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Article ; Online: Tribute to Hiro-o Hamaguchi: Expanding the Boundaries of Raman Spectroscopy.

Kano, Hideaki / Bonn, Mischa / Zanni, Martin / Tahara, Tahei

The journal of physical chemistry. B

2024 Volume 128, Issue 4, Page(s) 883–885

Language	English
Publishing date	2024-02-01
Publishing country	United States
Document type	Journal Article
ISSN	1520-5207
ISSN (online)	1520-5207
DOI	10.1021/acs.jpcb.3c08380
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Article ; Online: Pulsed-Interleaved-Excitation Two-Dimensional Fluorescence Lifetime Correlation Spectroscopy.

Sarkar, Bidyut / Ishii, Kunihiko / Tahara, Tahei

The journal of physical chemistry. B

2024 Volume 128, Issue 19, Page(s) 4685–4695

Abstract: We report on pulsed-interleaved-excitation two-dimensional fluorescence lifetime correlation spectroscopy (PIE 2D FLCS) to study biomolecular structural dynamics with high sensitivity and high time resolution using Förster resonance energy transfer (FRET) ...

Abstract	We report on pulsed-interleaved-excitation two-dimensional fluorescence lifetime correlation spectroscopy (PIE 2D FLCS) to study biomolecular structural dynamics with high sensitivity and high time resolution using Förster resonance energy transfer (FRET). PIE 2D FLCS is an extension of 2D FLCS, which is a unique single-molecule fluorescence method that uses fluorescence lifetime information to distinguish different fluorescence species in equilibrium and resolves their interconversion dynamics with a submicrosecond time resolution. Because 2D FLCS has used only a single-color excitation so far, it was difficult to distinguish a very low-FRET (or zero-FRET) species from only donor-labeled species. We overcome this difficulty by implementing the PIE scheme (i.e., alternate excitation of the donor and acceptor dyes using two temporally interleaved excitations with different colors) to 2D FLCS, realizing two-color excitation and two-color fluorescence detection in 2D FLCS. After proof-of-principle PIE 2D FLCS analysis on the photon data synthesized with Monte Carlo simulation, we apply PIE 2D FLCS to a DNA-hairpin sample and show that this method readily distinguishes four fluorescent species, i.e., high-FRET, low-FRET, and two single-dye-labeled species. In addition, we show that PIE 2D FLCS can also quantitatively evaluate the contributions of the donor-acceptor spectral crosstalk, which often appears as artifacts in FRET studies and degrades the information obtained.
Language	English
Publishing date	2024-05-01
Publishing country	United States
Document type	Journal Article
ISSN	1520-5207
ISSN (online)	1520-5207
DOI	10.1021/acs.jpcb.4c01224
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Article ; Online: Superresolution concentration measurement realized by sub-shot-noise absorption spectroscopy.

Matsuzaki, Korenobu / Tahara, Tahei

Nature communications

2022 Volume 13, Issue 1, Page(s) 953

Abstract: Absorption spectroscopy is one of the most widely used spectroscopic methods. The signal-to-noise ratio in conventional absorption spectroscopy is ultimately limited by the shot noise, which arises from the statistical property of the light used for the ... ...

Abstract	Absorption spectroscopy is one of the most widely used spectroscopic methods. The signal-to-noise ratio in conventional absorption spectroscopy is ultimately limited by the shot noise, which arises from the statistical property of the light used for the measurement. Here we show that the noise in absorption spectra can be suppressed below the shot-noise limit when entangled photon pairs are used for the light source. By combining broadband entangled photon pairs and multichannel detection, we realize the acquisition of sub-shot-noise absorption spectra in the entire visible wavelength. Furthermore, we demonstrate the strength of sub-shot-noise absorption spectroscopy for the identification and quantification of chemical species, which are two primary aims of absorption spectroscopy. For highly diluted binary mixture solutions, sub-shot-noise absorption spectroscopy enables us to determine the concentration of each chemical species with precision beyond the limit of conventional absorption spectroscopy. That is, sub-shot-noise absorption spectroscopy achieves superresolution in concentration measurements.
Language	English
Publishing date	2022-02-17
Publishing country	England
Document type	Journal Article
ZDB-ID	2553671-0
ISSN	2041-1723 ; 2041-1723
ISSN (online)	2041-1723
ISSN	2041-1723
DOI	10.1038/s41467-022-28617-w
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Article ; Online: Unified picture of vibrational relaxation of OH stretch at the air/water interface.

