Recent advances in the self-referencing embedded strings (SELFIES) library.

String-based molecular representations play a crucial role in cheminformatics applications, and with the growing success of deep learning in chemistry, have been readily adopted into machine learning pipelines. However, traditional string-based representations such as SMILES are often prone to syntactic and semantic errors when produced by generative models. To address these problems, a novel representation, SELF-referencing embedded strings (SELFIES), was proposed that is inherently 100% robust, alongside an accompanying open-source implementation called selfies. Since then, we have generalized SELFIES to support a wider range of molecules and semantic constraints, and streamlined its underlying grammar. We have implemented this updated representation in subsequent versions of selfies, where we have also made major advances with respect to design, efficiency, and supported features. Hence, we present the current status of selfies (version 2.1.1) in this manuscript. Our library, selfies, is available at GitHub (https://github.com/aspuru-guzik-group/selfies).

Multiphoton non-local quantum interference controlled by an undetected photon.

The interference of quanta lies at the heart of quantum physics. The multipartite generalization of single-quanta interference creates entanglement, the coherent superposition of states shared by several quanta. Entanglement allows non-local correlations between many quanta and hence is a key resource for quantum information technology. Entanglement is typically considered to be essential for creating non-local quantum interference. Here, we show that this is not the case and demonstrate multiphoton non-local quantum interference that does not require entanglement of any intrinsic properties of the photons. We harness the superposition of the physical origin of a four-photon product state, which leads to constructive and destructive interference with the photons' mere existence. With the intrinsic indistinguishability in the generation process of photons, we realize four-photon frustrated quantum interference. This allows us to observe the following noteworthy difference to quantum entanglement: We control the non-local multipartite quantum interference with a photon that we never detect, which does not require quantum entanglement. These non-local properties pave the way for the studies of foundations of quantum physics and potential applications in quantum technologies.

SELFIES and the future of molecular string representations.

Artificial intelligence (AI) and machine learning (ML) are expanding in popularity for broad applications to challenging tasks in chemistry and materials science. Examples include the prediction of properties, the discovery of new reaction pathways, or the design of new molecules. The machine needs to read and write fluently in a chemical language for each of these tasks. Strings are a common tool to represent molecular graphs, and the most popular molecular string representation, Smiles, has powered cheminformatics since the late 1980s. However, in the context of AI and ML in chemistry, Smiles has several shortcomings-most pertinently, most combinations of symbols lead to invalid results with no valid chemical interpretation. To overcome this issue, a new language for molecules was introduced in 2020 that guarantees 100% robustness: SELF-referencing embedded string (Selfies). Selfies has since simplified and enabled numerous new applications in chemistry. In this perspective, we look to the future and discuss molecular string representations, along with their respective opportunities and challenges. We propose 16 concrete future projects for robust molecular representations. These involve the extension toward new chemical domains, exciting questions at the interface of AI and robust languages, and interpretability for both humans and machines. We hope that these proposals will inspire several follow-up works exploiting the full potential of molecular string representations for the future of AI in chemistry and materials science.

On scientific understanding with artificial intelligence.

An oracle that correctly predicts the outcome of every particle physics experiment, the products of every possible chemical reaction or the function of every protein would revolutionize science and technology. However, scientists would not be entirely satisfied because they would want to comprehend how the oracle made these predictions. This is scientific understanding, one of the main aims of science. With the increase in the available computational power and advances in artificial intelligence, a natural question arises: how can advanced computational systems, and specifically artificial intelligence, contribute to new scientific understanding or gain it autonomously? Trying to answer this question, we adopted a definition of 'scientific understanding' from the philosophy of science that enabled us to overview the scattered literature on the topic and, combined with dozens of anecdotes from scientists, map out three dimensions of computer-assisted scientific understanding. For each dimension, we review the existing state of the art and discuss future developments. We hope that this Perspective will inspire and focus research directions in this multidisciplinary emerging field.

Beyond generative models: superfast traversal, optimization, novelty, exploration and discovery (STONED) algorithm for molecules using SELFIES.

Inverse design allows the generation of molecules with desirable physical quantities using property optimization. Deep generative models have recently been applied to tackle inverse design, as they possess the ability to optimize molecular properties directly through structure modification using gradients. While the ability to carry out direct property optimizations is promising, the use of generative deep learning models to solve practical problems requires large amounts of data and is very time-consuming. In this work, we propose STONED - a simple and efficient algorithm to perform interpolation and exploration in the chemical space, comparable to deep generative models. STONED bypasses the need for large amounts of data and training times by using string modifications in the SELFIES molecular representation. First, we achieve non-trivial performance on typical benchmarks for generative models without any training. Additionally, we demonstrate applications in high-throughput virtual screening for the design of drugs, photovoltaics, and the construction of chemical paths, allowing for both property and structure-based interpolation in the chemical space. Overall, we anticipate our results to be a stepping stone for developing more sophisticated inverse design models and benchmarking tools, ultimately helping generative models achieve wider adoption.

