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Alan Aspuru-Guzik

Publications and source records attributed to Alan Aspuru-Guzik.

At least 19 recordsLinked to original sources

DIA: Denoising Intermediate Advantage for Diffusion Policy Optimization

Diffusion-based robot policies have become widely used in robotic manipulation, where they are typically trained with behavior cloning. However, policies trained purely from demonstrations are limited by the quality and coverage of the available data. Reinforcement learning can further improve the performance of these pretrained policies through interaction. A common approach is to use policy-gradient methods that formulate diffusion-policy fine-tuning as an outer environment MDP together with an inner denoising MDP. However, existing methods typically assign the same environment-level credit to all denoising steps used to construct an action chunk, without distinguishing which intermediate decisions contributed most to the final return. We introduce Denoising Intermediate Advantage (DIA), a policy-gradient method that learns a value function over partially denoised actions and uses it to construct a denoising level advantage for each step of the generative process. DIA combines this inner credit signal with the standard environment-level PPO advantage, providing state-dependent credit throughout the denoising chain. Across Robomimic, FurnitureBench, Franka Kitchen, and D3IL, DIA consistently improves final performance over existing diffusion-policy fine-tuning methods. Beyond final reward, DIA reaches successful states more efficiently and can shift farther from the pretrained behavior distribution, enabling it to discover more effective and efficient task-level strategies and subtask sequences that baseline methods fail to reach.

cs.RO

HIP: Hessian Interatomic Potentials without derivatives

Molecular Hessians, the second derivatives of the potential energy, are fundamental to many workflows in computational chemistry. Usually, accurate Hessians are computationally expensive to calculate and scale poorly with system size, whether computed using quantum chemistry methods or machine-learning interatomic potentials (MLIPs). In this work, we introduce Hessian interatomic potentials (HIPs), a deep learning model that directly predicts Hessians without relying on automatic differentiation or finite differences. To do so, we construct SE(3)-equivariant, symmetric Hessians from irreducible representation (irrep) features up to degree $l$=2, computed by a graph neural network. HIP Hessians are one to two orders of magnitude faster, more accurate, more memory efficient, easier to train, and exhibit more favourable scaling with system size. We validate our predictions across a wide range of downstream tasks, demonstrating consistently superior performance in transition state search, geometry optimization, zero-point energy corrections, and vibrational analysis. We open-source the HIP code and model weights.

cs.LG

How Molecular Generative Models Organize Molecular Identity

Generative models for matter are often evaluated as samplers over output representations, and their latent spaces are commonly used as proxies for navigating chemical space. Much less is known about how these models internally arrange discrete chemical identities within those representations. We study this arrangement by making molecular identity explicit and pulling it back through the generative process. Through these pullbacks we probe the regions that generate the same object, exposing the trained model's internal repertoire: a fixed partition that determines which objects (novel or not) the model can produce. Across three molecular generative architectures, we find that this repertoire is arranged into piecewise-constant regions separated by recurring coarse-to-fine boundaries. Its organization depends on the representation probed, the identity convention, decoder stochasticity, and the metric used to compare coordinates. During training, local chemical organization stabilizes while the number of distinct molecular identities represented within each neighborhood continues to change. Internal organization must therefore be characterized, rather than assumed, before a generative space can be treated as chemically navigable.

cs.LG

Faster Algorithmic Quantum and Classical Simulations by Corrected Product Formulas

Hamiltonian simulation using product formulas is arguably the most straightforward and practical approach for algorithmic simulation of a quantum system's dynamics on a quantum computer. Here we present corrected product formulas (CPFs), a variation of product formulas achieved by injecting auxiliary terms called correctors into standard product formulas. We establish several correctors that improve the accuracy of standard product formulas by orders of magnitude when simulating Hamiltonians comprised of two exactly simulatable partitions, a common structure of lattice Hamiltonians. Importantly, injecting these correctors increases the overall simulation cost by only a small additive or multiplicative factor. We show that correctors are particularly advantageous for perturbed systems, where one partition has a relatively small norm compared to the other, as they allow the small norm to be utilized as an additional parameter for controlling the simulation error. We demonstrate the performance of CPFs by numerical simulations for several lattice Hamiltonians. Numerical results show that our theoretical error bounds for CPFs match or outperform the empirical error scaling of standard product formulas for these systems. We also demonstrate improvements offered by CPFs by implementing small-size systems on actual quantum hardware, as well as on noisy and noiseless quantum simulators. CPFs could be a valuable algorithmic tool for early fault-tolerant quantum computers with limited computing resources. As for standard product formulas, CPFs could also be used for simulations on a classical computer.

