The theorems of density functional theory (DFT) establish bijective maps between the local external potential of a many-body system and its electron density, wavefunction and, therefore, one-particle reduced density matrix. Building on this foundation, we show that machine learning models based on the one-electron reduced density matrix can be used to generate surrogate electronic structure methods. We generate surrogates of local and hybrid DFT, Hartree-Fock and full configuration interaction theories for systems ranging from small molecules such as water to more complex compounds like benzene and propanol. The surrogate models use the one-electron reduced density matrix as the central quantity to be learned. From the predicted density matrices, we show that either standard quantum chemistry or a second machine-learning model can be used to compute molecular observables, energies, and atomic forces. The surrogate models can generate essentially anything that a standard electronic structure method can, ranging from band gaps and Kohn-Sham orbitals to energy-conserving ab-initio molecular dynamics simulations and infrared spectra, which account for anharmonicity and thermal effects, without the need to employ computationally expensive algorithms such as self-consistent field theory. The algorithms are packaged in an efficient and easy to use Python code, QMLearn, accessible on popular platforms.
This content will become publicly available on September 21, 2024
Catalyzed by enormous success in the industrial sector, many research programs have been exploring data-driven, machine learning approaches. Performance can be poor when the model is extrapolated to new regions of chemical space, e.g., new bonding types, new many-body interactions. Another important limitation is the spatial locality assumption in model architecture, and this limitation cannot be overcome with larger or more diverse datasets. The outlined challenges are primarily associated with the lack of electronic structure information in surrogate models such as interatomic potentials. Given the fast development of machine learning and computational chemistry methods, we expect some limitations of surrogate models to be addressed in the near future; nevertheless spatial locality assumption will likely remain a limiting factor for their transferability. Here, we suggest focusing on an equally important effort—design of physics-informed models that leverage the domain knowledge and employ machine learning only as a corrective tool. In the context of material science, we will focus on semi-empirical quantum mechanics, using machine learning to predict corrections to the reduced-order Hamiltonian model parameters. The resulting models are broadly applicable, retain the speed of semiempirical chemistry, and frequently achieve accuracy on par with much more expensive ab initio calculations. These early results indicate that future work, in which machine learning and quantum chemistry methods are developed jointly, may provide the best of all worlds for chemistry applications that demand both high accuracy and high numerical efficiency.
more » « less- Award ID(s):
- 2202693
- NSF-PAR ID:
- 10479418
- Publisher / Repository:
- J. Chem. Phys.
- Date Published:
- Journal Name:
- The Journal of Chemical Physics
- Volume:
- 159
- Issue:
- 11
- ISSN:
- 0021-9606
- Page Range / eLocation ID:
- 110901-110912
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract The potential energy of molecular species and their conformers can be computed with a wide range of computational chemistry methods, from molecular mechanics to ab initio quantum chemistry. However, the proper choice of the computational approach based on computational cost and reliability of calculated energies is a dilemma, especially for large molecules. This dilemma is proved to be even more problematic for studies that require hundreds and thousands of calculations, such as drug discovery. On the other hand, driven by their pattern recognition capabilities, neural networks started to gain popularity in the computational chemistry community. During the last decade, many neural network potentials have been developed to predict a variety of chemical information of different systems. Neural network potentials are proved to predict chemical properties with accuracy comparable to quantum mechanical approaches but with the cost approaching molecular mechanics calculations. As a result, the development of more reliable, transferable, and extensible neural network potentials became an attractive field of study for researchers. In this review, we outlined an overview of the status of current neural network potentials and strategies to improve their accuracy. We provide recent examples of studies that prove the applicability of these potentials. We also discuss the capabilities and shortcomings of the current models and the challenges and future aspects of their development and applications. It is expected that this review would provide guidance for the development of neural network potentials and the exploitation of their applicability.
