{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,2,23]],"date-time":"2026-02-23T12:01:48Z","timestamp":1771848108517,"version":"3.50.1"},"reference-count":109,"publisher":"AIP Publishing","issue":"8","license":[{"start":{"date-parts":[[2026,2,20]],"date-time":"2026-02-20T00:00:00Z","timestamp":1771545600000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"DOI":"10.13039\/501100004359","name":"Vetenskapsr\u00e5det","doi-asserted-by":"publisher","award":["2020-05403"],"award-info":[{"award-number":["2020-05403"]}],"id":[{"id":"10.13039\/501100004359","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100003748","name":"Svenska S\u00e4llskapet f\u00f6r Medicinsk Forskning","doi-asserted-by":"publisher","award":["S20-0156"],"award-info":[{"award-number":["S20-0156"]}],"id":[{"id":"10.13039\/501100003748","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100009759","name":"Harald och Greta Jeanssons Stiftelse","doi-asserted-by":"publisher","award":["J2021-0114"],"award-info":[{"award-number":["J2021-0114"]}],"id":[{"id":"10.13039\/501100009759","id-type":"DOI","asserted-by":"publisher"}]},{"name":"National Academic Infrastructure for Supercomputing in Sweden","award":["NAISS 2025\/5-307"],"award-info":[{"award-number":["NAISS 2025\/5-307"]}]},{"name":"National Academic Infrastructure for Supercomputing in Sweden","award":["NAISS 2025\/6-203"],"award-info":[{"award-number":["NAISS 2025\/6-203"]}]},{"name":"National Academic Infrastructure for Supercomputing in Sweden","award":["NAISS 2025\/6-39"],"award-info":[{"award-number":["NAISS 2025\/6-39"]}]},{"name":"National Academic Infrastructure for Supercomputing in Sweden","award":["UPPMAX 2025\/2-237"],"award-info":[{"award-number":["UPPMAX 2025\/2-237"]}]},{"name":"National Academic Infrastructure for Supercomputing in Sweden","award":["NAISS 2022-06725"],"award-info":[{"award-number":["NAISS 2022-06725"]}]}],"content-domain":{"domain":["pubs.aip.org"],"crossmark-restriction":true},"short-container-title":[],"published-print":{"date-parts":[[2026,2,28]]},"abstract":"<jats:p>Two-dimensional infrared (2DIR) spectroscopy captures vibrational correlations on femtosecond timescales, offering direct insights into hydrogen(H)-bonding dynamics and other ultrafast molecular processes. However, interpreting these spectra requires simulations that accurately describe solute\u2013solvent interactions over realistic timescales and system sizes. While classical approaches using empirical frequency maps are common, ab\u00a0initio molecular dynamics (AIMD) offers a more rigorous alternative by treating dynamics and vibrational frequencies on a consistent theoretical level. The primary drawback of AIMD is its high computational cost, which typically limits simulations to short trajectories. Here, we introduce a hybrid strategy that combines linear-scaling density functional theory (LS-DFT) with a machine-learned (ML) interatomic potential. We use short LS-DFT simulations to generate reference energies, forces, and electron-density-derived dipole moments, which then serve as training data for a DeepMD model. The resulting ML potential allows nanosecond-scale dynamics at a fraction of the ab\u00a0initio cost. We demonstrate this approach for N-methylacetamide in methanol, a model system known to form distinct H-bonded subpopulations. A key advantage of our method is that it bypasses the need for empirical frequency maps. Instead, molecular dipoles are learned directly from the electron density, and instantaneous vibrational frequencies are calculated from stable numerical Hessians. The resulting linear and 2DIR spectra show excellent agreement with experiment, accurately reproducing the characteristic doublet structure of the amide I band. This framework provides a practical and accurate route to simulating vibrational spectra at the AIMD level of theory for a wide range of IR-active solutes and H-bonded complexes.<\/jats:p>","DOI":"10.1063\/5.0303526","type":"journal-article","created":{"date-parts":[[2026,2,23]],"date-time":"2026-02-23T11:10:53Z","timestamp":1771845053000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":0,"title":["Two-dimensional infrared spectroscopy of solute\u2013solvent complexes from linear-scaling DFT and machine learning"],"prefix":"10.1063","volume":"164","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-1567-9514","authenticated-orcid":false,"given":"Micha\u0142","family":"Maj","sequence":"first","affiliation":[{"name":"Department of Chemistry-\u00c5ngstr\u00f6m Laboratory, Uppsala University , SE-75120 Uppsala,","place":["Sweden"]}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"317","published-online":{"date-parts":[[2026,2,23]]},"reference":[{"key":"2026022306104828300_c1","doi-asserted-by":"publisher","first-page":"1331","DOI":"10.1021\/cr078377b","article-title":"Coherent two-dimensional optical spectroscopy","volume":"108","year":"2008","journal-title":"Chem. Rev."