quant-ph

QPILOTS: Efficient Test-Time Q-Steering for Flow Policies

Flow-matching and diffusion policies are expressive action generators, but optimizing them with temporal-difference reinforcement learning (RL) remains difficult. Effective policy extraction requires exploiting the critic's action gradient, yet directly backpropagating this signal through a multi-step denoising process can be numerically unstable. Existing methods work around this either by discarding gradient information, distilling the policy into a simpler one-step actor, or repeatedly fine-tuning the denoising policy as the critic improves. We propose QPILOTS, a method that leaves the original policy unmodified and steers the denoising process at inference time. At each denoising step, instead of evaluating the critic on the noisy intermediate action where critic predictions are unreliable, we first project that intermediate state to an estimate of the final clean action and compute the critic gradient there. We introduce two variants: QPILOTS-U uses a fast single-point approximation, while QPILOTS-M draws differentiable posterior samples via a learned auxiliary network. On a standard offline-to-online RL benchmark, QPILOTS achieves the best aggregate performance, reaching an average success rate of 90% across 50 tasks. We also apply QPILOTS to steer a large, frozen, pretrained Vision-Language Action (VLA) foundation model, outperforming or matching prior inference-time approaches across six manipulation tasks in simulation.

cs.LG

EGMOF: Efficient Generation of Metal-Organic Frameworks Using a Hybrid Diffusion-Transformer Architecture

Designing materials with targeted properties remains challenging due to the vastness of chemical space and the scarcity of property-labeled data. While recent advances in generative models offer a promising way for inverse design, most approaches require large datasets and must be retrained for every new target property. Here, we introduce the EGMOF (Efficient Generation of MOFs), a hybrid diffusion-transformer framework that overcomes these limitations through a modular, descriptor-mediated workflow. EGMOF decomposes inverse design into two steps: (1) a one-dimensional diffusion model (Prop2Desc) that maps desired properties to chemically meaningful descriptors followed by (2) a transformer model (Desc2MOF) that generates structures from these descriptors. This modular hybrid design enables minimal retraining and maintains high accuracy even under small-data conditions. On a hydrogen uptake dataset, EGMOF achieved over 94% validity and 91% hit rate, representing significant improvements of up to 39% in validity and 29% in hit rate compared to existing methods, while remaining effective with only 1,000 training samples. Moreover, our model successfully performed conditional generation across 29 diverse property datasets, including CoREMOF, QMOF, and text-mined experimental datasets, whereas previous models have not. This work presents a data-efficient, generalizable approach to the inverse design of diverse MOFs and highlights the potential of modular inverse design workflows for broader materials discovery.

cond-mat.mtrl-sci

Schema for In-Context Learning

In-Context Learning (ICL) enables transformer-based language models to adapt to new tasks by conditioning on demonstration examples. However, traditional example-driven in-context learning lacks explicit modules for knowledge retrieval and transfer at the abstraction level. Inspired by cognitive science, specifically schema theory, which holds that humans interpret new information by activating pre-existing mental frameworks (schemas) to structure understanding, we introduce Schema-Activated In-Context Learning (SA-ICL). This framework extracts the representation of the building blocks of cognition for the reasoning process instilled from prior examples, creating an abstracted schema, a lightweight, structured template of key inferential steps and their relationships, which is then used to augment a model's reasoning process when presented with a novel question. We demonstrate that a broad range of large language models (LLMs) lack the capacity to form and utilize internal schema-based learning representations implicitly, but instead benefit significantly from explicit schema-based scaffolding. Across chemistry and physics questions from the GPQA dataset, our experiments show that SA-ICL consistently boosts performance, up to 36.19 percent, when the single demonstration example is of high quality, which simultaneously reduces reliance on the number of demonstrations and enhances interpretability. Schema-Activated In-Context Learning not only bridges disparate ICL strategies ranging from pattern priming to Chain-of-Thought prompting, but also paves a new path for enhancing human-like reasoning in LLMs.

cs.CL

Auger Spectroscopy via Generative Quantum Eigensolver: A Quantum Approach to Molecular Excitations

