Quantum chemical accuracy from density functional approximations via machine learning.

Kohn-Sham density functional theory (DFT) is a standard tool in most branches of chemistry, but accuracies for many molecules are limited to 2-3 kcal â‹… mol-1 with presently-available functionals. Ab initio methods, such as coupled-cluster, routinely produce much higher accuracy, but computational costs limit their application to small molecules. In this paper, we leverage machine learning to calculate coupled-cluster energies from DFT densities, reaching quantum chemical accuracy (errors below 1 kcal â‹… mol-1) on test data. Moreover, density-based Δ-learning (learning only the correction to a standard DFT calculation, termed Δ-DFT ) significantly reduces the amount of training data required, particularly when molecular symmetries are included. The robustness of Δ-DFT  is highlighted by correcting "on the fly" DFT-based molecular dynamics (MD) simulations of resorcinol (C6H4(OH)2) to obtain MD trajectories with coupled-cluster accuracy. We conclude, therefore, that Δ-DFT  facilitates running gas-phase MD simulations with quantum chemical accuracy, even for strained geometries and conformer changes where standard DFT fails.

Implicit relevance feedback from electroencephalography and eye tracking in image search.

OBJECTIVE: Methods from brain-computer interfacing (BCI) open a direct access to the mental processes of computer users, which offers particular benefits in comparison to standard methods for inferring user-related information. The signals can be recorded unobtrusively in the background, which circumvents the time-consuming and distracting need for the users to give explicit feedback to questions concerning the individual interest. The obtained implicit information makes it possible to create dynamic user interest profiles in real-time, that can be taken into account by novel types of adaptive, personalised software. In the present study, the potential of implicit relevance feedback from electroencephalography (EEG) and eye tracking was explored with a demonstrator application that simulated an image search engine. APPROACH: The participants of the study queried for ambiguous search terms, having in mind one of the two possible interpretations of the respective term. Subsequently, they viewed different images arranged in a grid that were related to the query. The ambiguity of the underspecified search term was resolved with implicit information present in the recorded signals. For this purpose, feature vectors were extracted from the signals and used by multivariate classifiers that estimated the intended interpretation of the ambiguous query. MAIN RESULT: The intended interpretation was inferred correctly from a combination of EEG and eye tracking signals in 86% of the cases on average. Information provided by the two measurement modalities turned out to be complementary. SIGNIFICANCE: It was demonstrated that BCI methods can extract implicit user-related information in a setting of human-computer interaction. Novelties of the study are the implicit online feedback from EEG and eye tracking, the approximation to a realistic use case in a simulation, and the presentation of a large set of photographies that had to be interpreted with respect to the content.