Pulse-sequence approaches for multidimensional electronic spectroscopy of ultrafast photochemistry:
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Format: | Abschlussarbeit Buch |
Sprache: | German |
Veröffentlicht: |
2014
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Online-Zugang: | kostenfrei Inhaltsverzeichnis |
Beschreibung: | Zsfassung in dt. und engl. Sprache |
Beschreibung: | IX, 200 S. graph. Darst. |
Internformat
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Datensatz im Suchindex
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adam_text | PULSE-SEQUENCE APPROACHES FOR
MULTIDIMENSIONAL ELECTRONIC SPECTROSCOPY
OF ULTRAFAST PHOTOCHEMISTRY
DISSERTATION ZUR ERLANGUNG DES
NATURWISSENSCHAFTLICHEN DOKTORGRADES DER
JULIUS-MAXIMILIANS-UNIVERSITAT WIIRZBURG
VORGELEGT VON
STEFAN RIITZEL
AUS MARKTREDWITZ
WIIRZBURG 2014
HTTP://D-NB.INFO/1055055150
CONTENTS
LIST OF PUBLICATIONS III
1 INTRODUCTION 1
2 THEORETICAL BACKGROUND 5
* 2.1 MATHEMATICAL DESCRIPTION OF ULTRASHORT LASER PULSES 5
2.1.1 FREQUENCY- AND TIME-DOMAIN PICTURES 6
2.1.2 JOINT TIME-FREQUENCY DESCRIPTIONS 13
2.1.3 THE POLARIZATION STATE OF ULTRASHORT PULSES 17
2.1.4 SPATIAL BEAM PROPAGATION 21
2.2 NONLINEAR PROCESSES IN ULTRAFAST OPTICS 23
2.2.1 NONLINEAR POLARIZATION 24
2.2.2 FREQUENCY CONVERSION 24
2.3 PHOTOCHEMICAL PROCESSES 31
2.3.1 ELECTRONIC STATES AND TRANSITIONS 31
2.3.2 PHOTOCHEMICAL REACTIONS 34
2.3.3 MOLECULAR WAVE-PACKET DYNAMICS 35
3 EXPERIMENTAL TECHNIQUES 39
3.1 FEMTOSECOND LASER PULSE GENERATION 39
3.1.1 TI:SAPPHIRE LASERS AND CHIRPED PULSE AMPLIFICATION 39
3.1.2 NONCOLLINEAR OPTICAL PARAMETRIC AMPLIFICATION 43
3.2 ULTRAFAST PULSE SHAPING 45
3.3 PULSE CHARACTERIZATION AND COMPRESSION 47
3.4 TRANSIENT ABSORPTION SPECTROSCOPY 51
3.4.1 BASIC PRINCIPLE 51
3.4.2 DATA EVALUATION 55
3.4.3 CORRECTION OF PROBE CHIRP 57
3.4.4 TEMPORAL RESOLUTION 58
3.5 COHERENT TWO-DIMENSIONAL SPECTROSCOPY 59
3.5.1 MOTIVATION 59
3.5.2 THEORETICAL CONCEPTS 61
3.5.3 BEAM GEOMETRIES FOR 2D SPECTROSCOPY 64
4 EXPOSING REACTIVE MODES IN ULTRAFAST PHOTOCHEMISTRY BY THIRD-ORDER
THREE-
DIMENSIONAL ELECTRONIC SPECTROSCOPY 67
4.1 THE SPIROPYRAN-MEROCYANINE PHOTOSYSTEM 67
4.1.1 ISOMERISM OF THE MEROCYANINE FORM 68
STEFAN RQTZEL: PULSE-SEQUENCE APPROACHES FOR MULTIDIMENSIONAL ELECTRONIC
SPECTROSCOPY OF ULTRAFAST PHOTOCHEMISTRY (DISSERTATION UNIVERSITY OF
WURZBURG, 2014)
VIII CONTENTS