Auger electron spectroscopy, a way of characterizing electronic structure through core-level decay processes, is widely used in materials characterization; however direct calculation from molecular geometry requires accurate treatment of many excited states, posing a challenge for classical methods. We present a hybrid quantum-classical workflow for calculating Auger spectra that combines the generative quantum eigensolver (GQE) for ground-state preparation, the quantum self-consistent equation-of-motion method for excited-state calculations, and the one-centre approximation for Auger transition rates. GQE uses a GPT-2 model to generate quantum circuits for ground-state optimization, allowing our workflow to benefit from HPC parallelization and GPU-acceleration for favourable scaling with system size. We demonstrate the validity of our workflow by calculating the Auger spectrum of water with the STO-3G basis set and demonstrating qualitative and quantitative agreement with spectra obtained using completely classical full configuration interaction calculations, from the computational literature, and from the experimental literature. We also find that for water, substituting the variational quantum eigensolver (VQE) for GQE results in near-identical spectra, but that the ground state estimator generated by GQE contains about half the total gate count as that generated by VQE.

quant-ph

Application-Driven Innovation in Machine Learning

In this position paper, we argue that application-driven research has been systemically under-valued in the machine learning community. As applications of machine learning proliferate, innovative algorithms inspired by specific real-world challenges have become increasingly important. Such work offers the potential for significant impact not merely in domains of application but also in machine learning itself. In this paper, we describe the paradigm of application-driven research in machine learning, contrasting it with the more standard paradigm of methods-driven research. We illustrate the benefits of application-driven machine learning and how this approach can productively synergize with methods-driven work. Despite these benefits, we find that reviewing, hiring, and teaching practices in machine learning often hold back application-driven innovation. We outline how these processes may be improved.

cs.LG

SynTwins: A Retrosynthesis-Guided Framework for Synthesizable Molecular Analog Generation

The disconnect between AI-generated molecules with desirable properties and their synthetic feasibility remains a critical bottleneck in computational discovery of drugs and materials. While generative AI has accelerated the proposal of candidate molecules, many of these structures prove challenging or impossible to synthesize using established chemical reactions. Here, we introduce SynTwins, a novel retrosynthesis-guided molecule design framework that finds synthetically accessible molecular analogs by emulating expert chemists' strategies in three steps: retrosynthesis, searching similar building blocks, and virtual synthesis. Using a search algorithm instead of a stochastic data-driven generator, SynTwins outperforms state-of-the-art machine learning models at exploring synthetically accessible analogs while maintaining high structural similarity to original target molecules. Furthermore, when integrated into existing molecular property-optimization frameworks, our hybrid approach produces synthetically feasible analogs with minimal loss in property scores. Our comprehensive benchmarking across diverse molecular datasets demonstrates that SynTwins effectively bridges the gap between computational design and experimental synthesis, providing a practical solution for accelerating the discovery of synthesizable molecules with desired properties for a wide range of applications.

physics.chem-ph

RAISE: A self-driving laboratory for interfacial property formulation discovery

Surface wettability is a critical design parameter for biomedical devices, coatings, and textiles. Contact angle measurements quantify liquid-surface interactions, which depend strongly on liquid formulation. Herein, we present the Robotic Autonomous Imaging Surface Evaluator (RAISE), a closed-loop, self-driving laboratory that is capable of linking liquid formulation optimization with surface wettability assessment. RAISE comprises a full experimental orchestrator with the ability of mixing liquid ingredients to create varying formulation cocktails, transferring droplets of prepared formulations to a high-throughput stage, and using a pick-and-place camera tool for automated droplet image capture. The system also includes an automated image processing pipeline to measure contact angles. This closed loop experiment orchestrator is integrated with a Bayesian Optimization (BO) client, which enables iterative exploration of new formulations based on previous contact angle measurements to meet user-defined objectives. The system operates in a high-throughput manner and can achieve a measurement rate of approximately 1 contact angle measurement per minute. Here we demonstrate RAISE can be used to explore surfactant wettability and how surfactant combinations create tunable formulations that compensate for purity-related variations. Furthermore, multi-objective BO demonstrates how precise and optimal formulations can be reached based on application-specific goals. The optimization is guided by a desirability score, which prioritizes formulations that are within target contact angle ranges, minimize surfactant usage and reduce cost. This work demonstrates the capabilities of RAISE to autonomously link liquid formulations to contact angle measurements in a closed-loop system, using multi-objective BO to efficiently identify optimal formulations aligned with researcher-defined criteria.

cs.RO

Quantum Algorithm for Vibronic Dynamics: Case Study on Singlet Fission Solar Cell Design

