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Quantitative Measurements of Many-Body Exciton Dynamics in Gaas Quantum-Well Structures

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Quantitative Measurements of Many-Body Exciton Dynamics in Gaas Quantum-Well Structures Quantitative measurements of many-body exciton dynamics in GaAs quantum-well structures by Ryan P. Smith B.S. Physics, Georgia Institute of Technology, 2004 A thesis submitted to the Faculty of the Graduate School of the University of Colorado in partial fulfillment of the requirements for the degree of Doctor of Philosophy Department of Physics 2010 This thesis entitled: Quantitative measurements of many-body exciton dynamics in GaAs quantum-well structures written by Ryan P. Smith has been approved for the Department of Physics Dr. Steven T. Cundiff Dr. Chris H. Greene Date The final copy of this thesis has been examined by the signatories, and we find that both the content and the form meet acceptable presentation standards of scholarly work in the above mentioned discipline. iii Smith, Ryan P. (Ph.D., Physics) Quantitative measurements of many-body exciton dynamics in GaAs quantum-well struc- tures Thesis directed by Professor Dr. Steven T. Cundiff Heterostructures in semiconductors, such as quantum wells, give rise to new optoelec- tronic properties compared to bulk materials by confining the motion of carriers. We study quasiparticles in gallium arsenide (GaAs) quantum wells known as excitons. The absorp- tion spectrum of these excitons exhibits changes at elevated carrier-excitation levels because of many-body interactions between particles. While the spectral absorption changes from these interactions have been studied, a connection between measurements and a microscopic theory has been lacking. The quantitative spectrally resolved transient absorption measurements described in this thesis are combined with a microscopic theory. This combination relates observed spec- tral changes in the probe after ultrashort optical excitation to a unique mixture of electron- hole plasma, exciton, and polarization effects. Through theory-experiment comparison, we deduce the actual carrier-density levels, exciton populations, and other correlations in the system. We find that Coulomb scattering of polarization with free-carrier densities dom- inates the excitation-induced shifting and broadening of the exciton resonance and that exciton populations do not significantly contribute to the excitation-induced effects. We observe a strong transient gain and attribute this feature to a coherent transfer of energy between the pump and probe. Since the excitation-induced effects are strong, theory predicts that the system should display light-statistic-dependent excitation-induced effects. To demonstrate that light statis- tics of optical fields have a meaningful effect on the many-body dynamics, we develop a mea- surement technique involving optical pulse shaping. Our measurements are consistent with iv theoretical predictions that light with incoherent statistics gives rise to weaker excitation- induced effects than does a coherent source that creates the same density of electron-hole pairs. Preliminary results suggest that the observed effects are related to the increased tem- poral duration of the exciting light source. We explore the effects of different pulse shapes to elucidate the primary underlying effects that give rise to the observed weaker excitation- induced effects. Dedication To my parents, who have nurtured me and encouraged me on my path. vi Acknowledgements I would like to thank my advisor, Steve Cundiff, for his thoughtful and patient guidance as I explored uncharted territory. He has inspired me by his enthusiasm for exploring new ideas and for developing helpful intuitive models. Working with Mack Kira has been an incredible pleasure. He has been generous in taking the time to discuss his theories to me, and he continues to challenge me and inspires me to be curious about nature. I am grateful to all the group members of the Cundiff lab. They have helped me enor- mously to find empowerment and confidence in my work, and have been an incredible team. Pete Roos introduced me to the lab and helped me to develop my own system for successful research. Jared Wahlstrand guided me through the early stages of this project and encour- aged me to push forward even when I experienced uncertainties in the research. Andy Funk has inspired me to be inquisitive and to produce quality work through practice. I would like to thank Alan Bristow, Xingcan Dai, and Tianhao Zhang for helpful discussions, and Qing Chao, Hebin Li, Galan Moody, Andy Funk, Haipeng Zhang, Andy Hunter, Mark Siemans, Soobong Choi, and Martina Carsjens for their proof-reading help and encouragement with this thesis. My ‘chunch’ ( chess lunch ) buddy, John Willits, frequently brought me fresh per- | i ⊗ | i spective and kept my brain charged. A number of people