Atomistically resolved hot exciton relaxation dynamics in CdSe quantum dots: Experiment and theory

Ghosh, Arnab; Peng, Kaiyue; Brosseau, Patrick J.; Rabani, Eran; Kambhampati, Patanjali

doi:10.1063/5.0272621

Atomistically resolved hot exciton relaxation dynamics in CdSe quantum dots: Experiment and theory

Journal Article · Tue Sep 09 00:00:00 EDT 2025 · The Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0272621· OSTI ID:2998202

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McGill Univ., Montreal, QC (Canada)
University of California, Berkeley, CA (United States)
University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Tel Aviv Univ., Tel Aviv (Israel)

Semiconductor quantum dots (QDs) are well known to give rise to a quantum confined structure of excitons. Because of this quantum confinement, new physics of hot exciton relaxation dynamics arises. Decades of work using transient absorption (TA) spectroscopy have yielded initial simple observations, such as estimates of the cooling rate from single pump photon energy experiments. More detailed TA experiments employed variable pump photon energies to measure excitonic state-resolved transition rates. These TA measurements, usually the simplest form, have been employed to characterize QDs and their relaxation dynamics to this day. Yet, these TA measurements are fundamentally lacking in their ability to measure energy-resolved hot exciton cooling, which requires observation of the full cooling history through the real excitonic manifold. Here, we employ coherent multi-dimensional spectroscopy (CMDS) to perform an atomistically directed study of hot exciton cooling in CdSe QDs, revealing energy resolved relaxation dynamics. CMDS experiments are compared with simulations and prior TA measurements and simpler theories. Our findings reveal a hot exciton relaxation dynamics landscape. This relaxation dynamics landscape is a linear or sub-linear function of excess energy for different structures of QDs, with a strong size dependence. Furthermore, our model simulations parameterized by the empirical pseudopotential model reproduces the experimental functional form and the dependence upon QD diameter and shell.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), High Energy Physics (HEP); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 2998202

Journal Information:: The Journal of Chemical Physics, Journal Name: The Journal of Chemical Physics Journal Issue: 10 Vol. 163; ISSN 1089-7690; ISSN 0021-9606

Publisher:: AIP PublishingCopyright Statement

Country of Publication:: United States

Language:: English

References (114)

Intraband Cooling in All‐Inorganic and Hybrid Organic–Inorganic Perovskite Nanocrystals Diroll, Benjamin T.; Schaller, Richard D. Advanced Functional Materials, Vol. 29, Issue 37 https://doi.org/10.1002/adfm.201901725	journal	July 2019
Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
Breaking the phonon bottleneck in nanometer quantum dots: Role of Auger-like processes Efros, Al. L.; Kharchenko, V. A.; Rosen, M. Solid State Communications, Vol. 93, Issue 4, p. 281-284 https://doi.org/10.1016/0038-1098(94)00760-8	journal	January 1995
Two-dimensional electronic spectroscopy Hybl, John D.; Albrecht, Allison W.; Gallagher Faeder, Sarah M. Chemical Physics Letters, Vol. 297, Issue 3-4 https://doi.org/10.1016/S0009-2614(98)01140-3	journal	November 1998
Surface and interface effects on non-radiative exciton recombination and relaxation dynamics in CdSe/Cd,Zn,S nanocrystals Walsh, Brenna R.; Saari, Jonathan I.; Krause, Michael M. Chemical Physics, Vol. 471 https://doi.org/10.1016/j.chemphys.2015.11.004	journal	June 2016
