دورية أكاديمية
Ultrafast Transient Infrared Spectroscopy of Photoreceptors with Polarizable QM/MM Dynamics
| العنوان: | Ultrafast Transient Infrared Spectroscopy of Photoreceptors with Polarizable QM/MM Dynamics |
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| المؤلفون: | Macaluso V., Hashem S., Nottoli M., Lipparini F., Cupellini L., Mennucci B. |
| المساهمون: | Macaluso, V., Hashem, S., Nottoli, M., Lipparini, F., Cupellini, L., Mennucci, B. |
| سنة النشر: | 2021 |
| المجموعة: | ARPI - Archivio della Ricerca dell'Università di Pisa |
| الوصف: | Ultrafast transient infrared (TRIR) spectroscopy is widely used to measure the excitation-induced structural changes of protein-bound chromophores. Here, we design a novel and general strategy to compute TRIR spectra of photoreceptors by combining μs-long MM molecular dynamics with ps-long QM/AMOEBA Born-Oppenheimer molecular dynamics (BOMD) trajectories for both ground and excited electronic states. As a proof of concept, the strategy is here applied to AppA, a blue-light-utilizing flavin (BLUF) protein, found in bacteria. We first analyzed the short-time evolution of the embedded flavin upon excitation revealing that its dynamic Stokes shift is ultrafast and mainly driven by the internal reorganization of the chromophore. A different normal-mode representation was needed to describe ground- and excited-state IR spectra. In this way, we could assign all of the bands observed in the measured transient spectrum. In particular, we could characterize the flavin isoalloxazine-ring region of the spectrum, for which a full and clear description was missing. |
| نوع الوثيقة: | article in journal/newspaper |
| اللغة: | English |
| العلاقة: | info:eu-repo/semantics/altIdentifier/pmid/34476939; info:eu-repo/semantics/altIdentifier/wos/WOS:000697332700020; volume:125; issue:36; firstpage:10282; lastpage:10292; numberofpages:11; journal:JOURNAL OF PHYSICAL CHEMISTRY. B, CONDENSED MATTER, MATERIALS, SURFACES, INTERFACES & BIOPHYSICAL; info:eu-repo/grantAgreement/EC/H2020/786714; http://hdl.handle.net/11568/1109657Test; info:eu-repo/semantics/altIdentifier/scopus/2-s2.0-85114883016 |
| DOI: | 10.1021/acs.jpcb.1c05753 |
| الإتاحة: | https://doi.org/10.1021/acs.jpcb.1c05753Test http://hdl.handle.net/11568/1109657Test |
| حقوق: | info:eu-repo/semantics/openAccess |
| رقم الانضمام: | edsbas.6E9CB7F3 |
| قاعدة البيانات: | BASE |
| DOI: | 10.1021/acs.jpcb.1c05753 |
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