Article
Chemistry, Physical
Linyu Yan, Chu Li, Meng Li, Shuqi Mu, Kebin Shi, Qihuang Gong, Yan Li
Summary: This study experimentally verifies the ultrafast coherent energy transport among chlorophyll molecules inside the FMO complex and uncovers its dynamic process. The high similarities between experimental and theoretical results demonstrate precise control of the photonic lattices. These findings contribute to a deeper understanding of the mechanism and have significant applications in artificial light energy transport.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Multidisciplinary Sciences
Hong-Guang Duan, Ajay Jha, Lipeng Chen, Vandana Tiwari, Richard J. Cogdell, Khuram Ashraf, Valentyn I. Prokhorenko, Michael Thorwart, R. J. Dwanye Miller
Summary: Scientists have discovered that electronic coherence in light harvesting can be prolonged at extremely low temperatures, increasing the stability of the process against fragile quantum effects.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Physical
Ellen Mulvihill, Kristina M. Lenn, Xing Gao, Alexander Schubert, Barry D. Dunietz, Eitan Geva
Summary: The M-GQME approach captures the effect of nuclear degrees of freedom on the time evolution of the electronic density matrix through a memory kernel superoperator, providing accurate results in predicting energy transfer dynamics in complex molecular systems.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Zhe Huai, Zhengqing Tong, Ye Mei, Yan Mo
Summary: This study investigated the spectral differences between Fenna-Matthews-Olson proteins from C. tepidum and P. aestuarii mutants, revealing that a single-point mutation near BChl 6 can significantly affect the absorption spectrum and excitonic structures of neighboring pigments. The results are consistent with previous experiments and indicate the critical role of protein scaffold in modulating optical properties.
JOURNAL OF PHYSICAL CHEMISTRY B
(2021)
Article
Quantum Science & Technology
Zixuan Hu, Kade Head-Marsden, David A. Mazziotti, Prineha Narang, Sabre Kais
Summary: This paper introduces the research on using quantum algorithms to simulate complex physical processes and demonstrates the simulation of the dynamics of the FMO complex using a quantum algorithm. The study shows that quantum methods have a query complexity advantage in addressing open quantum dynamics.
Article
Chemistry, Physical
Yongbin Kim, Zach Mitchell, Jack Lawrence, Dmitry Morozov, Sergei Savikhin, Lyudmila V. Slipchenko
Summary: Multiscale molecular modeling is used to predict the optical absorption and circular dichroism spectra of two single-point mutants of the Fenna-Matthews-Olson photosynthetic pigment-protein complex. The modeling approach combines classical molecular dynamics simulations, structural refinement of photosynthetic pigments, and calculations of their excited states in a polarizable protein environment. The modeling demonstrates that a single-point mutation can induce long-range effects on the protein structure and that extensive structural changes near a pigment do not necessarily lead to significant changes in the electronic properties of that pigment.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Biochemistry & Molecular Biology
Francisco Delgado, Marco Enriquez
Summary: Fenna-Mathews-Olson complexes play a role in the photosynthetic process of Sulfur Green Bacteria, exhibiting quantum features such as multipartite entanglement and apparent tunnelling. A multidisciplinary approach involving experimental biology, spectroscopy, physics, and math modelling is required to study these aspects. The Hierarchical Equations of Motion are used to solve the open quantum system problem and a new measure of multipartite entanglement is employed. The study provides new insights into FMO multipartite entanglement and tracks the dynamical evolution of the initial state.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Article
Chemistry, Physical
XueYan Cui, YiJing Yan, JianHua Wei
Summary: This study investigates the impact of pigment-protein coupling on the dynamics of photosynthetic energy transport in chromophoric complexes, revealing that the heterogeneous local protein environment affects the excitation energy transfer process and leads to asymmetric excitation oscillation timescales at different pigment sites. The results suggest that the interaction between excited chromophores and their environment plays a critical role in coherent energy-transfer processes, with quantum dynamical simulations showing sustained oscillations of coherent excitation on a long timescale.
JOURNAL OF PHYSICAL CHEMISTRY B
(2021)
Article
Chemistry, Physical
Zhubin Hu, Zengkui Liu, Xiang Sun
Summary: The heterogeneous protein environment in the FMO complex of green sulfur bacteria affects excitation energy transfer. A more realistic model shows slower energy transfer dynamics than the traditional model. Larger reorganization energy, heterogeneity in spectral densities, and low-frequency modes facilitate energy dissipation.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Physical
Xuan Leng, Peng Lei, Wen-zhao Zhang
Summary: The absorption and two-dimensional rephasing spectra of the Fenna-Matthews-Olson (FMO) complex at 77K were simulated using hierarchical equations of motion method. Three cases of vibrational coupling were studied in the FMO complex model, showing that the vibrational mode significantly weakens the intensity of the absorption peak of high-energy electronic transitions. It was also observed that long-lived quantum beatings originate from vibration, while short-lived electronic coherence still exists. Furthermore, the speed-up of rephasing dynamics by electronic resonance mode is not directly proportional to the coupling strength, and the low-energy electronic-vibrational resonance dimer exhibits a greater speed-up.