},{"key":"2026022306104828300_c2","volume-title":"Concepts and Methods of 2D Infrared Spectroscopy","year":"2011"},{"key":"2026022306104828300_c3","doi-asserted-by":"publisher","first-page":"82","DOI":"10.1038\/s42004-024-01170-x","article-title":"Chasing weakly-bound biological water in aqueous environment near the peptide backbone by ultrafast 2D infrared spectroscopy","volume":"7","year":"2024","journal-title":"Commun. Chem."},{"key":"2026022306104828300_c4","doi-asserted-by":"publisher","first-page":"10726","DOI":"10.1021\/acs.chemrev.6b00582","article-title":"Watching proteins wiggle: Mapping structures with two-dimensional infrared spectroscopy","volume":"117","year":"2017","journal-title":"Chem. Rev."},{"key":"2026022306104828300_c5","doi-asserted-by":"publisher","first-page":"064501","DOI":"10.1063\/5.0041270","article-title":"On the role of hydrogen-bond exchanges in the spectral diffusion of water","volume":"154","year":"2021","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c6","doi-asserted-by":"publisher","first-page":"e202416091","DOI":"10.1002\/anie.202416091","article-title":"Fast collective hydrogen-bond dynamics in hexafluoroisopropanol related to its chemical activity","volume":"63","year":"2024","journal-title":"Angew. Chem., Int. Ed."},{"key":"2026022306104828300_c7","doi-asserted-by":"publisher","first-page":"160","DOI":"10.1126\/science.abe1951","article-title":"Crossover from hydrogen to chemical bonding","volume":"371","year":"2021","journal-title":"Science"},{"key":"2026022306104828300_c8","doi-asserted-by":"publisher","first-page":"6520","DOI":"10.1021\/jp0100093","article-title":"Heterodyned two-dimensional infrared spectroscopy of solvent-dependent conformations of acetylproline-NH2","volume":"105","year":"2001","journal-title":"J.\u00a0Phys. Chem. B"},{"key":"2026022306104828300_c9","doi-asserted-by":"publisher","first-page":"11316","DOI":"10.1021\/jp001546a","article-title":"Structure determination of trialanine in water using polarization sensitive two-dimensional vibrational spectroscopy","volume":"104","year":"2000","journal-title":"J.\u00a0Phys. Chem. B"},{"key":"2026022306104828300_c10","doi-asserted-by":"publisher","first-page":"e2206400119","DOI":"10.1073\/pnas.2206400119","article-title":"Vibrational couplings between protein and cofactor in bacterial phytochrome Agp1 revealed by 2D-IR spectroscopy","volume":"119","year":"2022","journal-title":"Proc. Natl. Acad. Sci. U. S. A."},{"key":"2026022306104828300_c11","doi-asserted-by":"publisher","first-page":"124501","DOI":"10.1063\/1.3212618","article-title":"Intermolecular vibrational energy exchange directly probed with ultrafast two dimensional infrared spectroscopy","volume":"131","year":"2009","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c12","doi-asserted-by":"publisher","first-page":"14209","DOI":"10.1073\/pnas.0700560104","article-title":"A relaxation-assisted 2D IR spectroscopy method","volume":"104","year":"2007","journal-title":"Proc. Natl. Acad. Sci. U. S. A."},{"key":"2026022306104828300_c13","doi-asserted-by":"publisher","first-page":"11063","DOI":"10.1021\/jp2066315","article-title":"Structure dependent energy transport: Relaxation-assisted 2DIR measurements and theoretical studies","volume":"115","year":"2011","journal-title":"J.\u00a0Phys. Chem. B"},{"key":"2026022306104828300_c14","doi-asserted-by":"publisher","first-page":"224201","DOI":"10.1063\/5.0153760","article-title":"Inhibition of vibrational energy flow within an aromatic scaffold via heavy atom effect","volume":"158","year":"2023","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c15","doi-asserted-by":"publisher","first-page":"761","DOI":"10.1021\/acsphyschemau.4c00073","article-title":"Two-dimensional infrared spectroscopy resolves the vibrational landscape in donor\u2013bridge\u2013acceptor complexes with site-specific isotopic labeling","volume":"4","year":"2024","journal-title":"ACS Phys. Chem. Au"},{"key":"2026022306104828300_c16","doi-asserted-by":"publisher","first-page":"11185","DOI":"10.1073\/pnas.0504865102","article-title":"Chemical exchange 2D IR of hydrogen-bond making and breaking","volume":"102","year":"2005","journal-title":"Proc. Natl. Acad. Sci. U. S. A."