Elucidating
structure–function relationships that determine
the photophysics of nanomaterials that upconvert high-power, near-infrared
(NIR) excitation to shorter wavelength NIR, visible, and UV emission
requires both compositional characterization and experimental designs
that rigorously define laser excitation conditions and the manner
in which emitted photons are collected. Presented herein are laser
power-dependent, total-emitted radiant flux (watts), and absolute
quantum yield measurements of homogeneous, solution-phase 28 nm [NaYF4; Yb (15%), Er (2%)] upconversion nanocrystals (UCNCs) determined
using a multidetector integrating sphere spectroscopy system. These
studies compare for the first time quantitative total radiant flux
and absolute quantum yield measurements of UCNCs determined as a function
of laser power density for both 970 nm continuous-wave (CW) and 976
nm pulsed Ti-sapphire (140 fs pulse width, 80 MHz) laser excitation.
This study illustrates that at intensities in the range 35–225
W/cm2, the total radiant flux is higher under CW excitation
by an average factor of 1.5, and for this range of laser powers the
high peak intensities associated with femtosecond-pulsed excitation
conditions do not drive further augmentation of the radiant flux magnitude.
This study has important ramifications for the field as it establishes
the total radiant flux as the most appropriate figure of merit relevant
for quantifying the emissive output intensity of UCNCs. In contrast
to an UCNC emission quantum yield measurement, the total radiant flux
may be determined with a high degree of accuracy; this point is critical,
as this parameter is more closely connected to UCNC performance metrics
important for imaging, emission fingerprinting, tracking, and energy
conversion applications.
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