Tracing excited-state photochemistry by multidimensional electronic spectroscopy:
Gespeichert in:
| 1. Verfasser: | |
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| Format: | Abschlussarbeit Buch |
| Sprache: | English |
| Veröffentlicht: |
2013
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| Schlagworte: | |
| Online-Zugang: | Volltext Inhaltsverzeichnis |
| Beschreibung: | Zsfassung in dt. und engl. Sprache |
| Beschreibung: | VI, 194 S. Ill., graph. Darst. |
Internformat
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| 100 | 1 | |a Kullmann, Martin |e Verfasser |0 (DE-588)1042639299 |4 aut | |
| 245 | 1 | 0 | |a Tracing excited-state photochemistry by multidimensional electronic spectroscopy |c von Martin Armin Kullmann |
| 246 | 1 | 3 | |a Auflösung der Photochemie von angeregten Zuständen mittels multidimensionaler elektronischer Spektroskopie |
| 264 | 1 | |c 2013 | |
| 300 | |a VI, 194 S. |b Ill., graph. Darst. | ||
| 336 | |b txt |2 rdacontent | ||
| 337 | |b n |2 rdamedia | ||
| 338 | |b nc |2 rdacarrier | ||
| 500 | |a Zsfassung in dt. und engl. Sprache | ||
| 502 | |a Würzburg, Univ., Diss., 2013 | ||
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Datensatz im Suchindex
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| adam_text | TABLE OF CONTENTS
