We present QDK/Chemistry, a software toolkit for quantum chemistry workflows targeting quantum computers. The toolkit addresses a key challenge in the field: while quantum algorithms for chemistry have matured considerably, the infrastructure connecting classical electronic structure calculations to quantum circuit execution remains fragmented. QDK/Chemistry provides this infrastructure through a modular architecture that separates data representations from computational methods, enabling researchers to compose workflows from interchangeable components. In addition to providing native implementations of targeted algorithms in the quantum-classical pipeline, the toolkit builds upon and integrates with widely used open-source quantum chemistry packages and quantum computing frameworks through a plugin system, allowing users to combine methods from different sources without modifying workflow logic. This paper describes the design philosophy, current capabilities, and role of QDK/Chemistry as a foundation for reproducible quantum chemistry experiments.

We describe a concrete device roadmap towards a fault-tolerant quantum computing architecture based on noise-resilient, topologically protected Majorana-based qubits. Our roadmap encompasses four generations of devices: a single-qubit device that enables a measurement-based qubit benchmarking protocol; a two-qubit device that uses measurement-based braiding to perform single-qubit Clifford operations; an eight-qubit device that can be used to show an improvement of a two-qubit operation when performed on logical qubits rather than directly on physical qubits; and a topological qubit array supporting lattice surgery demonstrations on two logical qubits. Devices that enable this path require a superconductor-semiconductor heterostructure that supports a topological phase, quantum dots and coupling between those quantum dots that can create the appropriate loops for interferometric measurements, and a microwave readout system that can perform fast, low-error single-shot measurements. We describe the key design components of these qubit devices, along with the associated protocols for demonstrations of single-qubit benchmarking, Clifford gate execution, quantum error detection, and quantum error correction, which differ greatly from those in more conventional qubits. Finally, we comment on implications and advantages of this architecture for utility-scale quantum computation.

We demonstrate the first end-to-end integration of high-performance computing (HPC), reliable quantum computing, and AI in a case study on catalytic reactions producing chiral molecules. We present a hybrid computation workflow to determine the strongly correlated reaction configurations and estimate, for one such configuration, its active site's ground state energy. We combine 1) the use of HPC tools like AutoRXN and AutoCAS to systematically identify the strongly correlated chemistry within a large chemical space with 2) the use of logical qubits in the quantum computing stage to prepare the quantum ground state of the strongly correlated active site, demonstrating the advantage of logical qubits compared to physical qubits, and 3) the use of optimized quantum measurements of the logical qubits with so-called classical shadows to accurately predict various properties of the ground state including energies. The combination of HPC, reliable quantum computing, and AI in this demonstration serves as a proof of principle of how future hybrid chemistry applications will require integration of large-scale quantum computers with classical computing to be able to provide a measurable quantum advantage.

Quantum computation for chemical problems will require the construction of guiding states with sufficient overlap with a target state. Since easily available and initializable mean-field states are characterized by an overlap that is reduced for multi-configurational electronic structures and even vanishes with growing system size, we here investigate the severity of state preparation for reaction chemistry. We emphasize weaknesses in current traditional approaches (even for weakly correlated molecules) and highlight the advantage of quantum phase estimation algorithms. An important result is the introduction of a new classification scheme for electronic structures based on orbital entanglement information. We identify two categories of multi-configurational molecules. Whereas class-1 molecules are dominated by very few determinants and often found in reaction chemistry, class-2 molecules do not allow one to single out a reasonably sized number of important determinants. The latter are particularly hard for traditional approaches and an ultimate target for quantum computation. Some open-shell iron-sulfur clusters belong to class 2. We discuss the role of the molecular orbital basis set and show that true class-2 molecules remain in this class independent of the choice of the orbital basis, with the iron-molybdenum cofactor of nitrogenase being a prototypical example. We stress that class-2 molecules can be build in a systematic fashion from open-shell centers or unsaturated carbon atoms. Our key result is that it will always be possible to initialize a guiding state for chemical reaction chemistry in the ground state based on initial low-cost approximate electronic structure information, which is facilitated by the finite size of the atomistic structures to be considered.

The theoretical analysis of the Adiabatic Quantum Computation protocol presents several challenges resulting from the difficulty of simulating, with classical resources, the unitary dynamics of a large quantum device. We present here a variational approach to substantially alleviate this problem in many situations of interest. Our approach is based on the time-dependent Variational Monte Carlo method, in conjunction with a correlated and time-dependent Jastrow ansatz. We demonstrate that accurate results can be obtained in a variety of problems, ranging from the description of defect generation through a dynamical phase transition in 1D to the complex dynamics of frustrated spin-glass problems both on fully-connected and Chimera graphs.

