Article
Optics
Hanqing Xiong, Naixin Qian, Yupeng Miao, Zhilun Zhao, Chen Chen, Wei Min
Summary: Super-resolution Raman imaging, which offers higher chemical specificity but lower vibrational contrasts than fluorescence imaging, has been a challenge in achieving biocompatible imaging in the optical far-field. Stimulated Raman Excited Fluorescence (SREF) was discovered as an ultrasensitive vibrational spectroscopy that combines Raman scattering's chemical specificity with fluorescence detection's sensitivity. By integrating STED with background-free FM-SREF, high-contrast super-resolution vibrational imaging with STED-FM-SREF was achieved, offering spatial resolution determined by the signal-to-noise ratio.
LIGHT-SCIENCE & APPLICATIONS
(2021)
Article
Chemistry, Physical
Li-lin Jiang, Yun-fei Song, Wei-long Liu, Hong-lin Wu, Xi-you Li, Yan-qiang Yang
Summary: Ultrafast vibrational dynamics in pure liquid tetrahydrofuran were studied using femtosecond coherent anti Stokes Raman scattering. Different vibrational modes were observed with oscillatory decay in time-resolved spectra, providing insights into chemical reaction mechanisms in condensed-phase systems.
CHEMICAL PHYSICS LETTERS
(2021)
Article
Chemistry, Physical
Ruihua Pu, Ziyu Wang, Ruixue Zhu, Jiaming Jiang, Tsu-Chien Weng, Yifan Huang, Weimin Liu
Summary: Phototherapy is an effective and safe method for reducing high levels of ZZ-BR in newborns' serum. The process involves photoinduced configurational and structural isomerization, which generates excretable isomers. However, the exact mechanism of ZZ-BR photoinduced isomerization is still not well understood.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Ruihua Pu, Ziyu Wang, Ruixue Zhu, Jiaming Jiang, Tsu-Chien Weng, Yifan Huang, Weimin Liu
Summary: Phototherapy is an effective and safe method for reducing high levels of ZZ-BR in the serum of newborns. This study used various spectroscopic techniques and quantum chemical calculations to investigate the primary configurational isomerization dynamics of ZZ-BR in organic solvents. The results showed that upon photoexcitation, ultrafast configurational isomerization occurred, followed by intramolecular hydrogen-bond distortion and large-scale rotation of the two dipyrrinone halves of the ZZ-BR isomer in a few picoseconds. Most of the population returned back to ZZ-BR, while a small amount converted into stable BR isomers via structural isomerization.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Qiaozhi Yu, Zhengjian Yao, Haolin Zhang, Zhibin Li, Zhixing Chen, Hanqing Xiong
Summary: Researchers have developed a new ultrafast time-domain spectroscopy technique called transient stimulated Raman excited fluorescence (T-SREF), which enables background-free Raman spectra of electronic-coupled vibrational modes. By exciting the sample with two successive broadband femtosecond pulse pairs and performing Fourier transform on the resulting time-domain fluorescence trace, T-SREF achieves high sensitivity at the level of a few molecules, paving the way for supermultiplexed fluorescence detection and molecular dynamics sensing.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Jingle Wei, Yuexia Wu, Ruihua Pu, Limin Shi, Jiaming Jiang, Juan Du, Zhiqian Guo, Yifan Huang, Weimin Liu
Summary: The anti-Kasha process allows for the development of novel applications using high-energy excited states. Research has shown that dual-emission fluorophores can be achieved by slowing down the internal conversion from the S-2 state to the S-1 state in the anti-Kasha mechanism.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Yusuke Yoneda, Hikaru Kuramochi
Summary: Photochemical reactions occur in the electronically excited state, which is effectively represented by a multidimensional potential energy surface (PES) with a vast degree of freedom of nuclear coordinates. Recently, fully time-domain resonant two-dimensional Raman spectroscopy has emerged as a potentially powerful tool to provide unique information about the coupling between vibrational manifolds in the excited state. In this study, we demonstrate time-domain resonant two-dimensional impulsive stimulated Raman spectroscopy (2D-ISRS) of excited states using sub-10fs pulses based on the rapid scan of the time delay, which facilitates the efficient collection of time-domain vibrational signals with high sensitivity.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Sofia Goia, Matthew A. P. Turner, Jack M. Woolley, Michael D. Horbury, Alexandra J. Borrill, Joshua J. Tully, Samuel J. Cobb, Michael Staniforth, Nicholas D. M. Hine, Adam Burriss, Julie Macpherson, Ben R. Robinson, Vasilios G. Stavros
Summary: The study introduces a TA-SEC approach using BDD mesh electrodes to investigate early-stage photoinduced dynamics of reactive species. By electrochemically generating intermediates, the relaxation mechanisms of AQS and AH(2)QS are unravelled in the first 2.5 ns following UV absorption.
