Coherence Vibrations and Electronic Excitation Dynamics in Molecular Aggregates and Photosynthetic Pigment-Proteins
|
|
- Jean Loren Powell
- 5 years ago
- Views:
Transcription
1 VILNIUS UNIVERSITY Coherence Vibrations and Electronic Excitation Dynamics in Molecular Aggregates and Photosynthetic Pigment-Proteins L. Valkunas Department of Theoretical Physics, Faculty of Physics, Vilnius University, Institute of Physics, Center for Physical Sciences and Technology, Vilnius Lithuania
2 Contents Coherent vs. Incoherent Processes Coherences and oscillations in 2D ES Model systems Coupled two-level systems (electronic dimer) Displaced harmonic oscillator Coupled displaced harmonic oscillators (molecular dimer) Real stuff PSII RC, FCP
3 Energy transfer and charge separation
4 Resonance of energy transfer Electronic excited state Vibronic states Resonance energy transfer to nearby molecule Electronic ground state Molecule 1 Molecule 2
5 Are excitons the excitons? The system evolves into new equilibrium with respect to the excited system configuration. The initial exciton becomes not the eigenstate A. Gelzinis, D. Abramavicius, L. Valkunas, Phys. Rev. B. 84, , 2011.
6 Are excitons the excitons? The systems evolves into new equilibrium with respect to the excited system configuration. The initial exciton becomes not the eigenstate Absorption A. Gelzinis, D. Abramavicius, L. Valkunas, Phys. Rev. B. 84, , 2011.
7 Are excitons the excitons? The systems evolves into new equilibrium with respect to the excited system configuration. The initial exciton becomes not the eigenstate Emission A. Gelzinis, D. Abramavicius, L. Valkunas, Phys. Rev. B. 84, , 2011.
8 Are excitons the excitons? The system evolves into new equilibrium with respect to the excited system configuration. The initial exciton becomes not the eigenstate Emission A. Gelzinis, D. Abramavicius, L. Valkunas, Phys. Rev. B. 84, , 2011.
9 Are excitons the excitons? The system evolves into new equilibrium with respect to the excited system configuration. The initial exciton becomes not the eigenstate Mixed picture where all excitons are more localized Emission A. Gelzinis, D. Abramavicius, L. Valkunas, Phys. Rev. B. 84, , 2011.
10 Search for the preferred basis The exciton basis is given by: The global basis is different: The density matrix is diagonal in the global basis at equilibrium What happens in the molecular representation? EFFECTIVE PARAMETERS A. Gelzinis, D. Abramavicius, L. Valkunas, Phys. Rev. B. 84, , 2011.
11 The effective polaronic Hamiltonian The real effective Hamiltonian is a function of the system-bath coupling Initial excitons are no longer relevant A. Gelzinis, D. Abramavicius, L. Valkunas, Phys. Rev. B. 84, , 2011.
12 Absorption lineshape calculations A. Gelzinis, D. Abramavicius, L. Valkunas, J. Chem. Phys. 142, , 2015.
13 Different levels of theory for off-diagonal fluctuations A. Gelzinis, D. Abramavicius, L. Valkunas, J. Chem. Phys. 142, , 2015.
14 Coherence vs. Incoherence
15 FMO G. S. Engel et al. Nature 446, 782 (2007) G. Panitchayangkoon et al. PNAS 107, (2010)
16 Scheme 2D photon echo spectroscopy (3) (3) r P (, t) dt dt dt S ( t, t, t ) E( r, t t ) E( r, t t t ) E( r, t t t t )
17 Classification of third order techniques: Possible phase-matching directions: ks u k u k u k Assuming that each laser pulse interacts with the system only once, we get 4 linearly independent signals ki k k k rephasing non-rephasing kii k k k double quantum coherence k k k k III 1 2 3
18 Two-level system Inhomogeneous linewidth Homogeneous linewidth
19 Noninteracting molecules Two diagonal peaks present Peaks getting round shape due to losing correlation
20 Interacting molecules (a dimer) Excited state absorption Excitation relaxation
21 Quantum transport in 2D spectroscopy Diagonal peaks represent state populations Off-diagonal peaks are mixed: populations and coherences Off-diagonal oscillate due to quantum coherences this does not show quantum transport Exponential decay/rise of the diagonal peaks signify Classical Transport regime Oscillatory diagonal peaks signify Quantum Transport regime
22 Oscillation Fourier maps One contribution of the rephasing signal Phase and amplitude of oscillations is obtained by Fourier transform of time-dependent spectra, assuming no bath-induced relaxation and Green s function, gives Oscillating cross-peak: V. Butkus, D. Zigmantas, L. Valkunas, D. Abramavicius, CPL 545, 40 (2012)
23 Purely electronic/vibrational systems Vibrational monomer Vibrational monomer Electronic dimer Electronic dimer V. Butkus, D. Zigmantas, L. Valkunas, D. Abramavicius, CPL 545, 40 (2012)
24 Intensity Intensyvumas Intensity Intensity Oscillations in model systems (rephasing signal only) Cross-peak oscillations IN PHASE Diagonal elements Off-diagonal elements Population time (fs) Population time (fs) Diagonal elements Population time (fs) Population time (fs) Off-diagonal elements V. Butkus, D. Zigmantas, L. Valkunas, D. Abramavicius, CPL 545, 40 (2012)
25 Purely electronic/vibrational systems Vibrational monomer Electronic dimer V. Tiwari et al. PNAS 110 (2013) V. Butkus, D. Zigmantas, L. Valkunas, D. Abramavicius, CPL 545, 40 (2012)
26 Oscillation map in experiment Jan Alster Water-Soluble Chlorophyll-Binding Protein from Lepidium virginicum J. Alster, H. Jokstein, J. Dostàl, A. Uchida, D. Zigmantas, JPCB 118, 3524 (2014)
