Revealing giant internal magnetic fields due to spin fluctuations in magnetically doped colloidal nanocrystals

Rice, William D.; Liu, Wenyong; Baker, Thomas A.; Sinitsyn, Nikolai A.; Klimov, Victor Ivanovich; Crooker, Scott A.

doi:10.1038/nnano.2015.258

Title: Revealing giant internal magnetic fields due to spin fluctuations in magnetically doped colloidal nanocrystals

Journal Article · Mon Nov 23 00:00:00 EST 2015 · Nature Nanotechnology

DOI:https://doi.org/10.1038/nnano.2015.258· OSTI ID:1335596

Rice, William D. ^[1]; Liu, Wenyong ^[2]; Baker, Thomas A. ^[2]; Sinitsyn, Nikolai A. ^[3]; Klimov, Victor Ivanovich ^[2]; Crooker, Scott A. ^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States). National High Magnetic Field Lab.
Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Chemistry Division
Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Theory Division

Strong quantum confinement in semiconductors can compress the wavefunctions of band electrons and holes to nanometre-scale volumes, significantly enhancing interactions between themselves and individual dopants. In magnetically doped semiconductors, where paramagnetic dopants (such as Mn²⁺, Co²⁺ and so on) couple to band carriers via strong sp–d spin exchange, giant magneto-optical effects can therefore be realized in confined geometries using few or even single impurity spins. Importantly, however, thermodynamic spin fluctuations become increasingly relevant in this few-spin limit. In nanoscale volumes, the statistical √N fluctuations of N spins are expected to generate giant effective magnetic fields B_eff, which should dramatically impact carrier spin dynamics, even in the absence of any applied field. In this paper, we directly and unambiguously reveal the large B_eff that exist in Mn²⁺-doped CdSe colloidal nanocrystals using ultrafast optical spectroscopy. At zero applied magnetic field, extremely rapid (300–600 GHz) spin precession of photoinjected electrons is observed, indicating B_eff ~ 15-30 T for electrons. Precession frequencies exceed 2 THz in applied magnetic fields. Finally, these signals arise from electron precession about the random fields due to statistically incomplete cancellation of the embedded Mn²⁺ moments, thereby revealing the initial coherent dynamics of magnetic polaron formation, and highlighting the importance of magnetization fluctuations on carrier spin dynamics in nanomaterials.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: AC52-06NA25396; DMR-1157490

OSTI ID:: 1335596

Report Number(s):: LA-UR-15-24701

Journal Information:: Nature Nanotechnology, Vol. 11, Issue 2; ISSN 1748-3387

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 44 works

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Hot-electron dynamics in quantum dots manipulated by spin-exchange Auger interactions Singh, Rohan; Liu, Wenyong; Lim, Jaehoon Nature Nanotechnology, Vol. 14, Issue 11 https://doi.org/10.1038/s41565-019-0548-1	journal	October 2019
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