have been generous and helpful to me while here at JILA. Jim Faller mentored me and helped me to cultivate an enthusiasm about science even when I was vii buried in technical challenges. Carl Sauer and Terry Brown assisted me and educated me in many electronics issues. Dave Erickson, Jeff Sauter, and Brian Lynch smoothed the road with their unrelenting dedication; it was always a pleasure talking with them – thank you for so many days in paradise. Loree Kaleth helped our group organization, and always brought light into the lab whenever she stepped foot inside. Mike Paige and J. R. Raith patiently helped me with many computing difficulties. Ariel Paul inspires me to continue striving to be a quality scientist, regardless of the path I take in life. Julie Phillips helped me to become a better writer. Dave Alchenberger assisted with many technical issues. I thank Rich Mirin of NIST for high quality quantum-well samples. Wayne Knox brings a smile to my face. I thank Rich Muller (of UC Berkeley) and Mike Dubson for creating the opportunity for me to teach “Physics for future presidents.” John Wood from Georgia Tech introduced me to the joys of physics. I thank my friends, who have been supportive and curious about my work and have offered insight and perspective on this long path; especially David Biagioni, Angela Janzen, Adam Israel Cohen, Elizabeth Merchant, Charles Philbrick, Tara Lanich-LaBrie, Charles Bloch, Stephanie Chasteen, Dana M¨uller-Hoeppe, Michael Barber, Janice Brahney, Ryan Wilson, James McCutchan, Sherry Gillespie, Justin Kuzcynski, Aaron Donner, Joseph Brit- ton, Ethan Townsend, Mark DeRespinis, Candace Gilet, Meghan Barritt, Michael Teves, Caroline Mitchell, Pam and John Bowlan, Rachel Weitz, Tom Phillip. I would lastly like to thank my incredible parents, and my three beautiful sisters: Mom, Dad, Meaghan, Caitlin, and Cara, for being a joyful blessing my life. Contents Chapter 1 Introduction 1 1.1 Thesisorganization ............................... 3 2 Background on excitons in semiconductors 5 2.1 InterestinsemiconductorsandGaAs . 5 2.2 Semiconductors and direct band-gap picture . ........ 6 2.3 ExcitonsinbulkGaAs .............................. 8 2.4 ExcitonsinGaAsquantumwells . 12 2.5 Polarization selection rules QW electronic transitions . ............ 16 2.6 OpticalBlochEquations . 20 2.7 Decoherence and relaxation dynamics of QW excitons . ......... 24 2.8 Homogeneous vs. inhomogeneous broadening . ..... 27 2.9 Spectroscopyofsemiconductors . 28 2.9.1 Drivenoscillatormodel. 28 2.9.2 Linearspectroscopy............................ 29 2.9.3 Nonlinearspectroscopy. 33 2.10 Many-bodyeffectsinGaAsQWs . 37 2.10.1 Excitation-induced dephasing and shifting . ...... 38 2.10.2 Bleaching the exciton resonance . 40 ix 2.10.3 Band-gap renormalization . 41 2.10.4 Excitonicgain............................... 42 2.10.5 Biexcitons................................. 43 3 Experimental techniques 45 3.1 Samplecharacterization . 45 3.2 Linearabsorptionspectrum . 49 3.3 Transient absorption in the nonlinear regime . ....... 49 3.3.1 Experimentalsetup............................ 50 3.3.2 Choosing appropriate pump and probe spot sizes . 53 3.3.3 Estimation of excitation densities . 55 3.3.4 Quantitative measurement of the probe and pump absorption . 58 3.4 Extractionoflineshapeparameters . ..... 60 3.5 Cross-correlation measurement of the pump . 62 3.6 Conclusion..................................... 63 4 Coulomb-induced nonlinearities in semiconductor quantum wells 64 4.1 Introduction.................................... 64 4.2 Theorydevelopment ............................... 64 4.3 Resultsanddiscussion .............................. 67 4.4 Conclusion..................................... 73 4.5 Transition to the study of QW system response to light statistics . ...... 74 5 Background on light statistics and predicted interaction with matter 75 5.1 Coherenceofaclassicalfield . 75 5.1.1 First-ordercoherence . 76 5.1.2 Second-ordercoherence. 79 5.2 Statistics of the quantized electromagnetic field . .......... 82 x 5.2.1 Quantum-mechanical representation of the field . ...... 82 5.2.2 Densitymatrix .............................. 83 5.2.3 Coherence properties of light sources . 83 5.2.4 Photonnumberdistributions. 86 5.2.5 Singletquantities . 88 5.2.6 Coherent state is the classical field . 88 5.3 Phase-space representations of light fields . ....... 89 5.4 Theoretical predictions concerning many-body interactions excited by light havingincoherentstatistics. 91 5.4.1 Why excitons in GaAs quantum wells? . 91 5.4.2 Semiconductor Bloch equations . 93 5.4.3 Coherent on-resonance excitation . 94 5.4.4 Radiative recombination of carriers and excitons . ......... 95 5.4.5 Impact of quantum light statistics on matter . 96 5.4.6 Quantum-opticalspectroscopy . 97 5.4.7 Jaynes-Cummingsmodel . 99 5.5 Summary: thermal vs. coherent light statistics . ....... 105 6 Toward
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