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Correlation spectroscopy of single emitters: fundamental studies and applications
KTH, Superseded Departments, Microelectronics and Information Technology, IMIT.ORCID iD: 0000-0002-5584-9170
2001 (English)Licentiate thesis, comprehensive summary (Other scientific)
Abstract [en]

Correlation analysis and correlation spectroscopy has eversince the first developments, to characterise light emittingprocesses and biomolecular dynamics, continued to extend itspractical applicability. Today, correlation spectroscopy can beused in life science to study dynamical processes even at thesingle molecule level. Correlation analysis can in one of itsextreme be applied to investigate single photon processes fromsolid-state emitters. This thesis is an account of my studiesof fluorescent emitter related to quantum optics and lifescience. It presents some fundamental results and discussesapplications of emitters like single quantum dots or singledyes attached to biomolecules. The studies were performed bythe means of correlation analysis and correlation spectroscopyon self-made optical setups. One task of this thesis was todevelop fluorescence correlation spectroscopy for ultravioletexcitation and emission. With ultraviolet excitation thenatural intrinsic chromophores of certain nucleotides and aminoacids can be used. No external labelling of biomolecules couldbecome a reality using ultraviolet excitation and emission. Asecond task was to apply correlation spectroscopy to performhigh spatial-resolution flow profiling and trafficking ofsingle dye-labeled biomolecules in microstructured channels.Future transports effects, flow monitoring, flow profiling andprolonged fluorescence detection in artificial microstructuresor in cells, could benefit from this application. An additionaltask was to apply correlation spectroscopy to so-calledmicroarrays for parallel acquisition of dynamical data at thesingle molecule level. Parallel excitation and detection wasachieved with the use of diffractive optical elements andintegrated semiconductor single-photon sensitive detectors. Thecurrent throughput rate in biological diagnostic or screeninganalysis could be increased dramatically with implementation ofthis parallel confocal excitation and detection technique. Yetanother task of this thesis was to investigations single-photongeneration by InAs-semiconductor quantum dots. We show that aquantum dots can be used for single-photon generation ondemand. Besides the single-photon generation in quantum dots,the possibility of two-photon generation, and generation ofentangled photon-pair, has also been investigated

Place, publisher, year, edition, pages
Stockholm: KTH , 2001. , xiv, 49 p.
Series
Trita-MVT, ISSN 0348-4467 ; 2001:3
National Category
Engineering and Technology
Identifiers
URN: urn:nbn:se:kth:diva-1314ISBN: 91-628-4876-3 (print)OAI: oai:DiVA.org:kth-1314DiVA: diva2:7134
Presentation
(English)
Note
QC 20100420 NR 20140805Available from: 2001-10-23 Created: 2001-10-23 Last updated: 2010-04-28Bibliographically approved
List of papers
1. Elliptical line focus in fluorescence spectroscopy: theory and application
Open this publication in new window or tab >>Elliptical line focus in fluorescence spectroscopy: theory and application
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(English)Manuscript (preprint) (Other academic)
National Category
Engineering and Technology
Identifiers
urn:nbn:se:kth:diva-12445 (URN)
Note
QC 20100423Available from: 2010-04-23 Created: 2010-04-23 Last updated: 2011-02-08Bibliographically approved
2. Parallel Fluorescence Detection of Single Biomolecules in Microarrays by a Diffractive-Optical-Designed 2 x 2 Fan-Out Element
Open this publication in new window or tab >>Parallel Fluorescence Detection of Single Biomolecules in Microarrays by a Diffractive-Optical-Designed 2 x 2 Fan-Out Element
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2002 (English)In: Applied Optics, ISSN 1559-128X, E-ISSN 2155-3165, Vol. 41, no 16, 3336-3342 p.Article in journal (Refereed) Published
Abstract [en]

We have developed a multifocal diffractive-optical fluorescence correlation spectroscopy system for parallel excitation and detection of single tetramethylrhodamine biomolecules in microarrays. Multifocal excitation was made possible through the use of a 2 × 2 fan-out diffractive-optical element with uniform intensity in all foci. Characterization of the 2 × 2 fan-out diffractive-optical element shows formation of almost perfect Gaussian foci of submicrometer lateral diameter, as analyzed by thermal motion of tetramethylrhodamine dye molecules in solution. Results of parallel excitation and detection in a high-density microarray of circular wells show single-biomolecule sensitivity in all four foci simultaneously.

