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Nico Grimm

Publications and source records attributed to Nico Grimm.

2 recordsLinked to original sources

Direct Message Approximation (DMA): A Consistency-Based Framework for Tractable Approximate Inference on Factor Graphs

Approximate message passing on factor graphs underlies two dominant families of probabilistic inference algorithms: expectation propagation (EP) and variational message passing (VMP). Both methods approximate the marginal at each factor edge, forcing an iterative round-robin schedule, risking negative-precision messages, and, for VMP, collapsing to point estimates at Dirac-delta factors. We introduce Direct Message Approximation (DMA), which approximates factor-to-variable messages directly rather than the marginal. For normalisable factors, we define a consistency condition (requiring exactness when all other incoming messages are Dirac deltas) to guide message construction. We prove a master theorem (proper messages, any graph) bounding marginal KL from message KL, with three structural corollaries: Dirac-input consistency, no EP-style inner-loop iteration, and no negative-precision messages. Further, we prove a complementary $O(1/r^2)$ guarantee for the inherently improper backward message of the product factor, whose closed-form treatment has resisted prior work. As a concrete instantiation, we derive explicit DMA messages for the product and leaky-ReLU factors and assemble a Bayesian neural network (BNN) inference algorithm with one forward/backward sweep per training example and no gradient learning-rate hyperparameter, validating that the structural guarantees translate to predictive uncertainty that widens in data-sparse regions, including under model mismatch.

cs.LG↗

Temperature-dependent EXAFS measurements of the Pb L3-edge allow quantification of the anharmonicity of the lead-halide bond of chlorine-substituted methylammonium (MA) lead triiodide

This article reports on studies of chlorine-substituted MAPbI3 using combined temperature-dependent XRD synchrotron and Pb-L3 edge EXAFS to analyze the anharmonicity of the lead halide bond. The EXAFS parameters were described in the orthorhombic phase by an Einstein or T2 type behavior, which was then compared with the experimental EXAFS parameters of the tetragonal/cubic phase. In the orthorhombic phase, it was observed that the asymmetry of the pair distribution function (cumulant C3) in MAPbCl3 is much lower than in MAPbI3. Compared with the behavior in the orthorhombic phase, the anharmonicity changed after the phase transition to the room temperature phase, with MAPbCl3 showing an increased anharmonicity and MAPbI3 a decrease. The differences between MAPbI3 and 2% chlorine substitution were small, both in the orthorhombic and tetragonal phases. By determining the structural parameters required to convert the effective force constants k0 and k3 resulting from the EXAFS analysis into the Morse potential parameters α and D, we could establish that our results agree with other experimental findings. Moreover, by using XRD we found that the [PbX6] octahedra shrink slightly in the tetragonal phase of MAPbI3 and MAPbI2.94Cl0.06, towards increasing temperatures. This behavior in the tetragonal phase is related to the dominant negative tension effects observed by EXAFS.

cond-mat.mtrl-sci↗