Quantum computing promises to help humanity solve problems that would otherwise be intractable on classical computers. Unlike today's machines, quantum computers use a novel computing process that leverages the foundational quantum mechanical laws of nature. This unlocks unparalleled compute power for certain applications and promises to help solve some of our generation's gravest challenges, including the climate crisis, food insecurity, and widespread disease. No one entity will be able to realize this end state alone. Developing a fault-tolerant quantum supercomputer and a vibrant ecosystem around it will require deep partnerships between industry, governments, and academia. It will also require collective action to enable and promote positive applications of quantum computing and ensure that the safe and responsible use of the technology is at the center of its development and deployment. Achieving these objectives will require focusing on three priorities: 1. Impact. Ensure quantum computing benefits all of humankind by developing quantum solutions to solve critical, global problems. 2. Use. Protect against malicious use by accelerating the deployment of quantum-safe cryptography and developing governance processes and controls for the responsible use of quantum machines. 3. Access. Democratize the potential for economic growth across all of society through skilling, workforce and ecosystem development, and digital infrastructure. This paper discusses each in turn.

Quantum computing is an emerging technology with potentially far-reaching implications for national prosperity and security. Understanding the timeframes over which economic benefits and national security risks may manifest themselves is vital for ensuring the prudent development of this technology. To inform security experts and policy decision makers on this matter, we review what is currently known on the potential uses and risks of quantum computers, leveraging current research literature. The maturity of currently-available quantum computers is not yet at a level such that they can be used in production for large-scale, industrially-relevant problems, but they are not believed to currently pose security risks. We identify 2 large-scale trends – new approximate methods (variational algorithms, error mitigation, and circuit knitting) and the commercial exploration of business-relevant quantum applications – which, together, may enable useful and practical quantum computing in the near future. Crucially, these methods do not appear likely to change the required resources for cryptanalysis on currently-used cryptosystems. From an analysis we perform of the current and known algorithms for cryptanalysis, we find they require circuits of a size exceeding those that can be run by current and near-future quantum computers (and which will require error correction), though we acknowledge improvements in quantum algorithms for these problems are taking place in the literature. In addition, the risk to cybersecurity can be well-managed by the migration to new, quantum-safe cryptographic protocols, which we survey and discuss. Given the above, we conclude there is a credible expectation that quantum computers will be capable of performing computations which are economically-impactful before they will be capable of performing ones which are cryptographically-relevant.

HPC and Cloud have evolved independently, specializing their innovations into performance or productivity. Acceleration as a Service (XaaS) is a recipe to empower both fields with a shared execution platform that provides transparent access to computing resources, regardless of the underlying cloud or HPC service provider. Bridging HPC and cloud advancements, XaaS presents a unified architecture built on performance-portable containers. Our converged model concentrates on low-overhead, high-performance communication and computing, targeting resource-intensive workloads from climate simulations to machine learning. XaaS lifts the restricted allocation model of Function-as-a-Service (FaaS), allowing users to benefit from the flexibility and efficient resource utilization of serverless while supporting long-running and performance-sensitive workloads from HPC.

Density functional theory (DFT) has been a cornerstone in computational chemistry, physics, and materials science for decades, benefiting from advancements in computational power and theoretical methods. This paper introduces a novel, cloud-native application, Accelerated DFT, which offers an order of magnitude acceleration in DFT simulations. By integrating state-of-the-art cloud infrastructure and redesigning algorithms for graphic processing units (GPUs), Accelerated DFT achieves high-speed calculations without sacrificing accuracy. It provides a user-friendly and scalable solution for the increasing demands of DFT calculations in scientific communities. The implementation details, examples, and benchmark results illustrate how Accelerated DFT can significantly expedite scientific discovery across various domains.

High-throughput computational materials discovery has promised significant acceleration of the design and discovery of new materials for many years. Despite a surge in interest and activity, the constraints imposed by large-scale computational resources present a significant bottleneck. Furthermore, examples of large-scale computational discovery carried through experimental validation remain scarce, especially for materials with product applicability. Here we demonstrate how this vision became reality by first combining state-of-the-art artificial intelligence (AI) models and traditional physics-based models on cloud high-performance computing (HPC) resources to quickly navigate through more than 32 million candidates and predict around half a million potentially stable materials. By focusing on solid-state electrolytes for battery applications, our discovery pipeline further identified 18 promising candidates with new compositions and rediscovered a decade's worth of collective knowledge in the field as a byproduct. By employing around one thousand virtual machines (VMs) in the cloud, this process took less than 80 hours. We then synthesized and experimentally characterized the structures and conductivities of our top candidates, the Na$_x$Li$_{3-x}$YCl$_6$ ($0 < x < 3$) series, demonstrating the potential of these compounds to serve as solid electrolytes. Additional candidate materials that are currently under experimental investigation could offer more examples of the computational discovery of new phases of Li- and Na-conducting solid electrolytes. We believe that this unprecedented approach of synergistically integrating AI models and cloud HPC not only accelerates materials discovery but also showcases the potency of AI-guided experimentation in unlocking transformative scientific breakthroughs with real-world applications.