LIST OF PUBLICATIONS I
1 INTRODUCTION 1
2 THEORETICAL BACKGROUND 5
2.1 MATHEMATICAL DESCRIPTION OF ULTRASHORT LASER PULSES 5
2.1.1 THE ELECTRICAL FIELD IN TIME AND FREQUENCY DOMAIN 6
2.1.2 OPTICAL OBSERVABLES 8
2.1.3 SPATIAL BEAM PROPAGATION 10
2.2 NONLINEAR OPTICS 11
2.2.1 NONLINEAR PROCESSES 12
2.2.2 LASER PULSE CHARACTERIZATION 14
2.3 MOLECULAR TRANSITIONS 16
3 EXPERIMENTED METHODS 21
3.1 LASER SYSTEM 21
3.2 TRANSIENT-ABSORPTION SPECTROSCOPY 22
3.2.1 OBSERVABLE SIGNAL CONTRIBUTIONS 23
3.2.2 SIGNAL EVOLUTION AND DATA ANALYSIS 25
3.2.3 TRANSIENT-ABSORPTION SPECTROMETER 28
3.3 COHERENT TWO-DIMENSIONAL SPECTROSCOPY 30
3.3.1 THEORETICAL DESCRIPTION OF P^(T,R) 31
3.3.2 EXTRACTION OF A TWO-DIMENSIONAL SPECTRUM 34
3.3.3 RELATIONSHIP OF TIME-RESOLVED SPECTROSCOPIC TECHNIQUES ... 36
3.3.4 TWO-DIMENSIONAL SPECTROMETER FOR THE ULTRAVIOLET REGIME . . 37
4 ULTRAFAST EXCITON DYNAMICS OF A BISPORPHYRIN 39
4.1 INTRODUCTION 39
4.2 PHYSICOCHEMICAL PROPERTIES OF PORPHYRINS 41
4.2.1 SPECTRAL CHARACTERIZATION OF PORPHYRINS 41
4.2.2 THE GOUTERMAN MODEL 43
4.2.3 MOLECULAR EXCITONS 44
4.3 EXPERIMENTAL CONDITIONS IN THE TRANSIENT-ABSORPTION EXPERIMENTS . .
49
4.4 ZNTPP * INTRODUCING A PHOTOPHYSICAL MODEL COMPOUND 52
4.4.1 LITERATURE OVERVIEW 52
III
HTTP://D-NB.INFO/1044047216
4.4.2 STEADY-STATE CHARACTERIZATION 54
4.4.3 TRANSIENT-ABSORPTION MEASUREMENTS 55
PHOTODYNAMICS AFTER SORET-BAND EXCITATION 55
PHOTODYNAMICS AFTER Q-BAND EXCITATION 58
4.4.4 DEVELOPMENT OF A TEMPORAL RELAXATION SCHEME 59
4.5 (ZNTPP)
2
* HOW DYNAMICS CHANGE UPON GOING FROM MONOMER TO
DIMER 62
4.5.1 LITERATURE OVERVIEW 63
4.5.2 STEADY-STATE CHARACTERIZATION 65
4.5.3 TRANSIENT-ABSORPTION MEASUREMENTS 66
PHOTODYNAMICS AFTER SORET-BAND EXCITATION 66
PHOTODYNAMICS AFTER Q-BAND EXCITATION 69
PHOTOINDUCED PROPERTIES ON THE PS TIME-SCALE 71
ULTRAFAST PHOTODYNAMICS IN THE NEAR-INFRARED REGIME 71
4.5.4 CREATION OF POSSIBLE TEMPORAL RELAXATION SCHEMES 74
4.6 (ZNTPP)
