The quantum many-electron problem is not just at the heart of condensed matter phenomena, but also essential for first-principles simulation of chemical phenomena. Strong correlation in chemical systems are prevalent and present a formidable challenge in the simulation of these systems, while predictive phenomena in this domain often also requires a demanding level of accuracy to inform chemical behavior. Efficient representations of the many-electron states of chemical systems are therefore also being inspired by machine learning principles to provide an alternative to established approaches. In this chapter, we review recent progress in this endeavor for quantum chemical problems represented in second quantization, and the particular challenges present in this field. In particular, we focus on the application of Gaussian Process States emerging from efficient representations of the many-body wavefunction with rigorous Bayesian modeling frameworks, allowing for the unification of multiple paradigms under a common umbrella. We show how such models (and other representations derived from machine learning) can be used as novel tools to compute ab initio chemical properties, while in turn also informing the design of machine learning models to extract correlation patterns in classical data.
The quantum many-electron problem is not just at the heart of condensed matter phenomena, but also essential for first-principles simulation of chemical phenomena. Strong correlation in chemical systems are prevalent and present a formidable challenge in the simulation of these systems, while predictive phenomena in this domain often also requires a demanding level of accuracy to inform chemical behavior. Efficient representations of the many-electron states of chemical systems are therefore also being inspired by machine learning principles to provide an alternative to established approaches. In this chapter, we review recent progress in this endeavor for quantum chemical problems represented in second quantization, and the particular challenges present in this field. In particular, we focus on the application of Gaussian Process States emerging from efficient representations of the many-body wavefunction with rigorous Bayesian modeling frameworks, allowing for the unification of multiple paradigms under a common umbrella. We show how such models (and other representations derived from machine learning) can be used as novel tools to compute ab initio chemical properties, while in turn also informing the design of machine learning models to extract correlation patterns in classical data.
Capturing the correlation emerging between constituents of many-body systems accurately is one of the key challenges for the appropriate description of various systems whose properties are underpinned by quantum mechanical fundamentals. This thesis discusses novel tools and techniques for the (classical) modelling of quantum many-body wavefunctions with the ultimate goal to introduce a universal framework for finding accurate representations from which system properties can be extracted efficiently. It is outlined how synergies with standard machine learning approaches can be exploited to enable an automated inference of the most relevant intrinsic characteristics through rigorous Bayesian regression techniques. Based on the probabilistic framework forming the foundation of the introduced ansatz, coined the Gaussian Process State, different compression techniques are explored to extract numerically feasible representations of relevant target states within stochastic schemes. By following intuitively motivated design principles, the resulting model carries a high degree of interpretability and offers an easily applicable tool for the numerical study of quantum systems, including ones which are notoriously difficult to simulate due to a strong intrinsic correlation. The practical applicability of the Gaussian Process States framework is demonstrated within several benchmark applications, in particular, ground state approximations for prototypical quantum lattice models, Fermi-Hubbard models and J1−J2 models, as well as simple ab-initio quantum chemical systems.
We present a general framework for the efficient simulation of realistic fermionic systems with modern machine-learning-inspired representations of quantum many-body states, towards a universal tool for ab initio electronic structure. These machine-learning-inspired Ans\"atze have recently come to the fore in both a (first-quantized) continuum and discrete Fock space representations, where, however, the inherent scaling of the latter approach for realistic interactions has so far limited practical applications. With application to the ``Gaussian Process State,'' a recently introduced Ansatz inspired by systematically improvable kernel models in machine learning, we discuss different choices to define the representation of the computational Fock space. We show how local representations are particularly suited for stochastic sampling of expectation values, while also indicating a route to overcome the discrepancy in the scaling compared with continuum-formulated models. We are able to show competitive accuracy for systems with up to 64 electrons, including a simplified (yet fully ab initio) model of the Mott transition in three-dimensional hydrogen, indicating a significant improvement over similar approaches, even for moderate numbers of configurational samples.