Article
Chemistry, Physical
Maxim F. Gelin, Raffaele Borrelli
Summary: A fully quantum, numerically accurate wave function-based approach for calculating third-order spectroscopic signals of polyatomic molecules and molecular aggregates at finite temperature has been developed. The approach, based on Thermo Field Dynamics (TFD) representation and tensor-train (TT) machinery, efficiently simulates the quantum evolution of systems with many degrees of freedom. The developed approach has been applied to calculate time- and frequency-resolved fluorescence spectra of the Fenna-Matthews-Olson (FMO) antenna complex at room temperature, considering various factors such as finite resolution, orientational averaging, and static disorder.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2021)
Proceedings Paper
Quantum Science & Technology
B. Gonzalez-Soria, F. Delgado
Summary: The high efficiency of excitation energy transfer in the Fenna-Matthews-Olson light-harvesting complex in green sulfur bacteria is determined by its array of bacteriochlorophylls, which are central to the photosynthetic process of these bacteria and controversially associated with long-lived coherence. This study investigates the temperature effects on entanglement and coherence in bacteriochlorophyll excitation energy transfer within the Fenna-Matthews-Olson complex, considering the latest arrangement of 8 bacteriochlorophylls. The Hierarchical Equations of Motion method is used to analyze the system evolution and obtain the global and semi-local entanglement, as well as coherence in the system.
INTERNATIONAL CONFERENCE ON QUANTUM PHENOMENA, QUANTUM CONTROL AND QUANTUM OPTICS, QUANTUM FEST 2021
(2023)
Article
Optics
Peter Schnauber, Jan Grosse, Arsenty Kaganskiy, Maximilian Ott, Pavel Anikin, Ronny Schmidt, Sven Rodt, Stephan Reitzenstein
Summary: The deterministic integration of self-assembled quantum dots in waveguide structures has been achieved using in situ electron beam lithography. Spectral fine-tuning of the QDs has been achieved by applying external bias voltages, with the potential to enable the scalable fabrication of integrated quantum photonic circuits in the future.
Article
Biochemistry & Molecular Biology
Katharine A. Michie, Stephen J. Harrop, Harry W. Rathbone, Krystyna E. Wilk, Chang Ying Teng, Kerstin Hoef-Emden, Roger G. Hiller, Beverley R. Green, Paul M. G. Curmi
Summary: In addition to the membrane-bound light-harvesting antenna, the cryptophyte algae have a unique antenna system located in the thylakoid lumen. This antenna system consists of alpha beta protomers with different combinations of chromophores. The diversity of the alpha subunit gene family produces a range of antenna proteins with differing spectral properties.
Article
Physics, Multidisciplinary
Gabriele Riva, Timothee Audinet, Matthieu Vladaj, Pina Romaniello, J. Arjan Berger
Summary: This article presents an original strategy for calculating direct and inverse photoemission spectra from first principles. The main goal is to go beyond standard Green's function approaches and accurately describe both quasiparticles and satellite structures in strongly correlated materials. The authors use the three-body Green's function as a key quantity and demonstrate how to retrieve the one-body Green's function from it. They also find that satellite information is already present in the non-interacting three-body Green's function and that simple approximations to the three-body self-energy can yield accurate spectral functions.
Article
Chemistry, Physical
Julian Adolphs, Franziska Maier, Thomas Renger
JOURNAL OF PHYSICAL CHEMISTRY B
(2018)
Article
Chemistry, Physical
Parveen Akhtar, Dominik Lindorfer, Monika Lingvay, Krzysztof Pawlak, Otto Zsiros, Giuliano Siligardi, Tamas Javorfi, Marta Dorogi, Bettina Ughy, Gyozo Garab, Thomas Renger, Petar H. Lambrev
JOURNAL OF PHYSICAL CHEMISTRY B
(2019)
Article
Chemistry, Physical
Lorenzo Cupellini, Stefano Caprasecca, Ciro A. Guido, Frank Mueh, Thomas Renger, Benedetta Mennucci
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2018)
Article
Chemistry, Physical
Alexander Klinger, Dominik Lindorfer, Frank Muh, Thomas Renger
JOURNAL OF CHEMICAL PHYSICS
(2020)
Article
Chemistry, Physical
Marten L. Chaillet, Florian Lengauer, Julian Adolphs, Frank Muh, Alexander S. Fokas, Daniel J. Cole, Alex W. Chin, Thomas Renger
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2020)
Article
Chemistry, Multidisciplinary
Svetoslav Nakov, Ekaterina Sobakinskaya, Thomas Renger, Johannes Kraus
Summary: An adaptive finite element solver for calculating electrostatic coupling between molecules in a solvent environment was developed and tested. The new solver, ARGOS, demonstrated significantly improved precision and computational efficiency compared to standard finite difference solvers, as confirmed through numerical experiments on problems with known solutions. The solver was also used to calculate electrostatic interactions between various molecules, showcasing its advantages over existing solvers like MEAD and APBS.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2021)
Article
Chemistry, Physical
Thomas Renger
Summary: A conceptual issue in transfer theories using semiclassical descriptions of electron-vibrational coupling is the neglect of correlation between nuclear momenta and coordinates, leading to violations of detailed balance principles and equal transfer rate constants obtained uphill and downhill. Reorganization effects due to partial localization of excited states promote preferential downhill relaxation of excitation energy, but are too small to compensate for missing coordinate-momentum uncertainty in realistic spectral densities of light-harvesting antennae. Semiclassical variants of generalized Forster theory fulfill detailed balance principles in weakly coupled pigment domains, providing qualitatively correct transfer descriptions at lower computational costs compared to quantum counterparts.
