scholarly journals Disentanglement of excited-state dynamics with implications for FRET measurements: two-dimensional electronic spectroscopy of a BODIPY-functionalized cavitand

2018 ◽  
Vol 9 (15) ◽  
pp. 3694-3703 ◽  
Author(s):  
John P. Otto ◽  
Lili Wang ◽  
Igor Pochorovski ◽  
Samuel M. Blau ◽  
Alán Aspuru-Guzik ◽  
...  
Keyword(s):  
Energy Transfer ◽  
Excited State ◽  
Conformational Changes ◽  
Electronic Spectroscopy ◽  
Two Dimensional ◽  
Excited State Dynamics ◽  
Competing Dynamics

Two-dimensional electronic spectroscopy of energy transfer and competing dynamics highlights how conformational changes create issues with lifetime-based FRET measurements.

scholarly journals Polyhydrogenated Graphene: Excited State Dynamics in Photo- and Electroactive Two-Dimensional Domains

2015 ◽  
Vol 137 (40) ◽  
pp. 13079-13086 ◽  
Author(s):  
Volker Strauss ◽  
Ricarda A. Schäfer ◽  
Frank Hauke ◽  
Andreas Hirsch ◽  
Dirk M. Guldi
Keyword(s):  
Excited State ◽  
Two Dimensional ◽  
Excited State Dynamics

scholarly journals Two-Dimensional Electronic Spectroscopy Reveals the Spectral Dynamics of Förster Resonance Energy Transfer

Chem ◽  
2019 ◽  
Vol 5 (8) ◽  
pp. 2111-2125 ◽  
Author(s):  
Brian K. Petkov ◽  
Tobias A. Gellen ◽  
Camille A. Farfan ◽  
William P. Carbery ◽  
Belinda E. Hetzler ◽  
...  
Keyword(s):  
Energy Transfer ◽  
Electronic Spectroscopy ◽  
Resonance Energy Transfer ◽  
Resonance Energy ◽  
Forster Resonance Energy Transfer ◽  
Förster Resonance Energy Transfer ◽  
Two Dimensional ◽  
Spectral Dynamics ◽  
Förster Resonance

scholarly journals Ultrabroadband two-dimensional electronic spectroscopy reveals energy flow pathways in LHCII across the visible spectrum

2019 ◽  
Vol 205 ◽  
pp. 09034
Author(s):  
Minjung Son ◽  
Alberta Pinnola ◽  
Roberto Bassi ◽  
Gabriela S. Schlau-Cohen
Keyword(s):  
Energy Transfer ◽  
Excited States ◽  
Energy Flow ◽  
Energy Levels ◽  
Electronic Spectroscopy ◽  
Visible Region ◽  
Visible Spectrum ◽  
Energy Relaxation ◽  
Two Dimensional ◽  
Flow Pathways

We utilise ultrabroadband two-dimensional electronic spectroscopy to map out pathways of energy flow in LHCII across the entire visible region. In addition to the well-established, low-lying chlorophyll Qy bands, our results reveal additional pathways of energy relaxation on the higher-lying excited states involving the S2 energy levels of carotenoids, including ultrafast carotenoid-to-chlorophyll energy transfer on 90-150 fs timescales.

scholarly journals Excitation energy transfer and equilibration process in LHCII studied by multidimensional electronic spectroscopy

2019 ◽  
Vol 205 ◽  
pp. 09038
Author(s):  
Thanh Nhut Do ◽  
Adriana Huerta-Viga ◽  
Cheng Zhang ◽  
Parveen Akhtar ◽  
Pawei J. Nowakowski ◽  
...  
Keyword(s):  
Energy Transfer ◽  
Light Harvesting ◽  
Electronic Spectroscopy ◽  
Excitation Energy Transfer ◽  
Phenomenological Analysis ◽  
Two Dimensional ◽  
Light Harvesting Complex ◽  
Light Harvesting Complex Ii ◽  
Equilibration Process ◽  
Light Harvesting Antenna

Light-harvesting complex II (LHCII) – the light-harvesting antenna of Photosystem II – is a naturally abundant system that plays an important role in photosynthesis. In this study, we present a phenomenological analysis of the excitonic energy transfer in LHCII using ultrafast two-dimensional electronic spectroscopy, that we find compares well with previous theoretical and experimental results.

