Quantum simulation algorithms often require numerous ancilla qubits and deep circuits, prohibitive for near-term hardware. We introduce a framework for simulating quantum channels using ensembles of low-depth circuits in place of many-qubit dilations. This naturally enables simulations of open systems, which we demonstrate by preparing damped many-qubit GHZ states on ibm_hanoi. The technique further inspires two Hamiltonian simulation algorithms with gate counts that are asymptotically independent of the spectral precision target, reducing resource requirements by several orders of magnitude for a benchmark system.

Accurate models for open quantum systems─quantum states that have nontrivial interactions with their environment─may aid in the advancement of a diverse array of fields, including quantum computation, informatics, and the prediction of static and dynamic molecular properties. In recent years, quantum algorithms have been leveraged for the computation of open quantum systems as the predicted quantum advantage of quantum devices over classical ones may allow previously inaccessible applications. Accomplishing this goal will require input and expertise from different research perspectives, as well as the training of a diverse quantum workforce, making a compilation of current quantum methods for treating open quantum systems both useful and timely. In this Review, we first provide a succinct summary of the fundamental theory of open quantum systems and then delve into a discussion on recent quantum algorithms. We conclude with a discussion of pertinent applications, demonstrating the applicability of this field to realistic chemical, biological, and material systems.

Simulating quantum systems with their environments often requires non-unitary operations, and mapping these to quantum devices often involves expensive dilations or prohibitive measurement costs to achieve desired precisions. Building on prior work with a finite-differences strategy, we introduce an efficient and exact single-ancilla unitary decomposition technique that addresses these challenges. Our approach is based on Lagrange-Sylvester interpolation, akin to analytical differentiation techniques for functional interpolation. As a result, we can exactly express any arbitrary non-unitary operator with no finite approximation error using an easily computable decomposition. This can lead to several orders of magnitude reduction in the measurement cost, which is highly desirable for practical quantum computations of open systems.

Bosonic quantum devices offer a novel approach to realize quantum computations, where the quantum two-level system (qubit) is replaced with the quantum (an)harmonic oscillator (qumode) as the fundamental building block of the quantum simulator. The simulation of chemical structure and dynamics can then be achieved by representing or mapping the system Hamiltonians in terms of bosonic operators. In this perspective, we review recent progress and future potential of using bosonic quantum devices for addressing a wide range of challenging chemical problems, including the calculation of molecular vibronic spectra, the simulation of gas-phase and solution-phase adiabatic and nonadiabatic chemical dynamics, the efficient solution of molecular graph theory problems, and the calculations of electronic structure.

Quantum computers have the potential for a significant speedup of molecular computations. However, existing algorithms have limitations; quantum phase estimation (QPE) is intractable on current hardware while variational quantum eigensolvers (VQE) are dependent upon approximate wave functions without guaranteed convergence. In this paper we present an algorithm that yields verifiably exact solutions of the many-electron Schrodinger equation. Rather than solve the Schrodinger equation directly, we solve its contraction over all electrons except two, known as the contracted Schrodinger equation (CSE). The CSE generates a wave-function Ansatz, constructed from an iterative product of nonunitary two-body transformations, whose energy gradient with respect to the two-body operator of the current iteration vanishes if and only if the CSE is satisfied. Because the CSE implies the Schrodinger equation, the two-electron Ansatz provides a verifiably exact Ansatz for solving the many-electron Schrodinger equation. The exactness property contrasts with that of Ansatze built from the product of unitary two-body transformations where the gradient-the residual of the anti-Hermitian part of the CSE (ACSE)-can vanish without implying a solution of the Schrodinger equation. We demonstrate the algorithm on both simulators and noisy quantum computers with H2 dissociation and the rectangle-to-square transition in H4.