JOURNAL OF PHYSICAL CHEMISTRY B
(2021)
Article
Chemistry, Physical
Christian Friedl, Dmitri G. Fedorov, Thomas Renger
Summary: This study combines fragment molecular orbital method and polarizable continuum model to calculate excitonic couplings between photosynthetic pigments. By calibrating the vacuum dipole strength, excellent agreement between calculated and experimental results is obtained. In addition, an expression for estimating Huang-Rhys factors of high-frequency pigment vibrations is presented, and the small impact of these factors on pigment transitions is found.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Multidisciplinary Sciences
F. Caycedo-Soler, A. Mattioni, J. Lim, T. Renger, S. F. Huelga, M. B. Plenio
Summary: Numerically exact simulations reveal that multimode vibronic mixing in model photosynthetic systems strongly affects optical responses and facilitates coherent dynamics. The generation, transport, and trapping of excitons in pigment-protein complexes (PPCs) are crucial for photosynthesis. The inclusion of full multi-mode vibronic dynamics in numerical calculations of linear spectra leads to significant corrections to electronic parameter estimation. These effects are relevant to the discussion on the origin of long-lived oscillations in multidimensional nonlinear spectra.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Vladislav Slama, Frank Mueh, Thomas Renger, Torng Mancal
Summary: We proposed an extension of the QM/MM approach to investigate the excited state properties of embedded systems under environmental effects. Our model, based on perturbation theory, allows a more general description of the environment, considering frequency-dependent atomic polarizabilities. By comparing with full quantum chemistry calculations and standard polarizable QM/MM approach, we demonstrated the importance of frequency dependence for accurately treating the effects of the environment on transition energy shifts and interaction energies.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Biochemistry & Molecular Biology
Ferdinand Horvath, Sascha Berlansky, Lena Maltan, Herwig Grabmayr, Marc Fahrner, Isabella Derler, Christoph Romanin, Thomas Renger, Heinrich Krobath
Summary: STIM1 is a protein located in the endoplasmic reticulum (ER) membrane that senses the concentration of calcium ions and plays a role in the activation of calcium channels. Through molecular docking simulations, a structural model of the resting state of STIM1 was established, and the binding interface was analyzed using molecular dynamics simulations. Experimental results confirmed the validity of the model and provided insights into the conformational dynamics of the resting state of STIM1.
Editorial Material
Chemistry, Physical
Graham R. Fleming, Jun Minagawa, Thomas Renger, Gabriela S. Schlau-Cohen
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Lea Ress, Pavel Maly, Jann B. Landgraf, Dominik Lindorfer, Michael Hofer, Joshua Selby, Christoph Lambert, Thomas Renger, Tobias Brixner
Summary: This article presents the experimental and theoretical foundations for femtosecond time-resolved circular dichroism (TRCD) spectroscopy of excitonic systems. A new experimental setup, with a polarization grating as the key element, is introduced to generate circularly polarized pulses for TRCD experiments. By applying a specific chopping scheme, left and right circular polarizations can be switched, and transient absorption (TA) and TRCD spectra can be detected simultaneously. Experiments on a squaraine polymer are performed to investigate excitonic dynamics, and a general theory for TRCD experiments of excitonically coupled systems is developed and applied to describe the experimental data.
Article
Chemistry, Physical
Alexander Klinger, Dominik Lindorfer, Frank Muh, Thomas Renger
Summary: Photosynthetic green sulfur bacteria can survive under extreme low light conditions. However, the light-harvesting efficiencies of Fenna-Matthews-Olson (FMO) protein-reaction center complex (RCC) supercomplexes are lower than those of photosystems in other species. This study presents evidence for a light-harvesting efficiency of around 95% under native anaerobic conditions, which can drop to 47% when the FMO protein switches to a photoprotective mode in the presence of molecular oxygen. Light-harvesting bottlenecks are observed between the FMO protein and the RCC, and between the antenna of the RCC and its reaction center, with forward energy transfer time constants of 39 ps and 23 ps, respectively.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Ekaterina Sobakinskaya, Heinrich Krobath, Thomas Renger, Frank Mueh
Summary: The SecYEG translocon in bacteria serves as a channel for protein transport while preventing water and ion leakage through the membrane. The pore ring (PR) plays a crucial role in maintaining a tight seal for the wild-type translocon, with hydrophobic interactions within the PR and between the PR and the plug being important for channel stability.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