Magnetic resonance fingerprinting (MRF) is a novel quantitative MR technique that simultaneously provides multiple tissue property maps. When optimizing MRF scans, modeling undersampling errors and field imperfections in cost functions for direct measurement of quantitative errors will make the optimization results more practical and robust. However, optimizing such cost function is computationally expensive and impractical for MRF optimization with tens of thousands of iterations. Here, we introduce a fast MRF simulator to simulate aliased images from actual scan scenarios including undersampling and system imperfections, which substantially reduces computational time and allows for direct error estimation of the quantitative maps and efficient sequence optimization. We evaluate the performance and computational speed of the proposed approach by simulations and in vivo experiments. The simulations from the proposed method closely approximate the signals and MRF maps from in vivo scans, with 158 times shorter processing time than the conventional simulation method using Non-uniform Fourier transform. We also demonstrate the power of applying the fast MRF simulator in MRF sequence optimization. The optimized sequences are validated with in vivo scans to assess the image quality and accuracy. The optimized sequences produce artifact-free T1 and T2 maps in 2D and 3D scans with equivalent mapping accuracy as the human-designed sequence but at shorter scan times. Incorporating the proposed simulator in the MRF optimization framework makes direct estimation of undersampling errors during the optimization process feasible, and provide optimized MRF sequences that are robust against undersampling artifacts and field inhomogeneity.

Detecting the impacts of natural and anthropogenic disturbances that cause declines in organisms or changes in community composition has long been a focus of ecology. However, a tradeoff often exists between the spatial extent over which relevant data can be collected, and the resolution of those data. Recent advances in underwater photogrammetry, as well as computer vision and machine learning tools that employ artificial intelligence (AI), offer potential solutions with which to resolve this tradeoff. Here, we coupled a rigorous photogrammetric survey method with novel AI-assisted image segmentation software in order to quantify the impact of a coral bleaching event on a tropical reef, both at an ecologically meaningful spatial scale and with high spatial resolution. In addition to outlining our workflow, we highlight three key results: (1) dramatic changes in the three-dimensional surface areas of live and dead coral, as well as the ratio of live to dead colonies before and after bleaching; (2) a size-dependent pattern of mortality in bleached corals, where the largest corals were disproportionately affected, and (3) a significantly greater decline in the surface area of live coral, as revealed by our approximation of the 3D shape compared to the more standard planar area (2D) approach. The technique of photogrammetry allows us to turn 2D images into approximate 3D models in a flexible and efficient way. Increasing the resolution, accuracy, spatial extent, and efficiency with which we can quantify effects of disturbances will improve our ability to understand the ecological consequences that cascade from small to large scales, as well as allow more informed decisions to be made regarding the mitigation of undesired impacts.

Quantum chemical calculations on atomistic systems have evolved into a standard approach to studying molecular matter. These calculations often involve a significant amount of manual input and expertise, although most of this effort could be automated, which would alleviate the need for expertise in software and hardware accessibility. Here, we present the AutoRXN workflow, an automated workflow for exploratory high-throughput electronic structure calculations of molecular systems, in which (i) density functional theory methods are exploited to deliver minimum and transition-state structures and corresponding energies and properties, (ii) coupled cluster calculations are then launched for optimized structures to provide more accurate energy and property estimates, and (iii) multi-reference diagnostics are evaluated to back check the coupled cluster results and subject them to automated multi-configurational calculations for potential multi-configurational cases. All calculations are carried out in a cloud environment and support massive computational campaigns. Key features of all components of the AutoRXN workflow are autonomy, stability, and minimum operator interference. We highlight the AutoRXN workflow with the example of an autonomous reaction mechanism exploration of the mode of action of a homogeneous catalyst for the asymmetric reduction of ketones.

What are the promising applications to realize quantum advantage?

Molecular science is governed by the dynamics of electrons and atomic nuclei, and by their interactions with electromagnetic fields. A faithful physicochemical understanding of these processes is crucial for the design and synthesis of chemicals and materials of value for our society and economy. Although some problems in this field can be adequately addressed by classical mechanics, many demand an explicit quantum mechanical description. Such quantum problems require a representation of wave functions that grows exponentially with system size and therefore should naturally benefit from quantum computation on a number of logical qubits that scales only linearly with system size. In this perspective, we elaborate on the potential benefits of quantum computing in the molecular sciences, i.e., in molecular physics, chemistry, biochemistry, and materials science.