Data-Driven Strategies for Accelerated Materials Design.

The ongoing revolution of the natural sciences by the advent of machine learning and artificial intelligence sparked significant interest in the material science community in recent years. The intrinsically high dimensionality of the space of realizable materials makes traditional approaches ineffective for large-scale explorations. Modern data science and machine learning tools developed for increasingly complicated problems are an attractive alternative. An imminent climate catastrophe calls for a clean energy transformation by overhauling current technologies within only several years of possible action available. Tackling this crisis requires the development of new materials at an unprecedented pace and scale. For example, organic photovoltaics have the potential to replace existing silicon-based materials to a large extent and open up new fields of application. In recent years, organic light-emitting diodes have emerged as state-of-the-art technology for digital screens and portable devices and are enabling new applications with flexible displays. Reticular frameworks allow the atom-precise synthesis of nanomaterials and promise to revolutionize the field by the potential to realize multifunctional nanoparticles with applications from gas storage, gas separation, and electrochemical energy storage to nanomedicine. In the recent decade, significant advances in all these fields have been facilitated by the comprehensive application of simulation and machine learning for property prediction, property optimization, and chemical space exploration enabled by considerable advances in computing power and algorithmic efficiency.In this Account, we review the most recent contributions of our group in this thriving field of machine learning for material science. We start with a summary of the most important material classes our group has been involved in, focusing on small molecules as organic electronic materials and crystalline materials. Specifically, we highlight the data-driven approaches we employed to speed up discovery and derive material design strategies. Subsequently, our focus lies on the data-driven methodologies our group has developed and employed, elaborating on high-throughput virtual screening, inverse molecular design, Bayesian optimization, and supervised learning. We discuss the general ideas, their working principles, and their use cases with examples of successful implementations in data-driven material discovery and design efforts. Furthermore, we elaborate on potential pitfalls and remaining challenges of these methods. Finally, we provide a brief outlook for the field as we foresee increasing adaptation and implementation of large scale data-driven approaches in material discovery and design campaigns.

Path identity as a source of high-dimensional entanglement.

We present an experimental demonstration of a general entanglement-generation framework, where the form of the entangled state is independent of the physical process used to produce the particles. It is the indistinguishability of multiple generation processes and the geometry of the setup that give rise to the entanglement. Such a framework, termed entanglement by path identity, exhibits a high degree of customizability. We employ one class of such geometries to build a modular source of photon pairs that are high-dimensionally entangled in their orbital angular momentum. We demonstrate the creation of three-dimensionally entangled states and show how to incrementally increase the dimensionality of entanglement. The generated states retain their quality even in higher dimensions. In addition, the design of our source allows for its generalization to various degrees of freedom and even for the implementation in integrated compact devices. The concept of entanglement by path identity itself is a general scheme and allows for construction of sources producing also customized states of multiple photons. We therefore expect that future quantum technologies and fundamental tests of nature in higher dimensions will benefit from this approach.

Computer-Inspired Concept for High-Dimensional Multipartite Quantum Gates.

An open question in quantum optics is how to manipulate and control complex quantum states in an experimentally feasible way. Here we present concepts for transformations of high-dimensional multiphotonic quantum systems. The proposals rely on two new ideas: (i) a novel high-dimensional quantum nondemolition measurement, (ii) the encoding and decoding of the entire quantum transformation in an ancillary state for sharing the necessary quantum information between the involved parties. Many solutions can readily be performed in laboratories around the world and thereby we identify important pathways for experimental research in the near future. The concepts have been found using the computer algorithm melvin for designing computer-inspired quantum experiments. As opposed to the field of machine learning, here the human learns new scientific concepts by interpreting and analyzing the results presented by the machine. This demonstrates that computer algorithms can inspire new ideas in science, which has a widely unexplored potential that goes far beyond experimental quantum information science.

Phenomenology of complex structured light in turbulent air.

