期刊
ACS ENERGY LETTERS
卷 2, 期 12, 页码 2647-2652出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.7b00862
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资金
- EPSRC [EP/L000202, EP/L01551X/1, EP/K016288/1]
- ERC [277757]
- EPSRC [EP/K016288/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/K016288/1] Funding Source: researchfish
Halide perovskites show unusual thermalization kinetics for above-bandgap photoexcitation. We explain this as a consequence of excess energy being deposited into discrete large polaron states. The crossover between low-fluence and high-fluence phonon bottleneck cooling is due to a Mott transition where the polarons overlap (n >= 10(18) cm(-3)) and the phonon subpopulations are shared. We calculate the initial rate of cooling (thermalization) from the scattering time in the Frohlich polaron model to be 78 meV ps(-1) for CH3NH3PbI3. This rapid initial thermalization involves heat transfer into optical phonon modes coupled by a polar dielectric interaction. Further cooling to equilibrium over hundreds of picoseconds is limited by the ultralow thermal conductivity of the perovskite lattice.
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