements. The algorithm’s effectiveness has been validated through both numerical simulations and quantum hardware experiments, demonstrating that using just one or two qubits per phonon mode can produce quantitatively accurate results across various coupling regimes. The integration of these innovations within the TenCirChem library represents a significant advancement in quantum computational chemistry. The software package provides researchers with a comprehensive toolkit for developing, testing, and implementing quantum algorithms, while the novel methods address fundamental challenges in circuit depth, parameter optimization, and resource efficiency. These developments collectively enhance the practicality of quantum computing for addressing real-world chemical problems in the NISQ era, offering improved accuracy, efficiency, and noise robustness.
Abstract Quantum chemistry (QC) is one of the most promising applications of quantum computing. However, present quantum processing units (QPUs) are still subject to large errors. Therefore, noisy intermediate‐scale quantum (NISQ) hardware is limited in terms of qubit counts/circuit depths. Variational quantum eigensolver (VQE) algorithms can potentially overcome such issues. Here, we introduce the OpenVQE open‐source QC package. It provides tools for using and developing chemically‐inspired adaptive methods derived from unitary coupled cluster (UCC). It facilitates the development and testing of VQE algorithms and is able to use the Atos Quantum Learning Machine (QLM), a general quantum programming framework enabling to write/optimize/simulate quantum computing programs. We present a specific, freely available QLM open‐source module, myQLM‐fermion. We review its key tools for facilitating QC computations (fermionic second quantization, fermion‐spin transforms, etc.). OpenVQE largely extends the QLM's QC capabilities by providing: (i) the functions to generate the different types of excitations beyond the commonly used UCCSD ansatz; (ii) a new Python implementation of the “adaptive derivative assembled pseudo‐Trotter method” (ADAPT‐VQE). Interoperability with other major quantum programming frameworks is ensured thanks to the myQLM‐interop package, which allows users to build their own code and easily execute it on existing QPUs. The combined OpenVQE/myQLM‐fermion libraries facilitate the implementation, testing and development of variational quantum algorithms, while offering access to large molecules as the noiseless Schrödinger‐style dense simulator can reach up to 41 qubits for any circuit. Extensive benchmarks are provided for molecules associated to qubit counts ranging from 4 to 24. We focus on reaching chemical accuracy, reducing the number of circuit gates and optimizing parameters and operators between “fixed‐length” UCC and ADAPT‐VQE ansätze. This article is categorized under: Software > Quantum Chemistry Quantum Computing > Algorithms
One of the first practical applications of quantum computers is expected to be molecular modelling. Performing this task would profoundly affect areas such as chemistry, materials science and drug synthesis. Modelling of molecules, which are classically intractable, can be achieved with just over
30 qubits, whereas state of the art quantum computers already have more than
50 qubits. The Variational Quantum Eigensolver (VQE) algorithm and VQE based protocols, are promising candidates to enable this task on emerging Noisy Intermediate-Scale Quantum (NISQ) computers. These protocols require short quantum circuits and short coherence times, and are particularly resilient to quantum errors. Nevertheless, there is still a significant gap between the accuracy and the coherence times of current NISQ computers, and the hardware requirements of VQE protocols to simulate practically interesting molecules. In this thesis, I present my contribution to narrowing this gap by developing VQE protocols for molecular modelling that are less demanding on quantum hardware. The VQE relies on the Rayleigh-Ritz variational principle to estimate the eigenvalues of a Hamiltonian operator, by minimizing its expectation value with respect to a trial quantum state, prepared by an ansatz. A major challenge for the practical realisation of VQE protocols on NISQ computers is to construct an ansatz that: (1) can accurately approximate the eigenstates of the Hamiltonian; (2) is easy to optimize; and (3) can be implemented by a shallow circuit, within the capabilities of a NISQ computer. The most widely used, unitary coupled cluster (UCC), type of ans\"atze mathematically correspond to a product of unitary evolutions of fermionic excitation operators. Owing to their fermionic structure, UCC ans\"atze preserve the symmetries of electronic wavefunctions, and thus are accurate and easy to optimize. Nevertheless, UCC ans\"atze are implemented by high depth circuits, which severely limit the size of the molecules that can be reliably simulated on NISQ computers. In this thesis, I begin by constructing efficient quantum circuits to perform evolutions of fermionic excitation operators. The circuits are optimized in the number of two-qubit entangling gates, which are the current bottleneck of NISQ computers. Compared to the standard circuits used to implement evolutions of fermionic excitation operators, the circuits derived in this thesis reduce the number of two-qubit entangling gates by more than