Spin relaxation in zinc blende and wurtzite CdSe quantum dots Huxter, Vanessa M.; Kim, Jeongho; Lo, Shun S. Chemical Physics Letters, Vol. 491, Issue 4-6 https://doi.org/10.1016/j.cplett.2010.03.081	journal	May 2010
Quantum size effect in semiconductor microcrystals Ekimov, A. I.; Efros, Al. L.; Onushchenko, A. A. Solid State Communications, Vol. 56, Issue 11, p. 921-924 https://doi.org/10.1016/s0038-1098(85)80025-9	journal	December 1985
Coherent Two-Dimensional and Broadband Electronic Spectroscopies Biswas, Somnath; Kim, JunWoo; Zhang, Xinzi Chemical Reviews, Vol. 122, Issue 3 https://doi.org/10.1021/acs.chemrev.1c00623	journal	January 2022
Spectroscopic and Device Aspects of Nanocrystal Quantum Dots Pietryga, Jeffrey M.; Park, Young-Shin; Lim, Jaehoon Chemical Reviews, Vol. 116, Issue 18 https://doi.org/10.1021/acs.chemrev.6b00169	journal	September 2016
Role of Atomic Structure on Exciton Dynamics and Photoluminescence in NIR Emissive InAs/InP/ZnSe Quantum Dots Enright, Michael J.; Jasrasaria, Dipti; Hanchard, Mathilde M. The Journal of Physical Chemistry C, Vol. 126, Issue 17 https://doi.org/10.1021/acs.jpcc.2c01499	journal	April 2022
Spectator Exciton Effects on Nanocrystal Photophysics II: PbS Dana, Jayanta; Ghosh, Tufan; Gdor, Itay The Journal of Physical Chemistry C, Vol. 126, Issue 45 https://doi.org/10.1021/acs.jpcc.2c06591	journal	November 2022
Controlling the Surface of Semiconductor Nanocrystals for Efficient Light Emission from Single Excitons to Multiexcitons Walsh, Brenna R.; Saari, Jonathan I.; Krause, Michael M. The Journal of Physical Chemistry C, Vol. 119, Issue 28 https://doi.org/10.1021/acs.jpcc.5b03853	journal	June 2015
Interfacial Electronic Structure in Graded Shell Nanocrystals Dictates Their Performance for Optical Gain Walsh, Brenna R.; Saari, Jonathan I.; Krause, Michael M. The Journal of Physical Chemistry C, Vol. 120, Issue 34 https://doi.org/10.1021/acs.jpcc.6b05836	journal	August 2016
Excited State Phononic Processes in Semiconductor Nanocrystals Revealed by Excitonic State-Resolved Pump/Probe Spectroscopy Walsh, Brenna R.; Sonnichsen, Colin; Mack, Timothy G. The Journal of Physical Chemistry C, Vol. 123, Issue 6 https://doi.org/10.1021/acs.jpcc.8b11099	journal	January 2019
Solving Quantum-Dot Excitonic Riddles with Absolute Pump–Probe Spectroscopy Ruhman, Sanford The Journal of Physical Chemistry Letters, Vol. 12, Issue 38 https://doi.org/10.1021/acs.jpclett.1c02408	journal	September 2021
Origin of Vibronic Coherences During Carrier Cooling in Colloidal Quantum Dots Hetherington, Caitlin V.; Mohan T. M., Nila; Tilluck, Ryan W. The Journal of Physical Chemistry Letters, Vol. 14, Issue 51 https://doi.org/10.1021/acs.jpclett.3c02384	journal	December 2023
Two-Dimensional Electronic Spectroscopy Reveals Dynamics within the Bright Fine Structure of CdSe Quantum Dots Brosseau, Patrick; Jasrasaria, Dipti; Ghosh, Arnab The Journal of Physical Chemistry Letters, Vol. 15, Issue 6 https://doi.org/10.1021/acs.jpclett.3c03378	journal	February 2024
Spin Blockades to Relaxation of Hot Multiexcitons in Nanocrystals Ghosh, Tufan; Dehnel, Joanna; Fabian, Marcel The Journal of Physical Chemistry Letters, Vol. 10, Issue 10 https://doi.org/10.1021/acs.jpclett.9b00992	journal	April 2019
Interplay of Surface and Interior Modes in Exciton–Phonon Coupling at the Nanoscale Jasrasaria, Dipti; Rabani, Eran Nano Letters, Vol. 21, Issue 20 https://doi.org/10.1021/acs.nanolett.1c02953	journal	October 2021
Polaritonic Bottleneck in Colloidal Quantum Dots Peng, Kaiyue; Rabani, Eran Nano Letters, Vol. 23, Issue 22 https://doi.org/10.1021/acs.nanolett.3c03508	journal	November 2023