The field of quantum chemistry has long been defined by the central computational challenge of the quantum many-body fermionic system problem, main the electronic Schrödinger equation. This exponential scaling makes it computationally intractable to solve, the exact governing electronic Schrödinger equation. Approximation methods have been developed, ranging from the widely used Density Functional Theory (DFT) to Coupled Cluster (CC) theory. While powerful, these conventional approaches often involve controlled truncations which caused a trade-off between accuracy, leaving many systems—particularly those with strong electron correlation—beyond the reach of ab initio simulation. Furthermore, the famous fermionic sign oscillation problem is particularly severe in stochastic methods like Quantum Monte Carlo (QMC). 1 Traditional Ansätze are also frequently engineered specifically for particular systems, which results in a fragmentation of results and fundamentally limits the transferability. Recent research demonstrates that with carefully designed architectures, ANNs can not only represent ground states of model systems with high precision but also tackle the sign problem, offering a promising path forward for strongly correlated electronic structure calculations.2,3 This review charts the paradigm shift driven by Neural Network Quantum States (NNQS), which leverage the representational power of deep learning to overcome these barriers. We detail the architectural evolution from Restricted Boltzmann Machines to autoregressive models like RNNs and Transformers, which enable exact, uncorrelated sampling and bypass critical bottlenecks.2,4,5Furthermore, we explore the geometric foundation of high-efficiency optimization via the neural networks, which decouples optimization cost from model complexity.6 The frontier of the field is marked by the integration of operator learning and hybrid quantum-classical frameworks, such as Reinforcement Learning for contracted quantum eigen-solvers and Quantum-Enhanced Neural Networks, which leverage quantum processors to enhance expressivity for hardware-efficient Ansätze.7,8 By framing the problem through the lens of computational resource allocation—specifically, trading exponential memory demands for polynomialcomplexity optimization and sampling—this review elucidates how recent advances at the intersection of artificial neural networks and quantum computing have evolved. The emergence of those methods not merely progress into a powerful simulation-tools, but also a hybrid computational interface.9 This convergence offers a versatile and systematically improvable framework for potentially addressing some of the most challenging problems in quantum physics and chemistry.
The field of quantum chemistry has long been defined by the central computational challenge of the quantum many-body fermionic system problem, main the electronic Schrödinger equation. This exponential scaling makes it computationally intractable to solve, the exact governing electronic Schrödinger equation. Approximation methods have been developed, ranging from the widely used Density Functional Theory (DFT) to Coupled Cluster (CC) theory. While powerful, these conventional approaches often involve controlled truncations which caused a trade-off between accuracy, leaving many systems—particularly those with strong electron correlation—beyond the reach of ab initio simulation. Furthermore, the famous fermionic sign oscillation problem is particularly severe in stochastic methods like Quantum Monte Carlo (QMC). 1 Traditional Ansätze are also frequently engineered specifically for particular systems, which results in a fragmentation of results and fundamentally limits the transferability. Recent research demonstrates that with carefully designed architectures, ANNs can not only represent ground states of model systems with high precision but also tackle the sign problem, offering a promising path forward for strongly correlated electronic structure calculations.2,3 This review charts the paradigm shift driven by Neural Network Quantum States (NNQS), which leverage the representational power of deep learning to overcome these barriers. We detail the architectural evolution from Restricted Boltzmann Machines to autoregressive models like RNNs and Transformers, which enable exact, uncorrelated sampling and bypass critical bottlenecks.2,4,5Furthermore, we explore the geometric foundation of high-efficiency optimization via the neural networks, which decouples optimization cost from model complexity.6 The frontier of the field is marked by the integration of operator learning and hybrid quantum-classical frameworks, such as Reinforcement Learning for contracted quantum eigen-solvers and Quantum-Enhanced Neural Networks, which leverage quantum processors to enhance expressivity for hardware-efficient Ansätze.7,8 By framing the problem through the lens of computational resource allocation—specifically, trading exponential memory demands for polynomialcomplexity optimization and sampling—this review elucidates how recent advances at the intersection of artificial neural networks and quantum computing have evolved. The emergence of those methods not merely progress into a powerful simulation-tools, but also a hybrid computational interface.9 This convergence offers a versatile and systematically improvable framework for potentially addressing some of the most challenging problems in quantum physics and chemistry.