27 Time-resolved phenomena Coherent beats of vibrational degrees of freedom (internal structure of excitons) V. Butkus, D. Zigmantas, L. Valkunas, D. Abramavicius, CPL 545, 40 (2012)
28 Exciton vibronic Hamiltonian of a dimer Electronic basis of a dimer consists of a common ground state 0 and molecular excited states m = B m 0. Hamiltonian of a single molecule: A. Ground-state basis B. Shifted basis A. Of a dimer: B. E. Basinskaite, V. Butkus, D. Abramavicius, L. Valkunas, Photosynth. Res. 121, (2014)
29 Choosing the basis GS basis and shifted basis are equivalent from the physical point of view In the GS basis approach, a larger number vibrational levels have to be considered A. Ground-state basis B. Shifted basis H = A. B. 0 (11) 0 0 (22) 0 H = 0 0 (21) (12) 0 0 Multi-particle states e i g j first molecule is vibronically excited; second molecule is vibrationally excited g i e j first molecule is vibrationally excited; second molecule is vibronically excited One-particle approximation e i g 0 first molecule is vibronically excited; second molecule in zero-quantum GS. g 0 e j first molecule is in zero-quantum GS; second molecule is vibronically excited E. Basinskaite, V. Butkus, D. Abramavicius, L. Valkunas, Photosynth. Res. 121, (2014)
30 In which cases the one-particle approximation works? Let s consider linear absorption dependence on resonant coupling Multi-particle states Two-particle approx. Electronic Vibronic Huang-Rhys s=0.05 Huang-Rhys s=0.5 One-particle approximation (OPA) can be used to simulate stationary spectra with low values of Huang Rhys factor or large inhomogeneous broadening OPA fails completely if the system is in the vicinity of the exciton vibronic resonance Validity of OPA in calculations with different laser pulse polarizations is highly questionable OPA will not give oscillations associated to mixed coherences. E. Basinskaite, V. Butkus, D. Abramavicius, L. Valkunas, Photosynth. Res. 121, (2014)
31 Effects of the inhomogeneous disorder on coherences The amplitude of the electronic-character beats is dramatically reduced by the disorder Vibrational-character beats weakly depend on the disorder σ σ D =20 σ D =0 D =50 cm -1-1 ω 0 =600 cm -1 ΔE=850 cm -1 s 1 =s 2 =0.05 σ D =200 cm -1 V. Butkus, D. Zigmantas, D. Abramavicius, L. Valkunas, CPL 587, 93 (2013)
32 Amplitude dependence on disorder σ D =0 σ D =200 cm -1 V. Butkus, D. Zigmantas, D. Abramavicius, L. Valkunas, CPL 587, 93 (2013)
33 Tight binding hamiltonian A. Gelzinis et al. New J. Phys. 15, (2013)
34 CT pathways A. Gelzinis et al. New J. Phys. 15, (2013)
35 CT states A. Gelzinis et al. New J. Phys. 15, (2013)
36 Spectral density A. Gelzinis et al. New J. Phys. 15, (2013)
37 Absorption of PSII RC A. Gelzinis et al. New J. Phys. 15, (2013)
38 Monomer absorption A. Gelzinis et al. New J. Phys. 15, (2013)
39 PSII RC 2D at 77 K A. Gelzinis et al. New J. Phys. 15, (2013 A. Gelzinis et al. New J. Phys. 15, (2013)
40 PSII RC 2D at 77 K A. Gelzinis et al. New J. Phys. 15, (2013)
41 PSII RC 2D at 77 K A. Gelzinis et al. New J. Phys. 15, (2013)
42 Excited state energy distributions A. Gelzinis et al. New J. Phys. 15, (2013)
43 2D spectrum of the PSII RC at 77K at a waiting time of 170 fs. F. D. Fuller, J. Pan, A. Gelzinis, V. Butkus, S. S. Senlik, D. E. Wilcox, C. F. Yocum, L. Valkunas, D. Abramavicius, J. P. Ogilvie, Vibronic coherence in oxygenic photosynthesis. Nature Chemistry 6, (2014)
44 Excitonic states Physical origin of coherences Experiment Theory Vibronic Experiment Theory F. D. Fuller, J. Pan, A. Gelzinis, V. Butkus, S. S. Senlik, D. E. Wilcox, C. F. Yocum, L. Valkunas, D. Abramavicius, J. P. Ogilvie, Vibronic coherence in oxygenic photosynthesis. Nature Chemistry 6, (2014)
45 Spectral density Population of CT state Enhancement of the charge transfer Separated charges Ground state CT state Excitonic splittings After the excitation, the electron appears in the initial state A. The transition along overdamped and underdamped coordinates are indicated as states B, C and D. The charge transfer may take place at any time while the most probable event happens in the state D. D. Abramavicius et al. Acceleration of charge separation by oscillations of the environment polarization. Chem Phys Lett 368 (2003) F. D. Fuller, J. Pan, A. Gelzinis, V. Butkus, S. S. Senlik, D. E. Wilcox, C. F. Yocum, L. Valkunas, D. Abramavicius, J. P. Ogilvie, Vibronic coherence in oxygenic photosynthesis. Nature Chemistry 6, (2014)
46 Enhancement of charge transfer D. Abramavicius, L. Valkunas, Photosynth. Res. (2015)
47 Fucoxanthin-chlorophyll protein - FCP V. Butkus et al. JCP 142 (2015)
48 FCP absorption V. Butkus et al. JCP 142 (2015)
49 V. Butkus et al. JCP 142 (2015)
50 Oscillation frequencies V. Butkus et al. JCP 142 (2015)
51 Fourier maps V. Butkus et al. JCP 142 (2015)
52 Proposed pigment arrangement V. Butkus et al. JCP 142 (2015)
53 Conclusions Two types of oscillations of either vibronic or electronic character can be distinguished by the use of Fourier oscillation maps, constructed from the sequences of time-resolved 2D spectra. Inhomogeneous disorder influences vibronic/electronic coherences differently. Vibrational coherences evolving in the ground state and vibronic coherences in the excited state are equally significant.
