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Correlation spectrosopy of single eitters: fundamental studies and applications related to quantum optics and life science
KTH, Superseded Departments, Microelectronics and Information Technology, IMIT.ORCID iD: 0000-0002-5584-9170
2003 (English)Doctoral 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 discussesapplicationsof 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 , 2003. , xviii, 85 p.
Series
Trita-MVT, ISSN 0348-4467 ; 2003:7
Keyword [en]
optics, analytical chemistry, solid states
National Category
Engineering and Technology
Identifiers
URN: urn:nbn:se:kth:diva-3593ISBN: 91-7283-520-6 (print)OAI: oai:DiVA.org:kth-3593DiVA: diva2:9415
Public defence
2003-09-23, 00:00 (English)
Note
QC 20100423 NR 20140805Available from: 2003-09-16 Created: 2003-09-16 Last updated: 2010-04-28Bibliographically approved
List of papers
1. Analysis of amyloid β-peptides in fluid microchannels
Open this publication in new window or tab >>Analysis of amyloid β-peptides in fluid microchannels
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(English)Manuscript (preprint) (Other academic)
National Category
Engineering and Technology
Identifiers
urn:nbn:se:kth:diva-12465 (URN)
Note

QC 20100429

Available from: 2010-04-26 Created: 2010-04-26 Last updated: 2012-10-01Bibliographically approved
2. Fluorescence correlation spectroscopy with Lorentzian intensity distribution
Open this publication in new window or tab >>Fluorescence correlation spectroscopy with Lorentzian intensity distribution
(English)Manuscript (preprint) (Other academic)
Keyword
Fluorescence correlation spectroscopy, Lorentzian intensity distribution, anlytical autocorrelation function
National Category
Engineering and Technology
Identifiers
urn:nbn:se:kth:diva-12466 (URN)
Note
QC 20100429Available from: 2010-04-26 Created: 2010-04-26 Last updated: 2011-02-08Bibliographically approved
3. Parallel Flow Measurements in Microstructures by Use of a Multifocal 4 x 1 Diffractive Optical Fan-Out Element
Open this publication in new window or tab >>Parallel Flow Measurements in Microstructures by Use of a Multifocal 4 x 1 Diffractive Optical Fan-Out Element
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2002 (English)In: Applied Optics, ISSN 1559-128X, E-ISSN 2155-3165, Vol. 41, no 31, 6614-6620 p.Article in journal (Refereed) Published
Abstract [en]

We have developed a multifocal optical fluorescence correlation spectroscopy system for parallel flow analyses. Multifocal excitation was made possible through a 4 x 1 diffractive optical fan-out element, which produces uniform intensity in all four foci. Autocorrelation flow analyses inside a 20 μm x 20 μm square microchannel, with the 4 x 1 fan-out foci perpendicular to the flow direction, made it possible to monitor different flows in all four foci simultaneously. We were able to perform cross-correlation flow analyses by turning the microstructure, thereby having all four foci parallel to the direction of flow. Transport effects of the diffusion as a function of flow and distance could then also be studied.

Keyword
fluorescence correlation spectroscopy, cross-correlation, gene-expression, arrays, identification, excitation, diffusion, genomics, design, laser
National Category
Engineering and Technology
Identifiers
urn:nbn:se:kth:diva-12447 (URN)10.1364/AO.41.006614 (DOI)000178847600010 ()
Note
QC 20100423Available from: 2010-04-23 Created: 2010-04-23 Last updated: 2017-12-12Bibliographically approved
4. 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
5. 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
6. Multi-focal dual-color cross-correlation spectroscopy of single biomolescules using diffractive-optical-elements
Open this publication in new window or tab >>Multi-focal dual-color cross-correlation spectroscopy of single biomolescules using diffractive-optical-elements
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2003 (English)In: Optics Letters, ISSN 0146-9592, E-ISSN 1539-4794Article in journal (Refereed) Submitted
National Category
Engineering and Technology
Identifiers
urn:nbn:se:kth:diva-12456 (URN)
Note
QC 20100426Available from: 2010-04-26 Created: 2010-04-23 Last updated: 2017-12-12Bibliographically approved
7. Parallel Fluorescence Correlation Spectroscopy with a fully integratedsingle photon 2x2 detector array made with conventional CMOS technology
Open this publication in new window or tab >>Parallel Fluorescence Correlation Spectroscopy with a fully integratedsingle photon 2x2 detector array made with conventional CMOS technology
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2003 (English)In: Optical Technologies in Biophysics and Medicine V: Proceedings of SPIE Vol. 5474 / [ed] Tuchin, Valery V., 2003, 248-258 p.Conference paper, Published paper (Refereed)
Abstract [en]

We present multipoint Fluorescence Correlation Spectroscopy (FCS) experiments with a fully integrated Complementary Metal Oxide Semiconductor (CMOS) single photon 2x2 detector array. Multifocal excitation was achieved with a diffractive optical element (DOE). Special emphasis was put on parallelization of the total system. In particular the performance of the single-photon CMOS detector was investigated and compared to a state-of-the art single-photon detecting module (actively quenched avalanche photo diode) by measurements on free difftising molecules at different concentrations. The potential of our new technique for high throughput FCS based systems is discussed.

Keyword
Fluorescent Correlation Spectroscopy, single-molecule detection, single-photon detector, CMOS technology, diffractive optics
National Category
Engineering and Technology
Identifiers
urn:nbn:se:kth:diva-12455 (URN)10.1117/12.578934 (DOI)2-s2.0-12144263207 (Scopus ID)0-8194-5397-8 (ISBN)
Conference
Saratov Fall Meeting 2003
Note
QC 20100423Available from: 2010-04-23 Created: 2010-04-23 Last updated: 2011-02-11Bibliographically approved
8. 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
9. 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
10. Correlation spectroscopy of excitons and biexcitons on a single quantum dot
Open this publication in new window or tab >>Correlation spectroscopy of excitons and biexcitons on a single quantum dot
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2002 (English)In: Physical Review A. Atomic, Molecular, and Optical Physics, ISSN 1050-2947, E-ISSN 1094-1622, Vol. 66, no 2, 053814-053814-7 p.Article in journal (Refereed) Published
Abstract [en]

We report the observation of antibunched emission from single self-assembled InAs quantum dots under various conditions. We have measured the correlation function of the photon emission pertaining to single emission lines from single quantum dots under continuous and pulsed laser excitation, as well as under continuous white light excitation. The measurements were performed under different excitation intensities at liquid helium temperatures on two samples with distinct structures. At higher temperatures ~30 K!, an antibunching dip was still observed. We have also observed antibunching on a second emission line in the quantum dot spectrum, attributed to the biexciton, demonstrating the possibility of generating photon pairs with a single quantum dot. Polarization correlations on the biexciton and exciton line were also measured in an attempt to generate entangled photon pairs.

Keyword
room-temperature, photons, time
National Category
Engineering and Technology
Identifiers
urn:nbn:se:kth:diva-12449 (URN)10.1103/PhysRevA.66.053814 (DOI)
Note
QC 20100423Available from: 2010-04-23 Created: 2010-04-23 Last updated: 2017-12-12Bibliographically approved

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  • harvard1
  • ieee
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  • Other locale
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Output format
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