Intrinsically Slow Cooling of Hot Electrons in CdSe Nanocrystals Compared to CdS Coley-O’Rourke, Matthew J.; Hou, Bokang; Sherman, Skylar J. Nano Letters, Vol. 25, Issue 1 https://doi.org/10.1021/acs.nanolett.4c04912	journal	December 2024
Origins of Stokes Shift in PbS Nanocrystals Voznyy, Oleksandr; Levina, Larissa; Fan, Fengjia Nano Letters, Vol. 17, Issue 12 https://doi.org/10.1021/acs.nanolett.7b01843	journal	November 2017
Tuning Electron–Phonon Interactions in Nanocrystals through Surface Termination Yazdani, Nuri; Bozyigit, Deniz; Vuttivorakulchai, Kantawong Nano Letters, Vol. 18, Issue 4 https://doi.org/10.1021/acs.nanolett.7b04729	journal	March 2018
Seeing Multiexcitons through Sample Inhomogeneity: Band-Edge Biexciton Structure in CdSe Nanocrystals Revealed by Two-Dimensional Electronic Spectroscopy Seiler, Hélène; Palato, Samuel; Sonnichsen, Colin Nano Letters, Vol. 18, Issue 5 https://doi.org/10.1021/acs.nanolett.8b00470	journal	March 2018
Phonon-Mediated and Weakly Size-Dependent Electron and Hole Cooling in CsPbBr ₃ Nanocrystals Revealed by Atomistic Simulations and Ultrafast Spectroscopy Boehme, Simon C.; Brinck, Stephanie ten; Maes, Jorick Nano Letters, Vol. 20, Issue 3 https://doi.org/10.1021/acs.nanolett.9b05051	journal	February 2020
Nanocrystal Quantum Dots: From Discovery to Modern Development Efros, Alexander L.; Brus, Louis E. ACS Nano, Vol. 15, Issue 4 https://doi.org/10.1021/acsnano.1c01399	journal	April 2021
Strongly Confined CsPbBr₃ Quantum Dots as Quantum Emitters and Building Blocks for Rhombic Superlattices Boehme, Simon C.; Bodnarchuk, Maryna I.; Burian, Max ACS Nano, Vol. 17, Issue 3 https://doi.org/10.1021/acsnano.2c07677	journal	January 2023
Breaking Phonon Bottlenecks through Efficient Auger Processes in Perovskite Nanocrystals Baker, Harry; Perez, Carlos Mora; Sonnichsen, Colin ACS Nano, Vol. 17, Issue 4 https://doi.org/10.1021/acsnano.2c12220	journal	February 2023
Ligands Slow Down Pure-Dephasing in Semiconductor Quantum Dots Liu, Jin; Kilina, Svetlana V.; Tretiak, Sergei ACS Nano, Vol. 9, Issue 9 https://doi.org/10.1021/acsnano.5b03255	journal	August 2015
Hole Cooling Is Much Faster than Electron Cooling in PbSe Quantum Dots Spoor, Frank C. M.; Kunneman, Lucas T.; Evers, Wiel H. ACS Nano, Vol. 10, Issue 1 https://doi.org/10.1021/acsnano.5b05731	journal	December 2015
Broadband Cooling Spectra of Hot Electrons and Holes in PbSe Quantum Dots Spoor, Frank C. M.; Tomić, Stanko; Houtepen, Arjan J. ACS Nano, Vol. 11, Issue 6 https://doi.org/10.1021/acsnano.7b02506	journal	May 2017
Origins of the Stokes Shift in PbS Quantum Dots: Impact of Polydispersity, Ligands, and Defects Liu, Yun; Kim, Donghun; Morris, Owen P. ACS Nano, Vol. 12, Issue 3 https://doi.org/10.1021/acsnano.8b00132	journal	February 2018
Unraveling the Structure and Dynamics of Excitons in Semiconductor Quantum Dots Kambhampati, Patanjali Accounts of Chemical Research, Vol. 44, Issue 1 https://doi.org/10.1021/ar1000428	journal	January 2011
Photoinduced Dynamics in Semiconductor Quantum Dots: Insights from Time-Domain ab Initio Studies Prezhdo, Oleg V. Accounts of Chemical Research, Vol. 42, Issue 12 https://doi.org/10.1021/ar900157s	journal	December 2009
Spectator Exciton Effects in Nanocrystals III: Unveiling the Stimulated Emission Cross Section in Quantum Confined CsPbBr₃ Nanocrystals De, Apurba; Bhunia, Soumyadip; Cai, Yichao Journal of the American Chemical Society, Vol. 146, Issue 29 https://doi.org/10.1021/jacs.4c05412	journal	July 2024
Mechanisms for Photogeneration and Recombination of Multiexcitons in Semiconductor Nanocrystals: Implications for Lasing and Solar Energy Conversion Klimov, Victor I. The Journal of Physical Chemistry B, Vol. 110, Issue 34 https://doi.org/10.1021/jp0615959	journal	August 2006
