The first microsolvation step for furans: New experiments and benchmarking strategies

被引：37

作者：

Gottschalk, Hannes C. ^{[1
]}

Poblotzki, Anja ^{[1
]}

Fatima, Mariyam ^{[2
]}

Obenchain, Daniel A. ^{[2
]}

Perez, Cristobal ^{[2
]}

Antony, Jens ^{[3
]}

Auer, Alexander A. ^{[4
]}

Baptista, Leonardo ^{[5
]}

Benoit, David M. ^{[6
,7
]}

Bistoni, Giovanni ^{[4
]}

Bohle, Fabian ^{[3
]}

Dahmani, Rahma ^{[8
]}

Firaha, Dzmitry ^{[9
]}

Grimme, Stefan ^{[3
]}

Hansen, Andreas ^{[3
]}

Harding, Michael E. ^{[10
]}

Hochlaf, Majdi ^{[8
]}

Holzer, Christof ^{[11
]}

Jansen, Georg ^{[12
]}

Klopper, Wim ^{[11
]}

Kopp, Wassja A. ^{[9
]}

Kroeger, Leif C. ^{[9
]}

Leonhard, Kai ^{[9
]}

Al-Mogren, Muneerah Mogren ^{[13
]}

Mouhib, Halima ^{[8
]}

Neese, Frank ^{[4
]}

Pereira, X. N. ^{[5
]}

Prakash, Muthuramalingam ^{[14
]}

Ulusoy, Inga S. ^{[15
]}

Mata, Ricardo A. ^{[1
]}

Suhm, Martin A. ^{[1
]}

Schnell, Melanie ^{[2
]}

机构：

[1] Univ Gottingen, Inst Physikal Chem, Tammannstr 6, D-37077 Gottingen, Germany

[2] DESY, Notkestr 85, D-22607 Hamburg, Germany

[3] Univ Bonn, Mulliken Ctr Theoret Chem, Beringstr 4, D-53115 Bonn, Germany

[4] Max Planck Inst Chem Energy Convers, Dept Mol Theory & Spect, Stiftstr 34-36, D-45470 Mulheim, Germany

[5] Univ Estado Rio de Janeiro, Fac Tecnol, Dept Quim & Ambiental, Resende, RJ, Brazil

[6] Univ Hull, EA Milne Ctr Astrophys, Dept Phys & Math, Kingston Upon Hull HU6 7RX, N Humberside, England

[7] Univ Hull, GW Gray Ctr Adv Mat Chem, Kingston Upon Hull HU6 7RX, N Humberside, England

[8] Univ Gustave Eiffel, COSYS LISIS, 5 Blvd Descartes, F-77454 Marne La Vallee, France

[9] Rhein Westfal TH Aachen, Lehrstuhl Tech Thermodynam, D-52062 Aachen, Germany

[10] Karlsruhe Inst Technol, Inst Nanotechnol, Hermann von Helm Holtz Pl 1, D-76344 Eggenstein Leopoldshafen, Germany

[11] Karlsruhe Inst Technol KIT, Inst Phys Chem, Theoret Chem Grp, POB 6980, D-76049 Karlsruhe, Germany

[12] Univ Duisburg Essen, Fak Chem, Univ Str 5, D-45117 Essen, Germany

[13] King Saud Univ, Fac Sci, Chem Dept, POB 2455, Riyadh 11451, Saudi Arabia

[14] SRM Inst Sci & Technol, Dept Chem, Kattankulathur 603203, Tamil Nadu, India

[15] Heidelberg Univ, Inst Phys Chem, Theoret Chem, Neuenheimer Feld 229, D-69120 Heidelberg, Germany

来源：

JOURNAL OF CHEMICAL PHYSICS | 2020年 / 152卷 / 16期

关键词：

DENSITY-FUNCTIONAL THEORY; INTERNAL-ROTATION SPLITTINGS; ADAPTED PERTURBATION-THEORY; CENTER-DOT-PI; MICROWAVE SPECTROSCOPY; GENERAL PROGRAM; WAVE-FUNCTION; AB-INITIO; WATER; PREDICTION;

D O I：

10.1063/5.0004465

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The site-specific first microsolvation step of furan and some of its derivatives with methanol is explored to benchmark the ability of quantum-chemical methods to describe the structure, energetics, and vibrational spectrum at low temperature. Infrared and microwave spectra in supersonic jet expansions are used to quantify the docking preference and some relevant quantum states of the model complexes. Microwave spectroscopy strictly rules out in-plane docking of methanol as opposed to the top coordination of the aromatic ring. Contrasting comparison strategies, which emphasize either the experimental or the theoretical input, are explored. Within the harmonic approximation, only a few composite computational approaches are able to achieve a satisfactory performance. Deuteration experiments suggest that the harmonic treatment itself is largely justified for the zero-point energy, likely and by design due to the systematic cancellation of important anharmonic contributions between the docking variants. Therefore, discrepancies between experiment and theory for the isomer abundance are tentatively assigned to electronic structure deficiencies, but uncertainties remain on the nuclear dynamics side. Attempts to include anharmonic contributions indicate that for systems of this size, a uniform treatment of anharmonicity with systematically improved performance is not yet in sight.

引用

页数：17

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