Journal
PHYSICAL REVIEW LETTERS
Volume 111, Issue 10, Pages -Publisher
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.111.107401
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Funding
- Center for Nanoscale Materials, a U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences User Facility [DE-AC02-06CH11357]
- NSF [DGE-0824162]
- Office of Basic Energy Sciences [DE-SC0004752]
- Camille and Henry Dreyfus Foundation Postdoctoral Program in Environmental Chemistry
- ANSER Center, an Energy Frontier Research Center
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-SC0001059]
- U.S. Department of Energy (DOE) [DE-SC0004752] Funding Source: U.S. Department of Energy (DOE)
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We report femtosecond stimulated Raman spectroscopy measurements of lattice dynamics in semiconductor nanocrystals and characterize longitudinal optical (LO) phonon production during confinement-enhanced, ultrafast intraband relaxation. Stimulated Raman signals from unexcited CdSe nanocrystals produce a spectral shape similar to spontaneous Raman signals. Upon photoexcitation, stimulated Raman amplitude decreases owing to experimentally resolved ultrafast phonon generation rates within the lattice. We find a similar to 600 fs, particle-size-independent depletion time attributed to hole cooling, evidence of LO-to-acoustic down-conversion, and LO phonon mode softening.
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