Quantum computing offers several new pathways toward finding many-body eigenstates, with variational approaches being some of the most flexible and near-term oriented. These require particular parameterizations of the state, and for solving multiple eigenstates must incorporate orthogonality. In this work, we use techniques from manifold optimization to arrive at solutions of the many-body eigenstate problem via direct minimization over the Stiefel and Grassmannian manifolds, avoiding parameterizations of the states and allowing for multiple eigenstates to be simultaneously calculated. These Riemannian manifolds naturally encode orthogonality constraints and have efficient quantum representations of the states and tangent vectors. We provide example calculations for quantum many-body molecular systems and discuss different pathways for solving the multiple eigenstate problem.

The aim of the Quantum Games workshop is to enable participants to develop an intuition for the particularly “non-intuitive” principles of quantum mechanics, such as superposition and wavefunction collapse (i.e., quantum measurement). These phenomena have important applications across the physical sciences, and some of the most exciting aspects are related to recent progress in quantum computing! The goal of the workshop is to teach participants to reason intuitively about quantum systems, thus enabling them to use their unique perspectives to become future leaders in the field of quantum information science!

Calculating ground and excited states is an exciting prospect for near-term quantum computing applications, and accurate and efficient algorithms are needed to assess viable directions. We develop an excited-state approach based on the contracted quantum eigensolver (ES-CQE), which iteratively attempts to find a solution to a contraction of the Schrödinger equation projected onto a subspace and does not require a priori information on the system. We focus on the anti-Hermitian portion of the equation, leading to a two-body unitary ansatz. We investigate the role of symmetries, initial states, constraints, and overall performance within the context of the model strongly correlated rectangular H4 system. We show that the ES-CQE achieves near-exact accuracy across the majority of states, covering regions of strong and weak electron correlation, while also elucidating challenging instances for two-body unitary ansatz.

Simulating physical systems on quantum devices is one of the most promising applications of quantum technology. Current quantum approaches to simulating open quantum systems are still practically challenging on NISQ-era devices, because they typically require ancilla qubits and extensive controlled sequences. In this work, we propose a hybrid quantum -classical approach for simulating a class of open system dynamics called random -unitary channels. These channels naturally decompose into a series of convex unitary evolutions, which can then be efficiently sampled and run as independent circuits. The method does not require deep ancilla frameworks and thus can be implemented with lower noise costs. We implement simulations of open quantum systems up to dozens of qubits and with large channel ranks.

The generation and control of entanglement in a quantum mechanical system are critical elements of nearly all quantum applications. Molecular systems are promising candidates, with numerous degrees of freedom able to be targeted. However, knowledge of intersystem entanglement mechanisms in such systems is limited. In this work, we demonstrate the generation of entanglement between vibrational degrees of freedom in molecules via strong coupling to a cavity mode driven by a weak coherent field. In a bimolecular system, we show that entanglement can be generated not only between the cavity and molecular system but also between molecules. This process also results in the generation of nonclassical states of light, providing potential pathways for harnessing entanglement in molecular systems.

Quantum computers may demonstrate significant advantages over classical devices, as they are able to exploit a purely quantum-mechanical phenomenon known as entanglement in which a single quantum state simultaneously populates two-or-more classical configurations. However, due to environmental noise and device errors, elaborate quantum entanglement can be difficult to prepare on modern quantum computers. In this paper, we introduce a metric based on the condensation of qubits to assess the ability of a quantum device to simulate many-electron systems. Qubit condensation occurs when the qubits on a quantum computer condense into a single, highly correlated particle-hole state. While conventional metrics like gate errors and quantum volume do not directly target entanglement, the qubit-condensation metric measures the quantum computer's ability to generate an entangled state that achieves nonclassical long-range order across the device. To demonstrate, we prepare qubit condensations on various quantum devices and probe the degree to which qubit condensation is realized via postmeasurement analysis. We show that the predicted ranking of the quantum devices is consistent with the errors obtained from molecular simulations of H2 using a contracted quantum eigensolver.

