دورية أكاديمية
Photophysical Outcomes of Water-Solvated Heterocycles: Single-Conformation Ultraviolet and Infrared Spectroscopy of Microsolvated 2‑Phenylpyrrole
| العنوان: | Photophysical Outcomes of Water-Solvated Heterocycles: Single-Conformation Ultraviolet and Infrared Spectroscopy of Microsolvated 2‑Phenylpyrrole |
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| المؤلفون: | Ruby W. Neisser, John P. Davis, Megan E. Alfieri, Hayden Harkins, Andrew S. Petit, Daniel P. Tabor, Nathanael M. Kidwell |
| سنة النشر: | 2023 |
| مصطلحات موضوعية: | Biophysics, Biochemistry, Sociology, Space Science, Biological Sciences not elsewhere classified, Chemical Sciences not elsewhere classified, Physical Sciences not elsewhere classified, vibrational spectral signatures, using resonant two, upon stepwise addition, pyrrole nh donor, nh stretching coordinates, mode hamiltonian approach, conjugated pyrrole derivative, analysis revealed evidence, pyrrole aromatic rings, h atom stabilization, specific 2phpy :<, 2 , aromatic rings, specific ultraviolet, n <, 2phpy :<, ultraviolet wavelengths, ultraviolet spectra, thus identifying, third h, theoretical methods, solvated heterocycles, photophysical outcomes |
| الوصف: | The molecular chromophores within brown carbon (BrC) aerosols absorb solar radiation at visible and near-ultraviolet wavelengths. This contributes to the overall warming of the troposphere and the photochemical aging of aerosols. In this investigation, we combine a suite of experimental and theoretical methods to reveal the conformation-specific ultraviolet and infrared spectroscopy of 2-phenylpyrrole (2PhPy)an extended π-conjugated pyrrole derivative and a model BrC chromophorealong with its water microsolvated molecular complexes (2PhPy: n H 2 O, n = 1–3). Using resonant two-photon ionization and double-resonance holeburning techniques alongside MP3 (ground state) and ADC(3) (excited state) torsional potential energy surfaces and discrete variable representation simulations, we characterized the ultraviolet spectra of 2PhPy and 2PhPy:1H 2 O. This analysis revealed evidence for Herzberg–Teller vibronic coupling along the CH wagging and NH stretching coordinates of the aromatic rings. Conformation-specific infrared spectroscopy revealed extended hydrogen-bonding networks of the 2PhPy: n H 2 O complexes. Upon stepwise addition of H 2 O solvation, the nearest H 2 O acceptor forms a strong, noncovalent interaction with the pyrrole NH donor, while the second and third H 2 O partners interface with the phenyl and pyrrole aromatic rings through growing van der Waals π/H atom stabilization. A local-mode Hamiltonian approach was employed for comparison with the experimental spectra, thus identifying the vibrational spectral signatures to specific 2PhPy: n H 2 O oscillators. |
| نوع الوثيقة: | article in journal/newspaper |
| اللغة: | unknown |
| العلاقة: | https://figshare.com/articles/journal_contribution/Photophysical_Outcomes_of_Water-Solvated_Heterocycles_Single-Conformation_Ultraviolet_and_Infrared_Spectroscopy_of_Microsolvated_2_Phenylpyrrole/24796381Test |
| DOI: | 10.1021/acs.jpca.3c04472.s001 |
| الإتاحة: | https://doi.org/10.1021/acs.jpca.3c04472.s001Test https://figshare.com/articles/journal_contribution/Photophysical_Outcomes_of_Water-Solvated_Heterocycles_Single-Conformation_Ultraviolet_and_Infrared_Spectroscopy_of_Microsolvated_2_Phenylpyrrole/24796381Test |
| حقوق: | CC BY-NC 4.0 |
| رقم الانضمام: | edsbas.F46C8C26 |
| قاعدة البيانات: | BASE |
| DOI: | 10.1021/acs.jpca.3c04472.s001 |
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