arXiv subjects

Matthias Troyer

Publications and source records attributed to Matthias Troyer.

At least 19 recordsLinked to original sources

arXiv2026

QDK/Chemistry: A Modular Toolkit for Quantum Chemistry Applications

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.

quant-ph↗

arXiv2024

Classification of electronic structures and state preparation for quantum computation of reaction chemistry

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.

physics.comp-ph↗

arXiv2024

End-to-End Quantum Simulation of a Chemical System

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.

quant-ph↗

arXiv2024

Acceleration without Disruption: DFT Software as a Service

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 an accessible 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.

physics.chem-ph↗

arXiv2024

Simulating adiabatic quantum computation with a variational approach

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.

quant-ph↗

arXiv2024

Quantum for Good and the Societal Impact of Quantum Computing

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.

physics.soc-ph↗

arXiv2024

Assessing the Benefits and Risks of Quantum Computers

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, and 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.

quant-ph↗

arXiv2024

XaaS: Acceleration as a Service to Enable Productive High-Performance Cloud Computing

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.

cs.DC↗

arXiv2024

Accelerating computational materials discovery with artificial intelligence and cloud high-performance computing: from large-scale screening to experimental validation

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.

cond-mat.mtrl-sci↗

arXiv2023

Disentangling Hype from Practicality: On Realistically Achieving Quantum Advantage

Quantum computers offer a new paradigm of computing with the potential to vastly outperform any imagineable classical computer. This has caused a gold rush towards new quantum algorithms and hardware. In light of the growing expectations and hype surrounding quantum computing we ask the question which are the promising applications to realize quantum advantage. We argue that small data problems and quantum algorithms with super-quadratic speedups are essential to make quantum computers useful in practice. With these guidelines one can separate promising applications for quantum computing from those where classical solutions should be pursued. While most of the proposed quantum algorithms and applications do not achieve the necessary speedups to be considered practical, we already see a huge potential in material science and chemistry. We expect further applications to be developed based on our guidelines.

quant-ph↗

arXiv2023

High-throughput ab initio reaction mechanism exploration in the cloud with automated multi-reference validation

Quantum chemical calculations on atomistic systems have evolved into a standard approach to study 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 lectronic 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 hem 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 omponents of the AutoRXN workflow are autonomy, stability, and minimum operator interference. We highlight the AutoRXN workflow at the example of an autonomous reaction mechanism exploration of the mode of action of a homogeneous catalyst for the asymmetric reduction of ketones.

physics.chem-ph↗

arXiv2022

Assessing requirements to scale to practical quantum advantage

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.

quant-ph↗

arXiv2022

Independent quality assessment of a commercial quantum random number generator

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.

quant-ph↗

arXiv2022

Automated Design of Pulse Sequences for Magnetic Resonance Fingerprinting using Physics-Inspired Optimization

Magnetic Resonance Fingerprinting (MRF) is a method to extract quantitative tissue properties such as T1 and T2 relaxation rates from arbitrary pulse sequences using conventional magnetic resonance imaging hardware. MRF pulse sequences have thousands of tunable parameters which can be chosen to maximize precision and minimize scan time. Here we perform de novo automated design of MRF pulse sequences by applying physics-inspired optimization heuristics. Our experimental data suggests systematic errors dominate over random errors in MRF scans under clinically-relevant conditions of high undersampling. Thus, in contrast to prior optimization efforts, which focused on statistical error models, we use a cost function based on explicit first-principles simulation of systematic errors arising from Fourier undersampling and phase variation. The resulting pulse sequences display features qualitatively different from previously used MRF pulse sequences and achieve fourfold shorter scan time than prior human-designed sequences of equivalent precision in T1 and T2. Furthermore, the optimization algorithm has discovered the existence of MRF pulse sequences with intrinsic robustness against shading artifacts due to phase variation.

physics.med-ph↗

arXiv2021

Scaling overhead of embedding optimization problems in quantum annealing

In order to treat all-to-all connected quadratic binary optimization problems (QUBO) with hardware quantum annealers, an embedding of the original problem is required due to the sparsity of the hardware's topology. Embedding fully-connected graphs - typically found in industrial applications - incurs a quadratic space overhead and thus a significant overhead in the time to solution. Here we investigate this embedding penalty of established planar embedding schemes such as minor embedding on a square lattice, minor embedding on a Chimera graph, and the Lechner-Hauke-Zoller scheme using simulated quantum annealing on classical hardware. Large-scale quantum Monte Carlo simulation suggest a polynomial time-to-solution overhead. Our results demonstrate that standard analog quantum annealing hardware is at a disadvantage in comparison to classical digital annealers, as well as gate-model quantum annealers and could also serve as benchmark for improvements of the standard quantum annealing protocol.

quant-ph↗

arXiv2021

A Fast MR Fingerprinting Simulator for Direct Error Estimation and Sequence Optimization

MR Fingerprinting is a novel quantitative MR technique that could simultaneously provide multiple tissue property maps. When optimizing MRF scans, modeling undersampling errors and field imperfections in cost functions will make the optimization results more practical and robust. However, this process is computationally expensive and impractical for sequence optimization algorithms when MRF signal evolutions need to be generated for each optimization iteration. 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 and efficient sequence optimization. By constraining the total number of tissues present in a brain phantom, MRF signals from highly undersampled scans can be simulated as the product of the spatial response functions based on sampling patterns and sequence-dependent temporal functions. During optimization, the spatial response function is independent of sequence design and does not need to be recalculated. We evaluate the performance and computational speed of the proposed approach by simulations and in vivo experiments. We also demonstrate the power of applying the simulator in MRF sequence optimization. The simulation results 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. 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 factors and system inhomogeneity.

eess.IV↗

arXiv2021

Prospects of Quantum Computing for Molecular Sciences

Molecular science is governed by the dynamics of electrons, atomic nuclei, and their interaction with electromagnetic fields. A reliable physicochemical understanding of these processes is crucial for the design and synthesis of chemicals and materials of economic value. Although some problems in this field are adequately addressed by classical mechanics, many require an explicit quantum mechanical description. Such quantum problems represented by exponentially large wave function should naturally benefit from quantum computation on a number of logical qubits that scales only linearly with system size. In this perspective, we focus on the potential of quantum computing for solving relevant problems in the molecular sciences -- molecular physics, chemistry, biochemistry, and materials science.

quant-ph↗

arXiv2021

Distributed Quantum Computing with QMPI

Practical applications of quantum computers require millions of physical qubits and it will be challenging for individual quantum processors to reach such qubit numbers. It is therefore timely to investigate the resource requirements of quantum algorithms in a distributed setting, where multiple quantum processors are interconnected by a coherent network. We introduce an extension of the Message Passing Interface (MPI) to enable high-performance implementations of distributed quantum algorithms. In turn, these implementations can be used for testing, debugging, and resource estimation. In addition to a prototype implementation of quantum MPI, we present a performance model for distributed quantum computing, SENDQ. The model is inspired by the classical LogP model, making it useful to inform algorithmic decisions when programming distributed quantum computers. Specifically, we consider several optimizations of two quantum algorithms for problems in physics and chemistry, and we detail their effects on performance in the SENDQ model.

quant-ph↗