Quantum computing has the potential to revolutionize computing for certain classes of problems with exponential scaling, and yet this potential is accompanied by significant sensitivity to noise, requiring sophisticated error correction and mitigation strategies. Here we simulate the relaxations of stationary states at different frequencies on several quantum computers to obtain unique spectroscopic fingerprints of their noise. Response functions generated from the data reveal a clear signature of non-Markovian dynamics, demonstrating that each of the quantum computers acts as a non-Markovian bath with a unique colored noise profile. The study suggest that noisy intermediate-scale quantum computers (NISQ) provide a built-in noisy bath that can be analyzed from their simulation of closed quantum systems with the results potentially being harnessed for error mitigation or open-system simulation.

Quantum computers potentially have an exponential advantage over classical computers for the quantum simulation of many-fermion quantum systems. Nonetheless, fermions are more expensive to simulate than bosons due to the fermionic encoding???a mapping by which the qubits are encoded with fermion statistics. Here we generalize the contracted quantum eigensolver (CQE) to avoid fermionic encoding of the wave function. In contrast to the variational quantum eigensolver, the CQE solves for a many-fermion stationary state by minimizing the contraction (projection) of the Schr??dinger equation onto two fermions. We avoid fermionic encoding of the wave function by contracting the Schr??dinger equation onto an unencoded pair of particles. Solution of the resulting contracted equation by a series of unencoded two-body exponential transformations generates an unencoded wave function from which the energy and two-fermion reduced density matrix (2-RDM) can be computed. We apply the unencoded and the encoded CQE algorithms to the hydrogen fluoride molecule, the dissociation of oxygen O2, and a series of hydrogen chains. Both algorithms show comparable convergence towards the exact ground-state energies and 2-RDMs, but the unencoded algorithm has computational advantages in terms of state preparation and tomography.

A contracted quantum eigensolver (CQE) finds a solution to the many-electron Schrödinger equation by solving its integration (or contraction) to the two-electron space─a contracted Schrödinger equation (CSE)─on a quantum computer. When applied to the anti-Hermitian part of the CSE (ACSE), the CQE iterations optimize the wave function, with respect to a general product ansatz of two-body exponential unitary transformations that can exactly solve the Schrödinger equation. In this work, we accelerate the convergence of the CQE and its wave function ansatz via tools from classical optimization theory. By treating the CQE algorithm as an optimization in a local parameter space, we can apply quasi-second-order optimization techniques, such as quasi-Newton approaches or nonlinear conjugate gradient approaches. Practically, these algorithms result in superlinear convergence of the wave function to a solution of the ACSE. Convergence acceleration is important because it can both minimize the accumulation of noise on near-term intermediate-scale quantum (NISQ) computers and achieve highly accurate solutions on future fault-tolerant quantum devices. We demonstrate the algorithm, as well as some heuristic implementations relevant for cost-reduction considerations, comparisons with other common methods such as variational quantum eigensolvers, and a Fermionic-encoding-free form of the CQE.

The simulation of strongly correlated many-electron systems is one of the most promising applications for near-term quantum devices. Here we use a class of eigenvalue solvers [presented in Smart and Mazziotti, Phys. Rev. Lett. 126, 070504 (2021)] in which a contraction of the Schrodinger equation is solved for the two-electron reduced density matrix (2-RDM) to resolve the energy splittings of the ortho-, meta-, and para-isomers of benzyne C6H4. In contrast to the traditional variational quantum eigensolver, the contracted quantum eigensolver can solve an integration (or contraction) of the many-electron Schrodinger equation onto the two-electron space. The quantum solution of the anti-Hermitian part of the contracted Schrodinger equation provides a scalable approach with few variational parameters that has its foundations in 2-RDM theory. Experimentally, a variety of error-mitigation strategies enable the calculation, including a linear shift in the 2-RDM targeting the iterative nature of the algorithm as well as a projection of the 2-RDM onto the convex set of approximately N-representable 2-RDMs defined by the 2-positive N-representability conditions. The relative energies exhibit single-digit millihartree errors, capturing a large part of the electron correlation energy, and the computed natural orbital occupations reflect the significant differences in the electron correlation of the isomers.

