Large two-photon cross sections and low-threshold multiphoton lasing of CdS/CdSe/CdS quantum shells

Diroll, Benjamin T.; Cassidy, James P.; Harankahage, Dulanjan; Hua, Muchuan; Lin, Xiao-Min; Zamkov, Mikhail

doi:10.1039/d3nr04203k

Large two-photon cross sections and low-threshold multiphoton lasing of CdS/CdSe/CdS quantum shells

Journal Article · Tue Nov 07 19:00:00 EST 2023 · Nanoscale

DOI:https://doi.org/10.1039/d3nr04203k· OSTI ID:2569775

^[1]; Cassidy, James P. ^[2]; Harankahage, Dulanjan ^[2]; ^[1]; ^[1]; ^[2]

Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
Bowling Green State Univ., OH (United States)

Colloidal quantum shells are spherical semiconductor quantum wells, which have shown strong promise as optical materials, particularly in classes of experiments requiring multiple excitons. The two-photon properties of CdS/CdSe/CdS quantum shell samples are studied here to demonstrate large non-linear absorption cross-sections while retaining advantageous multiexciton physics conferred by the geometrical structure. The quantum shells have large two-phonon cross sections (0.4–7.9 × 10⁶ GM), which highlights their potential use in upconversion imaging in which large per particle two-photon absorption is critical. Time-resolved measurements confirmed that the quantum shells have long biexciton lifetime (>10 ns in the largest core samples reported here) and large gain bandwidth (>300 meV). The combination of these attributes with large two-photon cross sections makes the CdS/CdSe/CdS quantum shells excellent gain media for two-photon excitation. With a broad gain bandwidth and long gain lifetime, quantum shell solids support multimodal amplified spontaneous emission from excitons, biexcitons, and higher excited states. In conclusion, thresholds for amplified spontaneous emission and lasing, which are as low as 1 mJ cm⁻², are comparable to, or lower than, the thresholds reported for other colloidal materials.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Science Foundation (NSF)

Grant/Contract Number:: SC0016872; AC02-06CH11357

OSTI ID:: 2569775

Alternate ID(s):: OSTI ID: 2205242

Journal Information:: Nanoscale, Journal Name: Nanoscale Journal Issue: 45 Vol. 15; ISSN 2040-3364; ISSN 2040-3372

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Quantum shell
amplified spontaneous emission
laser
optical gain
two photon absorption

Large two-photon cross sections and low-threshold multiphoton lasing of CdS/CdSe/CdS quantum shells

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