The study of light propagation has been a cornerstone of progress in physics and technology. Recently, advances in control and shaping of light have created significant interest in the propagation of complex structures of light - particularly under realistic terrestrial conditions. While theoretical understanding of this research question has significantly grown over the last two decades, outdoor experiments with complex light structures are rare, and comparisons with theory have been nearly lacking. Such situations show a significant gap between theoretical models of atmospheric light behaviour and current experimental effort. Here, in an attempt to reduce this gap, we describe an interesting result of atmospheric models that are feasible for empirical observation. We analyze in detail light propagation in different spatial bases and present results of the theory that the influence of atmospheric turbulence is basis-dependent. Concretely, light propagating as eigenstate in one complete basis is more strongly influenced by atmosphere than light propagating in a different, complete basis. We obtain these results by exploiting a family of the continuously adjustable, complete basis of spatial modes-the Ince-Gauss modes. Our concrete numerical results will hopefully inspire experimental efforts and bring the theoretical and empirical study of complex light patterns in realistic scenarios closer together.

Predicting research trends with semantic and neural networks with an application in quantum physics.

The vast and growing number of publications in all disciplines of science cannot be comprehended by a single human researcher. As a consequence, researchers have to specialize in narrow subdisciplines, which makes it challenging to uncover scientific connections beyond the own field of research. Thus, access to structured knowledge from a large corpus of publications could help push the frontiers of science. Here, we demonstrate a method to build a semantic network from published scientific literature, which we call SemNet We use SemNet to predict future trends in research and to inspire personalized and surprising seeds of ideas in science. We apply it in the discipline of quantum physics, which has seen an unprecedented growth of activity in recent years. In SemNet, scientific knowledge is represented as an evolving network using the content of 750,000 scientific papers published since 1919. The nodes of the network correspond to physical concepts, and links between two nodes are drawn when two concepts are concurrently studied in research articles. We identify influential and prize-winning research topics from the past inside SemNet, thus confirming that it stores useful semantic knowledge. We train a neural network using states of SemNet of the past to predict future developments in quantum physics and confirm high-quality predictions using historic data. Using network theoretical tools, we can suggest personalized, out-of-the-box ideas by identifying pairs of concepts, which have unique and extremal semantic network properties. Finally, we consider possible future developments and implications of our findings.

Quantum Teleportation in High Dimensions.

Quantum teleportation allows a "disembodied" transmission of unknown quantum states between distant quantum systems. Yet, all teleportation experiments to date were limited to a two-dimensional subspace of quantized multiple levels of the quantum systems. Here, we propose a scheme for teleportation of arbitrarily high-dimensional photonic quantum states and demonstrate an example of teleporting a qutrit. Measurements over a complete set of 12 qutrit states in mutually unbiased bases yield a teleportation fidelity of 0.75(1), which is well above both the optimal single-copy qutrit state-estimation limit of 1/2 and maximal qubit-qutrit overlap of 2/3, thus confirming a genuine and nonclassical three-dimensional teleportation. Our work will enable advanced quantum technologies in high dimensions, since teleportation plays a central role in quantum repeaters and quantum networks.

Quantum experiments and graphs II: Quantum interference, computation, and state generation.

We present an approach to describe state-of-the-art photonic quantum experiments using graph theory. There, the quantum states are given by the coherent superpositions of perfect matchings. The crucial observation is that introducing complex weights in graphs naturally leads to quantum interference. This viewpoint immediately leads to many interesting results, some of which we present here. First, we identify an experimental unexplored multiphoton interference phenomenon. Second, we find that computing the results of such experiments is #P-hard, which means it is a classically intractable problem dealing with the computation of a matrix function Permanent and its generalization Hafnian. Third, we explain how a recent no-go result applies generally to linear optical quantum experiments, thus revealing important insights into quantum state generation with current photonic technology. Fourth, we show how to describe quantum protocols such as entanglement swapping in a graphical way. The uncovered bridge between quantum experiments and graph theory offers another perspective on a widely used technology and immediately raises many follow-up questions.

Gouy Phase Radial Mode Sorter for Light: Concepts and Experiments.

We present an in principle lossless sorter for radial modes of light, using accumulated Gouy phases. The experimental setups have been found by a computer algorithm, and can be intuitively understood in a geometric way. Together with the ability to sort angular-momentum modes, we now have access to the complete two-dimensional transverse plane of light. The device can readily be used in multiplexing classical information. On a quantum level, it is an analog of the Stern-Gerlach experiment-significant for the discussion of fundamental concepts in quantum physics. As such, it can be applied in high-dimensional and multiphotonic quantum experiments.

Active learning machine learns to create new quantum experiments.

