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Wavelength-Dependent Spin Excitation with Circularly Polarized Light in CdSe Nanoplatelets
Abstract
Zinc-blende (ZB) cadmium selenide (CdSe) nanoplatelets (NPLs) have drawn increasing attention as an ideal condensed-phase material for facilitating photon-to-spin transduction in quantum networks. Yet, a systematic investigation of their fidelity in converting circularly polarized light (CPL) to exciton spin polarization as a function of excitation wavelength is lacking. Here, this work demonstrates using time-resolved transient absorption (TA) spectroscopy combined with density functional theory calculations that ZB CdSe NPLs exhibit wavelength-dependent CPL-induced spin polarization. The capacity of CPL to inject spin polarization is maximized for resonant excitation of band-edge valence-to-conduction band (VB/CB) transitions, and the degree to which CPL induces spin polarization can be modified for non-resonant excitation wavelengths as excitation occurs at k-points away from the Γ point from VB states with varying degrees of mixed heavy-hole (HH) and light-hole (LH) characters. Furthermore, it is highlighted that spin polarization within the LH exciton (LX) population created from resonant LH/CB excitation is retained upon LX → HH exciton (HX) relaxation due to the slow electron spin-flip rate (~1.1 ps) compared to the LH → HH inter-band relaxation rate (~200 fs).
- Authors:
-
[2];
[3];
[2]
- Northwestern University, Evanston, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Northwestern University, Evanston, IL (United States)
- Argonne National Laboratory (ANL), Argonne, IL (United States); University of Chicago, IL (United States); Northwestern University, Evanston, IL (United States)
- Publication Date:
- Research Org.:
- Northwestern Univ., Evanston, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 2001294
- Grant/Contract Number:
- SC0021314; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 127; Journal Issue: 29; Related Information: https://pubs.acs.org/doi/10.1021/acs.jpcc.3c02767.; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Cadmium selenide; Excitons; Polarization; Probes; Quantum mechanics
Citation Formats
Flor, Baxter, Zeman, Charles J., Ma, Xuedan, and Schatz, George C. Wavelength-Dependent Spin Excitation with Circularly Polarized Light in CdSe Nanoplatelets. United States: N. p., 2023.
Web. doi:10.1021/acs.jpcc.3c02767.
Flor, Baxter, Zeman, Charles J., Ma, Xuedan, & Schatz, George C. Wavelength-Dependent Spin Excitation with Circularly Polarized Light in CdSe Nanoplatelets. United States. https://doi.org/10.1021/acs.jpcc.3c02767
Flor, Baxter, Zeman, Charles J., Ma, Xuedan, and Schatz, George C. Wed .
"Wavelength-Dependent Spin Excitation with Circularly Polarized Light in CdSe Nanoplatelets". United States. https://doi.org/10.1021/acs.jpcc.3c02767.
@article{osti_2001294,
title = {Wavelength-Dependent Spin Excitation with Circularly Polarized Light in CdSe Nanoplatelets},
author = {Flor, Baxter and Zeman, Charles J. and Ma, Xuedan and Schatz, George C.},
abstractNote = {Zinc-blende (ZB) cadmium selenide (CdSe) nanoplatelets (NPLs) have drawn increasing attention as an ideal condensed-phase material for facilitating photon-to-spin transduction in quantum networks. Yet, a systematic investigation of their fidelity in converting circularly polarized light (CPL) to exciton spin polarization as a function of excitation wavelength is lacking. Here, this work demonstrates using time-resolved transient absorption (TA) spectroscopy combined with density functional theory calculations that ZB CdSe NPLs exhibit wavelength-dependent CPL-induced spin polarization. The capacity of CPL to inject spin polarization is maximized for resonant excitation of band-edge valence-to-conduction band (VB/CB) transitions, and the degree to which CPL induces spin polarization can be modified for non-resonant excitation wavelengths as excitation occurs at k-points away from the Γ point from VB states with varying degrees of mixed heavy-hole (HH) and light-hole (LH) characters. Furthermore, it is highlighted that spin polarization within the LH exciton (LX) population created from resonant LH/CB excitation is retained upon LX → HH exciton (HX) relaxation due to the slow electron spin-flip rate (~1.1 ps) compared to the LH → HH inter-band relaxation rate (~200 fs).},
doi = {10.1021/acs.jpcc.3c02767},
journal = {Journal of Physical Chemistry. C},
number = 29,
volume = 127,
place = {United States},
year = {Wed Jul 12 00:00:00 EDT 2023},
month = {Wed Jul 12 00:00:00 EDT 2023}
}
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Works referenced in this record:
The spin structure of quasi–two-dimensional biexcitons in quantum wells
journal, September 2002
- de-Leon, S. Ben-Tabou; Laikhtman, B.
