Spatially-resolved fluorescence-detected two-dimensional electronic spectroscopy probes varying excitonic structure in photosynthetic bacteria

  title={Spatially-resolved fluorescence-detected two-dimensional electronic spectroscopy probes varying excitonic structure in photosynthetic bacteria},
  author={Vivek Tiwari and Yassel Acosta Matutes and Alastair T. Gardiner and Thomas la Cour Jansen and Richard J. Cogdell and Jennifer P. Ogilvie},
  journal={Nature Communications},
Conventional implementations of two-dimensional electronic spectroscopy typically spatially average over ~1010 chromophores spread over ~104 micron square area, limiting their ability to characterize spatially heterogeneous samples. Here we present a variation of two-dimensional electronic spectroscopy that is capable of mapping spatially varying differences in excitonic structure, with sensitivity orders of magnitude better than conventional spatially-averaged electronic spectroscopies. The… 

Coherently and fluorescence-detected two-dimensional electronic spectroscopy: direct comparison on squaraine dimers.

This work directly compares, both experimentally and theoretically, four-wave mixing coherently and fluorescence-detected 2DES of a series of squaraine dimers of increasing electronic coupling and demonstrates the degree of complementarity of the techniques.

High-sensitivity Fluorescence-Detected Multidimensional Electronic Spectroscopy Through Continuous Pump-probe Delay Scan

Background-free fluorescence detection in multidimensional electronic spectroscopy promises high sensitivity compared to conventional approaches. Here we explore the sensitivity limits of

Simulating Fluorescence-Detected Two-Dimensional Electronic Spectroscopy of Multichromophoric Systems

The use of time-resolving fluorescence-detected two-dimensional spectroscopy to study state-resolved exciton–exciton annihilation is proposed and tested by comparison of the predicted spectra of the light-harvesting complex LH2 with experimental data.

Correlated spatially resolved two-dimensional electronic and linear absorption spectroscopy.

A multimodal method for correlating linear and nonlinear optical spectra with a spatial resolution is presented. Using a partially collinear pump-probe geometry and two-frame phase-cycling, ultrafast

Rapid multiple-quantum three-dimensional fluorescence spectroscopy disentangles quantum pathways

3D population-based three-dimensional electronic spectroscopy is introduced and the extraction of all fourth- and multiple sixth-order nonlinear signal contributions are extracted by employing 125-fold phase cycling of a four-pulse sequence.

Multidimensional Spectroscopy on the Microscale: Development of a Multimodal Imaging System Incorporating 2D White-Light Spectroscopy, Broadband Transient Absorption, and Atomic Force Microscopy.

A time-resolved non-linear microscopy system using white-light supercontinuum pulses as a broadband light source capable of correlating ~nm scale sample morphology determined from atomic force topography measurements with broadband transient absorption hyperspectral images and ultrafast 2D white- light spectra, all with a spatial resolution of ≤1 μm is presented.

Fluorescence‐Detected Pump–Probe Spectroscopy

A new approach, fluorescence-detected pump-probe (F-PP) spectroscopy, that overcomes several limitations of traditional PP and is broadly applicable to chemical systems in various environments and in different spectral regimes.

Fluorescence-detected Fourier transform electronic spectroscopy by phase-tagged photon counting.

An approach to low-signal fluorescence-detected FT spectroscopy, in which individual photon counts are assigned to a modulated interferometer phase ('phase-tagged photon counting,' or PTPC), and the resulting data are processed to construct optical spectra is introduced.

Molecular versus Excitonic Disorder in Individual Artificial Light-Harvesting Systems

The detailed characterization of static and dynamic disorder at the exciton as well as the molecular level presented here opens new avenues in analyzing and predicting dynamic exciton properties, such as excitation energy transport.

Signatures of exciton dynamics and interaction in coherently and fluorescence-detected four- and six-wave-mixing two-dimensional electronic spectroscopy.

A sixth-order fluorescence-detected EEI2D spectroscopy variant that focuses on the possibility to extract the dynamics arising from exciton-exciton interaction directly from the six-wave-mixing spectra.



Spatially Resolved Two-Dimensional Infrared Spectroscopy via Wide-Field Microscopy.

The first wide-field microscope for measuring two-dimensional infrared (2D IR) spectroscopic images is reported, which has diffraction-limited spatial resolution and enhanced contrast compared to FTIR microscopy and is found to have nonlinear scaling of the 2D IR signal to the absorptivity coefficient for the vibrational modes.

Methods of single-molecule fluorescence spectroscopy and microscopy

Optical spectroscopy at the ultimate limit of a single molecule has grown over the past dozen years into a powerful technique for exploring the individual nanoscale behavior of molecules in complex

Fluorescence-detected two-dimensional electronic coherence spectroscopy by acousto-optic phase modulation.

A new experimental scheme for phase-selective nonlinear ECS that combines acousto-optic phase modulation with ultrashort laser excitation to produce intensity modulated nonlinear fluorescence signals and decouples the relative temporal phases from the pulse envelopes of a collinear train of four sequential pulses is introduced.

Experimental implementations of two-dimensional fourier transform electronic spectroscopy.

The challenges of implementing 2DES are discussed, different approaches in terms of their information content, ease of implementation, and potential for broadband measurements are compared, and different approaches to spectroscopic signatures are compared.

Sub-10 fs Time-Resolved Vibronic Optical Microscopy

Femtosecond wide-field transient absorption microscopy combining sub-10 fs pump and probe pulses covering the complete visible and near-infrared spectrum with diffraction-limited optical resolution is introduced, opening up the possibility of studying ultrafast dynamics on nanometer length and femTosecond time scales in a variety of two-dimensional and nanoscopic systems.

Coherent two-dimensional fluorescence micro-spectroscopy.

We have developed coherent two-dimensional (2D) fluorescence micro-spectroscopy which probes the nonlinear optical response at surfaces via fluorescence detection with sub-micron spatial resolution.

Fourier Transform Fluorescence-Encoded Infrared Spectroscopy.

The development of Fourier transform FEIR is reported on as an alternate approach for high-sensitivity IR spectroscopy and the pathways observed in a 2D FEIR spectrum arise from the excitation of vibrational populations and coherences between coupled vibrations.

Bringing Far-Field Subdiffraction Optical Imaging to Electronically Coupled Optoelectronic Molecular Materials Using Their Endogenous Chromophores.

It is demonstrated that subdiffraction resolution can be achieved in fluorescence imaging of functional materials with densely packed, endogenous, electronically coupled chromophores by modifying stimulated emission depletion (STED) microscopy, which will transform the current understanding of these materials' structure-function relationships.

Two-dimensional femtosecond spectroscopy.

  • D. Jonas
  • Physics, Chemistry
    Annual review of physical chemistry
  • 2003
This review provides an introduction to two-dimensional Fourier transform experiments exploiting second- and third-order vibrational and electronic nonlinearities.

Imaging Electronic Trap States in Perovskite Thin Films with Combined Fluorescence and Femtosecond Transient Absorption Microscopy.

A comparative study on methylammonium lead tri-iodide perovskite thin films subject to different thermal annealing times using a combined photoluminescence (PL) and femtosecond transient absorption microscopy (TAM) approach to spatially map trap states suggests spatially dependent PL quantum efficiency, indicative of trapping events.