54 Acknowledgements Vilnius: Michigan: Saclay: D. Abramavicius J. P. Ogilvie B. Robert V. Butkus F. D. Fuller A. Gall A. Gelzinis Lund: Frankfurt: R. Augulis D. Zigmantas C. Büchel E. Basinskaite Financial support LSC grant no: VP1-3.1-ŠMM-07-K
Photosynthesis provides the energy source for essentially all lifes on Earth. The molecular details of photosynthesis are not yet fully elucidated
Photosynthesis provides the energy source for essentially all lifes on Earth The molecular details of photosynthesis are not yet fully elucidated Remarkable efficiency of photosynthesis processes is not
More informationDiversity of coherences and origin of electronic transitions of supermolecular nanoring
Diversity of coherences and origin of electronic transitions of supermolecular nanoring Fenna Matthews Olson (FMO) light-harvesting complex (whether electronic[4] or vibrational[2, 11, 12]) still causes
More informationSUPPLEMENTARY INFORMATION
Vibronic Coherence in Oxygenic Photosynthesis Franklin D. Fuller 1, Jie Pan 1, Andrius Gelzinis 2,, Vytautas Butkus 2,, S. Seckin Senlik 1, Daniel E. Wilcox 1, Charles F. Yocum 4, Leonas Valkunas 2,, Darius
More informationUltrafast 2D Spectroscopy of Photosynthetic Light-Harvesting Complexes
Ultrafast 2D Spectroscopy of Photosynthetic Light-Harvesting Complexes PETAR LAMBREV PREAMBLE LASERS IN LIFE SCIENCE LASERS IN MEDICINE AND LIFE SCIENCE, SZEGED 2017 2 Preamble LASERS IN MEDICINE AND LIFE
More information5.74 Introductory Quantum Mechanics II
MIT OpenCourseWare http://ocw.mit.edu 5.74 Introductory Quantum Mechanics II Spring 009 For information about citing these materials or our Terms of Use, visit: http://ocw.mit.edu/terms. Andrei Tokmakoff,
More informationInhomogeneous Broadening Induced Long-Lived Integrated Two- Color Coherence Photon Echo Signal
pubs.acs.org/jpcb Inhomogeneous Broadening Induced Long-Lived Integrated Two- Color Coherence Photon Echo Signal Hui Dong and Graham R. Fleming* Department of Chemistry, University of California, Berkeley,
More informationCorrelation spectroscopy
1 TWO-DIMENSIONAL SPECTROSCOPY Correlation spectroscopy What is two-dimensional spectroscopy? This is a method that will describe the underlying correlations between two spectral features. Our examination
More informationPRINCIPLES OF NONLINEAR OPTICAL SPECTROSCOPY
PRINCIPLES OF NONLINEAR OPTICAL SPECTROSCOPY Shaul Mukamel University of Rochester Rochester, New York New York Oxford OXFORD UNIVERSITY PRESS 1995 Contents 1. Introduction 3 Linear versus Nonlinear Spectroscopy
More information5.74 Introductory Quantum Mechanics II
MIT OpenCourseWare http://ocw.mit.edu 5.74 Introductory Quantum Mechanics II Spring 009 For information about citing these materials or our Terms of Use, visit: http://ocw.mit.edu/terms. Andrei Tokmakoff,
More informationSupplementary Information Direct Observation of the Ultrafast Exciton Dissociation in Lead-iodide Perovskite by 2D Electronic Spectroscopy
Supplementary Information Direct Observation of the Ultrafast Exciton Dissociation in Lead-iodide Perovskite by 2D Electronic Spectroscopy Ajay Jha 1, Hong-Guang Duan 1,2,3, Vandana Tiwari 1,4, Pabitra
More informationPathways of Energy Flow in LHCII from Two-Dimensional Electronic Spectroscopy
15352 J. Phys. Chem. B 2009, 113, 15352 15363 Pathways of Energy Flow in LHCII from Two-Dimensional Electronic Spectroscopy Gabriela S. Schlau-Cohen,, Tessa R. Calhoun,, Naomi S. Ginsberg,, Elizabeth L.
More informationAndrei V. Pisliakov, Tomáš Manal, and Graham R. Fleming
Two-dimensional optical three-pulse photon echo spectroscopy. II. Signatures of coherent electronic motion and exciton population transfer in dimer two-dimensional spectra Andrei V. Pisliakov, Tomáš Manal,
More information5.74 Introductory Quantum Mechanics II
MIT OpenCourseWare http://ocw.mit.edu 5.74 Introductory Quantum Mechanics II Spring 2009 For information about citing these materials or our Terms of Use, visit: http://ocw.mit.edu/terms. p. 10-0 10..
