Ultrafast Vibrational Energy Transfer through the Covalent Bond and Intra- and Intermolecular Hydrogen Bonds in a Supramolecular Dimer by Two-Dimensional Infrared Spectroscopy

Dong, Xueqian; Wang, Sumin; Yu, Pengyun; Yang, Fan; Zhao, Juan; Wu, Li‐Zhu; Tung, Chen‐Ho; Wang, Jianping

doi:10.1021/acs.jpcb.9b10431

Cited by 8 publications

(3 citation statements)

References 88 publications

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“…Presently, it would be logical to consider two possible mechanisms underlying the effect of contactless impact. The first mechanism is VRET (vibrational resonant energy transfer), which is carried out by intra-and intermolecular exchange, including through-space interaction [64]. However, VRET is very short-range, making it difficult to seriously consider it as a possible mechanism of the effect of one system on another through vessel walls.…”

Section: Discussionmentioning

confidence: 99%

Antibodies Processed Using High Dilution Technology Distantly Change Structural Properties of IFNγ Aqueous Solution

Penkov

2021

Pharmaceutics

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Terahertz spectroscopy allows for the analysis of vibrations corresponding to the large-scale structural movements and collective dynamics of hydrogen-bonded water molecules. Previously, differences had been detected in the emission spectra of interferon-gamma (IFNγ) solutions surrounded by extremely diluted solutions of either IFNγ or antibodies to IFNγ without direct contact compared to a control. Here we aimed to analyse the structural properties of water in a sample of an aqueous solution of IFNγ via terahertz time-domain spectroscopy (THz-TDS). Tubes with the IFNγ solution were immersed in fluidised lactose saturated with test samples (dilutions of antibodies to IFNγ or control) and incubated at 37 °C for 1, 1.5–2, 2.5–3, or 3.5–4 h. Fluidised lactose was chosen since it is an excipient in the manufacture of drugs based on diluted antibodies to IFNγ. After incubation, spectra were recorded within a wavenumber range of 10 to 110 cm−1 with a resolution of 4 cm−1. Lactose saturated with dilutions of antibodies to IFNγ (incubated for more than 2.5 h) changed the structural properties of an IFNγ aqueous solution without direct contact compared to the control. Terahertz spectra revealed stronger intermolecular hydrogen bonds and an increase in the relaxation time of free and weakly bound water molecules. The methodology developed on the basis of THz-TDS could potentially be applied to quality control of pharmaceuticals based on extremely diluted antibodies.

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Section: Discussionmentioning

confidence: 99%

Antibodies Processed Using High Dilution Technology Distantly Change Structural Properties of IFNγ Aqueous Solution

Penkov

2021

Pharmaceutics

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“…Interestingly, the kinetics of resonance energy transfer caused by plasmons is an open area for study [ 65 ]. The results of the study of the intra- and intermolecular transfer of vibrational energy in supramolecular structures state that the transfer of this energy occurs in a picosecond time scale [ 66 ]. The data obtained plays an important role both for the systematic view of the processes of intra- and intermolecular interactions, and for the scientific community in general.…”

Section: Resultsmentioning

confidence: 99%

Controlling the Quality of Nanodrugs According to Their New Property—Radiothermal Emission