},{"key":"2026022306104828300_c17","doi-asserted-by":"publisher","first-page":"21","DOI":"10.1146\/annurev-physchem-073108-112712","article-title":"Dynamics of liquids, molecules, and proteins measured with ultrafast 2D IR vibrational echo chemical exchange spectroscopy","volume":"60","year":"2009","journal-title":"Annu. Rev. Phys. Chem."},{"key":"2026022306104828300_c18","first-page":"MC4","volume-title":"Ultrafast chemical exchange 2D IR spectroscopy","year":"2006"},{"key":"2026022306104828300_c19","doi-asserted-by":"publisher","first-page":"7878","DOI":"10.1021\/acs.jpclett.9b03144","article-title":"Ultrafast chemical exchange dynamics of hydrogen bonds observed via isonitrile infrared sensors: Implications for biomolecular studies","volume":"10","year":"2019","journal-title":"J.\u00a0Phys. Chem. Lett."},{"key":"2026022306104828300_c20","doi-asserted-by":"publisher","first-page":"375","DOI":"10.1073\/pnas.0811489106","article-title":"Ion\u2013water hydrogen-bond switching observed with 2D IR vibrational echo chemical exchange spectroscopy","volume":"106","year":"2009","journal-title":"Proc. Natl. Acad. Sci. U. S. A."},{"key":"2026022306104828300_c21","doi-asserted-by":"publisher","first-page":"094505","DOI":"10.1063\/1.3079609","article-title":"Vibrational solvatochromism and electrochromism: Coarse-grained models and their relationships","volume":"130","year":"2009","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c22","doi-asserted-by":"publisher","first-page":"7152","DOI":"10.1021\/acs.chemrev.9b00813","article-title":"Vibrational spectroscopic map, vibrational spectroscopy, and intermolecular interaction","volume":"120","year":"2020","journal-title":"Chem. Rev."},{"key":"2026022306104828300_c23","doi-asserted-by":"publisher","first-page":"143","DOI":"10.1016\/j.chemphys.2007.06.043","article-title":"Are water simulation models consistent with steady-state and ultrafast vibrational spectroscopy experiments?","volume":"341","year":"2007","journal-title":"Chem. Phys."},{"key":"2026022306104828300_c24","doi-asserted-by":"publisher","first-page":"065001","DOI":"10.1088\/1367-2630\/12\/6\/065001","article-title":"Direct quantum mechanical\/molecular mechanical simulations of two-dimensional vibrational responses: N-methylacetamide in water","volume":"12","year":"2010","journal-title":"New J. Phys."},{"key":"2026022306104828300_c25","doi-asserted-by":"publisher","first-page":"134506","DOI":"10.1063\/1.2844787","article-title":"Nitrile and thiocyanate IR probes: Quantum chemistry calculation studies and multivariate least-square fitting analysis","volume":"128","year":"2008","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c26","doi-asserted-by":"publisher","first-page":"114307","DOI":"10.1063\/1.4751477","article-title":"Vibrational solvatochromism and electrochromism. II. Multipole analysis","volume":"137","year":"2012","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c27","doi-asserted-by":"publisher","first-page":"12658","DOI":"10.1039\/c0cp00214c","article-title":"Vibrational solvatochromism and electrochromism of cyanide, thiocyanate, and azide anions in water","volume":"12","year":"2010","journal-title":"Phys. Chem. Chem. Phys."},{"key":"2026022306104828300_c28","doi-asserted-by":"publisher","first-page":"014113","DOI":"10.1063\/5.0242857","article-title":"Solvatochromic charge model of isonitrile probes for investigating hydrogen-bond dynamics with 2DIR spectroscopy","volume":"162","year":"2025","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c29","doi-asserted-by":"publisher","first-page":"1406","DOI":"10.1021\/ct401118k","article-title":"Multiscale free energy simulations: An efficient method for connecting classical MD simulations to QM or QM\/MM free energies using non-Boltzmann Bennett reweighting schemes","volume":"10","year":"2014","journal-title":"J.\u00a0Chem. Theory Comput."},{"key":"2026022306104828300_c30","doi-asserted-by":"publisher","first-page":"6850","DOI":"10.1021\/acs.jctc.9b00698","article-title":"Machine learning for vibrational spectroscopic maps","volume":"15","year":"2019","journal-title":"J.\u00a0Chem. Theory Comput."},{"key":"2026022306104828300_c31","doi-asserted-by":"publisher","first-page":"19071","DOI":"10.1021\/jacs.0c06530","article-title":"A machine learning protocol for predicting protein infrared spectra","volume":"142","year":"2020","journal-title":"J.