Hot Exciton Relaxation Dynamics in Semiconductor Quantum Dots: Radiationless Transitions on the Nanoscale Kambhampati, Patanjali The Journal of Physical Chemistry C, Vol. 115, Issue 45 https://doi.org/10.1021/jp2058673	journal	October 2011
Theoretical Study of Electron–Phonon Relaxation in PbSe and CdSe Quantum Dots: Evidence for Phonon Memory Kilina, Svetlana V.; Kilin, Dmitri S.; Prezhdo, Victor V. The Journal of Physical Chemistry C, Vol. 115, Issue 44 https://doi.org/10.1021/jp206594e	journal	October 2011
Control of Phonons in Semiconductor Nanocrystals via Femtosecond Pulse Chirp-Influenced Wavepacket Dynamics and Polarization Mooney, Jonathan; Saari, Jonathan I.; Myers Kelley, Anne The Journal of Physical Chemistry B, Vol. 117, Issue 49 https://doi.org/10.1021/jp406323f	journal	September 2013
State-Resolved Exciton−Phonon Couplings in CdSe Semiconductor Quantum Dots Sagar, D. M.; Cooney, Ryan R.; Sewall, Samuel L. The Journal of Physical Chemistry C, Vol. 112, Issue 25 https://doi.org/10.1021/jp803386g	journal	May 2008
High-Energy Excitonic Transitions in CdSe Quantum Dots No authors listed The Journal of Physical Chemistry B, Vol. 102, Issue 34 https://doi.org/10.1021/jp981018n	journal	August 1998
Optical Nonlinearities and Ultrafast Carrier Dynamics in Semiconductor Nanocrystals Klimov, Victor I. The Journal of Physical Chemistry B, Vol. 104, Issue 26 https://doi.org/10.1021/jp9944132	journal	July 2000
Ultrafast Exciton Fine Structure Relaxation Dynamics in Lead Chalcogenide Nanocrystals Johnson, Justin C.; Gerth, Kathrine A.; Song, Qing Nano Letters, Vol. 8, Issue 5 https://doi.org/10.1021/nl080126a	journal	May 2008
Bulklike Hot Carrier Dynamics in Lead Sulfide Quantum Dots Cho, Byungmoon; Peters, William K.; Hill, Robert J. Nano Letters, Vol. 10, Issue 7 https://doi.org/10.1021/nl1010349	journal	July 2010
Controlling Piezoelectric Response in Semiconductor Quantum Dots via Impulsive Charge Localization Tyagi, Pooja; Cooney, Ryan R.; Sewall, Samuel L. Nano Letters, Vol. 10, Issue 8 https://doi.org/10.1021/nl101605r	journal	July 2010
Slow Hot-Carrier Relaxation in Colloidal Graphene Quantum Dots Mueller, Mallory L.; Yan, Xin; Dragnea, Bogdan Nano Letters, Vol. 11, Issue 1 https://doi.org/10.1021/nl102712x	journal	January 2011
Femtosecond Cooling of Hot Electrons in CdSe Quantum-Well Platelets Sippel, Philipp; Albrecht, Wiebke; van der Bok, Johanna C. Nano Letters, Vol. 15, Issue 4 https://doi.org/10.1021/nl504706w	journal	March 2015
Surface Ligands Increase Photoexcitation Relaxation Rates in CdSe Quantum Dots Kilina, Svetlana; Velizhanin, Kirill A.; Ivanov, Sergei ACS Nano, Vol. 6, Issue 7 https://doi.org/10.1021/nn302371q	journal	June 2012
Three-Pulse Femtosecond Spectroscopy of PbSe Nanocrystals: 1S Bleach Nonlinearity and Sub-Band-Edge Excited-State Absorption Assignment Gdor, Itay; Shapiro, Arthur; Yang, Chunfan ACS Nano, Vol. 9, Issue 2 https://doi.org/10.1021/nn5074868	journal	January 2015
Breaking the Phonon Bottleneck in PbSe and CdSe Quantum Dots: Time-Domain Density Functional Theory of Charge Carrier Relaxation Kilina, Svetlana V.; Kilin, Dmitri S.; Prezhdo, Oleg V. ACS Nano, Vol. 3, Issue 1 https://doi.org/10.1021/nn800674n	journal	December 2008
Observation of a phonon bottleneck in copper-doped colloidal quantum dots Wang, Lifeng; Chen, Zongwei; Liang, Guijie Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-12558-y	journal	October 2019
Two-dimensional electronic spectroscopy reveals liquid-like lineshape dynamics in CsPbI3 perovskite nanocrystals Seiler, Hélène; Palato, Samuel; Sonnichsen, Colin Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-12830-1	journal	October 2019