More informationQuantum dynamics in complex environments towards biological and nanostructured systems
Quantum dynamics in complex environments towards biological and nanostructured systems Chris Engelbrecht Summer School on Quantum Biology Lecture 4 Irene Burghardt Department of Physical and Theoretical
More informationLinear and nonlinear spectroscopy
Linear and nonlinear spectroscopy We ve seen that we can determine molecular frequencies and dephasing rates (for electronic, vibrational, or spin degrees of freedom) from frequency-domain or timedomain
More informationELECTRONIC AND VIBRATIONAL COHERENCE IN PHOTOSYNTHETIC COFACTORS: COMPARISON OF SOLUTIONS AND PROTEINS
Laser Chem., 1999, Vol. 19, pp. 195-199 Reprints available directly from the publisher Photocopying permitted by license only 0 1999 OPA (Overseas Publishers Association) N.V. Published by license under
More informationarxiv: v2 [physics.chem-ph] 2 Jul 2012
arxiv:15.3383v [physics.chem-ph] Jul 1 Molecular vibrations-induced quantum beats in two-dimensional electronic spectroscopy Vytautas Butkus, 1, Leonas Valkunas, 1, 1,3, a) and Darius Abramavicius 1) Department
More information11.6. TWO-DIMENSIONAL CORRELATION SPECTROSCOPY
Andrei Tokmakoff, MIT Department of Chemistry, 6/5/009 p. -54.6. TWO-DIMENSIONAL CORRELATION SPECTROSCOPY Our examination of pump-probe experiments indicates that the third-order response reports on the
More informationQuantum Coherence in Photosynthesis for Efficient Solar Energy Conversion
Europe PMC Funders Group Author Manuscript Published in final edited form as: Nat Phys. 2014 September 1; 10(9): 676 682. doi:10.1038/nphys3017. Quantum Coherence in Photosynthesis for Efficient Solar
More informationLight Harvesting Complexes
Light Harvesting Complexes a Multicromophoric approach to describe the energy transfer Gianluca Costagliola University of Turin, INFN 12 febbraio 2014 Photosynthesis: an overview It s one of the most important
More informationElectronic coherence transfer in photosynthetic complexes and its signatures in optical spectroscopy
Spectroscopy 22 (2008) 199 211 199 DOI 10.3233/SPE-2008-0334 IOS Press Electronic coherence transfer in photosynthetic complexes and its signatures in optical spectroscopy Tomáš Mančal a,,leonasvalkunas
More informationCharge and Energy Transfer Dynamits in Molecular Systems
Volkhard May, Oliver Kühn Charge and Energy Transfer Dynamits in Molecular Systems Second, Revised and Enlarged Edition WILEY- VCH WILEY-VCH Verlag GmbH & Co. KGaA Contents 1 Introduction 19 2 Electronic
More informationdoi: /nature22012 Humankind is facing an energy challenge: the urgent need to
2017MacmilanPublishersLimited,partofSpringerNature.AlrightQuantum design of photosynthesis for bio-inspired solar-energy conversion Elisabet Romero 1, Vladimir I. Novoderezhkin 2 & Rienk van Grondelle
More informationDirect evidence of quantum transport in photosynthetic light-harvesting complexes
Direct evidence of quantum transport in photosynthetic light-harvesting complexes Gitt Panitchayangkoon a,, Dmitri V. Voronine b,, Darius Abramavicius c,d, Justin R. Caram a, Nicholas H. C. Lewis a, Shaul
More informationModern Optical Spectroscopy
Modern Optical Spectroscopy With Exercises and Examples from Biophysics and Biochemistry von William W Parson 1. Auflage Springer-Verlag Berlin Heidelberg 2006 Verlag C.H. Beck im Internet: www.beck.de
More informationTwo-Color three-pulse Photon Echoes
Two-Color three-pulse Photon Echoes Intensity (normalized) 1 0.8 0.6 0.4 0.2 IR144 in Methanol 0 600 650 700 750 800 850 900 Wavelength (nm) 1 Intensity (normalized) 0.8 0.6 0.4 0.2 DTTCI in Methanol 0
More informationAn Open System Dynamics Approach for Polyatomic Molecules: Excitons in Chromophore Complexes
An Open System Dynamics Approach for Polyatomic Molecules: Excitons in Chromophore Complexes Volkhard May, Institute of Physics, Humboldt-University at Berlin Thanks to: Ben Brüggemann (Lund) Tomas Mancal
More informationCoherent or hopping like energy transfer in the chlorosome? Peter Nalbach
Coherent or hopping like energy transfer in the chlorosome? Peter Nalbach Photosynthesis 2 Photosynthesis Energy transfer incoherent Förster type or quantum coherent? Incoherent Förster type Strong environmental
More informationLong-lived quantum coherence in photosynthetic complexes at physiological temperature
Long-lived quantum coherence in photosynthetic complexes at physiological temperature Gitt Panitchayangkoon 1, Dugan Hayes 1, Kelly A. Fransted 1, Justin R. Caram 1, Elad Harel 1, Jianzhong Wen 2, Robert
More informationFundamentals of Spectroscopy for Optical Remote Sensing. Course Outline 2009
Fundamentals of Spectroscopy for Optical Remote Sensing Course Outline 2009 Part I. Fundamentals of Quantum Mechanics Chapter 1. Concepts of Quantum and Experimental Facts 1.1. Blackbody Radiation and
More informationVibronic quantum dynamics of exciton relaxation/trapping in molecular aggregates
Symposium, Bordeaux Vibronic quantum dynamics of exciton relaxation/trapping in molecular aggregates Alexander Schubert Institute of Physical and Theoretical Chemistry, University of Würzburg November
More informationarxiv: v1 [physics.chem-ph] 16 Mar 2018