\u00a0Am. Chem. Soc."},{"key":"2026022306104828300_c32","doi-asserted-by":"publisher","first-page":"3750","DOI":"10.1002\/anie.200802644","article-title":"Coherent multidimensional vibrational spectroscopy of biomolecules: Concepts, simulations, and challenges","volume":"48","year":"2009","journal-title":"Angew. Chem., Int. Ed."},{"key":"2026022306104828300_c33","doi-asserted-by":"publisher","first-page":"9839641","DOI":"10.1155\/2018\/9839641","article-title":"Computational methods for ab\u00a0initio molecular dynamics","volume":"2018","journal-title":"Adv. Chem."},{"key":"2026022306104828300_c34","doi-asserted-by":"publisher","first-page":"6654","DOI":"10.1073\/pnas.0500193102","article-title":"Ab initio molecular dynamics: Concepts, recent developments, and future trends","volume":"102","year":"2005","journal-title":"Proc. Natl. Acad. Sci. U. S. A."},{"key":"2026022306104828300_c35","doi-asserted-by":"publisher","first-page":"164103","DOI":"10.1063\/5.0046930","article-title":"Ab initio molecular dynamics on quantum computers","volume":"154","year":"2021","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c36","doi-asserted-by":"publisher","first-page":"24685","DOI":"10.1039\/c4cp03828b","article-title":"Resolving the anomalous infrared spectrum of the MeCN\u2013HCl molecular cluster using ab\u00a0initio molecular dynamics","volume":"16","year":"2014","journal-title":"Phys. Chem. Chem. Phys."},{"key":"2026022306104828300_c37","doi-asserted-by":"publisher","first-page":"1902765","DOI":"10.1002\/adma.201902765","article-title":"Machine learning interatomic potentials as emerging tools for materials science","volume":"31","year":"2019","journal-title":"Adv. Mater."},{"key":"2026022306104828300_c38","doi-asserted-by":"publisher","first-page":"1085","DOI":"10.1103\/revmodphys.71.1085","article-title":"Linear scaling electronic structure methods","volume":"71","year":"1999","journal-title":"Rev. Mod. Phys."},{"key":"2026022306104828300_c39","doi-asserted-by":"publisher","first-page":"044502","DOI":"10.1063\/1.2148409","article-title":"A transferable electrostatic map for solvation effects on amide I vibrations and its application to linear and two-dimensional spectroscopy","volume":"124","year":"2006","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c40","doi-asserted-by":"publisher","first-page":"1477","DOI":"10.1063\/1.1633549","article-title":"Non-Gaussian statistics of amide I mode frequency fluctuation of N-methylacetamide in methanol solution: Linear and nonlinear vibrational spectra","volume":"120","year":"2004","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c41","doi-asserted-by":"publisher","first-page":"772","DOI":"10.1021\/ct050029z","article-title":"Infrared spectroscopy of N-Methylacetamide revisited by ab\u00a0initio molecular dynamics simulations","volume":"1","year":"2005","journal-title":"J.\u00a0Chem. Theory Comput."},{"key":"2026022306104828300_c42","doi-asserted-by":"publisher","first-page":"12868","DOI":"10.1039\/c7cp00690j","article-title":"Probing the dynamics of N-methylacetamide in methanol via ab\u00a0initio molecular dynamics","volume":"19","year":"2017","journal-title":"Phys. Chem. Chem. Phys."},{"key":"2026022306104828300_c43","doi-asserted-by":"publisher","first-page":"1113","DOI":"10.1002\/(sici)1096-987x(19970715)18:9&lt;1113::aid-jcc1&gt;3.0.co;2-u","article-title":"Voronoi cell: New method for allocation of space among atoms: Elimination of avoidable errors in calculation of atomic volume and density","volume":"18","year":"1997","journal-title":"J.\u00a0Comput. Chem."},{"key":"2026022306104828300_c44","volume-title":"Principles of Nonlinear Optical Spectroscopy","year":"1995"},{"key":"2026022306104828300_c45","volume-title":"Two-Dimensional Optical Spectroscopy","year":"2009","edition":"1"},{"key":"2026022306104828300_c46","doi-asserted-by":"publisher","first-page":"12974","DOI":"10.1021\/jp960669l","article-title":"Density functional theory of electronic structure","volume":"100","year":"1996","journal-title":"J.\u00a0Phys. Chem."},{"key":"2026022306104828300_c47","doi-asserted-by":"publisher","first-page":"20120488","DOI":"10.1098\/rsta.2012.0488","article-title":"Density functional theory across chemistry, physics and biology","volume":"372","year":"2014","journal-title":"Philos. Trans. R. Soc., A"},{"key":"2026022306104828300_c48","doi-asserted-by":"publisher","first-page":"A1133","DOI":"10.1103\/physrev.140.a1133","article-title":"Self-consistent equations including exchange and correlation effects","volume":"140","year":"1965","journal-title":"Phys. Rev."