Circumventing the phonon bottleneck by multiphonon-mediated hot exciton cooling at the nanoscale Jasrasaria, Dipti; Rabani, Eran npj Computational Materials, Vol. 9, Issue 1 https://doi.org/10.1038/s41524-023-01102-8	journal	August 2023
Ultrafast hole relaxation dynamics in quantum dots revealed by two-dimensional electronic spectroscopy Brosseau, Patrick J.; Geuchies, Jaco J.; Jasrasaria, Dipti Communications Physics, Vol. 6, Issue 1 https://doi.org/10.1038/s42005-023-01169-1	journal	March 2023
Two-dimensional electronic spectroscopy Fresch, Elisa; Camargo, Franco V. A.; Shen, Qijie Nature Reviews Methods Primers, Vol. 3, Issue 1 https://doi.org/10.1038/s43586-023-00267-2	journal	November 2023
Testing the fate of nascent holes in CdSe nanocrystals with sub-10 fs pump–probe spectroscopy Dana, Jayanta; Haggag, Omer S.; Dehnel, Joanna Nanoscale, Vol. 13, Issue 3 https://doi.org/10.1039/d0nr07651a	journal	January 2021
Colloidal chemical synthesis and characterization of InAs nanocrystal quantum dots Guzelian, A. A.; Banin, U.; Kadavanich, A. V. Applied Physics Letters, Vol. 69, Issue 10 https://doi.org/10.1063/1.117605	journal	September 1996
Comparison of the k⋅p and the direct diagonalization approaches for describing the electronic structure of quantum dots Fu, Huaxiang; Wang, Lin-Wang; Zunger, Alex Applied Physics Letters, Vol. 71, Issue 23 https://doi.org/10.1063/1.120421	journal	December 1997
Comment on “Comparison of the k⋅p and the direct diagonalization approaches for describing the electron structure of quantum dots” [Appl. Phys. Lett. 71, 3433 (1997)] Efros, Al. L.; Rosen, M. Applied Physics Letters, Vol. 73, Issue 8 https://doi.org/10.1063/1.122114	journal	August 1998
Two-dimensional Fourier transform electronic spectroscopy Hybl, John D.; Albrecht Ferro, Allison; Jonas, David M. The Journal of Chemical Physics, Vol. 115, Issue 14, p. 6606-6622 https://doi.org/10.1063/1.1398579	journal	October 2001
State-resolved studies of biexcitons and surface trapping dynamics in semiconductor quantum dots Sewall, Samuel L.; Cooney, Ryan R.; Anderson, Kevin E. H. The Journal of Chemical Physics, Vol. 129, Issue 8 https://doi.org/10.1063/1.2971181	journal	August 2008
Experimental tests of effective mass and atomistic approaches to quantum dot electronic structure: Ordering of electronic states Sewall, Samuel L.; Cooney, Ryan R.; Kambhampati, Patanjali Applied Physics Letters, Vol. 94, Issue 24 https://doi.org/10.1063/1.3157269	journal	June 2009
Electron–electron and electron‐hole interactions in small semiconductor crystallites: The size dependence of the lowest excited electronic state Brus, L. E. The Journal of Chemical Physics, Vol. 80, Issue 9 https://doi.org/10.1063/1.447218	journal	May 1984
The band edge luminescence of surface modified CdSe nanocrystallites: Probing the luminescing state Kuno, M.; Lee, J. K.; Dabbousi, B. O. The Journal of Chemical Physics, Vol. 106, Issue 23 https://doi.org/10.1063/1.473875	journal	June 1997
Kilohertz generation of high contrast polarization states for visible femtosecond pulses via phase-locked acousto-optic pulse shapers Seiler, Hélène; Walsh, Brenna; Palato, Samuel Journal of Applied Physics, Vol. 118, Issue 10 https://doi.org/10.1063/1.4929954	journal	September 2015
Coherent multi-dimensional spectroscopy at optical frequencies in a single beam with optical readout Seiler, Hélène; Palato, Samuel; Kambhampati, Patanjali The Journal of Chemical Physics, Vol. 147, Issue 9 https://doi.org/10.1063/1.4990500	journal	September 2017
Investigating exciton structure and dynamics in colloidal CdSe quantum dots with two-dimensional electronic spectroscopy Seiler, H.; Palato, S.; Kambhampati, P. The Journal of Chemical Physics, Vol. 149, Issue 7 https://doi.org/10.1063/1.5037223	journal	August 2018
