Molecular Coherent Three-Quantum Two-Dimensional Fluorescence Spectroscopy

The Journal of Physical Chemistry Letters
Stefan Mueller, Tobias Brixner

Abstract

We introduce molecular coherent three-quantum (3Q) two-dimensional (2D) fluorescence spectroscopy with phase cycling via shot-to-shot pulse shaping at a 1 kHz repetition rate. This allows us to acquire simultaneously, within a single scan, three fourth-order and six sixth-order signals correlating various one-quantum, two-quantum, and 3Q coherences. We demonstrate the approach on the dye molecule rhodamine 700 and reproduce all nine 2D data sets, including their absolute signal strengths, with simulations using a single, consistent set of model parameters. We observe a linear concentration dependence of all nonlinear signals, evidencing the absence of cascades and many-particle signals of noninteracting molecules. The single-beam, background-free implementation allows direct comparability between various nonlinear signal types and provides information about multiple excited states. Apart from molecules, the method is expected to be applicable to supramolecular systems, polymers, and solid-state materials with the prospect of revealing signatures of bi- and triexcitonic states.

References

Jun 7, 2003·Science·Peifang TianWarren S Warren
Mar 3, 2005·The Journal of Chemical Physics·Eric C FulmerMartin T Zanni
Mar 24, 2005·Physical Review Letters·Eric C FulmerMartin T Zanni
Oct 6, 2006·The Journal of Physical Chemistry. B·Soohwan SulNien-Hui Ge
Dec 11, 2007·The Journal of Chemical Physics·Patrick F TekavecAndrew H Marcus
Dec 18, 2007·The Journal of Chemical Physics·Shaul MukamelLijun Yang
May 2, 2009·The Journal of Chemical Physics·Sean Garrett-Roe, Peter Hamm
May 30, 2009·Science·Katherine W StoneKeith A Nelson
Jun 26, 2009·Accounts of Chemical Research·Jeongho KimGregory D Scholes
Aug 7, 2009·The Review of Scientific Instruments·A D BristowS T Cundiff
Aug 21, 2009·Accounts of Chemical Research·Katherine W StoneKeith A Nelson
Aug 27, 2010·Nature·Daniel B Turner, Keith A Nelson
Sep 14, 2010·The Journal of Chemical Physics·Alexandra NemethNiklas Christensson
Jun 7, 2012·The Journal of Chemical Physics·Oliver BixnerNiklas Christensson
Jul 3, 2013·The Journal of Physical Chemistry. B·Zhengyang ZhangHowe-Siang Tan
Dec 2, 2010·The Journal of Physical Chemistry Letters·Niklas ChristenssonJürgen Hauer
Sep 1, 1995·Journal of Fluorescence·M SauerK H Drexhage
May 9, 2014·Physical Chemistry Chemical Physics : PCCP·Kym L WellsHowe-Siang Tan
Dec 19, 2014·Nature Communications·Khadga J KarkiAndrew H Marcus
Jun 22, 2016·Nature Chemistry·Jakub DostálDonatas Zigmantas
Aug 31, 2016·The Journal of Physical Chemistry Letters·William O HutsonElad Harel
Dec 9, 2016·Nature Communications·Antonietta De SioChristoph Lienau
Dec 17, 2016·The Journal of Physical Chemistry Letters·Parveen AkhtarHowe-Siang Tan
Mar 11, 2017·Nature Communications·Austin P SpencerElad Harel
Sep 25, 2017·The Journal of Chemical Physics·Pascal GrégoireCarlos Silva
Mar 3, 2018·The Journal of Chemical Physics·Loni KringleAndrew H Marcus
Apr 3, 2018·The Journal of Physical Chemistry Letters·Stefan MuellerTobias Brixner
Jun 27, 2018·Nature Communications·Jakub DostálTobias Brixner
Nov 18, 2018·Physical Chemistry Chemical Physics : PCCP·Lukas BruderFrank Stienkemeier
Nov 18, 2018·Nature Communications·Lukas BruderFrank Stienkemeier
Oct 12, 2019·Nature Communications·Björn KrieteMaxim S Pshenichnikov
Oct 20, 2019·Nature Communications·Stefan MuellerTobias Brixner
Nov 2, 2019·Chemical Science·Khadga J KarkiTönu Pullerits
Feb 7, 2020·The Journal of Physical Chemistry Letters·Oliver KühnTõnu Pullerits

❮ Previous
Next ❯

Related Concepts

Trending Feeds

COVID-19

Coronaviruses encompass a large family of viruses that cause the common cold as well as more serious diseases, such as the ongoing outbreak of coronavirus disease 2019 (COVID-19; formally known as 2019-nCoV). Coronaviruses can spread from animals to humans; symptoms include fever, cough, shortness of breath, and breathing difficulties; in more severe cases, infection can lead to death. This feed covers recent research on COVID-19.

Blastomycosis

Blastomycosis fungal infections spread through inhaling Blastomyces dermatitidis spores. Discover the latest research on blastomycosis fungal infections here.

Nuclear Pore Complex in ALS/FTD

Alterations in nucleocytoplasmic transport, controlled by the nuclear pore complex, may be involved in the pathomechanism underlying multiple neurodegenerative diseases including Amyotrophic Lateral Sclerosis and Frontotemporal Dementia. Here is the latest research on the nuclear pore complex in ALS and FTD.

Applications of Molecular Barcoding

The concept of molecular barcoding is that each original DNA or RNA molecule is attached to a unique sequence barcode. Sequence reads having different barcodes represent different original molecules, while sequence reads having the same barcode are results of PCR duplication from one original molecule. Discover the latest research on molecular barcoding here.

Chronic Fatigue Syndrome

Chronic fatigue syndrome is a disease characterized by unexplained disabling fatigue; the pathology of which is incompletely understood. Discover the latest research on chronic fatigue syndrome here.

Evolution of Pluripotency

Pluripotency refers to the ability of a cell to develop into three primary germ cell layers of the embryo. This feed focuses on the mechanisms that underlie the evolution of pluripotency. Here is the latest research.

Position Effect Variegation

Position Effect Variagation occurs when a gene is inactivated due to its positioning near heterochromatic regions within a chromosome. Discover the latest research on Position Effect Variagation here.

STING Receptor Agonists

Stimulator of IFN genes (STING) are a group of transmembrane proteins that are involved in the induction of type I interferon that is important in the innate immune response. The stimulation of STING has been an active area of research in the treatment of cancer and infectious diseases. Here is the latest research on STING receptor agonists.

Microbicide

Microbicides are products that can be applied to vaginal or rectal mucosal surfaces with the goal of preventing, or at least significantly reducing, the transmission of sexually transmitted infections. Here is the latest research on microbicides.