},{"key":"2026022306104828300_c49","doi-asserted-by":"publisher","first-page":"163","DOI":"10.1016\/s0301-0104(03)00118-6","article-title":"An approach to reduce the computational effort in accurate DFT calculations","volume":"290","year":"2003","journal-title":"Chem. Phys."},{"key":"2026022306104828300_c50","doi-asserted-by":"publisher","first-page":"11635","DOI":"10.1073\/pnas.0505436102","article-title":"Nearsightedness of electronic matter","volume":"102","year":"2005","journal-title":"Proc. Natl. Acad. Sci. U. S. A."},{"key":"2026022306104828300_c51","doi-asserted-by":"publisher","first-page":"036503","DOI":"10.1088\/0034-4885\/75\/3\/036503","article-title":"Methods in electronic structure calculations","volume":"75","year":"2012","journal-title":"Rep. Prog. Phys."},{"key":"2026022306104828300_c52","doi-asserted-by":"publisher","first-page":"084114","DOI":"10.1063\/1.1853378","article-title":"Comparison of two genres for linear scaling in density functional theory: Purification and density matrix minimization methods","volume":"122","year":"2005","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c53","doi-asserted-by":"publisher","first-page":"164112","DOI":"10.1063\/5.0005074","article-title":"Large scale and linear scaling DFT with the CONQUEST code","volume":"152","year":"2020","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c54","doi-asserted-by":"publisher","first-page":"102920","DOI":"10.1016\/j.parco.2022.102920","article-title":"Towards electronic structure-based ab-initio molecular dynamics simulations with hundreds of millions of atoms","volume":"111","year":"2022","journal-title":"Parallel Comput."},{"key":"2026022306104828300_c55","doi-asserted-by":"publisher","first-page":"3865","DOI":"10.1103\/physrevlett.77.3865","article-title":"Generalized gradient approximation made simple","volume":"77","year":"1996","journal-title":"Phys. Rev. Lett."},{"key":"2026022306104828300_c56","doi-asserted-by":"publisher","first-page":"3098","DOI":"10.1103\/physreva.38.3098","article-title":"Density-functional exchange-energy approximation with correct asymptotic behavior","volume":"38","year":"1988","journal-title":"Phys. Rev. A"},{"key":"2026022306104828300_c57","doi-asserted-by":"publisher","first-page":"785","DOI":"10.1103\/physrevb.37.785","article-title":"Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density","volume":"37","year":"1988","journal-title":"Phys. Rev. B"},{"key":"2026022306104828300_c58","doi-asserted-by":"publisher","first-page":"024112","DOI":"10.1063\/5.0208103","article-title":"Efficient all-electron hybrid density functionals for atomistic simulations beyond 10 000 atoms","volume":"161","year":"2024","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c59","doi-asserted-by":"publisher","first-page":"112396","DOI":"10.1016\/j.commatsci.2023.112396","article-title":"Linear-scaling density functional theory (DFT) simulations of point, Frenkel and Schottky defects in CeO2","volume":"229","year":"2023","journal-title":"Comput. Mater. Sci."},{"key":"2026022306104828300_c60","doi-asserted-by":"publisher","first-page":"2007","DOI":"10.1021\/ci200217w","article-title":"TRAVIS\u2014A free analyzer and visualizer for Monte Carlo and molecular dynamics trajectories","volume":"51","year":"2011","journal-title":"J.\u00a0Chem. Inf. Model."},{"key":"2026022306104828300_c61","doi-asserted-by":"publisher","first-page":"3207","DOI":"10.1039\/c4cp05272b","article-title":"Voronoi dipole moments for the simulation of bulk phase vibrational spectra","volume":"17","year":"2015","journal-title":"Phys. Chem. Chem. Phys."},{"key":"2026022306104828300_c62","doi-asserted-by":"publisher","first-page":"4137","DOI":"10.3390\/molecules30204137","article-title":"Polarizabilities of atoms in molecules: Choice of the partitioning scheme and applications for secondary interactions","volume":"30","year":"2025","journal-title":"Molecules"},{"key":"2026022306104828300_c63","doi-asserted-by":"publisher","first-page":"1875","DOI":"10.3390\/molecules26071875","article-title":"Optimized atomic partial charges and radii defined by radical Voronoi tessellation of bulk phase simulations","volume":"26","year":"2021","journal-title":"Molecules"},{"key":"2026022306104828300_c64","doi-asserted-by":"publisher","first-page":"189","DOI":"10.1002\/jcc.10351","article-title":"Voronoi deformation density (VDD) charges: Assessment of the Mulliken, Bader, Hirshfeld, Weinhold, and VDD methods for charge analysis","volume":"25","year":"2004","journal-title":"J.