Article
Chemistry, Physical
Grace H. Taumoefolau, Robert B. Best
Summary: In a two-state molecular system, transition paths involve the trajectories during which the system transitions between stable states. Single-molecule experiments can estimate transition-path durations, although there may be a tendency to underestimate. Greater flexibility in the transition-path model can lead to more accurate extraction of transition-path times.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Aljaz Godec, Dmitrii E. Makarov
Summary: In this paper, we discuss the practical challenges of using stochastic thermodynamics to determine the directionality of molecular machines from experimental single-molecule trajectories. Due to the limitations of spatiotemporal resolution in these experiments and the inability to detect both forward and backward transitions between the same states, distinguishing the forward and backward directions of ATP-consuming periodic molecular machines becomes a nontrivial task. By extending the commonly used Markov-state model to analyze single-molecule transition-path measurements, we show how irreversibility can be hidden in these measurements but can be revealed when non-Markov effects in low-dimensional single-molecule trajectories are considered.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Kevin Song, Raymond Park, Atanu Das, Dmitrii E. Makarov, Etienne Vouga
Summary: A milestone-based method for information-theoretical analysis of continuous trajectories is developed and shown to be useful in both Markov and non-Markov models and in trajectories obtained from molecular simulations.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Irina V. Gopich, Jae-Yeol Kim, Hoi Sung Chung
Summary: In single-molecule free diffusion experiments, accurate determination of individual molecule species' brightness and diffusivity from selected bursts of photons is crucial. New methods are presented to analyze the bursts, considering the bias introduced by the burst selection criteria. These methods, utilizing Maximum Likelihood (ML) approach, perform well on simulated photon trajectories and experimental data.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Review
Biochemistry & Molecular Biology
Rafayel Petrosyan, Abhishek Narayan, Michael T. Woodside
Summary: Single-molecule force spectroscopy (SMFS) is a powerful tool for studying protein folding dynamics, uncovering energy landscapes of folding, complex folding pathways, mechanisms of chaperones in assisting folding, effects of ribosomes on co-translational folding, and monitoring membrane protein folding.
JOURNAL OF MOLECULAR BIOLOGY
(2021)
Article
Chemistry, Physical
Kevin Song, Dmitrii E. Makarov, Etienne Vouga
Summary: Single-molecule and single-particle tracking experiments often cannot accurately measure thermal motion details on short timescales due to continuous trajectories. We demonstrate that the error in measuring the first passage time to a specific domain can be significantly larger than the time resolution when a diffusive trajectory xt is sampled at finite time intervals delta t. This error arises from unobserved trajectory entries and exits, which artificially lengthen the apparent first passage time by more than delta t. These systematic errors are particularly important in single-molecule studies of barrier crossing dynamics. However, we show that the correct first passage times and other trajectory properties can be recovered using a stochastic algorithm that reintroduces unobserved first passage events probabilistically.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Analytical
Xueping Yang, Jingyun Li, Suixin Zhang, Chao Li, Jiehua Ma
Summary: CRISPR/Cas-based systems have intrinsic merits for developing diagnostic technologies, but nucleic acid amplification is still required for high sensitivity. This study presents a one-step and amplification-free detection method using Cas12a-based assay and a single-microbead detection platform, which allows single-molecule level detection of DNA. The method has been successfully applied for specific identification in real samples without extra nucleic acid amplification.
ANALYTICAL CHEMISTRY
(2022)
Article
Chemistry, Analytical
Hong Sun, Chuan Yao, Kaibo You, Can Chen, Shuoshuo Liu, Zhihong Xu
Summary: In this study, a dynamic monitoring approach based on nanopore single-molecule biosensor was developed to detect the folding and unfolding transitions of proteins. By gradually increasing the concentration of denaturant guanidine hydrochloride (GdmCl), sensitive responses were observed with lysozyme unfolding. The existence of a stable intermediate was experimentally confirmed, providing insights into the conformation of the intermediate and the manner of denaturant towards lysozyme.
ANALYTICA CHIMICA ACTA
(2023)
Article
Optics
H-H Boltz, A. Sirbu, N. Stelzer, M. J. Lohse, C. Schuette, P. Annibale
Summary: Single molecule fluorescence tracking offers nanometer-scale and millisecond-temporal resolution insights into dynamics and interaction of individual molecules in a biological environment, but faces limitations in quantitatively characterizing interactions between indistinguishable molecules. A theoretical foundation for spectroscopy of interaction times is developed to infer interactions from imaging data, highlighting a non-trivial crossover between power law and exponential behavior in the distribution of interaction times, depending on microscopic reaction affinity. Validation is done with simulated and experimental datasets.