4.1.2 STEADY-STATE PROPERTIES OF RING-OPEN 6-NITRO BIPS 70
4.1.3 CURRENT STATE OF RESEARCH 71
4.2 FEMTOSECOND TRANSIENT ABSORPTION SPECTROSCOPY 73
4.2.1 DYNAMICS AFTER EXCITATION AT VARIOUS WAVELENGTHS 73
4.2.2 GLOBAL DATA ANALYSIS 75
4.2.3 ISOMERIZATION QUANTUM YIELD 78
4.2.4 ANALYSIS OF WAVE-PACKET DYNAMICS 80
4.3 REACTION SCHEME 86
4.4 COHERENT TWO-DIMENSIONAL ELECTRONIC SPECTROSCOPY 88
4.4.1 DETECTION OF PHOTOCHEMICAL EXCHANGE IN MULTIDIMENSIONAL ELEC
TRONIC SPECTROSCOPY 88
4.4.2 EXPERIMENTAL IMPLEMENTATION OF 2D SPECTROSCOPY IN THE PUMP-
PROBE BEAM GEOMETRY 90
4.4.3 TWO-DIMENSIONAL SPECTROSCOPY - LONG-TIME DYNAMICS 94
4.4.4 TWO-DIMENSIONAL SPECTROSCOPY - ULTRAFAST PRIMARY PHOTODYNAMICS 97
4.5 THIRD-ORDER THREE-DIMENSIONAL ELECTRONIC SPECTROSCOPY 99
4.6 QUANTUM CHEMICAL CALCULATIONS 103
4.6.1 POTENTIAL ENERGY SURFACES 103
4.6.2 NORMAL MODE ANALYSIS 106
4.7 CONCLUSION 107
5 EXPERIMENTAL IMPLEMENTATION OF FIFTH-ORDER TRIGGERED-EXCHANGE TWO-DI
MENSIONAL ELECTRONIC SPECTROSCOPY 109
5.1 PULSE SEQUENCES IN ULTRAFAST SPECTROSCOPY 110
5.2 6,8-DINITRO BIPS ILL
5.2.1 STEADY-STATE PROPERTIES ILL
5.2.2 PHOTOPHYSICAL AND PHOTOCHEMICAL PROPERTIES 114
5.3 TWO-DIMENSIONAL ELECTRONIC SPECTROSCOPY OF 6,8-DINITRO BIPS 114
5.3.1 ISOMERIZATION SCENARIOS FOR RING-OPEN 6,8-DINITRO BIPS 115
5.3.2 2D ELECTRONIC SPECTRA 117
5.3.3 DISCUSSION OF THE 2D SPECTRA 120
5.4 PUMP-REPUMP-PROBE SPECTROSCOPY 121
5.4.1 EXPERIMENTAL IMPLEMENTATION 121
5.4.2 PUMP-REPUMP-PROBE RESULTS 123
5.5 TRIGGERED-EXCHANGE TWO-DIMENSIONAL ELECTRONIC SPECTROSCOPY 125
5.6 REACTION SCHEME 128
5.7 CONCLUSION 129
6 POLARIZATION PULSE SHAPING IN THE VON NEUMANN FORMALISM FOR ARBITRARY-
ORDER NONLINEARITIES 131
6.1 MOTIVATION 132
6.2 THE VON NEUMANN REPRESENTATION FOR LINEARLY POLARIZED PULSES 135
6.3 GENERALIZATION TO POLARIZATION SHAPED LASER PULSES 140
6.4 EXAMPLE PULSE SHAPES 144
6.5 ACCURACY OF FORWARD- AND BACKWARD-TRANSFORMATIONS 147
STEFAN RQTZEL: PULSE-SEQUENCE APPROACHES FOR MULTIDIMENSIONAL ELECTRONIC
SPECTROSCOPY OF ULTRAFAST PHOTOCHEMISTRY (DISSERTATION UNIVERSITY OF
WSRZBURG, 2014)
CONTENTS IX
6.6 INTERPRETATION OF THE VON NEUMANN PARAMETERS FOR POLARIZATION-SHAPED
PULSES 148
6.7 CONCLUSION 149
7 SUMMARY 151
ZUSAMMENFASSUNG 155
APPENDIX 159
A.L MOLECULAR GEOMETRY OF RING-OPEN 6-NITRO
BIPS
IN THE
FIRST EXCITED STATE
159
A.2 NORMAL MODES OF RING-OPEN 6-NITRO BIPS IN THE FIRST EXCITED STATE .