Petrov,

Galkina,

Koldina

et al. 2024

Pharmaceutics

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Previous studies have shown that complexly shaped nanoparticles (NPs) have their intrinsic radiothermal emission in the millimeter range. This article presents a method for controlling the quality of nanodrugs—immunobiological preparations (IBPs)—based on the detection of their intrinsic radiothermal emissions. The emissivity of interferon (IFN) medicals, determined without opening the primary package, is as follows (µW/m2): IFN-α2b—80 ± 9 (105 IU per package), IFN-β1a—40 ± 5 (24 × 106 IU per package), IFN-γ—30 ± 4 (105 IU per package). The emissivity of virus-like particles (VLP), determined using vaccines Gam-VLP-multivac (120 μg) in an injection bottle (crimp cap vials), was as follows: 12 ± 1 µW/m2, Gam-VLP—rota vaccines—9 ± 1 µW/m2. This study shows the reproducibility of emissivity over the course of a year, subject to the storage conditions of the immunobiological products. It has been shown that accelerated aging and a longer shelf life are accompanied by the coagulation of active NPs, and lead to a manyfold drop in emissivity. The dependence of radiothermal emission on temperature has a complex, non-monotonic nature. The emission intensity depends on the form of dosage, but remains within the order of magnitude for IFN-α2b for intranasal aqueous solution, ointments, and suppositories. The possibility of the remote quantitative control of the first phases of the immune response (increased synthesis of IFNs) to the intranasal administration of VLP vaccines has been demonstrated in experimental animals.

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“…2D IR spectra of the bR samples were collected using a pulseshaper-based 2D IR spectrometer. 66 Briefly, a commercial ultrafast Ti:sapphire laser amplifier with 3 mJ, sub 25 fs, 800 nm pulse at 1 kHz repetition rate was used to pump an optical parametric amplifier so as to generate mid-IR pulses with a pulse energy of ca. 9 μJ, a center frequency of 1645 cm −1 , and a spectral width (full width at halfmaximum) of ca.…”

Section: Discussionmentioning

confidence: 99%

Ultrafast Two-Dimensional Infrared Spectroscopy Resolved a Structured Lysine 159 on the Cytoplasmic Surface of the Microbial Photoreceptor Bacteriorhodopsin

Ding

et al. 2022

J. Am. Chem. Soc.

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Bacteriorhodopsin (bR) is a light-driven microbial receptor, and lysine 159 (K159) is a charged residue on the cytoplasmic (CP) side of its E−F loop. However, its conformation and function remain unknown due to fast surface dynamics. By utilizing a 13 C, 15 N-labeled lysine (K) as an isotope probe, we created a network of site-specific amide-I vibrational signatures (backbone carbonyl stretch) to identify the frequency contribution of the labeled residues to the amide-I excitonic band structure. Thus, the red-shifted amide-I frequency in the 13 C, 15 N-lysinelabeled bR (uK-bR) to the unlabeled bR (WT-bR) could be differentiated and examined by ultrafast two-dimensional vibrational echo infrared (2D IR) spectroscopy. Our results showed that the backbone carbonyl of K159 is located at a high frequency of ca. 1693 cm −1 and has a vibrational excited-state relaxation time shorter than the bulk helical amide-I mode at the same frequency, suggesting that K159 may possess a hydrogen-bonded γ-turn structure with E161, one of the carboxylate residues on the CP surface of bR. The 2D solid-state NMR study of uK-bR also revealed conformational dependent lysine residues, from which K159 was found to involve the turn motif. This γ-turn structure maintained by K159 may help to stabilize the E−F loop and support E161 in attracting protons from the bulk during the late stage of the bR photocycle. The combined spectroscopic approach illustrated in this work may be applied to map residue-specific local structures and dynamics of other receptors and large proteins.

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Ultrafast Vibrational Energy Transfer through the Covalent Bond and Intra- and Intermolecular Hydrogen Bonds in a Supramolecular Dimer by Two-Dimensional Infrared Spectroscopy

Cited by 8 publications

References 88 publications

Antibodies Processed Using High Dilution Technology Distantly Change Structural Properties of IFNγ Aqueous Solution

Antibodies Processed Using High Dilution Technology Distantly Change Structural Properties of IFNγ Aqueous Solution

Controlling the Quality of Nanodrugs According to Their New Property—Radiothermal Emission

Ultrafast Two-Dimensional Infrared Spectroscopy Resolved a Structured Lysine 159 on the Cytoplasmic Surface of the Microbial Photoreceptor Bacteriorhodopsin

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