While quantum computers promise to solve some scientifically and commercially valuable problems thought intractable for classical machines, delivering on this promise will require a large-scale quantum machine. Understanding the impact of architecture design choices for a scaled quantum stack for specific applications, prior to full realization of the quantum system, is an important open challenge. To this end, we develop a framework for quantum resource estimation, abstracting the layers of the stack, to estimate resources required across these layers for large-scale quantum applications. Using a tool that implements this framework, we assess three scaled quantum applications and find that hundreds of thousands to millions of physical qubits are needed to achieve practical quantum advantage. We identify three qubit parameters, namely size, speed, and controllability, that are critical at scale to rendering these applications practical. A goal of our work is to accelerate progress towards practical quantum advantage by enabling the broader community to explore design choices across the stack, from algorithms to qubits.

The development of quantum computing across several technologies and platforms has reached the point of having an advantage over classical computers for an artificial problem, a point known as 'quantum advantage'. As a next step along the development of this technology, it is now important to discuss 'practical quantum advantage', the point at which quantum devices will solve problems of practical interest that are not tractable for traditional supercomputers. Many of the most promising short-term applications of quantum computers fall under the umbrella of quantum simulation: modelling the quantum properties of microscopic particles that are directly relevant to modern materials science, high-energy physics and quantum chemistry. This would impact several important real-world applications, such as developing materials for batteries, industrial catalysis or nitrogen fixing. Much as aerodynamics can be studied either through simulations on a digital computer or in a wind tunnel, quantum simulation can be performed not only on future fault-tolerant digital quantum computers but also already today through special-purpose analogue quantum simulators. Here we overview the state of the art and future perspectives for quantum simulation, arguing that a first practical quantum advantage already exists in the case of specialized applications of analogue devices, and that fully digital devices open a full range of applications but require further development of fault-tolerant hardware. Hybrid digital-analogue devices that exist today already promise substantial flexibility in near-term applications.

We reverse-engineer, test and analyse hardware and firmware of the commercial quantum-optical random number generator Quantis from ID Quantique. We show that > 99% of its output data originates in physically random processes: random timing of photon absorption in a semiconductor material, and random growth of avalanche owing to impact ionisation. Under a strong assumption that these processes correspond to a measurement of an initially pure state of the components, our analysis implies the unpredictability of the generated randomness. We have also found minor non-random contributions from imperfections in detector electronics and an internal processing algorithm, specific to this particular device. Our work shows that the design quality of a commercial quantum-optical randomness source can be verified without cooperation of the manufacturer and without access to the engineering documentation.

The rapid development in hardware for quantum computing and simulation has led to much interest in problems where these devices can exceed the capabilities of existing classical computers and known methods. Approaching this for problems that go beyond testing the performance of a quantum device is an important step, and quantum simulation of many-body quench dynamics is one of the most promising candidates for early practical quantum advantage. We analyse the requirements for quantitatively reliable quantum simulation beyond the capabilities of existing classical methods for analogue quantum simulators with neutral atoms in optical lattices and trapped ions. Considering the primary sources of error in analogue devices and how they propagate after a quench in studies of the Hubbard or long-range transverse field Ising model, we identify the level of error expected in quantities we extract from experiments. We conclude for models that are directly implementable that regimes of practical quantum advantage are attained in current experiments with analogue simulators. We also identify the hardware requirements to reach the same level of accuracy with future fault-tolerant digital quantum simulation. Verification techniques are already available to test the assumptions we make here, and demonstrating these in experiments will be an important next step.

The quantum computation of electronic energies can break the curse of dimensionality that plagues many-particle quantum mechanics. It is for this reason that a universal quantum computer has the potential to fundamentally change computational chemistry and materials science, areas in which strong electron correlations present severe hurdles for traditional electronic structure methods. Here, we present a state-of-the-art analysis of accurate energy measurements on a quantum computer for computational catalysis, using improved quantum algorithms with more than an order of magnitude improvement over the best previous algorithms. As a prototypical example of local catalytic chemical reactivity we consider the case of a ruthenium catalyst that can bind, activate, and transform carbon dioxide to the high-value chemical methanol. We aim at accurate resource estimates for the quantum computing steps required for assessing the electronic energy of key intermediates and transition states of its catalytic cycle. In particular, we present new quantum algorithms for double-factorized representations of the four-index integrals that can significantly reduce the computational cost over previous algorithms, and we discuss the challenges of increasing active space sizes to accurately deal with dynamical correlations. We address the requirements for future quantum hardware in order to make a universal quantum computer a successful and reliable tool for quantum computing enhanced computational materials science and chemistry, and identify open questions for further research.