70% on average. As an intermediate result, I also derive efficient circuits to perform evolutions of qubit excitation operators (excitation operators that account for qubit, rather than fermionic commutation relations). Even with the fermionic-excitation-evolution circuits derived here, UCC ans\"atze still require very long circuits, with a particularly large number of two-qubit entangling gates. In this thesis, I consider the use of alternative VQE ans\"atze, based on evolutions of qubit excitation operators. Due to not accounting for fermionic anticommutation, evolutions of qubit excitation operators can be performed by circuits that require asymptotically fewer two-qubit entangling gates. Furthermore, qubit excitation operators preserve many of the physical properties of fermionic excitation operators. Performing a number of classical numerical VQE simulations for small molecules, I show that qubit-excitation-based ans\"atze can approximate molecular electronic wavefunctions almost as accurately as fermionic-excitation-based ans\"atze. Hence, I argue that evolutions of qubit excitation operators are more suitable to construct molecular ans\"atze than evolutions of fermionic excitation operators, especially in the era of NISQ computers. Motivated by the advantage of qubit-excitation-based ans\"atze, I introduce the qubit-excitation-based adaptive variational quantum eigensolver (QEB-ADAPT-VQE). The QEB-ADAPT-VQE belongs to a family of ADAPT-VQE protocols for molecular modelling that grow a problem-tailored ansatz by iteratively appending unitary operators sampled from a predefined finite-size pool of operators. The operator at each iteration is sampled based on an ansatz-growing strategy, which aims to achieve the lowest estimate for the Hamiltonian expectation value at each iteration. In this way, ADAPT-VQE protocols construct shallow-circuit, few-parameter ans\"atze tailored specifically to the molecular systems of interest. In the case of the QEB-ADAPT-VQE, the operator pool is defined by a set of evolutions of single and double qubit excitation operators. I benchmark the performance of the QEB-ADAPT-VQE, by performing classical numerical simulations. I demonstrate that it can construct ans\"atze that are several orders of magnitude more accurate, and require significantly shallower circuits, than standard UCC ans\"atze. I also compare the QEB-ADAPT-VQE against the original fermionic-ADAPT-VQE, which utilizes a pool of fermionic excitation evolutions, and the qubit-ADAPT-VQE, which utilizes a pool of Pauli-string evolutions. I demonstrate that, in terms of circuit efficiency and convergence speed, the QEB-ADAPT-VQE systematically outperforms the qubit-ADAPT-VQE, which to my knowledge was the previous most circuit-efficient, scalable VQE protocol for molecular modeling. The QEB-ADAPT-VQE protocol, therefore represents a significant improvement in the field of VQE protocols for molecular modelling and brings us closer to achieving practical quantum advantage. Lastly, I outline a modified version of the QEB-ADAPT-VQE, the excited-QEB-ADAPT-VQE, designed to estimate energies of excited molecular states. The excited-QEB-ADAPT-VQE is more robust to initial simulation conditions, at the expense of increased computational complexity.
In this work, we present a comprehensive comparative study between two different Ansatz quantum circuits , specifically the Unitary Vibrational Coupled Cluster (UVCC) and the Compact Heuristic Circuit (CHC) with use in computational chemistry . By incorporating these circuits into the Variational Quantum Eigensolver (VQE), we aim to find the vibrational ground state energy of small molecules. Our results, obtained using both the UVCC and CHC ansatzes with and without quantum hardware noise, are benchmarked against classical computational methods for energy state determination. We emphasize the efficiency and accuracy of the CHC Ansatz , which significantly reduces circuit complexity without sacrificing the fidelity of the results. This characteristic demonstrates the potential of the CHC Ansatz for scalable quantum chemistry applications, particularly in the Noisy Intermediate-Scale Quantum (NISQ) era. Furthermore, we employ the CHC Ansatz in conjunction with the Variational Quantum Deflation (VQD) algorithm to determine the excited vibrational state energies, which is compared against the reliable method of quantum Equation of Motion(qEOM). Through this comparative study, we aim to provide valuable insights into the practical applications of these Ansatz in quantum simulations of molecular systems, highlighting their respective advantages and potential for future quantum chemistry research.
We present example quantum chemistry programs written with JaqalPaq, a python meta-programming language used to code in Jaqal (Just Another Quantum Assembly Language). These JaqalPaq algorithms are intended to be run on the Quantum Scientific Computing Open User Testbed (QSCOUT) platform at Sandia National Laboratories. Our exemplars use the variational quantum eigensolver (VQE) quantum algorithm to compute the ground state energies of the H2, HeH+, and LiH molecules. Since the exemplars focus on how to program in JaqalPaq, the calculations of the second-quantized Hamiltonians are performed with the PySCF python package, and the mappings of the fermions to qubits are obtained from the OpenFermion python package. Using the emulator functionality of JaqalPaq, we emulate how these exemplars would be executed on an error-free QSCOUT platform and compare the emulated computation of the bond-dissociation curves for these molecules with their exact forms within the relevant basis.
Abstract Quantum computing is aimed to solve tasks, which are believed to be exponentially hard to existing computational devices and tools. A prominent example of such classically hard problems is simulating complex quantum many-body systems, in particular, for quantum chemistry. However, solving realistic quantum chemistry problems with quantum computers encounters various difficulties, which are related, first, to limited computational capabilities of existing quantum devices and, second, to the efficiency of algorithmic approaches. In the present work, we address the algorithmic side of quantum chemistry applications by introducing a Python 3 code library, whose primary objective is to speed up the development of variational quantum algorithms for electronic structure problems. We describe the various features and capabilities of this library, including its ease in constructing customized versions of variational quantum algorithms. We elucidate how the developed library allows one to design quantum circuits and enable for the efficient execution of quantum algorithms. Furthermore, the library facilitates the integration of classical and quantum algorithms for hybrid computations and helps to realize the cross-verification of data with traditional computational methods, thereby enhancing the overall reliability of quantum chemistry simulations.