Lixue Cheng, P. Bernát Szabó, Zeno Schätzle et al. · microsoft-research
Variational ab-initio methods in quantum chemistry stand out among other methods in providing direct access to the wave function. This allows in principle straightforward extraction of any other observable of interest, besides the energy, but in practice this extraction is often technically difficult and computationally impractical. Here, we consider the electron density as a central observable in quantum chemistry and introduce a novel method to obtain accurate densities from real-space many-electron wave functions by representing the density with a neural network that captures known asymptotic properties and is trained from the wave function by score matching and noise-contrastive estimation. We use variational quantum Monte Carlo with deep-learning ansätze (deep QMC) to obtain highly accurate wave functions free of basis set errors, and from them, using our novel method, correspondingly accurate electron densities, which we demonstrate by calculating dipole moments, nuclear forces, contact densities, and other density-based properties.
A faithful description of chemical processes requires exploring extended regions of the molecular potential energy surface (PES), which remains challenging for strongly correlated systems. Transferable deep-learning variational Monte Carlo (VMC) offers a promising route by efficiently solving the electronic Schrödinger equation jointly across molecular geometries at consistently high accuracy, yet its stochastic nature renders direct exploration of molecular configuration space nontrivial. Here, we present a framework for highly accurate ab initio exploration of PESs that combines transferable deep-learning VMC with a cost-effective estimation of energies, forces, and Hessians. By continuously sampling nuclear configurations during VMC optimization of electronic wave functions, we obtain transferable descriptions that achieve zero-shot chemical accuracy within chemically relevant distributions of molecular geometries. Throughout the subsequent characterization of molecular configuration space, the PES is evaluated only sparsely, with local approximations constructed by estimating VMC energies and forces at sampled geometries and aggregating the resulting noisy data using Gaussian process regression. Our method enables accurate and efficient exploration of complex PES landscapes, including structure relaxation, transition-state searches, and minimum-energy pathways, for both ground and excited states. This opens the door to studying bond breaking, formation, and large structural rearrangements in systems with pronounced multi-reference character.
Adam Foster, Zeno Schätzle, P. Bernát Szabó et al. · microsoft-research
Reliable description of bond breaking remains a major challenge for quantum chemistry due to the multireferential character of the electronic structure in dissociating species. Multireferential methods in particular suffer from large computational cost, which under the normal paradigm has to be paid anew for each system at a full price, ignoring commonalities in electronic structure across molecules. Quantum Monte Carlo with deep neural networks (deep QMC) uniquely offers to exploit such commonalities by pretraining transferable wavefunction models, but all such attempts were so far limited in scope. Here, we bring this new paradigm to fruition with Orbformer, a novel transferable wavefunction model pretrained on 22,000 equilibrium and dissociating structures that can be fine-tuned on unseen molecules reaching an accuracy-cost ratio rivalling classical multireferential methods. On established benchmarks as well as more challenging bond dissociations and Diels-Alder reactions, Orbformer is the only method that consistently converges to chemical accuracy (1 kcal/mol). This work turns the idea of amortizing the cost of solving the Schrödinger equation over many molecules into a practical approach in quantum chemistry.
Alireza Furutanpey, Pantelis A. Frangoudis, Patrik Szabo et al.
This paper investigates the adversarial robustness of Deep Neural Networks (DNNs) using Information Bottleneck (IB) objectives for task-oriented communication systems. We empirically demonstrate that while IB-based approaches provide baseline resilience against attacks targeting downstream tasks, the reliance on generative models for task-oriented communication introduces new vulnerabilities. Through extensive experiments on several datasets, we analyze how bottleneck depth and task complexity influence adversarial robustness. Our key findings show that Shallow Variational Bottleneck Injection (SVBI) provides less adversarial robustness compared to Deep Variational Information Bottleneck (DVIB) approaches, with the gap widening for more complex tasks. Additionally, we reveal that IB-based objectives exhibit stronger robustness against attacks focusing on salient pixels with high intensity compared to those perturbing many pixels with lower intensity. Lastly, we demonstrate that task-oriented communication systems that rely on generative models to extract and recover salient information have an increased attack surface. The results highlight important security considerations for next-generation communication systems that leverage neural networks for goal-oriented compression.