Electronic spectroscopy and excited state dynamics of the Al–N2 complex

1998 ◽  
Vol 239 (1-3) ◽  
pp. 207-221 ◽  
Author(s):  
Xin Yang ◽  
Irina Gerasimov ◽  
Paul J. Dagdigian
Keyword(s):  
Excited State ◽  
Electronic Spectroscopy ◽  
Excited State Dynamics

Excitonic couplings and interband energy transfer in a double-wall molecular aggregate imaged by coherent two-dimensional electronic spectroscopy

2009 ◽  
Vol 131 (5) ◽  
pp. 054510 ◽  
Author(s):  
F. Milota ◽  
J. Sperling ◽  
A. Nemeth ◽  
D. Abramavicius ◽  
S. Mukamel ◽  
...  
Keyword(s):  
Energy Transfer ◽  
Electronic Spectroscopy ◽  
Two Dimensional ◽  
Molecular Aggregate ◽  
Double Wall

scholarly journals Observation of dissipative chlorophyll-to-carotenoid energy transfer in light-harvesting complex II in membrane nanodiscs

2019 ◽  
Author(s):  
Minjung Son ◽  
Alberta Pinnola ◽  
Samuel C. Gordon ◽  
Roberto Bassi ◽  
Gabriela S. Schlau-Cohen
Keyword(s):  
Energy Transfer ◽  
Conformational Changes ◽  
Light Harvesting ◽  
Electronic Spectroscopy ◽  
Local Environment ◽  
Light Harvesting Complex ◽  
Complex Ii ◽  
Light Harvesting Complex Ii ◽  
Photosynthetic Antenna

<pre><p><a></a>Green plants prevent photodamage under high light conditions by dissipating excess energy as heat. Conformational changes of the photosynthetic antenna complexes activate dissipation by leveraging the sensitivity of the photophysics of the chlorophyll and carotenoids to their surrounding protein. However, the mechanisms and site of dissipation are still debated, largely due to two challenges. First, because of the ultrafast timescales and large energy gaps involved, measurements lacked the temporal or spectral requirements. Second, experiments have been performed in detergent, which can induce non-native conformations, or <i>in vivo</i>, where contributions from the multiple complexes cannot be disentangled and are further obfuscated by laser-induced artifacts. Here, we overcome both challenges by applying ultrabroadband two-dimensional electronic spectroscopy to the principal antenna complex, light-harvesting complex II, in a near-native membrane. The membrane enhances two dissipative pathways, one of which was previously uncharacterized chlorophyll-to-carotenoid energy transfer. Our results highlight the sensitivity of the photophysics to the local environment, which may be used to control the balance between light harvesting and dissipation <i>in vivo</i>.</p></pre>

Redox conditions correlated with vibronic coupling modulate quantum beats in photosynthetic pigment–protein complexes

2021 ◽  
Vol 118 (49) ◽  
pp. e2112817118
Author(s):  
Jacob S. Higgins ◽  
Marco A. Allodi ◽  
Lawson T. Lloyd ◽  
John P. Otto ◽  
Sara H. Sohail ◽  
...  
Keyword(s):  
Energy Transfer ◽  
Excited State ◽  
Photosynthetic Pigment ◽  
Electronic Spectroscopy ◽  
Power Spectra ◽  
Phase Relationship ◽  
Vibronic Coupling ◽  
Redox Conditions ◽  
Efficient Energy Transfer ◽  
Reducing Conditions

Quantum coherences, observed as time-dependent beats in ultrafast spectroscopic experiments, arise when light–matter interactions prepare systems in superpositions of states with differing energy and fixed phase across the ensemble. Such coherences have been observed in photosynthetic systems following ultrafast laser excitation, but what these coherences imply about the underlying energy transfer dynamics remains subject to debate. Recent work showed that redox conditions tune vibronic coupling in the Fenna–Matthews–Olson (FMO) pigment–protein complex in green sulfur bacteria, raising the question of whether redox conditions may also affect the long-lived (>100 fs) quantum coherences observed in this complex. In this work, we perform ultrafast two-dimensional electronic spectroscopy measurements on the FMO complex under both oxidizing and reducing conditions. We observe that many excited-state coherences are exclusively present in reducing conditions and are absent or attenuated in oxidizing conditions. Reducing conditions mimic the natural conditions of the complex more closely. Further, the presence of these coherences correlates with the vibronic coupling that produces faster, more efficient energy transfer through the complex under reducing conditions. The growth of coherences across the waiting time and the number of beating frequencies across hundreds of wavenumbers in the power spectra suggest that the beats are excited-state coherences with a mostly vibrational character whose phase relationship is maintained through the energy transfer process. Our results suggest that excitonic energy transfer proceeds through a coherent mechanism in this complex and that the coherences may provide a tool to disentangle coherent relaxation from energy transfer driven by stochastic environmental fluctuations.

Sign in / Sign up

Export Citation Format

Share Document