Keyword
correlation spectroscopy, oligonucleotide arrays, gene-expression, molecules, identification, genomics, diagnostics
National Category
Engineering and Technology
Identifiers
urn:nbn:se:kth:diva-12446 (URN)10.1364/AO.41.003336 (DOI)000175917600045 ()
Note
QC 20100423Available from: 2010-04-23 Created: 2010-04-23 Last updated: 2017-12-12Bibliographically approved
3. Hydrodynamic Flow Profiling in Microchannel Structures by Single Molecule Fluorescence Correlation Spectroscopy
Open this publication in new window or tab >>Hydrodynamic Flow Profiling in Microchannel Structures by Single Molecule Fluorescence Correlation Spectroscopy
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2000 (English)In: Analytical Chemistry, ISSN 0003-2700, E-ISSN 1520-6882, Vol. 72, no 14, 3260-3265 p.Article in journal (Refereed) Published
Abstract [en]

In this paper we demonstrate high spatial resolution hydrodynamic flow profiling in silicon wafer based microchannels using single molecule fluorescence correlation spectroscopy (FCS). We have used confocal fluorescence microscopy to detect single tetramethylrhodamine (TMR-4-dUTP) biomolecules traversing a l fL volume element defined by an argon laser beam focus. By elevating a (10-10 M) reservoir of diluted analyte, a continuous hydrodynamic flow through the microstructure could be accomplished. The microchannel was then scanned with a diffraction-limited focus in 1-μm steps in both the vertical and the horizontal directions to determine the flow profile across a 50 × 50 μm2 channel. The flow profile measured was parabolic in both dimensions, thereby showing a Poiseuille laminar flow profile. Future microstructures can hereby be nondestructively investigated with the use of high spatial resolution confocal correlation microscopy.

National Category
Engineering and Technology
Identifiers
urn:nbn:se:kth:diva-12417 (URN)10.1021/ac991448p (DOI)000088347100038 ()
Note
QC 20100420Available from: 2010-04-20 Created: 2010-04-20 Last updated: 2017-12-12Bibliographically approved
4. UV-Fluorescence Correlation Spectroscopy of 2-Aminopurine
Open this publication in new window or tab >>UV-Fluorescence Correlation Spectroscopy of 2-Aminopurine
2001 (English)In: Biological chemistry (Print), ISSN 1431-6730, E-ISSN 1437-4315, Vol. 382, no 3, 393-397 p.Article in journal (Refereed) Published
Abstract [en]

We have built a fluorescence correlation spectroscopy (FCS) microscope for ultraviolet excitation (280 300 nm) and emission. With UV excitation the fluorescence of natural fluorophores such as the modified nucleotide 2-aminopurine can be analyzed. The sensitivity of a natural fluorophore toward conformational changes can reveal dynamics in biomolecules. UVFCS is well suited for detection of intensity fluctuations related to such conformational dynamics. Here we show UVFCS measured on pQuarterphenyl and on 2-aminopurine (2-AP). The triplet state rate constants and the excitation cross section for 2- AP were estimated to k[23]=1 x 10[6] s[-1], k[31]=3 x 10[5] s[-1], and σ=2 x 10[-17] cm[2].

Keyword
dynamics of nucleic acids, FCS, UV fluorescence
National Category
Engineering and Technology
Identifiers
urn:nbn:se:kth:diva-12416 (URN)10.1515/BC.2001.048 (DOI)000168406100007 ()
Note
QC 20100420Available from: 2010-04-20 Created: 2010-04-20 Last updated: 2017-12-12Bibliographically approved
5. Single quantum dots emit single photons at a time: Antibunching experiments
Open this publication in new window or tab >>Single quantum dots emit single photons at a time: Antibunching experiments
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2001 (English)In: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 78, no 17, 2476- p.Article in journal (Refereed) Published
Abstract [en]

We have studied the photoluminescence correlation from a single InAs/GaAs self-assembled Stranski–Krastanow quantum dot under continuous, as well as under pulsed excitation. Under weak continuous excitation, where the single dot luminescence is due primarily to single exciton recombinations, antibunching is observed in the single dot emission correlation. Under weak pulsed excitation, the number of photons emitted by the quantum dot per pulse is close to one. We present data obtained under both conditions and are able to show that devices based on single quantum dots can be used to generate single photons.

Keyword
room-temperature, fluorescence, molecule, gaas
National Category
Engineering and Technology
Identifiers
urn:nbn:se:kth:diva-12418 (URN)10.1063/1.1366367 (DOI)000168304600021 ()
Note
QC 20100420Available from: 2010-04-20 Created: 2010-04-20 Last updated: 2017-12-12Bibliographically approved

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