Sung, Woongmo / Inoue, Ken-Ichi / Nihonyanagi, Satoshi / Tahara, Tahei

Nature communications

2024 Volume 15, Issue 1, Page(s) 1258

Abstract: The elucidation of the energy dissipation process is crucial for understanding various phenomena occurring in nature. Yet, the vibrational relaxation and its timescale at the water interface, where the hydrogen-bonding network is truncated, are not well ... ...

Abstract	The elucidation of the energy dissipation process is crucial for understanding various phenomena occurring in nature. Yet, the vibrational relaxation and its timescale at the water interface, where the hydrogen-bonding network is truncated, are not well understood and are still under debate. In the present study, we focus on the OH stretch of interfacial water at the air/water interface and investigate its vibrational relaxation by femtosecond time-resolved, heterodyne-detected vibrational sum-frequency generation (TR-HD-VSFG) spectroscopy. The temporal change of the vibrationally excited hydrogen-bonded (HB) OH stretch band (ν=1→2 transition) is measured, enabling us to determine reliable vibrational relaxation (T
Language	English
Publishing date	2024-02-10
Publishing country	England
Document type	Journal Article
ZDB-ID	2553671-0
ISSN	2041-1723 ; 2041-1723
ISSN (online)	2041-1723
ISSN	2041-1723
DOI	10.1038/s41467-024-45388-8
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Article ; Online: Complex phase of the nonresonant background in sum frequency generation spectroscopy.

Matsuzaki, Korenobu / Yamaguchi, Shoichi / Tahara, Tahei

The Journal of chemical physics

2023 Volume 159, Issue 22

Abstract: Sum frequency generation (SFG) spectroscopy is an interface-selective spectroscopic technique that enables us to selectively observe the vibrational or electronic resonances of molecules within a very thin interface layer. The interfacial properties ... ...

Abstract	Sum frequency generation (SFG) spectroscopy is an interface-selective spectroscopic technique that enables us to selectively observe the vibrational or electronic resonances of molecules within a very thin interface layer. The interfacial properties probed by SFG are contained in a complex quantity called the second-order nonlinear susceptibility (χ2). It is usually believed that the imaginary part of χ2 (Im χ2) exhibits the resonant responses of the system, whereas the nonresonant responses appear solely in the real part of χ2 (Re χ2). However, it was recently theoretically pointed out that a portion of the nonresonant responses actually contributes to the observed Im χ2 spectra when the finite thickness of the interface layer is taken into account. In this study, by considering a simple air/liquid interface without any solutes as a model system, we theoretically evaluate the nonresonant contribution to experimentally accessible Im χ2 as well as to Re χ2, from which the complex phase of the nonresonant background is estimated. It is shown that the deviation of the complex phase from 0° or 180° is less than 1° even if the thickness of the interface layer is taken into account. This means that the nonresonant contribution to Im χ2 is practically negligible, and it is a very good approximation to think that the nonresonant background appears solely in Re χ2 in the case of air/liquid interfaces. This result implies that Im χ2 practically contains only the resonant responses of the system, and molecular resonances at the interface can be conveniently studied using Im χ2 spectra at such interfaces.
Language	English
Publishing date	2023-12-11
Publishing country	United States
Document type	Journal Article
ZDB-ID	3113-6
ISSN	1089-7690 ; 0021-9606
ISSN (online)	1089-7690
ISSN	0021-9606
DOI	10.1063/5.0169712
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Article ; Online: Photoexcited Plasmon-Driven Ultrafast Dynamics of the Adsorbate Probed by Femtosecond Time-Resolved Surface-Enhanced Time-Domain Raman Spectroscopy.

Kumar, Pardeep / Kuramochi, Hikaru / Takeuchi, Satoshi / Tahara, Tahei

The journal of physical chemistry letters

2023 Volume 14, Issue 11, Page(s) 2845–2853

Abstract: Metal nanoparticles have high potential in light-harvesting applications by transferring absorbed photon energy to the adsorbates. However, photoexcited plasmon-driven ultrafast dynamics of the adsorbate on metal nanoparticles have not been clearly ... ...

