Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Near shot-noise limited time-resolved circular dichroism pump-probe spectrometer

Journal Article · · Review of Scientific Instruments
DOI:https://doi.org/10.1063/1.5009468· OSTI ID:1470599
 [1];  [2];  [2];  [1]
  1. Purdue Univ., West Lafayette, IN (United States). Dept. of Physics and Astronomy
  2. Washington Univ., St. Louis, MO (United States). Dept. of Biology and Chemistry, Photosynthetic Antenna Research Center

We describe an optical near shot-noise limited time-resolved circular dichroism (TRCD) pump-probe spectrometer capable of reliably measuring circular dichroism signals in the order of $$\mu$$deg with nanosecond time resolution. Such sensitivity is achieved through a modification of existing TRCD designs and introduction of a new data processing protocol that eliminates approximations that have caused substantial nonlinearities in past measurements and allows the measurement of absorption and circular dichroism transients simultaneously with a single pump pulse. The exceptional signal-to-noise ratio of the described setup makes the TRCD technique applicable to a large range of non-biological and biological systems. Finally, the spectrometer was used to record, for the first time, weak TRCD kinetics associated with the triplet state energy transfer in the photosynthetic Fenna-Matthews-Olson antenna pigment-protein complex.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Photosynthetic Antenna Research Center (PARC)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
SC0001035
OSTI ID:
1470599
Alternate ID(s):
OSTI ID: 1425540
Journal Information:
Review of Scientific Instruments, Journal Name: Review of Scientific Instruments Journal Issue: 3 Vol. 89; ISSN 0034-6748
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

References (51)

Stopped-flow circular dichroism: A new fast-kinetic system journal February 1974
Circular Dichroism and the Conformational Analysis of Biomolecules book January 1996
Recent advances in time resolved circular dichroism spectroscopy journal October 1987
Linear dichroism and circular dichroism in photosynthesis research journal May 2009
Revisiting the optical properties of the FMO protein journal March 2010
Ultrasensitive time-resolved linear dichroism spectral measurements using near-crossed linear polarizers journal July 1994
Perturbation of bacteriochlorophyll molecules in Fenna–Matthews–Olson protein complexes through mutagenesis of cysteine residues journal September 2016
How to study proteins by circular dichroism journal August 2005
Application of time-resolved circular dichroism to the study of conformational changes in photochemical and photobiological processes journal May 2009
Quantum coherence in photosynthesis journal January 2011
Nanosecond time-resolved polarization spectroscopies: Tools for probing protein reaction mechanisms journal September 2010
A picosecond circular dichroism study of photosynthetic reaction centers from Rhodobacter sphaeroides journal March 1991
Time-resolved circular dichroism and absorption studies of the photolysis reaction of (carbonmonoxy)myoglobin journal May 1988
Nanosecond optical rotatory dispersion spectroscopy: application to photolyzed hemoglobin-CO kinetics journal January 1995
Oscillating anisotropies in a bacteriochlorophyll protein: Evidence for quantum beating between exciton levels journal November 1997
Effect of Spectral Density Shapes on the Excitonic Structure and Dynamics of the Fenna–Matthews–Olson Trimer from Chlorobaculum tepidum journal August 2016
Allosteric Intermediates in Hemoglobin. 1. Nanosecond Time-Resolved Circular Dichroism Spectroscopy journal January 1996
Nanosecond circular dichroism spectral measurements: extension to the far-ultraviolet region journal May 1993
Analysis of optical artifacts in ellipsometric measurements of time-resolved circular dichroism journal June 1991
New technique for measuring circular dichroism changes on a nanosecond time scale. Application to (carbonmonoxy)myoglobin and (carbonmonoxy)hemoglobin journal January 1985
Birefringence effects in transient circular dichroism measurements with applications to the photolysis of carbon monoxyhemoglobin and carbon monoxymyoglobin journal August 1985
Time-resolved circular dichroism of native oat phytochrome photointermediates journal June 1992
Ultrafast Carbonyl Motion of the Photoactive Yellow Protein Chromophore Probed by Femtosecond Circular Dichroism journal September 2013
Conformational Changes in Photoexcited ( R )-(+)-1,1′-Bi-2-naphthol Studied by Time-Resolved Circular Dichroism journal September 2008
Exciton Analysis in 2D Electronic Spectroscopy journal June 2005
From Atomistic Modeling to Excitation Transfer and Two-Dimensional Spectra of the FMO Light-Harvesting Complex journal July 2011
Intensity Dependence of the Excited State Lifetimes and Triplet Conversion Yield in the Fenna–Matthews–Olson Antenna Protein journal February 2014
Comparative Study of the Folding/Unfolding Dynamics of Poly(glutamic acid) in Light and Heavy Water journal May 2014
The Fate of the Triplet Excitations in the Fenna–Matthews–Olson Complex journal April 2015
Effect of Diagonal Energy Disorder on Circular Dichroism Spectra of Fenna−Matthews−Olson Trimers journal October 1997
Fast Time-Resolved Magnetic Optical Rotatory Dispersion Measurements. 1. Mueller Analysis of Optical and Photoselection-Induced Artifacts journal November 1998
Exciton Simulations of Optical Spectra of the FMO Complex from the Green Sulfur Bacterium Chlorobium tepidum at 6 K journal November 1998
The FMO Protein journal January 2004
Chlorophyll arrangement in a bacteriochlorophyll protein from Chlorobium limicola journal December 1975
Evidence for wavelike energy transfer through quantum coherence in photosynthetic systems journal April 2007
Picosecond time‐resolved circular dichroism spectroscopy: experimental details and applications journal August 1989
Nanosecond time‐resolved circular dichroism measurements using an upconverted Ti:sapphire laser journal September 1996
The measurement of transient circular dichroism: A new kinetic technique journal November 1974
Broadband femtosecond circular dichroism spectrometer with white-light polarization control journal April 2010
Communication: Broadband and ultrasensitive femtosecond time-resolved circular dichroism spectroscopy journal September 2015
Evidence for a cysteine-mediated mechanism of excitation energy regulation in a photosynthetic antenna complex journal June 2016
Measurement of circular dichroism at millisecond time resolution: a stopped-flow circular dichroism system journal June 1974
Towards a coherent picture of excitonic coherence in the Fenna–Matthews–Olson complex journal July 2012
Circular Dichroism Techniques: Biomolecular and Nanostructural Analyses- A Review journal August 2009
Measuring the dynamics of circular dichroism in a pump-probe experiment with a Babinet-Soleil compensator: erratum journal January 2007
Picosecond circular dichroism spectroscopy: a Jones matrix analysis journal January 1990
Broadband near UV to visible optical activity measurement using self-heterodyned method journal January 2011
Broadband transient dichroism spectroscopy in chiral molecules journal January 2010
How Proteins Trigger Excitation Energy Transfer in the FMO Complex of Green Sulfur Bacteria journal October 2006
The Use of Circular Dichroism in the Investigation of Protein Structure and Function journal December 2000
Probing Kinetic Mechanisms of Protein Function and Folding with Time-Resolved Natural and Magnetic Chiroptical Spectroscopies journal January 2012

Cited By (2)

Ultrafast broadband circular dichroism in the deep ultraviolet journal January 2019
Ultrafast broadband circular dichroism in the deep ultraviolet text January 2019