arxiv:803.06389v [physics.chem-ph] 6 Mar 208 Mechanistic Regimes of Vibronic Transport in a Heterodimer and the Design Principle of Incoherent Vibronic Transport in Phycobiliproteins Doran I. G. Bennett,,,
More informationMulti-Dimensional IR Spectroscopy of Acetic Acid Dimers and Liquid Water
Multi-Dimensional IR Spectroscopy of Acetic Acid Dimers and Liquid Water N. Huse 1, J. Dreyer 1, E.T.J.Nibbering 1, T. Elsaesser 1 B.D. Bruner 2, M.L. Cowan 2, J.R. Dwyer 2, B. Chugh 2, R.J.D. Miller 2
More informationSpectroscopy in frequency and time domains
5.35 Module 1 Lecture Summary Fall 1 Spectroscopy in frequency and time domains Last time we introduced spectroscopy and spectroscopic measurement. I. Emphasized that both quantum and classical views of
More informationLong-lived quantum coherence in photosynthetic complexes at physiological temperature
Long-lived quantum coherence in photosynthetic complexes at physiological temperature Gitt Panitchayangkoon a, Dugan Hayes a, Kelly A. Fransted a, Justin R. Caram a, Elad Harel a, Jianzhong Wen b, Robert
More informationProbing correlated spectral motion: Two-color photon echo study of Nile blue
Probing correlated spectral motion: Two-color photon echo study of Nile blue Bradley S. Prall, Dilworth Y. Parkinson, and Graham R. Fleming Citation: The Journal of Chemical Physics 123, 054515 (2005);
More informationSupporting Materials
Supporting Materials Figure S1 Experimental Setup Page Figure S (a) (b) (c) Feynman Diagrams Page 3-6 Figure S3 D IR Spectra Page 7 Figure S4 Kinetic Model Page 8 Figure S5 Van t Hoff Plots Page 9 1 k
More informationSpin Dynamics Basics of Nuclear Magnetic Resonance. Malcolm H. Levitt
Spin Dynamics Basics of Nuclear Magnetic Resonance Second edition Malcolm H. Levitt The University of Southampton, UK John Wiley &. Sons, Ltd Preface xxi Preface to the First Edition xxiii Introduction
More information12.2 MARCUS THEORY 1 (12.22)
Andrei Tokmakoff, MIT Department of Chemistry, 3/5/8 1-6 1. MARCUS THEORY 1 The displaced harmonic oscillator (DHO) formalism and the Energy Gap Hamiltonian have been used extensively in describing charge
More informationPhysics 221 Lecture 31 Line Radiation from Atoms and Molecules March 31, 1999
Physics 221 Lecture 31 Line Radiation from Atoms and Molecules March 31, 1999 Reading Meyer-Arendt, Ch. 20; Möller, Ch. 15; Yariv, Ch.. Demonstrations Analyzing lineshapes from emission and absorption
More informationRole of coherence and delocalization in photo-induced electron transfer at organic interfaces
Supplementary Information to Role of coherence and delocalization in photo-induced electron transfer at organic interfaces V. Abramavicius,, V. Pranckevičius, A. Melianas, O. Inganäs, V. Gulbinas, D. Abramavicius
More informationOptical coherence spectroscopy in solution: Determining the system-bath correlation function
Optical coherence spectroscopy in solution: Determining the system-bath correlation function Lewis D. Book a, David C. Arnett b and Norbert F. Scherer a a Department of Chemistry and The James Franck Institute,
More informationThe mechanism of energy transfer in the antenna of photosynthetic purple bacteria
Journal of Photochemistry and Photobiology A: Chemistry 142 (2001) 107 119 The mechanism of energy transfer in the antenna of photosynthetic purple bacteria Mino Yang, Ritesh Agarwal, Graham R. Fleming
More information5.80 Small-Molecule Spectroscopy and Dynamics
MIT OpenCourseWare http://ocw.mit.edu 5.80 Small-Molecule Spectroscopy and Dynamics Fall 2008 For information about citing these materials or our Terms of Use, visit: http://ocw.mit.edu/terms. Lectures
More informationRole of Electronic-Vibrational Mixing in Enhancing Vibrational Coherences in the Ground Electronic States of Photosynthetic Bacterial Reaction Center
pubs.acs.org/jpcb Role of Electronic-Vibrational Mixing in Enhancing Vibrational Coherences in the Ground Electronic States of Photosynthetic Bacterial Reaction Center Ian Seungwan Ryu, Hui Dong, and Graham
More informationDynamics of Light Harvesting in Photosynthesis
Annu. Rev. Phys. Chem. 2009. 60:241 62 First published online as a Review in Advance on November 14, 2008 The Annual Review of Physical Chemistry is online at physchem.annualreviews.org This article s
More informationVisualizing Light Harvesting Processes Beyond Heisenberg s Uncertainty
WDS'13 Proceedings of Contributed Papers, Part III, 165 170, 2013. ISBN 978-80-7378-252-8 MATFYZPRESS Visualizing Light Harvesting Processes Beyond Heisenberg s Uncertainty D. Paleček, R. Dědic Charles
More informationVibronic Coupling in Quantum Wires: Applications to Polydiacetylene
Vibronic Coupling in Quantum Wires: Applications to Polydiacetylene An Exhaustively Researched Report by Will Bassett and Cole Johnson Overall Goal In order to elucidate the absorbance spectra of different
More informationTransduction of Light Energy in Chloroplasts
Module 0210101: Molecular Biology and Biochemistry of the Cell Lecture 16 Transduction of Light Energy in Chloroplasts Dale Sanders 9 March 2009 Objectives By the end of the lecture you should understand
More informationElements of Quantum Optics
Pierre Meystre Murray Sargent III Elements of Quantum Optics Fourth Edition With 124 Figures fya Springer Contents 1 Classical Electromagnetic Fields 1 1.1 Maxwell's Equations in a Vacuum 2 1.2 Maxwell's