2
* ACCESSING POPULATION AND ENERGY TRANSFER IN EXCITED
STATES 83
4.6.1 EXPERIMENTAL CONDITIONS 84
4.6.2 TRANSIENT ABSORPTION WITH ULTRAFAST TIME RESOLUTION 85
4.6.3 TRANSIENT-GRATING MEASUREMENTS *
TRANSFER INTO THE BOX GEOMETRY 87
4.6.4 COHERENT ELECTRONIC 2D SPECTROSCOPY 89
4.6.5 VALIDATION OF THE PURELY EXCITONIC REACTION SCHEME 93
4.7 CONCLUSION 98
5 6,8-DINITRO BIPS * COMPREHENSIVE STUDY OF A MOLECULAR SWITCH 101
5.1 INTRODUCTION 101
5.2 MOLECULAR SWITCHES 103
5.2.1 PROPERTIES OF A MOLECULAR SWITCH 104
5.2.2 PERICYCLIC REACTIONS 106
5.2.3 MEROCYANINES AND SPIROPYRANS 108
5.3 SAMPLE CHARACTERISTICS AND PREPARATION 112
5.4 FOLLOWING AN ELECTROCYCLIC RING-OPENING REACTION 113
5.4.1 STEADY-STATE CHARACTERIZATION 113
5.4.2 TRANSIENT-ABSORPTION MEASUREMENTS 115
RELAXATION DYNAMICS AFTER EXCITATION AT 560 NM 115
RELAXATION DYNAMICS AFTER EXCITATION AT 620 NM 118
5.4.3 SIMPLE SPIROPYRAN-MEROCYANINE REACTION SCHEME 120
5.5 ASSESSING POSSIBLE ISOMERIZATION DYNAMICS IN THE EXCITED STATE . . .
124
5.5.1 2D SETUP WITH A CONTINUUM PROBE IN PUMP-PROBE GEOMETRY 125
5.5.2 EXPERIMENTAL PARAMETERS 130
5.5.3 POSSIBLE ISOMERIZATION SCHEMES OF 6,8-DINITRO BIPS 131
5.5.4 2D MEASUREMENTS UNVEILING THE DYNAMICS OF BOTH ISOMERS . . 134
5.5.5 DISCUSSION OF THE ISOMERIZATION SCHEMES 136
5.6 EXPLORING MULTI-STEP REACTION PATHWAYS 139
IV
5.6.1 PUMP-REPUMP-PROBE SPECTROSCOPY: IMPLEMENTATION AND
DATA ANALYSIS 140
5.6.2 RESOLUTION OF TWO ULTRAFAST SUBSEQUENT ELECTROCYCLIC REACTIONS 143
EXPERIMENTAL PARAMETERS 143
TRACKING A CLOSING-OPENING CYCLE 144
TRACKING AN OPENING-CLOSING CYCLE 146
5.6.3 ASSESSING REACTION PATHWAYS ORIGINATING FROM EXCITED STATES
ONLY 149
SPECTRO-TEMPORAL PUMP-REPUMP-PROBE RESULTS 149
VALIDATING CATION FORMATION AFTER TWOFOLD EXCITATION 152
5.6.4 CONCLUSION 154
5.7 TRACING MULTI-STEP PHOTOREACTIONS OF TWO ISOMERIC SPECIES AT ONCE .
155
5.7.1 TRIGGERED-EXCHANGE 2D SPECTROSCOPY 155
5.7.2 RESULTS OF TRIGGERED-EXCHANGE 2D SPECTROSCOPY 157
5.8 COMBINING ALL RESULTS INTO A REACTION SCHEME 159
6 SUMMARY AND OUTLOOK 163
ZUSAMMENFASSUNG 167
LIST OF ABBREVIATIONS 171
BIBLIOGRAPHY 173
ACKNOWLEDGMENTS 195
V
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| spelling | Kullmann, Martin Verfasser (DE-588)1042639299 aut Tracing excited-state photochemistry by multidimensional electronic spectroscopy von Martin Armin Kullmann Auflösung der Photochemie von angeregten Zuständen mittels multidimensionaler elektronischer Spektroskopie 2013 VI, 194 S. Ill., graph. Darst. txt rdacontent n rdamedia nc rdacarrier Zsfassung in dt. und engl. Sprache Würzburg, Univ., Diss., 2013 Angeregter Zustand (DE-588)4142423-2 gnd rswk-swf Fotochemie (DE-588)4045873-8 gnd rswk-swf Femtosekundenspektroskopie (DE-588)4276916-4 gnd rswk-swf Elektronenspektroskopie (DE-588)4014332-6 gnd rswk-swf (DE-588)4113937-9 Hochschulschrift gnd-content Fotochemie (DE-588)4045873-8 s Angeregter Zustand (DE-588)4142423-2 s Elektronenspektroskopie (DE-588)4014332-6 s Femtosekundenspektroskopie (DE-588)4276916-4 s DE-604 Erscheint auch als Online-Ausgabe urn:nbn:de:bvb:20-opus-81276 https://nbn-resolving.org/urn:nbn:de:bvb:20-opus-81276 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=026792962&sequence=000001&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA Inhaltsverzeichnis |
| spellingShingle | Kullmann, Martin Tracing excited-state photochemistry by multidimensional electronic spectroscopy Angeregter Zustand (DE-588)4142423-2 gnd Fotochemie (DE-588)4045873-8 gnd Femtosekundenspektroskopie (DE-588)4276916-4 gnd Elektronenspektroskopie (DE-588)4014332-6 gnd |
| subject_GND | (DE-588)4142423-2 (DE-588)4045873-8 (DE-588)4276916-4 (DE-588)4014332-6 (DE-588)4113937-9 |
| title | Tracing excited-state photochemistry by multidimensional electronic spectroscopy |
| title_alt | Auflösung der Photochemie von angeregten Zuständen mittels multidimensionaler elektronischer Spektroskopie |
| title_auth | Tracing excited-state photochemistry by multidimensional electronic spectroscopy |
| title_exact_search | Tracing excited-state photochemistry by multidimensional electronic spectroscopy |
| title_full | Tracing excited-state photochemistry by multidimensional electronic spectroscopy von Martin Armin Kullmann |
| title_fullStr | Tracing excited-state photochemistry by multidimensional electronic spectroscopy von Martin Armin Kullmann |
| title_full_unstemmed | Tracing excited-state photochemistry by multidimensional electronic spectroscopy von Martin Armin Kullmann |
| title_short | Tracing excited-state photochemistry by multidimensional electronic spectroscopy |
| title_sort | tracing excited state photochemistry by multidimensional electronic spectroscopy |
| topic | Angeregter Zustand (DE-588)4142423-2 gnd Fotochemie (DE-588)4045873-8 gnd Femtosekundenspektroskopie (DE-588)4276916-4 gnd Elektronenspektroskopie (DE-588)4014332-6 gnd |
| topic_facet | Angeregter Zustand Fotochemie Femtosekundenspektroskopie Elektronenspektroskopie Hochschulschrift |
| url | https://nbn-resolving.org/urn:nbn:de:bvb:20-opus-81276 http://bvbr.bib-bvb.de:8991/F?func=service&doc_library=BVB01&local_base=BVB01&doc_number=026792962&sequence=000001&line_number=0001&func_code=DB_RECORDS&service_type=MEDIA |
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