- Europhysics Letters (EPL), Vol. 59, Issue 5
Room-temperature exciton coherence and dephasing in two-dimensional nanostructures
journal, January 2015
- Cassette, Elsa; Pensack, Ryan D.; Mahler, Benoît
- Nature Communications, Vol. 6, Issue 1
Circularly Polarized Optical Stark Effect in CdSe Colloidal Quantum Wells
journal, October 2020
- Diroll, Benjamin T.
- Nano Letters, Vol. 20, Issue 11
Directed Two-Photon Absorption in CdSe Nanoplatelets Revealed by k -Space Spectroscopy
journal, September 2017
- Heckmann, Jan; Scott, Riccardo; Prudnikau, Anatol V.
- Nano Letters, Vol. 17, Issue 10
Coherent manipulation of single spins in semiconductors
journal, June 2008
- Hanson, Ronald; Awschalom, David D.
- Nature, Vol. 453, Issue 7198
Optical properties and applications of two‐dimensional CdSe nanoplatelets
journal, April 2020
- Yu, Jiahao; Chen, Rui
- InfoMat, Vol. 2, Issue 5
Excitons and fundamental absorption in quantum wells
journal, May 1995
- Winkler, R.
- Physical Review B, Vol. 51, Issue 20
Tuning Spin-Polarized Lifetime in Two-Dimensional Metal–Halide Perovskite through Exciton Binding Energy
journal, November 2021
- Chen, Xihan; Lu, Haipeng; Wang, Kang
- Journal of the American Chemical Society, Vol. 143, Issue 46
Dependence of the light-hole—heavy-hole splitting on layer thickness and substrate orientation in GaAs-(GaAl) As single quantum wells
journal, June 1989
- El Khalifi, Y.; Gil, B.; Mathieu, H.
- Physical Review B, Vol. 39, Issue 18
Hybrid functionals based on a screened Coulomb potential
journal, May 2003
- Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias
- The Journal of Chemical Physics, Vol. 118, Issue 18
Surface spin magnetism controls the polarized exciton emission from CdSe nanoplatelets
journal, January 2020
- Shornikova, Elena V.; Golovatenko, Aleksandr A.; Yakovlev, Dmitri R.
- Nature Nanotechnology, Vol. 15, Issue 4
Colloidal CdSe/CdS Dot-in-Plate Nanocrystals with 2D-Polarized Emission
journal, July 2012
- Cassette, Elsa; Mahler, Benoît; Guigner, Jean-Michel
- ACS Nano, Vol. 6, Issue 8
Distinct Excitonic Circular Dichroism between Wurtzite and Zincblende CdSe Nanoplatelets
journal, October 2018
- Gao, Xiaoqing; Zhang, Xiuwen; Zhao, Luyang
- Nano Letters, Vol. 18, Issue 11
Spin relaxation in intrinsic GaAs quantum wells: Influence of excitonic localization
journal, February 1995
- Muñoz, L.; Pérez, E.; Viña, L.
- Physical Review B, Vol. 51, Issue 7
Size-Dependent Biexciton Quantum Yields and Carrier Dynamics of Quasi-Two-Dimensional Core/Shell Nanoplatelets
journal, September 2017
- Ma, Xuedan; Diroll, Benjamin T.; Cho, Wooje
- ACS Nano, Vol. 11, Issue 9
Manipulation of the Optical Properties of Colloidal 2D CdSe Nanoplatelets
journal, June 2021
- Zhang, Zitong; Sun, Handong
- Advanced Photonics Research, Vol. 2, Issue 8
Spin dynamics of exciton states in GaAS/AlGaAs multiple quantum wells
journal, April 1993
- Dareys, B.; Marie, X.; Amand, T.