More informationThird-order nonlinear time domain probes of solvation dynamics
Third-order nonlinear time domain probes of solvation dynamics Taiha Joo, Yiwei Jia, Jae-Young Yu, Matthew J. Lang, and Graham R. Fleming Department of Chemistry and the James Franck Research Institute,
More informationFemtosecond nonlinear coherence spectroscopy of carrier dynamics in porous silicon
JOURNAL OF APPLIED PHYSICS 98, 083508 2005 Femtosecond nonlinear coherence spectroscopy of carrier dynamics in porous silicon Lap Van Dao a and Peter Hannaford Centre for Atom Optics and Ultrafast Spectroscopy,
More informationCONTENTS. 2 CLASSICAL DESCRIPTION 2.1 The resonance phenomenon 2.2 The vector picture for pulse EPR experiments 2.3 Relaxation and the Bloch equations
CONTENTS Preface Acknowledgements Symbols Abbreviations 1 INTRODUCTION 1.1 Scope of pulse EPR 1.2 A short history of pulse EPR 1.3 Examples of Applications 2 CLASSICAL DESCRIPTION 2.1 The resonance phenomenon
More informationPhoton echo studies of photosynthetic light harvesting
Photosynth Res (2009) 101:233 243 DOI 10.1007/s11120-009-9464-9 REVIEW Photon echo studies of photosynthetic light harvesting Elizabeth L. Read Æ Hohjai Lee Æ Graham R. Fleming Received: 26 November 2008
More informationSpectral Resolution. Spectral resolution is a measure of the ability to separate nearby features in wavelength space.
Spectral Resolution Spectral resolution is a measure of the ability to separate nearby features in wavelength space. R, minimum wavelength separation of two resolved features. Delta lambda often set to
More informationSupporting Online Information
Photosynthesis Research manuscript No. (will be inserted by the editor) Supporting Online Information Maaike T.W. Milder Ben Brüggemann Rienk van Grondelle Jennifer L. Herek Received: date / Accepted:
More informationFrequency- and Time-Domain Spectroscopy
Frequency- and Time-Domain Spectroscopy We just showed that you could characterize a system by taking an absorption spectrum. We select a frequency component using a grating or prism, irradiate the sample,
More informationModels for Time-Dependent Phenomena
Models for Time-Dependent Phenomena I. Phenomena in laser-matter interaction: atoms II. Phenomena in laser-matter interaction: molecules III. Model systems and TDDFT Manfred Lein p. Outline Phenomena in
More informationSupplementary Figure 1 Level structure of a doubly charged QDM (a) PL bias map acquired under 90 nw non-resonant excitation at 860 nm.
Supplementary Figure 1 Level structure of a doubly charged QDM (a) PL bias map acquired under 90 nw non-resonant excitation at 860 nm. Charging steps are labeled by the vertical dashed lines. Intensity
More informationDisordered Exciton Model for the Core Light-Harvesting Antenna of Rhodopseudomonas viridis
666 Biophysical Journal Volume 77 August 1999 666 681 Disordered Exciton Model for the Core Light-Harvesting Antenna of Rhodopseudomonas viridis Vladimir Novoderezhkin,* René Monshouwer, # and Rienk van
More informationAdvanced Photon-In Photon-Out Hard X-ray Spectroscopy
FLS 2010, ICFA Beam Dynamics Workshop, SLAC, Menlo Park, CA, March 2, 2010 ħω ħω e - Advanced Photon-In Photon-Out Hard X-ray Spectroscopy Uwe Bergmann Linac Coherent Light Source SLAC National Accelerator
More informationThird-order nonlinear optical response of energy transfer systems
hird-order nonlinear optical response of energy transfer systems Mino Yang and Graham R. Fleming Citation: he Journal of Chemical Physics 111, 27 (1999); doi: 1.163/1.479359 View online: http://dx.doi.org/1.163/1.479359
More informationMultidimensional femtosecond coherence spectroscopy for study of the carrier dynamics in photonics materials
International Workshop on Photonics and Applications. Hanoi, Vietnam. April 5-8,24 Multidimensional femtosecond coherence spectroscopy for study of the carrier dynamics in photonics materials Lap Van Dao,
More informationPart II Course Content. Outline Lecture 9. Frequency Correlations & Lineshapes. Nonlinear Spectroscopic Methods
Part II Course Content Outline Lecture 9 Optical Bloch equations Nonlinear polarizations in matter: the perturbative expansion approach. Ultrafast Fourier-transform spectroscopy: two and more dimensions.
More informationQuantum Master Equations for the Electron Transfer Problem
20/01/2010 Quantum Master Equations for the Electron Transfer Problem Seminarvortrag Dekohaerenz und Dissipation in Quantensystemen Antonio A. Gentile The general transport problem in micro/mesoscopic
More information11.1. FÖRSTER RESONANCE ENERGY TRANSFER
11-1 11.1. FÖRSTER RESONANCE ENERGY TRANSFER Förster resonance energy transfer (FRET) refers to the nonradiative transfer of an electronic excitation from a donor molecule to an acceptor molecule: D *
More informationSimulation of Two-Dimensional Electronic Spectra of Phycoerythrin 545 at Ambient Temperature
pubs.acs.org/jpcb Simulation of Two-Dimensional Electronic Spectra of Phycoerythrin 545 at Ambient Temperature Xuan Leng and Xian-Ting Liang* Department of Physics and Institute of Optics, ingbo University,
More informationIntensities and rates in the spectral domain without eigenvectors.