How useful can machine learning be in a quantum laboratory? Here we raise the question of the potential of intelligent machines in the context of scientific research. A major motivation for the present work is the unknown reachability of various entanglement classes in quantum experiments. We investigate this question by using the projective simulation model, a physics-oriented approach to artificial intelligence. In our approach, the projective simulation system is challenged to design complex photonic quantum experiments that produce high-dimensional entangled multiphoton states, which are of high interest in modern quantum experiments. The artificial intelligence system learns to create a variety of entangled states and improves the efficiency of their realization. In the process, the system autonomously (re)discovers experimental techniques which are only now becoming standard in modern quantum optical experiments-a trait which was not explicitly demanded from the system but emerged through the process of learning. Such features highlight the possibility that machines could have a significantly more creative role in future research.

Twisted photons: new quantum perspectives in high dimensions.

Twisted photons can be used as alphabets to encode information beyond one bit per single photon. This ability offers great potential for quantum information tasks, as well as for the investigation of fundamental questions. In this review article, we give a brief overview of the theoretical differences between qubits and higher dimensional systems, qudits, in different quantum information scenarios. We then describe recent experimental developments in this field over the past three years. Finally, we summarize some important experimental and theoretical questions that might be beneficial to understand better in the near future.

Quantum Experiments and Graphs: Multiparty States as Coherent Superpositions of Perfect Matchings.

We show a surprising link between experimental setups to realize high-dimensional multipartite quantum states and graph theory. In these setups, the paths of photons are identified such that the photon-source information is never created. We find that each of these setups corresponds to an undirected graph, and every undirected graph corresponds to an experimental setup. Every term in the emerging quantum superposition corresponds to a perfect matching in the graph. Calculating the final quantum state is in the #P-complete complexity class, thus it cannot be done efficiently. To strengthen the link further, theorems from graph theory-such as Hall's marriage problem-are rephrased in the language of pair creation in quantum experiments. We show explicitly how this link allows one to answer questions about quantum experiments (such as which classes of entangled states can be created) with graph theoretical methods, and how to potentially simulate properties of graphs and networks with quantum experiments (such as critical exponents and phase transitions).

High-Dimensional Single-Photon Quantum Gates: Concepts and Experiments.

Transformations on quantum states form a basic building block of every quantum information system. From photonic polarization to two-level atoms, complete sets of quantum gates for a variety of qubit systems are well known. For multilevel quantum systems beyond qubits, the situation is more challenging. The orbital angular momentum modes of photons comprise one such high-dimensional system for which generation and measurement techniques are well studied. However, arbitrary transformations for such quantum states are not known. Here we experimentally demonstrate a four-dimensional generalization of the Pauli X gate and all of its integer powers on single photons carrying orbital angular momentum. Together with the well-known Z gate, this forms the first complete set of high-dimensional quantum gates implemented experimentally. The concept of the X gate is based on independent access to quantum states with different parities and can thus be generalized to other photonic degrees of freedom and potentially also to other quantum systems.

Erratum: Entanglement by Path Identity [Phys. Rev. Lett. 118, 080401 (2017)].

This corrects the article DOI: 10.1103/PhysRevLett.118.080401.

Entanglement by Path Identity.

Quantum entanglement is one of the most prominent features of quantum mechanics and forms the basis of quantum information technologies. Here we present a novel method for the creation of quantum entanglement in multipartite and high-dimensional systems. The two ingredients are (i) superposition of photon pairs with different origins and (ii) aligning photons such that their paths are identical. We explain the experimentally feasible creation of various classes of multiphoton entanglement encoded in polarization as well as in high-dimensional Hilbert spaces-starting only from nonentangled photon pairs. For two photons, arbitrary high-dimensional entanglement can be created. The idea of generating entanglement by path identity could also apply to quantum entities other than photons. We discovered the technique by analyzing the output of a computer algorithm. This shows that computer designed quantum experiments can be inspirations for new techniques.

Orbital angular momentum of photons and the entanglement of Laguerre-Gaussian modes.

The identification of orbital angular momentum (OAM) as a fundamental property of a beam of light nearly 25 years ago has led to an extensive body of research around this topic. The possibility that single photons can carry OAM has made this degree of freedom an ideal candidate for the investigation of complex quantum phenomena and their applications. Research in this direction has ranged from experiments on complex forms of quantum entanglement to the interaction between light and quantum states of matter. Furthermore, the use of OAM in quantum information has generated a lot of excitement, as it allows for encoding large amounts of information on a single photon. Here, we explain the intuition that led to the first quantum experiment with OAM 15 years ago. We continue by reviewing some key experiments investigating fundamental questions on photonic OAM and the first steps to applying these properties in novel quantum protocols. At the end, we identify several interesting open questions that could form the subject of future investigations with OAM.This article is part of the themed issue 'Optical orbital angular momentum'.