Article
Multidisciplinary Sciences
Yi Wang, Zhuodong Tang, Hong-Yuan Chen, Wei Wang, Nongjian Tao, Hui Wang
Summary: A nanoparticle-based technique has been developed to probe the energetic contributions of single-molecule binding events, introducing a single-molecule calorimeter that uncovers the complexity of molecular interactions and provides a comprehensive thermodynamic profile.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Chemistry, Physical
Ruizheng Hou, Zhisong Wang
Summary: This study introduces a method to deduce the effective potential from motor trajectories and finds that it can yield a motor's stall force. This finding reduces the difficulty of stall force measurement and provides a method for measuring an important quantity relevant to efficient energy conversion of molecular motors.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Review
Chemistry, Analytical
Elba Mauriz, Laura M. Lechuga
Summary: This review summarizes the latest advances in plasmonic technologies for monitoring clinically relevant biomarkers at the single-molecule level, discussing design and functional applications targeting individual molecules, and a wide variety of analytes involved in new analytical developments. It also provides an overview of the utility of plasmonic-based single-molecule analysis for personalized medicine.
Article
Multidisciplinary Sciences
Devin T. Edwards, Marc-Andre Leblanc, Thomas T. Perkins
Summary: Single-molecule force spectroscopy was used to study protein folding dynamics, revealing intrinsic changes in protein folding dynamics and transition state height under different pH conditions. Despite differences in destabilization mechanisms, constant-force landscapes showed minimal differences in transition state height, while force-dependent rates increased as pH decreased. This study provides insights for future AFM-based studies of mechanoresponsive proteins.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Physics, Multidisciplinary
Yu-Hang Zhang, Zhen-Yong Xue, Hao Sun, Zhu-Wei Zhang, Hu Chen
Summary: There are significant differences in mechanical stability and unfolding dynamics among proteins with different structural compositions. Magnetic tweezers, which can precisely control forces on a pico-Newton scale, are suitable to measure force-induced conformation transitions of proteins. In this study, ACBP was stretched using magnetic tweezers and the unfolding forces at different loading rates were measured. The results showed that ACBP has an extraordinarily long unfolding distance and unfolding of α-helices is less cooperative than β-sheet structures.
ACTA PHYSICA SINICA
(2023)
Review
Chemistry, Multidisciplinary
Stefano Gianni, Maria Ines Freiberger, Per Jemth, Diego U. Ferreiro, Peter G. Wolynes, Monika Fuxreiter
Summary: Proteins and their complexes can be described as ensembles that populate an energy landscape, where the diversity arises from the conflicts between interactions shaping the energy landscape. Within this framework, alternative sets of suboptimal contacts can encode specificity without achieving a single structural optimum. The interplay between frustration and fuzziness offers insights into the structural and dynamical continuum of protein assemblies.
ACCOUNTS OF CHEMICAL RESEARCH
(2021)
Article
Multidisciplinary Sciences
Hao Yu, Derek R. Dee, Xia Liu, Angela M. Brigley, Iveta Sosova, Michael T. Woodside
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2015)
Article
Multidisciplinary Sciences
Krishna Neupane, Daniel A. N. Foster, Derek R. Dee, Hao Yu, Feng Wang, Michael T. Woodside
Article
Multidisciplinary Sciences
Hao Yu, Matthew G. W. Siewny, Devin T. Edwards, Aric W. Sanders, Thomas T. Perkins
Article
Chemistry, Physical
Patrick R. Heenan, Hao Yu, Matthew G. W. Siewny, Thomas T. Perkins
JOURNAL OF CHEMICAL PHYSICS
(2018)
Article
Physics, Multidisciplinary
Amar Nath Gupta, Abhilash Vincent, Krishna Neupane, Hao Yu, Feng Wang, Michael T. Woodside
Article
Biochemistry & Molecular Biology
Krishna Neupane, Hao Yu, Daniel A. N. Foster, Feng Wang, Michael T. Woodside
NUCLEIC ACIDS RESEARCH
(2011)
Article
Biochemistry & Molecular Biology
Hao Yu, Derek R. Dee, Michael T. Woodside
Article
Multidisciplinary Sciences
Hao Yu, Xia Liu, Krishna Neupane, Amar Nath Gupta, Angela M. Brigley, Allison Solanki, Iveta Sosova, Michael T. Woodside
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2012)
Article
Multidisciplinary Sciences
Hao Yu, Amar Nath Gupta, Xia Liu, Krishna Neupane, Angela M. Brigley, Iveta Sosova, Michael T. Woodside
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2012)
Article
Chemistry, Multidisciplinary
Hao Yu, Patrick R. Heenan, Devin T. Edwards, Lyle Uyetake, Thomas T. Perkins
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2019)