UNIVERSITY OF ILLINOIS URBANA-CHAMPAIGN: DEPARTMENT OF CHEMISTRY Intensities and rates in the spectral domain without eigenvectors. By: Dr. Martin Gruebele Authors: Brian Nguyen and Drishti Guin 12/10/2013
More informationi) impact of interchain interactions
i) impact of interchain interactions multiple experimental observations: in dilute solutions or inert matrices: the photoluminescence quantum yield of a given conjugated polymers can be very large: up
More information12. Spectral diffusion
1. Spectral diffusion 1.1. Spectral diffusion, Two-Level Systems Until now, we have supposed that the optical transition frequency of each single molecule is a constant (except when we considered its variation
More informationLecture 10. Lidar Effective Cross-Section vs. Convolution
Lecture 10. Lidar Effective Cross-Section vs. Convolution q Introduction q Convolution in Lineshape Determination -- Voigt Lineshape (Lorentzian Gaussian) q Effective Cross Section for Single Isotope --
More informationCoherence and Its Role in Excitation Energy. Transfer in Fenna-Matthews-Olson Complex
Coherence and Its Role in Excitation Energy arxiv:1708.00933v1 [physics.chem-ph] 2 Aug 2017 Transfer in Fenna-Matthews-Olson Complex Davinder Singh and Shubhrangshu Dasgupta Department of Physics, Indian
More informationSpectral Broadening Mechanisms
Spectral Broadening Mechanisms Lorentzian broadening (Homogeneous) Gaussian broadening (Inhomogeneous, Inertial) Doppler broadening (special case for gas phase) The Fourier Transform NC State University
More informationSupporting Information
Supporting Information Temperature Dependence of Emission Linewidths from Semiconductor Nanocrystals Reveals Vibronic Contributions to Line Broadening Processes Timothy G. Mack, Lakshay Jethi, Patanjali
More informationDensity-matrix theory for time-resolved dynamics of superconductors in non-equilibrium
Max Planck Institute for Solid State Research Density-matrix theory for time-resolved dynamics of superconductors in non-equilibrium co-workers and papers: (1) (2) (3) (4) Dirk Manske A. Knorr (TU Berlin),
More informationVibrational Coherence Transfer and Trapping as Sources for Long-Lived Quantum Beats in Polarized Emission from Energy Transfer Complexes
11196 J. Phys. Chem. A 2004, 108, 11196-11208 Vibrational Coherence Transfer and Trapping as Sources for Long-Lived Quantum Beats in Polarized Emission from Energy Transfer Complexes Jeffrey A. Cina*,,
More informationNon-Adiabatic Mechanism for Photosynthetic Energy Transfer and All-Optical Determination of Concentration using Femtosecond Lasers
University of Colorado, Boulder CU Scholar Chemistry & Biochemistry Graduate Theses & Dissertations Chemistry & Biochemistry Spring 1-1-2014 Non-Adiabatic Mechanism for Photosynthetic Energy Transfer and
More informationModels for Time-Dependent Phenomena. I. Laser-matter interaction: atoms II. Laser-matter interaction: molecules III. Model systems and TDDFT
Models for Time-Dependent Phenomena I. Laser-matter interaction: atoms II. Laser-matter interaction: molecules III. Model systems and TDDFT Manfred Lein, TDDFT school Benasque 22 p. Outline Laser-matter
More informationEntangled Photon Generation via Biexciton in a Thin Film
Entangled Photon Generation via Biexciton in a Thin Film Hiroshi Ajiki Tokyo Denki University 24,Apr. 2017 Emerging Topics in Optics (IMA, Univ. Minnesota) Entangled Photon Generation Two-photon cascade
More informationQuantum control of dissipative systems. 1 Density operators and mixed quantum states
Quantum control of dissipative systems S. G. Schirmer and A. I. Solomon Quantum Processes Group, The Open University Milton Keynes, MK7 6AA, United Kingdom S.G.Schirmer@open.ac.uk, A.I.Solomon@open.ac.uk
More informationFEMTOSECOND MID-INFRARED SPECTROSCOPY OF HYDROGEN-BONDED LIQUIDS
Laser Chem., 1999, Vol. 19, pp. 83-90 Reprints available directly from the publisher Photocopying permitted by license only (C) 1999 OPA (Overseas Publishers Association) N.V. Published by license under
More informationarxiv: v1 [physics.chem-ph] 11 May 2016
How can the green sulfur bacteria use quantum computing for light harvesting? D Drakova 1 and G Doyen 2 1 State University of Sofia, Faculty of Chemistry, Sofia, Bulgaria 2 Ludwig-Maximilians-University,
More information5.74 Introductory Quantum Mechanics II
MIT OpenCourseWare http://ocw.mit.edu 5.74 Introductory Quantum Mechanics II Spring 9 For information about citing these materials or our Terms of Use, visit: http://ocw.mit.edu/terms. Andrei Tokmakoff,
More informationOf Electrons, Energy, and Excitons
Of,, and Gert van der Zwan July 17, 2014 1 / 35 Bacterial 2 / 35 Bacterial Bacterial LH1, LH2: excitonic interaction and energy transfer. RC, cytochromes: electron transfer reactions. Q, UQ: proton transfer
More informationPigment Organization and Energy Level Structure in Light-Harvesting Complex 4: Insights from Two-Dimensional Electronic Spectroscopy