Article
Chemistry, Physical
Pardeep Kumar, Hikaru Kuramochi, Satoshi Takeuchi, Tahei Tahara
Summary: Metal nanoparticles have the potential to transfer absorbed photon energy to adsorbates in light-harvesting applications. However, the ultrafast plasmon-driven dynamics of adsorbates on metal nanoparticles are not well understood. In this study, we investigated the 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). Our results show that photoexcitation of the localized surface plasmon resonance (LSPR) band of GNAs alters the chemical interaction between BPE and GNAs on an ultrafast time scale.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Tahei Tahara, Pardeep Kumar, Hikaru Kuramochi, Satoshi Takeuchi
Summary: Metal nanoparticles can transfer absorbed photon energy to adsorbates, making them highly potential in light-harvesting applications. However, the ultrafast plasmon-driven dynamics of adsorbates on metal nanoparticles are not well understood. In this study, we used TR-SE-ISRS to investigate the ultrafast plasmon-driven processes of trans-1,2-bis(4-pyridyl)ethylene (BPE) adsorbed on gold nanoparticle assemblies (GNAs). Our results revealed that photoexcitation of the localized surface plasmon resonance (LSPR) band of GNAs altered the chemical interaction between BPE and GNAs on an ultrafast timescale.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Analytical
Steven A. Diaz, David W. Mccamant
Summary: By improving the collection optics, we have developed two new diffuse reflectance-based femtosecond stimulated Raman spectroscopy (drFSRS) techniques for collecting Raman spectra of opaque systems. The experimental results demonstrate the current capabilities of collecting high-quality Raman spectra using drFSRS.
ANALYTICAL CHEMISTRY
(2023)
Article
Biochemical Research Methods
Rajeev Ranjan, Giovanni Costa, Maria Antonietta Ferrara, Mario Sansone, Luigi Sirleto
Summary: In this study, the relationship between hardware characteristics and image processing in SRS microscopy literature was explored, with a focus on statistical analysis of image noise. The results demonstrated an improvement in image denoising with the adapted singular spectrum analysis method.
JOURNAL OF BIOPHOTONICS
(2022)
Article
Biochemistry & Molecular Biology
Janak Solaris, Taylor D. Krueger, Cheng Chen, Chong Fang
Summary: Proton transfer processes are crucial in biological systems. Excited-state intramolecular proton transfer (ESIPT) reactions involve quick and efficient charge transfer and ultrafast proton motions. This study investigates the ESIPT reaction of the fungal pigment Draconin Red using femtosecond transient absorption and excited-state femtosecond stimulated Raman spectroscopy. The results provide insights into the relaxation pathways and excited-state dynamics of the chromophore in solvent. The findings have implications for modeling potential energy surfaces and understanding reaction mechanisms in natural chromophores.