An analysis of hollow-core fiber for applications in coherent femtosecond spectroscopies Palato, Samuel; Seiler, Hélène; Baker, Harry Journal of Applied Physics, Vol. 128, Issue 10 https://doi.org/10.1063/1.5113691	journal	September 2020
Investigating the electronic structure of confined multiexcitons with nonlinear spectroscopies Palato, S.; Seiler, H.; Baker, H. The Journal of Chemical Physics, Vol. 152, Issue 10 https://doi.org/10.1063/1.5142180	journal	March 2020
Fifth-order two-quantum absorptive two-dimensional electronic spectroscopy of CdSe quantum dots Brosseau, Patrick; Palato, Samuel; Seiler, Hélène The Journal of Chemical Physics, Vol. 153, Issue 23 https://doi.org/10.1063/5.0021381	journal	December 2020
Simulations of nonradiative processes in semiconductor nanocrystals Jasrasaria, Dipti; Weinberg, Daniel; Philbin, John P. The Journal of Chemical Physics, Vol. 157, Issue 2 https://doi.org/10.1063/5.0095897	journal	July 2022
Exciton–polaron interactions in metal halide perovskite nanocrystals revealed via two-dimensional electronic spectroscopy Brosseau, Patrick; Ghosh, Arnab; Seiler, Helene The Journal of Chemical Physics, Vol. 159, Issue 18 https://doi.org/10.1063/5.0173369	journal	November 2023
Polariton-assisted incoherent to coherent excitation energy transfer between colloidal nanocrystal quantum dots Peng, Kaiyue; Rabani, Eran The Journal of Chemical Physics, Vol. 161, Issue 15 https://doi.org/10.1063/5.0223369	journal	October 2024
Atomic fluctuations in electronic materials revealed by dephasing Palato, Samuel; Seiler, Hélène; Nijjar, Parmeet Proceedings of the National Academy of Sciences, Vol. 117, Issue 22 https://doi.org/10.1073/pnas.1916792117	journal	May 2020
State-to-state exciton dynamics in semiconductor quantum dots Sewall, Samuel L.; Cooney, Ryan R.; Anderson, Kevin E. H. Physical Review B, Vol. 74, Issue 23 https://doi.org/10.1103/PhysRevB.74.235328	journal	December 2006
Unified picture of electron and hole relaxation pathways in semiconductor quantum dots Cooney, Ryan R.; Sewall, Samuel L.; Dias, Eva A. Physical Review B, Vol. 75, Issue 24 https://doi.org/10.1103/PhysRevB.75.245311	journal	June 2007
Size dependent, state-resolved studies of exciton-phonon couplings in strongly confined semiconductor quantum dots Sagar, D. M.; Cooney, Ryan R.; Sewall, Samuel L. Physical Review B, Vol. 77, Issue 23 https://doi.org/10.1103/PhysRevB.77.235321	journal	June 2008
Direct observation of the structure of band-edge biexcitons in colloidal semiconductor CdSe quantum dots Sewall, Samuel L.; Franceschetti, Alberto; Cooney, Ryan R. Physical Review B, Vol. 80, Issue 8 https://doi.org/10.1103/PhysRevB.80.081310	journal	August 2009
State-resolved observation in real time of the structural dynamics of multiexcitons in semiconductor nanocrystals Sewall, Samuel L.; Cooney, Ryan R.; Dias, Eva A. Physical Review B, Vol. 84, Issue 23 https://doi.org/10.1103/PhysRevB.84.235304	journal	December 2011
Gain Control in Semiconductor Quantum Dots via State-Resolved Optical Pumping Cooney, Ryan R.; Sewall, Samuel L.; Sagar, D. M. Physical Review Letters, Vol. 102, Issue 12 https://doi.org/10.1103/PhysRevLett.102.127404	journal	March 2009
Spectral Analysis of Photoemissive Yields in Si, Ge, GaAs, GaSb, InAs, and InSb Cohen, M. L.; Phillips, J. C. Physical Review, Vol. 139, Issue 3A https://doi.org/10.1103/physrev.139.a912	journal	August 1965
Band Structures and Pseudopotential Form Factors for Fourteen Semiconductors of the Diamond and Zinc-blende Structures Cohen, Marvin L.; Bergstresser, T. K. Physical Review, Vol. 141, Issue 2 https://doi.org/10.1103/physrev.141.789	journal	January 1966