Abstract	Metal nanoparticles have high potential in light-harvesting applications by transferring absorbed photon energy to the adsorbates. However, photoexcited plasmon-driven ultrafast dynamics of the adsorbate on metal nanoparticles have not been clearly understood. We studied ultrafast plasmon-driven processes of trans-1,2-bis(4-pyridyl)ethylene (BPE) adsorbed on gold nanoparticle assemblies (GNAs) using time-resolved surface-enhanced impulsive stimulated Raman spectroscopy (TR-SE-ISRS). After photoexciting the localized surface plasmon resonance (LSPR) band of the GNAs, we measured femtosecond time-resolved surface-enhanced Raman spectra of the adsorbate, which exhibited transient bleach in the Raman signal and following biphasic recovery that proceeds on the time scale of a few tens of picoseconds. The TR-SE-ISRS data were analyzed with singular value decomposition, and the obtained species-associated Raman spectra indicated that photoexcitation of the LSPR band alters chemical interaction between BPE and the GNAs on an ultrafast time scale; initial steady-state BPE is recovered through a precursor state that has weaker interaction with the GNAs.
Language	English
Publishing date	2023-03-14
Publishing country	United States
Document type	Journal Article
ISSN	1948-7185
ISSN (online)	1948-7185
DOI	10.1021/acs.jpclett.2c03813
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Article ; Online: Local pH at Nonionic and Zwitterionic Lipid/Water Interfaces Revealed by Heterodyne-Detected Electronic Sum-Frequency Generation: A Unified View to Predict Interfacial pH of Biomembranes.

Kundu, Achintya / Yamaguchi, Shoichi / Tahara, Tahei

The journal of physical chemistry. B

2023 Volume 127, Issue 24, Page(s) 5445–5452

Abstract: For biomembranes, which are composed of neutral as well as charged lipids, the local pH at lipid/water interfaces is extremely important in their structural formation and functional activity. In our previous study of the charged lipid/water interfaces, ... ...

Abstract	For biomembranes, which are composed of neutral as well as charged lipids, the local pH at lipid/water interfaces is extremely important in their structural formation and functional activity. In our previous study of the charged lipid/water interfaces, we found that the local pH at the interface is governed by the positive or negative sign of the charge of the lipid: i.e., the local pH is dictated by the repulsive or attractive electrostatic interaction between the charged lipid headgroup and the proton. Because of the lack of net charge in the headgroup of the neutral lipid, the factor determining the local pH at neutral lipid/water interfaces is less straightforward, and therefore it is more challenging to predict the local pH. Here we apply heterodyne-detected electronic sum frequency generation (HD-ESFG) spectroscopy to nonionic and zwitterionic lipids to investigate the local pH at the neutral lipid/water interfaces. The obtained results indicate that the local pH at the nonionic lipid/water interface is higher than in bulk water by 0.8 whereas the local pH at the zwitterionic lipid/water interface is lower by 0.6, although the latter is subject to significant uncertainty. The present HD-ESFG study on neutral lipids, combined with the previous study on charged lipids, presents a unified view to consider the local pH at biomembranes based on the balance between the electrostatic interaction and the hydrophobicity provided by the lipid.
MeSH term(s)	Surface Properties ; Water/chemistry ; Spectrum Analysis ; Lipids/chemistry ; Hydrogen-Ion Concentration
Chemical Substances	Water (059QF0KO0R) ; Lipids
Language	English
Publishing date	2023-06-12
Publishing country	United States
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ISSN	1520-5207
ISSN (online)	1520-5207
DOI	10.1021/acs.jpcb.3c02002
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Article ; Online: Tracking Ultrafast Structural Dynamics by Time-Domain Raman Spectroscopy.

Kuramochi, Hikaru / Tahara, Tahei

Journal of the American Chemical Society

2021 Volume 143, Issue 26, Page(s) 9699–9717

Abstract: In traditional Raman spectroscopy, narrow-band light is irradiated on a sample, and its inelastic scattering, i.e., Raman scattering, is detected. The energy difference between the Raman scattering and the incident light corresponds to the vibrational ... ...