\u00a0Comput. Chem."},{"key":"2026022306104828300_c65","doi-asserted-by":"publisher","first-page":"3409","DOI":"10.1021\/acs.jpclett.7b01616","article-title":"Computing bulk phase Raman optical activity spectra from ab\u00a0initio molecular dynamics simulations","volume":"8","year":"2017","journal-title":"J.\u00a0Phys. Chem. Lett."},{"key":"2026022306104828300_c66","doi-asserted-by":"publisher","first-page":"170901","DOI":"10.1063\/1.4966192","article-title":"Perspective: Machine learning potentials for atomistic simulations","volume":"145","year":"2016","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c67","doi-asserted-by":"publisher","first-page":"178","DOI":"10.1016\/j.cpc.2018.03.016","article-title":"DeePMD-kit: A deep learning package for many-body potential energy representation and molecular dynamics","volume":"228","year":"2018","journal-title":"Comput. Phys. Commun."},{"key":"2026022306104828300_c68","doi-asserted-by":"publisher","first-page":"054801","DOI":"10.1063\/5.0155600","article-title":"DeePMD-kit v2: A software package for deep potential models","volume":"159","year":"2023","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c69","doi-asserted-by":"publisher","first-page":"4375","DOI":"10.1021\/acs.jctc.5c00340","article-title":"DeePMD-kit v3: A multiple-backend framework for machine learning potentials","volume":"21","year":"2025","journal-title":"J.\u00a0Chem. Theory Comput."},{"key":"2026022306104828300_c70","first-page":"992","volume-title":"SchNet: A continuous-filter convolutional neural network for modeling quantum interactions","year":"2017"},{"key":"2026022306104828300_c71","doi-asserted-by":"publisher","first-page":"10073","DOI":"10.1021\/acs.chemrev.1c00022","article-title":"Gaussian process regression for materials and molecules","volume":"121","year":"2021","journal-title":"Chem. Rev."},{"key":"2026022306104828300_c72","doi-asserted-by":"publisher","first-page":"024112","DOI":"10.1103\/physrevb.100.024112","article-title":"Optimizing many-body atomic descriptors for enhanced computational performance of machine learning based interatomic potentials","volume":"100","year":"2019","journal-title":"Phys. Rev. B"},{"key":"2026022306104828300_c73","article-title":"End-to-end symmetry preserving inter-atomic potential energy model for finite and extended systems","volume-title":"Advances in Neural Information Processing Systems","year":"2018"},{"key":"2026022306104828300_c74","doi-asserted-by":"publisher","first-page":"035101","DOI":"10.1063\/1.2426344","article-title":"Computation of the amide I band of polypeptides and proteins using a partial Hessian approach","volume":"126","year":"2007","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c75","doi-asserted-by":"publisher","first-page":"174505","DOI":"10.1063\/1.3409561","article-title":"On the calculation of rotational anisotropy decay, as measured by ultrafast polarization-resolved vibrational pump-probe experiments","volume":"132","year":"2010","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c76","doi-asserted-by":"publisher","first-page":"9496","DOI":"10.1063\/1.465484","article-title":"Two-dimensional femtosecond vibrational spectroscopy of liquids","volume":"99","year":"1993","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c77","doi-asserted-by":"publisher","first-page":"100901","DOI":"10.1063\/1.5083966","article-title":"Theory of coherent two-dimensional vibrational spectroscopy","volume":"150","year":"2019","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c78","doi-asserted-by":"publisher","first-page":"5258","DOI":"10.1021\/jp0219247","article-title":"Coherent 2D IR spectroscopy: Molecular structure and dynamics in solution","volume":"107","year":"2003","journal-title":"J.\u00a0Phys. Chem. A"},{"key":"2026022306104828300_c79","doi-asserted-by":"publisher","first-page":"1100","DOI":"10.1143\/jpsj.17.1100","article-title":"Generalized cumulant expansion method","volume":"17","year":"1962","journal-title":"J.\u00a0Phys. Soc. Jpn."