Article
Chemistry, Physical
Pardeep Kumar, Eduard Fron, Haruko Hosoi, Hikaru Kuramochi, Satoshi Takeuchi, Hideaki Mizuno, Tahei Tahara
Summary: LSSmOrange exhibits a large energy gap between absorption and emission due to excited-state proton transfer, and the bimodal ESPT dynamics is attributed to structural heterogeneity of the chromophore.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Multidisciplinary
Mason L. L. Valentine, Guoxin Yin, Julius J. J. Oppenheim, Mircea Dinca, Wei Xiong
Summary: We investigated the water H-bond network and its dynamics in Ni2Cl2BTDD using linear and ultrafast IR spectroscopy. We found that water forms an extensive H-bonding network in Ni2Cl2BTDD, which can rearrange within a confined cone up to 50 degrees within 1.3 ps. This reorientation indicates H-bond rearrangement, similar to bulk water. The picosecond H-bond rearrangement in Ni2Cl2BTDD supports its reversibility in water sorption.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Ziyu Wang, Ya Zhang, Cheng Chen, Ruixue Zhu, Jiaming Jiang, Tsu-Chien Weng, Quanjiang Ji, Yifan Huang, Chong Fang, Weimin Liu
Summary: This study utilized femtosecond stimulated Raman spectroscopy and various time-resolved electronic spectroscopies, aided by quantum calculations, to investigate the red fluorescent protein mKeima with a large Stokes shift. It revealed the photocycle and isomerization process of mKeima, and identified the trans-isomer as the dominant contributor to the large Stokes shift emission.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Zhiyuan Zhao, Ruihua Pu, Ziyu Wang, Jiaming Jiang, Weimin Liu
Summary: Light-induced reduction of graphene oxide (GO) is a promising method to produce reduced GO (rGO) without using harsh chemicals. However, the physicochemical mechanisms underlying photoreduction are still controversial, whether GO is reduced through direct excitation or through solvated electron production. Distinguishing GO photoreduction dynamics from solvated electron dynamics is challenging due to the similar electronic absorption responses.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Ruihua Pu, Ziyu Wang, Ruixue Zhu, Jiaming Jiang, Tsu-Chien Weng, Yifan Huang, Weimin Liu
Summary: Phototherapy is an effective and safe method for reducing high levels of ZZ-BR in the serum of newborns. This study used various spectroscopic techniques and quantum chemical calculations to investigate the primary configurational isomerization dynamics of ZZ-BR in organic solvents. The results showed that upon photoexcitation, ultrafast configurational isomerization occurred, followed by intramolecular hydrogen-bond distortion and large-scale rotation of the two dipyrrinone halves of the ZZ-BR isomer in a few picoseconds. Most of the population returned back to ZZ-BR, while a small amount converted into stable BR isomers via structural isomerization.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Biochemistry & Molecular Biology
Sullivan Bailey-Darland, Taylor D. Krueger, Chong Fang
Summary: In this work, the excited-state dynamics of a group of nitrophenols with different substituents were systematically studied using spectroscopic techniques and quantum calculations. The location of the substituents was found to have a significant impact on the properties of the compounds, providing important insights for the development of functional molecules for environmental applications.
Article
Biochemistry & Molecular Biology
Taylor D. D. Krueger, Longteng Tang, Cheng Chen, Liangdong Zhu, Isabella L. L. Breen, Rebekka M. M. Wachter, Chong Fang
Summary: Green-to-red photoconvertible fluorescent proteins are important tools for super-resolution imaging. The key residue Ala69 was identified to enhance the green-to-red photoconversion, and Thr69 promoted a stronger pi-pi stacking interaction between the chromophore and His193. These findings can be used to improve other green-to-red photoconvertible proteins for deeper biophysical and molecular biology insights, as well as bioimaging advancements.
Article
Chemistry, Analytical
Taylor D. Krueger, Longteng Tang, Chong Fang
Summary: Fluorescent proteins (FPs) are important tools for noninvasive bioimaging and sensing. REX-GECO1, a red-green emission and excitation ratiometric FP-based biosensor, shows a high dynamic range in measuring cellular calcium concentrations. The potential energy surfaces of these biosensors are revealed using electronic and spectroscopic techniques, uncovering details of their behavior. These findings can inform the design of biosensors with improved efficiency for calcium imaging.
