TY - JOUR A1 - Fischer, Eric Wolfgang A1 - Werther, Michael A1 - Bouakline, Foudhil A1 - Grossmann, Frank A1 - Saalfrank, Peter T1 - Non-Markovian vibrational relaxation dynamics at surfaces JF - The journal of chemical physics : bridges a gap between journals of physics and journals of chemistr N2 - Vibrational dynamics of adsorbates near surfaces plays both an important role for applied surface science and as a model lab for studying fundamental problems of open quantum systems. We employ a previously developed model for the relaxation of a D-Si-Si bending mode at a D:Si(100)-(2 x 1) surface, induced by a "bath " of more than 2000 phonon modes [Lorenz and P. Saalfrank, Chem. Phys. 482, 69 (2017)], to extend previous work along various directions. First, we use a Hierarchical Effective Mode (HEM) model [Fischer et al., J. Chem. Phys. 153, 064704 (2020)] to study relaxation of higher excited vibrational states than hitherto done by solving a high-dimensional system-bath time-dependent Schrodinger equation (TDSE). In the HEM approach, (many) real bath modes are replaced by (much less) effective bath modes. Accordingly, we are able to examine scaling laws for vibrational relaxation lifetimes for a realistic surface science problem. Second, we compare the performance of the multilayer multiconfigurational time-dependent Hartree (ML-MCTDH) approach with that of the recently developed coherent-state-based multi-Davydov-D2 Ansatz [Zhou et al., J. Chem. Phys. 143, 014113 (2015)]. Both approaches work well, with some computational advantages for the latter in the presented context. Third, we apply open-system density matrix theory in comparison with basically "exact " solutions of the multi-mode TDSEs. Specifically, we use an open-system Liouville-von Neumann (LvN) equation treating vibration-phonon coupling as Markovian dissipation in Lindblad form to quantify effects beyond the Born-Markov approximation. Published under an exclusive license by AIP Publishing. KW - phonons KW - Vibrational states KW - Chemical dynamics KW - Adsorption KW - Surface science KW - Open quantum systems KW - Density-matrix KW - Coherent states KW - Markov processes Y1 - 2022 U6 - https://doi.org/10.1063/5.0092836 SN - 0021-9606 SN - 1089-7690 SN - 1520-9032 VL - 156 IS - 21 PB - AIP Publishing CY - Melville ER - TY - JOUR A1 - Thon, Ingo A1 - Landwehr, Niels A1 - De Raedt, Luc T1 - Stochastic relational processes efficient inference and applications JF - Machine learning N2 - One of the goals of artificial intelligence is to develop agents that learn and act in complex environments. Realistic environments typically feature a variable number of objects, relations amongst them, and non-deterministic transition behavior. While standard probabilistic sequence models provide efficient inference and learning techniques for sequential data, they typically cannot fully capture the relational complexity. On the other hand, statistical relational learning techniques are often too inefficient to cope with complex sequential data. In this paper, we introduce a simple model that occupies an intermediate position in this expressiveness/efficiency trade-off. It is based on CP-logic (Causal Probabilistic Logic), an expressive probabilistic logic for modeling causality. However, by specializing CP-logic to represent a probability distribution over sequences of relational state descriptions and employing a Markov assumption, inference and learning become more tractable and effective. Specifically, we show how to solve part of the inference and learning problems directly at the first-order level, while transforming the remaining part into the problem of computing all satisfying assignments for a Boolean formula in a binary decision diagram. We experimentally validate that the resulting technique is able to handle probabilistic relational domains with a substantial number of objects and relations. KW - Statistical relational learning KW - Stochastic relational process KW - Markov processes KW - Time series KW - CP-Logic Y1 - 2011 U6 - https://doi.org/10.1007/s10994-010-5213-8 SN - 0885-6125 VL - 82 IS - 2 SP - 239 EP - 272 PB - Springer CY - Dordrecht ER -