Spectroscopic Probe Molecule Selection Using Quantum Theory, First-Principles Calculations, and Machine Learning

ACS Nano
Joshua L Lansford, Dionisios G Vlachos

Abstract

Probe molecule vibrational spectra have a long history of being used to characterize materials including metals, oxides, metal-organic frameworks, and even human proteins. Furthermore, recent advances in machine learning have enabled computationally generated spectra to aid in detailed characterization of complex surfaces with probe molecules. Despite widespread use of probe molecules, the science of probe molecule selection is underdeveloped. Here, we develop physical concepts, including orbital interaction energy and the energy overlap integral, to explain and predict the ability of probe molecules to discriminate structural descriptors. We resolve the crystal orbital overlap population (COOP) to specific molecular orbitals and quantify their bonding character, which directly influences vibrational frequencies. Using only a single adsorbate calculation from density function theory (DFT), we compute the interaction energy of individual adsorbate molecular orbitals with adsorption site atomic orbitals across many different sites. Combining the molecular orbital resolved COOP and changes in orbital interaction energy enables probe molecule selection for improved discrimination of various sites. We demonstrate these concepts by c...Continue Reading

References

Oct 2, 1998·Science·G Marnellos, M Stoukides
Oct 15, 1996·Physical Review. B, Condensed Matter·G Kresse, J Furthmüller
Sep 27, 2000·Physical Review Letters·N Lorente, M Persson
Sep 15, 1944·Proceedings of the National Academy of Sciences of the United States of America·F D Murnaghan
Aug 21, 2007·Journal of the American Chemical Society·Ismaila DaboNicola Marzari
Feb 10, 2009·Journal of the American Chemical Society·Eranda NikollaSuljo Linic
Sep 17, 2009·Physical Chemistry Chemical Physics : PCCP·Beth A LindquistSteven A Corcelli
Mar 20, 2010·Nature·Jian Feng LiZhong Qun Tian
Jun 24, 2010·Journal of the American Chemical Society·Adam R BrownEric N Jacobsen
Aug 17, 2010·Journal of the American Chemical Society·Insun ParkSergei S Sheiko
Jan 15, 2011·Science·Franklin Feng Tao, Miquel Salmeron
May 18, 2013·Chemical Reviews·Heejae Kim, Minhaeng Cho
Apr 3, 2014·Annual Review of Physical Chemistry·Aditya Savara, Eric Weitz
Oct 10, 2015·Science·Federico Calle-VallejoAliaksandr S Bandarenka
Feb 26, 2016·Journal of Computational Chemistry·Stefan MaintzRichard Dronskowski
Jun 10, 2016·Journal of the American Chemical Society·Alexander V Mironenko, Dionisios G Vlachos
Feb 6, 2017·Physical Review Letters·Xianfeng Ma, Hongliang Xin
Mar 28, 2017·Science Advances·Stephen W T PriceJ Frederick W Mosselmans
Jul 12, 2017·Cancer Cell·Julian Blagg, Paul Workman
Dec 1, 2017·Nature Communications·Joshua L LansfordDionisios G Vlachos
Feb 26, 2019·Advanced Materials·Dmitry I SharapaSilke Behrens
Apr 21, 2020·ACS Nano·Thomas HartmanBert M Weckhuysen

❮ Previous
Next ❯

Citations

Jul 16, 2021·Journal of Chemical Information and Modeling·Zachary J BaumQiongqiong Zhou
Nov 25, 2021·Physical Chemistry Chemical Physics : PCCP·Hao LiuChunxiao Gao

❮ Previous
Next ❯

Related Concepts

Trending Feeds

COVID-19

Coronaviruses encompass a large family of viruses that cause the common cold as well as more serious diseases, such as the ongoing outbreak of coronavirus disease 2019 (COVID-19; formally known as 2019-nCoV). Coronaviruses can spread from animals to humans; symptoms include fever, cough, shortness of breath, and breathing difficulties; in more severe cases, infection can lead to death. This feed covers recent research on COVID-19.

Blastomycosis

Blastomycosis fungal infections spread through inhaling Blastomyces dermatitidis spores. Discover the latest research on blastomycosis fungal infections here.

Nuclear Pore Complex in ALS/FTD

Alterations in nucleocytoplasmic transport, controlled by the nuclear pore complex, may be involved in the pathomechanism underlying multiple neurodegenerative diseases including Amyotrophic Lateral Sclerosis and Frontotemporal Dementia. Here is the latest research on the nuclear pore complex in ALS and FTD.

Applications of Molecular Barcoding

The concept of molecular barcoding is that each original DNA or RNA molecule is attached to a unique sequence barcode. Sequence reads having different barcodes represent different original molecules, while sequence reads having the same barcode are results of PCR duplication from one original molecule. Discover the latest research on molecular barcoding here.

Chronic Fatigue Syndrome

Chronic fatigue syndrome is a disease characterized by unexplained disabling fatigue; the pathology of which is incompletely understood. Discover the latest research on chronic fatigue syndrome here.

Evolution of Pluripotency

Pluripotency refers to the ability of a cell to develop into three primary germ cell layers of the embryo. This feed focuses on the mechanisms that underlie the evolution of pluripotency. Here is the latest research.

Position Effect Variegation

Position Effect Variagation occurs when a gene is inactivated due to its positioning near heterochromatic regions within a chromosome. Discover the latest research on Position Effect Variagation here.

STING Receptor Agonists

Stimulator of IFN genes (STING) are a group of transmembrane proteins that are involved in the induction of type I interferon that is important in the innate immune response. The stimulation of STING has been an active area of research in the treatment of cancer and infectious diseases. Here is the latest research on STING receptor agonists.

Microbicide

Microbicides are products that can be applied to vaginal or rectal mucosal surfaces with the goal of preventing, or at least significantly reducing, the transmission of sexually transmitted infections. Here is the latest research on microbicides.