- Superlattices and Microstructures, Vol. 13, Issue 3
Colloidal CdSe Nanoplatelets, A Model for Surface Chemistry/Optoelectronic Property Relations in Semiconductor Nanocrystals
journal, September 2018
- Singh, Shalini; Tomar, Renu; ten Brinck, Stephanie
- Journal of the American Chemical Society, Vol. 140, Issue 41
Exploiting chemistry and molecular systems for quantum information science
journal, July 2020
- Wasielewski, Michael R.; Forbes, Malcolm D. E.; Frank, Natia L.
- Nature Reviews Chemistry, Vol. 4, Issue 9
Spin-polarized exciton quantum beating in hybrid organic–inorganic perovskites
journal, May 2017
- Odenthal, Patrick; Talmadge, William; Gundlach, Nathan
- Nature Physics, Vol. 13, Issue 9
Colloidal nanoplatelets with two-dimensional electronic structure
journal, October 2011
- Ithurria, S.; Tessier, M. D.; Mahler, B.
- Nature Materials, Vol. 10, Issue 12
Experimental Determination of the Absorption Cross-Section and Molar Extinction Coefficient of Colloidal CdSe Nanoplatelets
journal, November 2015
- Yeltik, Aydan; Delikanli, Savas; Olutas, Murat
- The Journal of Physical Chemistry C, Vol. 119, Issue 47
Directed emission of CdSe nanoplatelets originating from strongly anisotropic 2D electronic structure
journal, September 2017
- Scott, Riccardo; Heckmann, Jan; Prudnikau, Anatol V.
- Nature Nanotechnology, Vol. 12, Issue 12
Electron and Hole Spin Relaxation in CdSe Colloidal Nanoplatelets
journal, December 2020
- Xiang, Dongmei; Li, Yulu; Wang, Lifeng
- The Journal of Physical Chemistry Letters, Vol. 12, Issue 1
Enhanced emission directivity from asymmetrically strained colloidal quantum dots
journal, February 2022
- Song, Yang; Liu, Ruixiang; Wang, Zhibo
- Science Advances, Vol. 8, Issue 8
Chloride-Induced Thickness Control in CdSe Nanoplatelets
journal, September 2018
- Christodoulou, Sotirios; Climente, Juan I.; Planelles, Josep
- Nano Letters, Vol. 18, Issue 10
Optical orientation of electron spins in GaAs quantum wells
journal, April 2005
- Pfalz, S.; Winkler, R.; Nowitzki, T.
- Physical Review B, Vol. 71, Issue 16
Optical investigation of the heavy hole-light hole splitting in thin GaAs/GaAlAs quantum wells
journal, February 1988
- Laruelle, F.; Etienne, B.
- Solid State Communications, Vol. 65, Issue 7
Origin of Low Temperature Trion Emission in CdSe Nanoplatelets
journal, November 2021
- Vong, Albert F.; Irgen-Gioro, Shawn; Wu, Yue
- Nano Letters, Vol. 21, Issue 23
Molecular qubits based on photogenerated spin-correlated radical pairs for quantum sensing
journal, June 2022
- Mani, Tomoyasu
- Chemical Physics Reviews, Vol. 3, Issue 2
Thermodynamic Equilibrium between Excitons and Excitonic Molecules Dictates Optical Gain in Colloidal CdSe Quantum Wells
journal, June 2019
- Geiregat, Pieter; Tomar, Renu; Chen, Kai
- The Journal of Physical Chemistry Letters, Vol. 10, Issue 13
Excitonic Spin-Coherence Lifetimes in CdSe Nanoplatelets Increase Significantly with Core/Shell Morphology
journal, February 2023
- Martin, Phillip I.; Panuganti, Shobhana; Portner, Joshua C.
- Nano Letters, Vol. 23, Issue 4
Charge Carrier Resolved Relaxation of the First Excitonic State in CdSe Quantum Dots Probed with Near-Infrared Transient Absorption Spectroscopy †
journal, November 2010
- McArthur, Eric A.; Morris-Cohen, Adam J.; Knowles, Kathryn E.
- The Journal of Physical Chemistry B, Vol. 114, Issue 45
Electronic structure and absorption spectrum of biexciton obtained by using exciton basis
journal, September 2013
- Shiau, Shiue-Yuan; Combescot, Monique; Chang, Yia-Chung
- Annals of Physics, Vol. 336