Vibronic interactions between nuclear motion and electronic states are critical for the accurate modeling of photochemistry. However, accurate simulations of fully quantum non-adiabatic dynamics are often prohibitively expensive for classical methods beyond small systems. In this work, we present a quantum algorithm based on product formulas for simulating time evolution under a general vibronic Hamiltonian in real space, capable of handling an arbitrary number of electronic states and vibrational modes. We develop the first trotterization scheme for vibronic Hamiltonians beyond two electronic states and introduce an array of optimization techniques for the exponentiation of each fragment in the product formula, resulting in a remarkably low cost of implementation. To demonstrate practical relevance, we outline a proof-of-principle integration of our algorithm into a materials discovery pipeline for designing more efficient singlet fission-based organic solar cells. We estimate that $100$ fs of propagation using a second-order Trotter product formula for a $6$-state, $21$-mode model of exciton transport at an anthracene dimer requires $154$ qubits and $2.76 \times 10^6$ Toffoli gates. While a $4$-state, $246$-mode model describing charge transfer at an anthracene-fullerene interface requires $1053$ qubits and $2.66 \times 10^7$ Toffoli gates.

quant-ph

Learning Zero-Shot Material States Segmentation, by Implanting Natural Image Patterns in Synthetic Data

Visual recognition of materials and their states is essential for understanding the physical world, from identifying wet regions on surfaces or stains on fabrics to detecting infected areas on plants or minerals in rocks. Collecting data that captures this vast variability is complex due to the scattered and gradual nature of material states. Manually annotating real-world images is constrained by cost and precision, while synthetic data, although accurate and inexpensive, lacks real-world diversity. This work aims to bridge this gap by infusing patterns automatically extracted from real-world images into synthetic data. Hence, patterns collected from natural images are used to generate and map materials into synthetic scenes. This unsupervised approach captures the complexity of the real world while maintaining the precision and scalability of synthetic data. We also present the first comprehensive benchmark for zero-shot material state segmentation, utilizing real-world images across a diverse range of domains, including food, soils, construction, plants, liquids, and more, each appears in various states such as wet, dry, infected, cooked, burned, and many others. The annotation includes partial similarity between regions with similar but not identical materials and hard segmentation of only identical material states. This benchmark eluded top foundation models, exposing the limitations of existing data collection methods. Meanwhile, nets trained on the infused data performed significantly better on this and related tasks. The dataset, code, and trained model are available. We also share 300,000 extracted textures and SVBRDF/PBR materials to facilitate future datasets generation.

cs.CV

Ranking over Regression for Bayesian Optimization and Molecule Selection

Bayesian optimization (BO) has become an indispensable tool for autonomous decision-making across diverse applications from autonomous vehicle control to accelerated drug and materials discovery. With the growing interest in self-driving laboratories, BO of chemical systems is crucial for machine learning (ML) guided experimental planning. Typically, BO employs a regression surrogate model to predict the distribution of unseen parts of the search space. However, for the selection of molecules, picking the top candidates with respect to a distribution, the relative ordering of their properties may be more important than their exact values. In this paper, we introduce Rank-based Bayesian Optimization (RBO), which utilizes a ranking model as the surrogate. We present a comprehensive investigation of RBO's optimization performance compared to conventional BO on various chemical datasets. Our results demonstrate similar or improved optimization performance using ranking models, particularly for datasets with rough structure-property landscapes and activity cliffs. Furthermore, we observe a high correlation between the surrogate ranking ability and BO performance, and this ability is maintained even at early iterations of BO optimization when using ranking surrogate models. We conclude that RBO is an effective alternative to regression-based BO, especially for optimizing novel chemical compounds.

cs.LG

qSWIFT: High-order randomized compiler for Hamiltonian simulation

Hamiltonian simulation is known to be one of the fundamental building blocks of a variety of quantum algorithms such as its most immediate application, that of simulating many-body systems to extract their physical properties. In this work, we present qSWIFT, a high-order randomized algorithm for Hamiltonian simulation. In qSWIFT, the required number of gates for a given precision is independent of the number of terms in Hamiltonian, while the systematic error is exponentially reduced with regards to the order parameter. In this respect, our qSWIFT is a higher-order counterpart of the previously proposed quantum stochastic drift protocol (qDRIFT), in which the number of gates scales linearly with the inverse of the precision required. We construct the qSWIFT channel and establish a rigorous bound for the systematic error quantified by the diamond norm. qSWIFT provides an algorithm to estimate given physical quantities using a system with one ancilla qubit, which is as simple as other product-formula-based approaches such as regular Trotter-Suzuki decompositions and qDRIFT. Our numerical experiment reveals that the required number of gates in qSWIFT is significantly reduced compared to qDRIFT. Particularly, the advantage is significant for problems where high precision is required; for example, to achieve a systematic relative propagation error of $10^{-6}$, the required number of gates in third-order qSWIFT is 1000 times smaller than that of qDRIFT.