},{"key":"2026022306104828300_c80","doi-asserted-by":"publisher","first-page":"044513","DOI":"10.1063\/1.1961472","article-title":"Pronounced non-Condon effects in the ultrafast infrared spectroscopy of water","volume":"123","year":"2005","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c81","doi-asserted-by":"publisher","first-page":"124503","DOI":"10.1063\/1.2772269","article-title":"Frequency-frequency correlation functions and apodization in two-dimensional infrared vibrational echo spectroscopy: A new approach","volume":"127","year":"2007","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c82","doi-asserted-by":"publisher","first-page":"4424","DOI":"10.1063\/1.1389844","article-title":"Nonlinear response functions for the three-dimensional spectroscopies","volume":"115","year":"2001","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c83","doi-asserted-by":"publisher","first-page":"224507","DOI":"10.1063\/1.2801538","article-title":"Liquid methanol Monte Carlo simulations with a refined potential which includes polarizability, nonadditivity, and intramolecular relaxation","volume":"127","year":"2007","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c84","doi-asserted-by":"publisher","first-page":"137","DOI":"10.1016\/s0301-0104(01)00224-5","article-title":"Hydrogen-bond lifetime measured by time-resolved 2D-IR spectroscopy: N-methylacetamide in methanol","volume":"266","year":"2001","journal-title":"Chem. Phys."},{"key":"2026022306104828300_c85","doi-asserted-by":"publisher","first-page":"1157","DOI":"10.1002\/jcc.20035","article-title":"Development and testing of a general amber force field","volume":"25","year":"2004","journal-title":"J.\u00a0Comput. Chem."},{"key":"2026022306104828300_c86","doi-asserted-by":"publisher","first-page":"332","DOI":"10.1021\/je00037a032","article-title":"Binary liquid mixture viscosities and densities","volume":"29","year":"1984","journal-title":"J.\u00a0Chem. Eng. Data"},{"key":"2026022306104828300_c87","doi-asserted-by":"publisher","first-page":"2102","DOI":"10.1039\/tf9656102102","article-title":"Adiabatic compressibilities of binary liquid mixtures","volume":"61","year":"1965","journal-title":"Trans. Faraday Soc."},{"key":"2026022306104828300_c88","doi-asserted-by":"publisher","first-page":"15","DOI":"10.1002\/wcms.1159","article-title":"cp2k: Atomistic simulations of condensed matter systems","volume":"4","year":"2014","journal-title":"Wiley Interdiscip. Rev.: Comput. Mol. Sci."},{"key":"2026022306104828300_c89","doi-asserted-by":"publisher","first-page":"154104","DOI":"10.1063\/1.3382344","article-title":"A consistent and accurate ab\u00a0initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu","volume":"132","year":"2010","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c90","doi-asserted-by":"publisher","first-page":"114105","DOI":"10.1063\/1.2770708","article-title":"Gaussian basis sets for accurate calculations on molecular systems in gas and condensed phases","volume":"127","year":"2007","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c91","doi-asserted-by":"publisher","first-page":"1703","DOI":"10.1103\/physrevb.54.1703","article-title":"Separable dual-space Gaussian pseudopotentials","volume":"54","year":"1996","journal-title":"Phys. Rev. B"},{"key":"2026022306104828300_c92","doi-asserted-by":"publisher","first-page":"1159","DOI":"10.1080\/00268979909483060","article-title":"The structure of liquid methanol revisited: A neutron diffraction experiment at \u201380 \u00b0and +25 \u00b0C","volume":"96","year":"1999","journal-title":"Mol. Phys."},{"key":"2026022306104828300_c93","doi-asserted-by":"publisher","first-page":"94","DOI":"10.1038\/s41524-024-01278-7","article-title":"Pretraining of attention-based deep learning potential model for molecular simulation","volume":"10","year":"2024","journal-title":"npj Comput. Mater."},{"key":"2026022306104828300_c94","doi-asserted-by":"publisher","first-page":"107206","DOI":"10.1016\/j.cpc.2020.107206","article-title":"DP-GEN: A concurrent learning platform for the generation of reliable deep learning based potential energy models","volume":"253","year":"2020","journal-title":"Comput. Phys. Commun."},{"key":"2026022306104828300_c95","doi-asserted-by":"publisher","first-page":"108171","DOI":"10.1016\/j.cpc.2021.108171","article-title":"LAMMPS\u2014A flexible simulation tool for particle-based materials modeling at the atomic, meso, and continuum scales","volume":"271","year":"2022","journal-title":"Comput. Phys. Commun."},{"key":"2026022306104828300_c96","doi-asserted-by":"publisher","first-page":"1359","DOI":"10.1142\/s0218127401002766","article-title":"Time-frequency analysis of classical trajectories of polyatomic molecules","volume":"11","year":"2001","journal-title":"Int. J. Bifurcation Chaos"},{"key":"2026022306104828300_c97","doi-asserted-by":"publisher","first-page":"18973","DOI":"10.1021\/jp0603334","article-title":"The anharmonic vibrational potential and relaxation pathways of the amide I and II modes of N-methylacetamide","volume":"110","year":"2006","journal-title":"J.