The field of quantum chemistry has long been defined by the central computational challenge of the quantum many-body fermionic system problem, main the electronic Schrödinger equation. This exponential scaling makes it computationally intractable to solve, the exact governing electronic Schrödinger equation. Approximation methods have been developed, ranging from the widely used Density Functional Theory (DFT) to Coupled Cluster (CC) theory. While powerful, these conventional approaches often involve controlled truncations which caused a trade-off between accuracy, leaving many systems—particularly those with strong electron correlation—beyond the reach of ab initio simulation. Furthermore, the famous fermionic sign oscillation problem is particularly severe in stochastic methods like Quantum Monte Carlo (QMC). 1 Traditional Ansätze are also frequently engineered specifically for particular systems, which results in a fragmentation of results and fundamentally limits the transferability. Recent research demonstrates that with carefully designed architectures, ANNs can not only represent ground states of model systems with high precision but also tackle the sign problem, offering a promising path forward for strongly correlated electronic structure calculations.2,3 This review charts the paradigm shift driven by Neural Network Quantum States (NNQS), which leverage the representational power of deep learning to overcome these barriers. We detail the architectural evolution from Restricted Boltzmann Machines to autoregressive models like RNNs and Transformers, which enable exact, uncorrelated sampling and bypass critical bottlenecks.2,4,5Furthermore, we explore the geometric foundation of high-efficiency optimization via the neural networks, which decouples optimization cost from model complexity.6 The frontier of the field is marked by the integration of operator learning and hybrid quantum-classical frameworks, such as Reinforcement Learning for contracted quantum eigen-solvers and Quantum-Enhanced Neural Networks, which leverage quantum processors to enhance expressivity for hardware-efficient Ansätze.7,8 By framing the problem through the lens of computational resource allocation—specifically, trading exponential memory demands for polynomialcomplexity optimization and sampling—this review elucidates how recent advances at the intersection of artificial neural networks and quantum computing have evolved. The emergence of those methods not merely progress into a powerful simulation-tools, but also a hybrid computational interface.9 This convergence offers a versatile and systematically improvable framework for potentially addressing some of the most challenging problems in quantum physics and chemistry.
The field of quantum chemistry has long been defined by the central computational challenge of the quantum many-body fermionic system problem, main the electronic Schrödinger equation. This exponential scaling makes it computationally intractable to solve, the exact governing electronic Schrödinger equation. Approximation methods have been developed, ranging from the widely used Density Functional Theory (DFT) to Coupled Cluster (CC) theory. While powerful, these conventional approaches often involve controlled truncations which caused a trade-off between accuracy, leaving many systems—particularly those with strong electron correlation—beyond the reach of ab initio simulation. Furthermore, the famous fermionic sign oscillation problem is particularly severe in stochastic methods like Quantum Monte Carlo (QMC). 1 Traditional Ansätze are also frequently engineered specifically for particular systems, which results in a fragmentation of results and fundamentally limits the transferability. Recent research demonstrates that with carefully designed architectures, ANNs can not only represent ground states of model systems with high precision but also tackle the sign problem, offering a promising path forward for strongly correlated electronic structure calculations.2,3 This review charts the paradigm shift driven by Neural Network Quantum States (NNQS), which leverage the representational power of deep learning to overcome these barriers. We detail the architectural evolution from Restricted Boltzmann Machines to autoregressive models like RNNs and Transformers, which enable exact, uncorrelated sampling and bypass critical bottlenecks.2,4,5Furthermore, we explore the geometric foundation of high-efficiency optimization via the neural networks, which decouples optimization cost from model complexity.6 The frontier of the field is marked by the integration of operator learning and hybrid quantum-classical frameworks, such as Reinforcement Learning for contracted quantum eigen-solvers and Quantum-Enhanced Neural Networks, which leverage quantum processors to enhance expressivity for hardware-efficient Ansätze.7,8 By framing the problem through the lens of computational resource allocation—specifically, trading exponential memory demands for polynomialcomplexity optimization and sampling—this review elucidates how recent advances at the intersection of artificial neural networks and quantum computing have evolved. The emergence of those methods not merely progress into a powerful simulation-tools, but also a hybrid computational interface.9 This convergence offers a versatile and systematically improvable framework for potentially addressing some of the most challenging problems in quantum physics and chemistry.