quant-ph

Efficient Quantum Algorithm for All Quantum Wavelet Transforms

Wavelet transforms are widely used in various fields of science and engineering as a mathematical tool with features that reveal information ignored by the Fourier transform. Unlike the Fourier transform, which is unique, a wavelet transform is specified by a sequence of numbers associated with the type of wavelet used and an order parameter specifying the length of the sequence. While the quantum Fourier transform, a quantum analog of the classical Fourier transform, has been pivotal in quantum computing, prior works on quantum wavelet transforms~(QWTs) were limited to the second and fourth order of a particular wavelet, the Daubechies wavelet. Here we develop a simple yet efficient quantum algorithm for executing any wavelet transform on a quantum computer. Our approach is to decompose the kernel matrix of a wavelet transform as a linear combination of unitaries (LCU) that are compilable by easy-to-implement modular quantum arithmetic operations and use the LCU technique to construct a probabilistic procedure to implement a QWT with a \textit{known} success probability. We then use properties of wavelets to make this approach deterministic by a few executions of the amplitude amplification strategy. We extend our approach to a multilevel wavelet transform and a generalized version, the packet wavelet transform, establishing computational complexities in terms of three parameters: the wavelet order $M$, the dimension $N$ of the transformation matrix, and the transformation level $d$. We show the cost is logarithmic in $N$, linear in $d$ and superlinear in $M$. Moreover, we show the cost is independent of $M$ for practical applications. Our proposed quantum wavelet transforms could be used in quantum computing algorithms in a similar manner to their well-established counterpart, the quantum Fourier transform.

quant-ph

Tartarus: A Benchmarking Platform for Realistic And Practical Inverse Molecular Design

The efficient exploration of chemical space to design molecules with intended properties enables the accelerated discovery of drugs, materials, and catalysts, and is one of the most important outstanding challenges in chemistry. Encouraged by the recent surge in computer power and artificial intelligence development, many algorithms have been developed to tackle this problem. However, despite the emergence of many new approaches in recent years, comparatively little progress has been made in developing realistic benchmarks that reflect the complexity of molecular design for real-world applications. In this work, we develop a set of practical benchmark tasks relying on physical simulation of molecular systems mimicking real-life molecular design problems for materials, drugs, and chemical reactions. Additionally, we demonstrate the utility and ease of use of our new benchmark set by demonstrating how to compare the performance of several well-established families of algorithms. Surprisingly, we find that model performance can strongly depend on the benchmark domain. We believe that our benchmark suite will help move the field towards more realistic molecular design benchmarks, and move the development of inverse molecular design algorithms closer to designing molecules that solve existing problems in both academia and industry alike.

cs.CE

One-shot recognition of any material anywhere using contrastive learning with physics-based rendering

Visual recognition of materials and their states is essential for understanding most aspects of the world, from determining whether food is cooked, metal is rusted, or a chemical reaction has occurred. However, current image recognition methods are limited to specific classes and properties and can't handle the vast number of material states in the world. To address this, we present MatSim: the first dataset and benchmark for computer vision-based recognition of similarities and transitions between materials and textures, focusing on identifying any material under any conditions using one or a few examples. The dataset contains synthetic and natural images. The synthetic images were rendered using giant collections of textures, objects, and environments generated by computer graphics artists. We use mixtures and gradual transitions between materials to allow the system to learn cases with smooth transitions between states (like gradually cooked food). We also render images with materials inside transparent containers to support beverage and chemistry lab use cases. We use this dataset to train a siamese net that identifies the same material in different objects, mixtures, and environments. The descriptor generated by this net can be used to identify the states of materials and their subclasses using a single image. We also present the first few-shot material recognition benchmark with images from a wide range of fields, including the state of foods and drinks, types of grounds, and many other use cases. We show that a net trained on the MatSim synthetic dataset outperforms state-of-the-art models like Clip on the benchmark and also achieves good results on other unsupervised material classification tasks.

cs.CV