Measurement in quantum simulations provides a means for extracting meaningful information from a complex quantum state, and for quantum computing, reducing the complexity of measurement will be vital for near-term applications. For most quantum simulations, the targeted state will obey several symmetries inherent to the system Hamiltonian. We obtain an alternative symmetry projected basis of measurement that reduces the number of measurements needed by a constant factor. Our scheme can be implemented at no additional cost on a quantum computer, can be implemented under various measurement or tomography schemes, and is reasonably resilient under noise.

The simulation of strongly correlated many-electron systems is one of the most promising applications for near-term quantum devices. Here we develop and apply a family of quantum simulation algorithms for electronic structure, based on the integration (or contraction) of the Schrodinger equation onto the two-electron space. We showcase the family of algorithms by resolving the energy splittings of the ortho-, meta-, and para-isomers of benzyne ${\textrm C_6} {\textrm H_4}$ including the strongly correlated biradical para-benzyne. The quantum solution of the anti-Hermitian part of the contracted Schrodinger equation (qACSE) provides a scalable approach with low circuit depth and few variational parameters that has its foundations in two-electron reduced density matrix (2-RDM) theory. Error in the 2-RDM is mitigated through projection of the 2-RDM measured by tomography onto the approximate set of physically realistic 2-RDMs defined by the 2-positive $N$-representability conditions. The relative energies exhibit single-digit millihartree errors, and the computed natural-orbital occupations capture significant differences in the electron correlation of the isomers including the biradical nature of the {\em para}-isomer.

While chemical systems containing hundreds to thousands of electrons remain beyond the reach of quantum devices, hybrid quantum-classical algorithms present a promising pathway toward a quantum advantage. Hybrid algorithms treat the exponentially scaling part of the calculation-the static correlation-on the quantum computer and the non-exponentially scaling part-the dynamic correlation-on the classical computer. While a variety of algorithms have been proposed, the dependence of many methods on the total wave function limits the development of easy-to-use classical post-processing implementations. Here, we present a novel combination of quantum and classical algorithms, which computes the all-electron energy of a strongly correlated molecular system on the classical computer from the 2-electron reduced density matrix (2-RDM) evaluated on the quantum device. Significantly, we circumvent the wave function in the all-electron calculations by using density matrix methods that only require input of the statically correlated 2-RDM. Although the algorithm is completely general, we test it with two classical density matrix methods, the anti-Hermitian contracted Schrödinger equation (ACSE) and multiconfiguration pair-density functional theories, using the recently developed quantum ACSE method for simulating the statically correlated 2-RDM. We obtain experimental accuracy for the relative energies of all three benzyne isomers and thereby demonstrate the ability of the developed algorithm to achieve chemically relevant and accurate results on noisy intermediate-scale quantum devices.

The accurate computation of ground and excited states of many-fermion quantum systems is one of the most consequential, contemporary challenges in the physical and computational sciences whose solution stands to benefit significantly from the advent of quantum computing devices. Existing methodologies using phase estimation or variational algorithms have potential drawbacks such as deep circuits requiring substantial error correction or nontrivial high-dimensional classical optimization. Here, we introduce a quantum solver of contracted eigenvalue equations, the quantum analog of classical methods for the energies and reduced density matrices of ground and excited states. The solver does not require deep circuits or difficult classical optimization and achieves an exponential speed-up over its classical counterpart. We demonstrate the algorithm though computations on both a quantum simulator and two IBM quantum processing units.

Molecular simulations generally require fermionic encoding in which fermion statistics are encoded into the qubit representation of the wave function. Recent calculations suggest that fermionic encoding of the wave function can be bypassed, leading to more efficient quantum computations. Here we show that the two-electron reduced density matrix (2-RDM) can be expressed as a unique functional of the unencoded N-qubit-particle wave function without approximation, and hence, the energy can be expressed as a functional of the 2-RDM without fermionic encoding of the wave function. In contrast to current hardware-efficient methods, the derived functional has a unique, one-to-one (and onto) mapping between the qubit-particle wave functions and 2-RDMs, which avoids the over-parametrization that can lead to optimization difficulties such as barren plateaus. An application to computing the ground-state energy and 2-RDM of H4 is presented.