Phonon scattering and energy relaxation in two-, one-, and zero-dimensional electron gases Bockelmann, U.; Bastard, G. Physical Review B, Vol. 42, Issue 14 https://doi.org/10.1103/physrevb.42.8947	journal	November 1990
Local-density-derived semiempirical pseudopotentials Wang, Lin-Wang; Zunger, Alex Physical Review B, Vol. 51, Issue 24 https://doi.org/10.1103/physrevb.51.17398	journal	June 1995
Measurement and assignment of the size-dependent optical spectrum in CdSe quantum dots Norris, D. J.; Bawendi, M. G. Physical Review B, Vol. 53, Issue 24 https://doi.org/10.1103/physrevb.53.16338	journal	June 1996
Size dependence of exciton fine structure in CdSe quantum dots Norris, D. J.; Efros, Al. L.; Rosen, M. Physical Review B, Vol. 53, Issue 24 https://doi.org/10.1103/physrevb.53.16347	journal	June 1996
Band-edge exciton in quantum dots of semiconductors with a degenerate valence band: Dark and bright exciton states Efros, Al. L.; Rosen, M.; Kuno, M. Physical Review B, Vol. 54, Issue 7 https://doi.org/10.1103/physrevb.54.4843	journal	August 1996
Electron and hole relaxation pathways in semiconductor quantum dots Klimov, V. I.; McBranch, D. W.; Leatherdale, C. A. Physical Review B, Vol. 60, Issue 19 https://doi.org/10.1103/physrevb.60.13740	journal	November 1999
Many-body pseudopotential theory of excitons in InP and CdSe quantum dots Franceschetti, A.; Fu, H.; Wang, L. W. Physical Review B, Vol. 60, Issue 3 https://doi.org/10.1103/physrevb.60.1819	journal	July 1999
Ultrafast dynamics of inter- and intraband transitions in semiconductor nanocrystals: Implications for quantum-dot lasers Klimov, V. I.; Schwarz, Ch. J.; McBranch, D. W. Physical Review B, Vol. 60, Issue 4 https://doi.org/10.1103/physrevb.60.r2177	journal	July 1999
Mechanisms for intraband energy relaxation in semiconductor quantum dots: The role of electron-hole interactions Klimov, V. I.; Mikhailovsky, A. A.; McBranch, D. W. Physical Review B, Vol. 61, Issue 20 https://doi.org/10.1103/physrevb.61.r13349	journal	May 2000
Electron-hole excitations and optical spectra from first principles Rohlfing, Michael; Louie, Steven G. Physical Review B, Vol. 62, Issue 8 https://doi.org/10.1103/physrevb.62.4927	journal	August 2000
Hole intraband relaxation in strongly confined quantum dots: Revisiting the “phonon bottleneck” problem Xu, S.; Mikhailovsky, A. A.; Hollingsworth, J. A. Physical Review B, Vol. 65, Issue 4 https://doi.org/10.1103/physrevb.65.045319	journal	January 2002
Optical transitions and nature of Stokes shift in spherical CdS quantum dots Demchenko, D. O.; Wang, Lin-Wang Physical Review B, Vol. 73, Issue 15 https://doi.org/10.1103/physrevb.73.155326	journal	April 2006
Stillinger-Weber potential for the II-VI elements Zn-Cd-Hg-S-Se-Te Zhou, X. W.; Ward, D. K.; Martin, J. E. Physical Review B, Vol. 88, Issue 8 https://doi.org/10.1103/physrevb.88.085309	journal	August 2013
Long-Range Electronic-to-Vibrational Energy Transfer from Nanocrystals to Their Surrounding Matrix Environment Aharoni, Assaf; Oron, Dan; Banin, Uri Physical Review Letters, Vol. 100, Issue 5 https://doi.org/10.1103/physrevlett.100.057404	journal	February 2008
Observation of the "Dark Exciton" in CdSe Quantum Dots Nirmal, M.; Norris, D. J.; Kuno, M. Physical Review Letters, Vol. 75, Issue 20 https://doi.org/10.1103/physrevlett.75.3728	journal	November 1995
Direct Pseudopotential Calculation of Exciton Coulomb and Exchange Energies in Semiconductor Quantum Dots Franceschetti, Alberto; Zunger, Alex Physical Review Letters, Vol. 78, Issue 5 https://doi.org/10.1103/physrevlett.78.915	journal	February 1997