. 160
A.3 ANALYSIS OF THE NORMAL MODES OF RING-OPEN 6-NITRO BIPS IN THE FIRST
EXCITED STATE 161
A.3.1 MODULATION OF BOND LENGTHS 161
A.3.2 BENDING OF BOND ANGLES 162
A.3.3 TORSIONAL MOTIONS 163
A.4 AUXILIARY CALCULATIONS FOR SECTION 6.3 165
LIST OF ABBREVIATIONS 167
BIBLIOGRAPHY 169
ACKNOWLEDGEMENTS 199
STEFAN RUTZEL: PULSE-SEQUENCE APPROACHES FOR MULTIDIMENSIONAL ELECTRONIC
SPECTROSCOPY OF ULTRAFAST PHOTOCHEMISTRY (DISSERTATION UNIVERSITY OF
WURZBURG, 2014)
|
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author | Rützel, Stefan |
author_GND | (DE-588)1054565422 |
author_facet | Rützel, Stefan |
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spelling | Rützel, Stefan Verfasser (DE-588)1054565422 aut Pulse-sequence approaches for multidimensional electronic spectroscopy of ultrafast photochemistry von Stefan Rützel Pulssequenzmethoden zur multidimensionalen elektronischen Spektroskopie ultraschneller Photochemie 2014 IX, 200 S. graph. Darst. txt rdacontent n rdamedia nc rdacarrier Zsfassung in dt. und engl. Sprache Würzburg, Univ., Diss., 2014 Ultrakurzzeitspektroskopie (DE-588)4209051-9 gnd rswk-swf (DE-588)4113937-9 Hochschulschrift gnd-content Ultrakurzzeitspektroskopie (DE-588)4209051-9 s DE-604 Erscheint auch als Online-Ausgabe urn:nbn:de:bvb:20-opus-98993 https://nbn-resolving.org/urn:nbn:de:bvb:20-opus-98993 Resolving-System kostenfrei Volltext DNB Datenaustausch application/pdf http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=027447851&sequence=000001&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA Inhaltsverzeichnis |
spellingShingle | Rützel, Stefan Pulse-sequence approaches for multidimensional electronic spectroscopy of ultrafast photochemistry Ultrakurzzeitspektroskopie (DE-588)4209051-9 gnd |
subject_GND | (DE-588)4209051-9 (DE-588)4113937-9 |
title | Pulse-sequence approaches for multidimensional electronic spectroscopy of ultrafast photochemistry |
title_alt | Pulssequenzmethoden zur multidimensionalen elektronischen Spektroskopie ultraschneller Photochemie |
title_auth | Pulse-sequence approaches for multidimensional electronic spectroscopy of ultrafast photochemistry |
title_exact_search | Pulse-sequence approaches for multidimensional electronic spectroscopy of ultrafast photochemistry |
title_full | Pulse-sequence approaches for multidimensional electronic spectroscopy of ultrafast photochemistry von Stefan Rützel |
title_fullStr | Pulse-sequence approaches for multidimensional electronic spectroscopy of ultrafast photochemistry von Stefan Rützel |
title_full_unstemmed | Pulse-sequence approaches for multidimensional electronic spectroscopy of ultrafast photochemistry von Stefan Rützel |
title_short | Pulse-sequence approaches for multidimensional electronic spectroscopy of ultrafast photochemistry |
title_sort | pulse sequence approaches for multidimensional electronic spectroscopy of ultrafast photochemistry |
topic | Ultrakurzzeitspektroskopie (DE-588)4209051-9 gnd |
topic_facet | Ultrakurzzeitspektroskopie Hochschulschrift |
url | https://nbn-resolving.org/urn:nbn:de:bvb:20-opus-98993 http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=027447851&sequence=000001&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA |
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