Abstract	In traditional Raman spectroscopy, narrow-band light is irradiated on a sample, and its inelastic scattering, i.e., Raman scattering, is detected. The energy difference between the Raman scattering and the incident light corresponds to the vibrational energy of the molecule, providing the Raman spectrum that contains rich information about the molecular-level properties of the materials. On the other hand, by using ultrashort optical pulses, it is possible to induce Raman-active coherent nuclear motion of the molecule and to observe the molecular vibration in real time. Moreover, this time-domain Raman measurement can be combined with femtosecond photoexcitation, triggering chemical changes, which enables tracking ultrafast structural dynamics in a form of "time-resolved" time-domain Raman spectroscopy, also known as time-resolved impulsive stimulated Raman spectroscopy. With the advent of stable, ultrashort laser pulse sources, time-resolved impulsive stimulated Raman spectroscopy now realizes high sensitivity and a wide detection frequency window from THz to 3000 cm
Language	English
Publishing date	2021-06-07
Publishing country	United States
Document type	Journal Article ; Research Support, Non-U.S. Gov't
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.1c02545
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Article: Tracking Ultrafast Structural Dynamics by Time-Domain Raman Spectroscopy

Kuramochi, Hikaru / Tahara, Tahei

Journal of the American Chemical Society. 2021 June 07, v. 143, no. 26

2021

Abstract	In traditional Raman spectroscopy, narrow-band light is irradiated on a sample, and its inelastic scattering, i.e., Raman scattering, is detected. The energy difference between the Raman scattering and the incident light corresponds to the vibrational energy of the molecule, providing the Raman spectrum that contains rich information about the molecular-level properties of the materials. On the other hand, by using ultrashort optical pulses, it is possible to induce Raman-active coherent nuclear motion of the molecule and to observe the molecular vibration in real time. Moreover, this time-domain Raman measurement can be combined with femtosecond photoexcitation, triggering chemical changes, which enables tracking ultrafast structural dynamics in a form of “time-resolved” time-domain Raman spectroscopy, also known as time-resolved impulsive stimulated Raman spectroscopy. With the advent of stable, ultrashort laser pulse sources, time-resolved impulsive stimulated Raman spectroscopy now realizes high sensitivity and a wide detection frequency window from THz to 3000 cm–¹, and has seen success in unveiling the molecular mechanisms underlying the efficient functions of complex molecular systems. In this Perspective, we overview the present status of time-domain Raman spectroscopy, particularly focusing on its application to the study of femtosecond structural dynamics. We first explain the principle and a brief history of time-domain Raman spectroscopy and then describe the apparatus and recent applications to the femtosecond dynamics of complex molecular systems, including proteins, molecular assemblies, and functional materials. We also discuss future directions for time-domain Raman spectroscopy, which has reached a status allowing a wide range of applications.
Keywords	Raman spectroscopy ; energy ; photochemical reactions ; vibration
Language	English
Dates of publication	2021-0607
Size	p. 9699-9717.
Publishing place	American Chemical Society
Document type	Article
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.1c02545
Database	NAL-Catalogue (AGRICOLA)

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Article: Why the Photochemical Reaction of Phenol Becomes Ultrafast at the Air–Water Interface: The Effect of Surface Hydration

Ishiyama, Tatsuya / Tahara, Tahei / Morita, Akihiro

Journal of the American Chemical Society. 2022 Apr. 04, v. 144, no. 14

2022

Abstract: Photochemical reactions at the air–water interface can show remarkably different rates from those in bulk water. The present study elucidates the reaction mechanism of phenol characteristic at the air–water interface by the combination of molecular ... ...

Abstract	Photochemical reactions at the air–water interface can show remarkably different rates from those in bulk water. The present study elucidates the reaction mechanism of phenol characteristic at the air–water interface by the combination of molecular dynamics simulation and quantum chemical calculations of the excited states. We found that incomplete hydrogen bonding to phenol at the air–water interface affects excited states associated with the conical intersection and significantly reduces the reaction barrier, resulting in the distinctively facilitated rate in comparison with the bulk phase. The present study indicates that the reaction dynamics can be substantially different at the interfaces in general, reflecting the difference in the stabilization energy of the electronic states in markedly different solvation at the interface.
Keywords	energy ; hydrogen ; liquid-air interface ; molecular dynamics ; phenol ; photochemical reactions ; quantum mechanics ; reaction mechanisms ; solvation
Language	English
Dates of publication	2022-0404
Size	p. 6321-6325.
Publishing place	American Chemical Society
Document type	Article
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.1c13336
Database	NAL-Catalogue (AGRICOLA)

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