Article
Biochemistry & Molecular Biology
Janak Solaris, Taylor D. Krueger, Cheng Chen, Chong Fang
Summary: Proton transfer processes are crucial in biological systems. Excited-state intramolecular proton transfer (ESIPT) reactions involve quick and efficient charge transfer and ultrafast proton motions. This study investigates the ESIPT reaction of the fungal pigment Draconin Red using femtosecond transient absorption and excited-state femtosecond stimulated Raman spectroscopy. The results provide insights into the relaxation pathways and excited-state dynamics of the chromophore in solvent. The findings have implications for modeling potential energy surfaces and understanding reaction mechanisms in natural chromophores.
Article
Green & Sustainable Science & Technology
Heng Jiang, Longteng Tang, Yanke Fu, Shitong Wang, Sean K. Sandstrom, Alexis M. Scida, Guoxing Li, David Hoang, Jessica J. Hong, Nan-Chieh Chiu, Kyriakos C. Stylianou, William F. Stickle, Donghai Wang, Ju Li, P. Alex Greaney, Chong Fang, Xiulei Ji
Summary: Rechargeable aqueous zinc batteries are gaining popularity in stationary storage applications due to their safety, cost-effectiveness, scalability, and low carbon footprint. However, the challenge of hydrogen evolution reaction (HER) at the zinc surface hinders the utilization of this reversible redox chemistry. In this study, a concentrated electrolyte design is developed to eliminate HER and achieve high Coulombic efficiency for Zn plating/stripping. The hybrid electrolyte not only enables the formation of a protective solid electrolyte interphase but also enhances battery performance, allowing for sustainable energy storage with high energy density.
NATURE SUSTAINABILITY
(2023)
Review
Chemistry, Multidisciplinary
Taylor D. Krueger, Cheng Chen, Chong Fang
Summary: Red fluorescent proteins (RFPs) are a popular class of genetically encodable bioprobes and biomarkers that can advance breakthroughs in imaging and life sciences. Understanding their working mechanisms requires suitable spectroscopic techniques to delineate key structural features and dynamic steps. Progress has been made in designing RFPs with improved functions and versatility.
CHEMISTRY-AN ASIAN JOURNAL
(2023)
Article
Biochemistry & Molecular Biology
Cheng Chen, J. Nathan Henderson, Dmitry A. Ruchkin, Jacob M. Kirsh, Mikhail S. Baranov, Alexey M. Bogdanov, Jeremy H. Mills, Steven G. Boxer, Chong Fang
Summary: This study systematically analyzed the vibrational properties of FP chromophores by using FSRS and quantum calculations. A bond-stretching mode characteristic of the quinoidal resonance structure was found to be present in most FPs and model chromophores, which can serve as a vibrational marker for interpreting chromophore-environment interactions and structural effects on the electronic properties of the chromophore.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Article
Materials Science, Multidisciplinary
Xueqiao Zhang, Ye Liu, Chieh-Hsi Kuan, Longteng Tang, Taylor D. Krueger, Sanjida Yeasmin, Ahasan Ullah, Chong Fang, Li-Jing Cheng
Summary: Researchers have discovered red carbon dots with large Stokes shifts and demonstrated their potential for display applications by creating multicolor patterns and color-conversion LEDs using printable carbon dot inks.
JOURNAL OF MATERIALS CHEMISTRY C
(2023)
Article
Chemistry, Physical
Cheng Chen, Hao Zhang, Jing Zhang, Hui-wang Ai, Chong Fang
Summary: The incorporation of ncAAs into fluorescent proteins has the potential to red-shift their fluorescence and improve tissue imaging. However, ncAA-based RFPs are rare. The recent advance of 3-aminotyrosine modified sfGFP has provided insights into the molecular mechanism of red-shifted fluorescence, but its dim fluorescence limits its applications.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)