Predicting Vibrational Spectroscopy for Flexible Molecules and Molecules with Non‐Idle Environments

Kirchner, Barbara; Blasius, Jan; Esser, Lars; Reckien, Werner

doi:10.1002/adts.202000223

Cited by 21 publications

(48 citation statements)

References 121 publications

(215 reference statements)

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Similarly, the peak at 1475 cm −1 is more intense in both calculated spectra than in the experimental spectrum. In this case, a shift to higher wavenumbers is observable which renders the scaling [ 100 ] of the peak locations difficult.…”

Section: Parameter Dependence Of the Calculated Spectramentioning

confidence: 99%

Benchmarking the Computational Costs and Quality of Vibrational Spectra from Ab Initio Simulations

Taherivardanjani¹,

Elfgen²,

Reckien³

et al. 2021

Advcd Theory and Sims

Self Cite

View full text Add to dashboard Cite

The scaling behavior of ab initio molecular dynamics simulations for the different size bulk systems of liquid methanol is presented and thereby the characteristics of every system performing on either a local compute cluster or a supercomputer are analyzed. Additionally, the influence of different parameters on the quality of the infrared and Raman spectra is investigated using different simulation frameworks, including time step, convergence criteria, density functional approximation, and basis set. Both the maximally localized Wannier functions and the radical Voronoi tessellation approaches are employed to evaluate vibrational spectra from the trajectories. The results of infrared and Raman spectra are classified in two frequency regions, 500 to 1600 cm−1 and 2500 to 4000 cm−1, in order to compare and discuss the experimental spectra and the results derived from ab initio molecular dynamics simulations comprehensively. The outcome of this study guides future experimental and theoretical researchers in order to acquire a profound perception into vibrational spectra, which evolves the way of elucidating molecular structure.

show abstract

Section: Parameter Dependence Of the Calculated Spectramentioning

confidence: 99%

Benchmarking the Computational Costs and Quality of Vibrational Spectra from Ab Initio Simulations

Taherivardanjani¹,

Elfgen²,

Reckien³

et al. 2021

Advcd Theory and Sims

Self Cite

View full text Add to dashboard Cite

show abstract

“…Another obstacle is the dynamical smearing of the vibrational features recorded experimentally, where the discrete structure of the spectral bands tends to be lost. These challenges were recognized by Kirchner and co-workers, resulting in the development of new methodologies for accurate predictions of the vibrational spectra of molten ILs via the use of AIMD simulations. − Further developments on this front can account for statistical averaging in complex molten-salt environments, as recently illustrated in ref . In the present work, we follow an alternative strategy by capitalizing from our knowledge of the crystal environment and provide a comprehensive multispectral analysis.…”

Section: Resultsmentioning

confidence: 99%

Spectroscopic Signatures of Hydrogen-Bonding Motifs in Protonic Ionic Liquid Systems: Insights from Diethylammonium Nitrate in the Solid State

et al. 2021

View full text Add to dashboard Cite

Diethylammonium nitrate, [N 0 0 2 2 ][NO 3 ], and its perdeuterated analogue, [N D D 2 2 ] [NO 3 ], were structurally characterized and studied by infrared, Raman, and inelastic neutron scattering (INS) spectroscopy. Using these experimental data along with state-of-the-art computational materials modeling, we report unambiguous spectroscopic signatures of hydrogen-bonding interactions between the two counterions. An exhaustive assignment of the spectral features observed with each technique has been provided, and a number of distinct modes related to NH···O dynamics have been identified. We put a particular emphasis on a detailed interpretation of the high-resolution, broadband INS experiments. In particular, the INS data highlight the importance of conformational degrees of freedom within the alkyl chains, a ubiquitous feature of ionic liquid (IL) systems. These findings also enable an in-depth physicochemical understanding of protonic IL systems, a first and necessary step to the tailoring of hydrogen-bonding networks in this important class of materials.

show abstract

“…In the mentioned study of (R)‐butan‐2‐ol 130 a temperature of 400 K has been applied to enhance the sampling, and the study compares results for the bulk and gas‐phase, showcasing the influence of intermolecular interactions on IR and VCD spectra. Such an exploration of the conformation space is most important in gas‐phase calculations, where no intermolecular energy exchange can mediate conformational changes, which are naturally present in bulk calculations.…”

Section: Types Of Spectroscopymentioning

confidence: 99%

“…Such an exploration of the conformation space is most important in gas‐phase calculations, where no intermolecular energy exchange can mediate conformational changes, which are naturally present in bulk calculations. As a result, an FPMD run in gas‐phase will tend only to sample a single conformer 130 . The group of Gaigeot studied flexible polypeptides in the gas‐phase extensively, computing, among others, IR spectra of a protonated polypeptide.…”

Section: Types Of Spectroscopymentioning

confidence: 99%

See 1 more Smart Citation

Vibrational spectroscopy by means of first‐principles molecular dynamics simulations

Ditler

Luber

2022

WIREs Comput Mol Sci

View full text Add to dashboard Cite

Vibrational spectroscopy is one of the most important experimental techniques for the characterization of molecules and materials. Spectroscopic signatures retrieved in experiments are not always easy to explain in terms of the structure and dynamics of the studied samples. Computational studies are a crucial tool for helping to understand and predict experimental results. Molecular dynamics simulations have emerged as an attractive method for the simulation of vibrational spectra because they explicitly treat the vibrational motion present in the compound under study, in particular in large and condensed systems, subject to complex intramolecular and intermolecular interactions. In this context, first‐principles molecular dynamics (FPMD) has been proven to provide an accurate realistic description of many compounds. This review article summarizes the field of vibrational spectroscopy by means of FPDM and highlights recent advances made such as the simulation of Infrared, vibrational circular dichroism, Raman, Raman optical activity, sum frequency generation, and nonlinear spectroscopies. This article is categorized under: Electronic Structure Theory > Ab Initio Electronic Structure Methods Theoretical and Physical Chemistry > Spectroscopy Molecular and Statistical Mechanics > Molecular Mechanics Electronic Structure Theory > Density Functional Theory

show abstract

Predicting Vibrational Spectroscopy for Flexible Molecules and Molecules with Non‐Idle Environments

Cited by 21 publications

References 121 publications

Benchmarking the Computational Costs and Quality of Vibrational Spectra from Ab Initio Simulations

Benchmarking the Computational Costs and Quality of Vibrational Spectra from Ab Initio Simulations

Spectroscopic Signatures of Hydrogen-Bonding Motifs in Protonic Ionic Liquid Systems: Insights from Diethylammonium Nitrate in the Solid State

Vibrational spectroscopy by means of first‐principles molecular dynamics simulations

Contact Info

Product

Resources

About