\u00a0Phys. Chem. B"},{"key":"2026022306104828300_c98","doi-asserted-by":"publisher","first-page":"1703","DOI":"10.1021\/acs.jpcb.9b11793","article-title":"The amide I spectrum of proteins\u2014Optimization of transition dipole coupling parameters using density functional theory calculations","volume":"124","year":"2020","journal-title":"J.\u00a0Phys. Chem. B"},{"key":"2026022306104828300_c99","doi-asserted-by":"publisher","first-page":"3379","DOI":"10.1021\/ct2003622","article-title":"GROMOS++ software for the analysis of biomolecular simulation trajectories","volume":"7","year":"2011","journal-title":"J.\u00a0Chem. Theory Comput."},{"key":"2026022306104828300_c100","doi-asserted-by":"publisher","first-page":"6123","DOI":"10.1021\/jp9813286","article-title":"Structure of the amide I band of peptides measured by femtosecond nonlinear-infrared spectroscopy","volume":"102","year":"1998","journal-title":"J.\u00a0Phys. Chem. B"},{"key":"2026022306104828300_c101","doi-asserted-by":"publisher","first-page":"212408","DOI":"10.1063\/1.4914156","article-title":"Dynamics of water, methanol, and ethanol in a room temperature ionic liquid","volume":"142","year":"2015","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c102","first-page":"422","article-title":"Solvation dynamics of N-methylacetamide in D2O, CDCI3 and DMSO-d6","volume-title":"Ultrafast Phenomena XIV","year":"2005"},{"key":"2026022306104828300_c103","doi-asserted-by":"publisher","first-page":"592","DOI":"10.1021\/jp807528q","article-title":"Empirical amide I vibrational frequency map: Application to 2D-IR line shapes for isotope-edited membrane peptide bundles","volume":"113","year":"2009","journal-title":"J.\u00a0Phys. Chem. B"},{"key":"2026022306104828300_c104","volume-title":"Computer Simulation of Liquids","year":"2017","edition":"2"},{"key":"2026022306104828300_c105","doi-asserted-by":"publisher","first-page":"224503","DOI":"10.1063\/1.3454733","article-title":"Two-dimensional infrared spectroscopy and ultrafast anisotropy decay of water","volume":"132","year":"2010","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c106","doi-asserted-by":"publisher","first-page":"1405","DOI":"10.1021\/ar900025a","article-title":"Waiting time dynamics in two-dimensional infrared spectroscopy","volume":"42","year":"2009","journal-title":"Acc. Chem. Res."},{"key":"2026022306104828300_c107","doi-asserted-by":"publisher","first-page":"22910","DOI":"10.1021\/jp064795t","article-title":"Nonadiabatic effects in the two-dimensional infrared spectra of peptides: Application to alanine dipeptide","volume":"110","year":"2006","journal-title":"J.\u00a0Phys. Chem. B"},{"key":"2026022306104828300_c108","doi-asserted-by":"publisher","first-page":"064106","DOI":"10.1063\/5.0138958","article-title":"Simulation of two-dimensional infrared Raman spectroscopy with application to proteins","volume":"158","year":"2023","journal-title":"J.\u00a0Chem. Phys."},{"key":"2026022306104828300_c109","doi-asserted-by":"crossref","unstructured":"D.\n            Zhang\n          , A.Peng, C.Cai, W.Li, Y.Zhou, J.Zeng, M.Guo, C.Zhang, B.Li, H.Jiang, T.Zhu, W.Jia, L.Zhang, and H.Wang, \u201cA graph neural network for the era of large atomistic models,\u201d arXiv:2506.01686 (2025).","DOI":"10.21203\/rs.3.rs-7075747\/v1"}],"container-title":["The Journal of Chemical Physics"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/pubs.aip.org\/aip\/jcp\/article-pdf\/doi\/10.1063\/5.0303526\/20914570\/084106_1_5.0303526.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/pubs.aip.org\/aip\/jcp\/article-pdf\/doi\/10.1063\/5.0303526\/20914570\/084106_1_5.0303526.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,2,23]],"date-time":"2026-02-23T11:10:57Z","timestamp":1771845057000},"score":1,"resource":{"primary":{"URL":"https:\/\/pubs.aip.org\/jcp\/article\/164\/8\/084106\/3380874\/Two-dimensional-infrared-spectroscopy-of-solute"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,2,23]]},"references-count":109,"journal-issue":{"issue":"8","published-print":{"date-parts":[[2026,2,28]]}},"URL":"https:\/\/doi.org\/10.1063\/5.0303526","relation":{},"ISSN":["0021-9606","1089-7690"],"issn-type":[{"value":"0021-9606","type":"print"},{"value":"1089-7690","type":"electronic"}],"subject":[],"published-other":{"date-parts":[[2026,2,28]]},"published":{"date-parts":[[2026,2,23]]},"article-number":"084106"}}