Femtosecond 1 P -to- 1 S Electron Relaxation in Strongly Confined Semiconductor Nanocrystals Klimov, Victor I.; McBranch, Duncan W. Physical Review Letters, Vol. 80, Issue 18 https://doi.org/10.1103/physrevlett.80.4028	journal	May 1998
Pseudopotential Theory of Auger Processes in CdSe Quantum Dots Wang, Lin-Wang; Califano, Marco; Zunger, Alex Physical Review Letters, Vol. 91, Issue 5 https://doi.org/10.1103/physrevlett.91.056404	journal	July 2003
Breaking the Phonon Bottleneck in Semiconductor Nanocrystals via Multiphonon Emission Induced by Intrinsic Nonadiabatic Interactions Schaller, Richard D.; Pietryga, Jeffrey M.; Goupalov, Serguei V. Physical Review Letters, Vol. 95, Issue 19 https://doi.org/10.1103/physrevlett.95.196401	journal	October 2005
Direct Observation of Electron-to-Hole Energy Transfer in CdSe Quantum Dots Hendry, E.; Koeberg, M.; Wang, F. Physical Review Letters, Vol. 96, Issue 5 https://doi.org/10.1103/physrevlett.96.057408	journal	February 2006
Breaking the Phonon Bottleneck for Holes in Semiconductor Quantum Dots Cooney, Ryan R.; Sewall, Samuel L.; Anderson, Kevin E. H. Physical Review Letters, Vol. 98, Issue 17 https://doi.org/10.1103/physrevlett.98.177403	journal	April 2007
Polaronic quantum confinement in bulk CsPbBr3 perovskite crystals revealed by state-resolved pump/probe spectroscopy Sonnichsen, Colin D.; Strandell, Dallas P.; Brosseau, Patrick J. Physical Review Research, Vol. 3, Issue 2 https://doi.org/10.1103/physrevresearch.3.023147	journal	May 2021
Relations between absorption, emission, and excited state chemical potentials from nanocrystal 2D spectra Ryu, Jisu; Park, Samuel D.; Baranov, Dmitry Science Advances, Vol. 7, Issue 22 https://doi.org/10.1126/sciadv.abf4741	journal	May 2021
CHEMISTRY: Multidimensional Snapshots of Chemical Dynamics Stolow, A. Science, Vol. 305, Issue 5690 https://doi.org/10.1126/science.1103195	journal	September 2004
Slow Electron Cooling in Colloidal Quantum Dots Pandey, A.; Guyot-Sionnest, P. Science, Vol. 322, Issue 5903 https://doi.org/10.1126/science.1159832	journal	November 2008
The Electronic Structure of Semiconductor Nanocrystals Efros, Al. L.; Rosen, M. Annual Review of Materials Science, Vol. 30, Issue 1 https://doi.org/10.1146/annurev.matsci.30.1.475	journal	August 2000
The Quantum Mechanics of Larger Semiconductor Clusters ("Quantum Dots") Bawendi, M. G.; Steigerwald, M. L.; Brus, L. E. Annual Review of Physical Chemistry, Vol. 41, Issue 1 https://doi.org/10.1146/annurev.pc.41.100190.002401	journal	October 1990
S PECTROSCOPY AND H OT E LECTRON R ELAXATION D YNAMICS IN S EMICONDUCTOR Q UANTUM W ELLS AND Q UANTUM D OTS Nozik, Arthur J. Annual Review of Physical Chemistry, Vol. 52, Issue 1 https://doi.org/10.1146/annurev.physchem.52.1.193	journal	October 2001
T WO -D IMENSIONAL F EMTOSECOND S PECTROSCOPY Jonas, David M. Annual Review of Physical Chemistry, Vol. 54, Issue 1 https://doi.org/10.1146/annurev.physchem.54.011002.103907	journal	October 2003
Spectral and Dynamical Properties of Multiexcitons in Semiconductor Nanocrystals Klimov, Victor I. Annual Review of Physical Chemistry, Vol. 58, Issue 1 https://doi.org/10.1146/annurev.physchem.58.032806.104537	journal	May 2007
OPA-driven hollow-core fiber as a tunable, broadband source for coherent multidimensional spectroscopy Sonnichsen, Colin; Brosseau, Patrick; Reid, Cameron Optics Express, Vol. 29, Issue 18 https://doi.org/10.1364/oe.431988	journal	August 2021
Simple fiber-based solution for coherent multidimensional spectroscopy in the visible regime Seiler, Hélène; Palato, Samuel; Schmidt, Bruno E. Optics Letters, Vol. 42, Issue 3 https://doi.org/10.1364/ol.42.000643	journal	January 2017

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