J. Phys. Chem. B 2009, 113, 6495 6504 6495 Pigment Organization and Energy Level Structure in Light-Harvesting Complex 4: Insights from Two-Dimensional Electronic Spectroscopy Elizabeth L. Read,,, Gabriela
More informationProbing dynamics of complex molecular systems with ultrafast 2D IR vibrational echo spectroscopy
/ Journal Homepage / Table of Contents for this issue INVITED ARTICLE www.rsc.org/pccp Physical Chemistry Chemical Physics Probing dynamics of complex molecular systems with ultrafast 2D IR vibrational
More informationSupplementary for Disorder Dependent Valley Properties in Monolayer WSe 2
Supplementary for Disorder Dependent Valley Properties in Monolayer WSe 2 Kha Tran 1, Akshay Singh 1,*, Joe Seifert 1, Yiping Wang 1, Kai Hao 1, Jing-Kai Huang 2, Lain-Jong Li 2, Takashi Taniguchi 4, Kenji
More informationIntroduction to Modern Quantum Optics
Introduction to Modern Quantum Optics Jin-Sheng Peng Gao-Xiang Li Huazhong Normal University, China Vfe World Scientific» Singapore* * NewJerseyL Jersey* London* Hong Kong IX CONTENTS Preface PART I. Theory
More informationAndrea Morello. Nuclear spin dynamics in quantum regime of a single-molecule. magnet. UBC Physics & Astronomy
Nuclear spin dynamics in quantum regime of a single-molecule magnet Andrea Morello UBC Physics & Astronomy Kamerlingh Onnes Laboratory Leiden University Nuclear spins in SMMs Intrinsic source of decoherence
More informationSupporting information for the manuscript. Excited state structural evolution during charge-transfer reactions in Betaine-30
Electronic Supplementary Material (ESI) for Physical Chemistry Chemical Physics. This journal is the Owner Societies 2015 Supporting information for the manuscript Excited state structural evolution during
More informationInfrared analogs of heteronuclear nuclear magnetic resonance coherence transfer experiments in peptides
JOURNAL OF CHEMICAL PHYSICS VOLUME 116, NUMBER 15 15 APRIL 2002 Infrared analogs of heteronuclear nuclear magnetic resonance coherence transfer experiments in peptides C. Scheurer a) and S. Mukamel b)
More informationControl and Characterization of Intramolecular Dynamics with Chirped Femtosecond Three-Pulse Four-Wave Mixing
106 J. Phys. Chem. A 1999, 103, 106-1036 Control and Characterization of Intramolecular Dynamics with Chirped Femtosecond Three-Pulse Four-Wave Mixing Igor Pastirk, Vadim V. Lozovoy, Bruna I. Grimberg,
More informationEran Rabani, S. A. Egorov, a) and B. J. Berne Department of Chemistry, Columbia University, 3000 Broadway, New York, New York 10027
JOURNAL OF CHEMICAL PHYSICS VOLUME 109, NUMBER 15 15 OCTOBER 1998 A comparison of exact quantum mechanical and various semiclassical treatments for the vibronic absorption spectrum: The case of fast vibrational
More informationTWO-DIMENSIONAL RAMAN SPECTROSCOPY N. Y , USA. (Received 28 June 1998)
Laser Chem., 1999, Vol. 19, pp. 109-116 Reprints available directly from the publisher Photocopying permitted by license only (C) 1999 OPA (Overseas Publishers Association) N.V. Published by license under
More information5.74 Introductory Quantum Mechanics II
MIT OpenCourseWare http://ocw.mit.edu 5.74 Introductory Quantum Mechanics II Spring 9 For information about citing these materials or our Terms of Use, visit: http://ocw.mit.edu/terms. Andrei Tokmakoff,
More informationΓ43 γ. Pump Γ31 Γ32 Γ42 Γ41
Supplementary Figure γ 4 Δ+δe Γ34 Γ43 γ 3 Δ Ω3,4 Pump Ω3,4, Ω3 Γ3 Γ3 Γ4 Γ4 Γ Γ Supplementary Figure Schematic picture of theoretical model: The picture shows a schematic representation of the theoretical
More informationMolecular Vibronic Structures of HDITC in Solutions Studied by Femtosecond Wavelength-Resolved Pump-Probe Spectroscopy
Journal of the Chinese Chemical Society, 1999,46,409-416 409 Molecular Vibronic Structures of HDITC in Solutions Studied by Femtosecond Wavelength-Resolved Pump-Probe Spectroscopy. - T.-S. Yang*a ( &FB
More informationAccidental vibrational degeneracy in vibrational excited states observed with ultrafast two-dimensional IR vibrational echo spectroscopy
THE JOURNAL OF CHEMICAL PHYSICS 13, 164301 005 Accidental vibrational degeneracy in vibrational excited states observed with ultrafast two-dimensional IR vibrational echo spectroscopy Junrong Zheng, Kyungwon
More informationFour-Wave Mixing Techniques Applied to the Investigation of Non-Adiabatic Dynamics in Polyatomic Molecules
Four-Wave Mixing Techniques Applied to the Investigation of Non-Adiabatic Dynamics in Polyatomic Molecules Dissertation zur Erlangung des naturwissenschaftlichen Doktorgrades der Bayerischen Julius Maximilians
More informationQuantum Condensed Matter Physics Lecture 9
Quantum Condensed Matter Physics Lecture 9 David Ritchie QCMP Lent/Easter 2018 http://www.sp.phy.cam.ac.uk/drp2/home 9.1 Quantum Condensed Matter Physics 1. Classical and Semi-classical models for electrons
More information