This article is categorized under:
Data Science > Artificial Intelligence/Machine Learning
Molecular and Statistical Mechanics > Molecular Interactions
Software > Molecular Modeling
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Modern semiempirical electronic structure methods have considerable promise in drug discovery as universal “force fields” that can reliably model biological and drug-like molecules, including alternative tautomers and protonation states. Herein, we compare the performance of several neglect of diatomic differential overlap-based semiempirical (MNDO/d, AM1, PM6, PM6-D3H4X, PM7, and ODM2), density-functional tight-binding based (DFTB3, DFTB/ChIMES, GFN1-xTB, and GFN2-xTB) models with pure machine learning potentials (ANI-1x and ANI-2x) and hybrid quantum mechanical/machine learning potentials (AIQM1 and QD π) for a wide range of data computed at a consistent ωB97X/6-31G* level of theory (as in the ANI-1x database). This data includes conformational energies, intermolecular interactions, tautomers, and protonation states. Additional comparisons are made to a set of natural and synthetic nucleic acids from the artificially expanded genetic information system that has important implications for the design of new biotechnology and therapeutics. Finally, we examine the acid/base chemistry relevant for RNA cleavage reactions catalyzed by small nucleolytic ribozymes, DNAzymes, and ribonucleases. Overall, the hybrid quantum mechanical/machine learning potentials appear to be the most robust for these datasets, and the recently developed QD π model performs exceptionally well, having especially high accuracy for tautomers and protonation states relevant to drug discovery.more » « less
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BACKGROUND Optical sensing devices measure the rich physical properties of an incident light beam, such as its power, polarization state, spectrum, and intensity distribution. Most conventional sensors, such as power meters, polarimeters, spectrometers, and cameras, are monofunctional and bulky. For example, classical Fourier-transform infrared spectrometers and polarimeters, which characterize the optical spectrum in the infrared and the polarization state of light, respectively, can occupy a considerable portion of an optical table. Over the past decade, the development of integrated sensing solutions by using miniaturized devices together with advanced machine-learning algorithms has accelerated rapidly, and optical sensing research has evolved into a highly interdisciplinary field that encompasses devices and materials engineering, condensed matter physics, and machine learning. To this end, future optical sensing technologies will benefit from innovations in device architecture, discoveries of new quantum materials, demonstrations of previously uncharacterized optical and optoelectronic phenomena, and rapid advances in the development of tailored machine-learning algorithms. ADVANCES Recently, a number of sensing and imaging demonstrations have emerged that differ substantially from conventional sensing schemes in the way that optical information is detected. A typical example is computational spectroscopy. In this new paradigm, a compact spectrometer first collectively captures the comprehensive spectral information of an incident light beam using multiple elements or a single element under different operational states and generates a high-dimensional photoresponse vector. An advanced algorithm then interprets the vector to achieve reconstruction of the spectrum. This scheme shifts the physical complexity of conventional grating- or interference-based spectrometers to computation. Moreover, many of the recent developments go well beyond optical spectroscopy, and we discuss them within a common framework, dubbed “geometric deep optical sensing.” The term “geometric” is intended to emphasize that in this sensing scheme, the physical properties of an unknown light beam and the corresponding photoresponses can be regarded as points in two respective high-dimensional vector spaces and that the sensing process can be considered to be a mapping from one vector space to the other. The mapping can be linear, nonlinear, or highly entangled; for the latter two cases, deep artificial neural networks represent a natural choice for the encoding and/or decoding processes, from which the term “deep” is derived. In addition to this classical geometric view, the quantum geometry of Bloch electrons in Hilbert space, such as Berry curvature and quantum metrics, is essential for the determination of the polarization-dependent photoresponses in some optical sensors. In this Review, we first present a general perspective of this sensing scheme from the viewpoint of information theory, in which the photoresponse measurement and the extraction of light properties are deemed as information-encoding and -decoding processes, respectively. We then discuss demonstrations in which a reconfigurable sensor (or an array thereof), enabled by device reconfigurability and the implementation of neural networks, can detect the power, polarization state, wavelength, and spatial features of an incident light beam. OUTLOOK As increasingly more computing resources become available, optical sensing is becoming more computational, with device reconfigurability playing a key role. 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