Nanoscopic thermometry with 30 mk precision: a quantitative study of cathodoluminescence in lanthanide-doped nanomaterials
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1 Nanoscopic thermometry with 30 mk precision: a quantitative study of cathodoluminescence in lanthanide-doped nanomaterials Clarice D. Aiello Inorganic Nanostructures Molecular Foundry, 03/16/17
2 Measuring temperature of tiny objects requires tiny sensor contact-based thermometry not applicable biology applications: cellular events marked by few- C temperature changes industrial applications: temperature diagnostics for nano-electronics, materials... Aigouy et al., Appl. Phys. Lett. 87, (2005)
3 Measuring temperature of tiny objects requires tiny sensor State-of-the-art: map how light from photostable nanomaterials changes as a function of temperature nanomaterials doped with lanthanide ions: sharp emission, long lifetimes, stability up to 1000 C optical excitation: works even for single nanoparticles......but diffraction-limited (we don t see the nanothermometer!) Idea: study cathodoluminescence of nanomaterials: nanoscopic localization (we see the nanothermometer!) nanomaterial can form a film or barrier to protect sample from radiation damage
4 Overview of experimental conditions
5 Nanoscopic thermometry with 30 mk precision: a quantitative study of cathodoluminescence in lanthanide-doped nanomaterials Intensity ratio thermometry Lifetime thermometry
6 Nanoscopic thermometry with 30 mk precision: a quantitative study of cathodoluminescence in lanthanide-doped nanomaterials Intensity ratio thermometry Lifetime thermometry
7 Can use a static signal to do thermometry study steady-state light while e-beam on signal is derived from ratio of intensity in spectral bands spectral peaks are linked thru phonon pathway: expect temperature dependence
8 Under cathodoluminescence, spectral behavior with temperature is akin to that under photoluminescence a Cathodoluminescence emission spectrum (Hz), 1kX mag C 60 C 50 C 40 C 30 C 25 C Wavelength (nm) b Cathodoluminescence emission spectrum (a.u.), 1kX mag Cathodoluminescence emission spectrum (a.u.), 1kX mag Wavelength (nm) Wavelength (nm)
9 Can use a static signal to do thermometry study steady-state light while e-beam on signal is derived from ratio of intensity in spectral bands spectral peaks are linked thru phonon pathway: expect temperature dependence use empirical law Signal(t, T) = R(T) G(T) a T2 + b T + c low signal-to-noise levels (all counts Poisson!), ratio is susceptible to fluctuations unrelated to temperature...
10 Cathodoluminescence intensity ratio thermometry is on par with with optical... a 25 C 30 C 40 C 50 C 60 C 70 C 100 nm b c Intensity thermometry signal, norm. to 25 C (a.u.) S = 0.1 S T = 2 C Temperature at sample ( C) T (signal)/ T (% C 1 ) previously reported (fluorescence ratio of intensity) Temperature at sample ( C)
11 Cathodoluminescence intensity ratio thermometry is on par with with optical... plus the nanometric localization a 25 C 30 C 40 C 50 C 60 C 70 C 100 nm b c Intensity thermometry signal, norm. to 25 C (a.u.) S = 0.1 S T = 2 C Temperature at sample ( C) T (signal)/ T (% C 1 ) previously reported (fluorescence ratio of intensity) Temperature at sample ( C)
12 Drawbacks and advantages of these static signals to do thermometry measured signal dependence on pixel size (none), e-beam energy (?) and current ( exponential)... nanothermometer exposure to e-beam is prolonged dependent on light collection fluctuations, local concentration of nanothermometers... need to correlate observations of multiple spectral lines
13 Nanoscopic thermometry with 30 mk precision: a quantitative study of cathodoluminescence in lanthanide-doped nanomaterials Intensity ratio thermometry Lifetime thermometry
14 Can use a dynamic signal to do thermometry study transient light after fast blanking of e-beam extremely low signal-to-noise levels......but noise averaged over by using transient light intensity as probability distribution Signal(t, T) = τ(t, T) empirical model available τ(t, T) α(t) T + β(t) t 0 I(t, T)t dt t 0 I(t, T)dt enables study of nanothermometer sensitivity as a function of acquisition time
15 Cathodoluminescence lifetime thermometry is on par with with optical... a Green band τ (µs) time in 50 µs intervals Red band τ (µs) Temperature at sample ( C) Temperature at sample ( C) b 1 1 c Abs. of norm. slope ᾱ τ/ T /τ 25 C (% C 1 ) 0.5 previously reported (fluorescence lifetime) 0.1 Sensitivity δt στ/ τ/ T ( C) Transient cathodoluminescence acquisition time (µs) Transient cathodoluminescence acquisition time (µs) 0.01
16 Cathodoluminescence lifetime thermometry is on par with with optical... plus the nanometric localization a Green band τ (µs) time in 50 µs intervals Red band τ (µs) Temperature at sample ( C) Temperature at sample ( C) b 1 1 c Abs. of norm. slope ᾱ τ/ T /τ 25 C (% C 1 ) 0.5 previously reported (fluorescence lifetime) 0.1 Sensitivity δt στ/ τ/ T ( C) Transient cathodoluminescence acquisition time (µs) Transient cathodoluminescence acquisition time (µs) 0.01
17 Drawbacks and advantages of this dynamic signal to do thermometry measured signal dependence on pixel size (none), e-beam energy ( none) and current (strongly non-linear)... nanothermometer exposure to e-beam is minimized independent of light collection fluctuations, local concentration of nanothermometers... only needs to measure one spectral line
18 Nanoscopic thermometry with 30 mk precision: a quantitative study of cathodoluminescence in lanthanide-doped nanomaterials Clarice D. Aiello Inorganic Nanostructures Molecular Foundry, 03/16/17
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