Shamrock 303i

TRLFS measurements were performed
at 298 K using a Nd/YAG (Surelite II laser, Continuum) pumped dye
laser system (NarrowScan D-R; Radiant Dyes Laser Accessories GmbH).
The wavelengths of 396.6 nm and 394 nm were used to excite Cm(III)
and Eu(III) ions, respectively. A spectrograph (Shamrock 303i, ANDOR)
with 300, 1199, and 2400 lines per mm gratings was used for spectral
decomposition. The fluorescence emission was detected using an ICCD
camera (iStar Gen III, ANDOR) after a delay time of 1 μs to
discriminate short-lived organic fluorescence and light scattering.

The device was characterized using an inverted optical microscope (Nikon, Eclipse Ti-E) equipped with an EMCCD (Andor, iXon Ultra 897) and a spectrometer (Andor, Shamrock 303i). The device emissions were collected from the backside of the substrates with an oil-immersed objective (Nikon, 100×, NA 1.49), when the devices were biased using a source meter (Keithley 6430). Fourier-plane images were captured by projecting the back focal plane of the objective on the EMCCD using a Bertrand lens. Spectral data are corrected for the detection efficiency of the optical system (see Supplementary Fig. S4).

The generated laser was first collimated by an f = 30 cm lens and then passed through a dichroic mirror (DM3) to filter out the residual pump pulses. To minimize the measurement error caused by a possible spatial anisotropy of the laser and a polarization dependent response of the spectrometer, we used an integral sphere (IS) to collect the signals and directed them into a grating spectrometer (Andor, Shamrock 303i). Another Glan-Taylor prism (GT2) was placed before the IS to measure the polarization of the laser pulses.
Throughout the experiment, we fixed the polarization direction of the pump pulses. We tuned the polarization direction of the seed pulses by rotating the HWP, and measured the intensity of the laser as a function of the angle of GT2. The zero degree of the angle of GT2 corresponds to that the optical axis of GT2 is parallel to the polarization direction of the pump pulses.

A microscope was built by mounting the following items onto a 2′′ post (Thorlabs Inc., Newton, MA, USA);

a quarz halogen lamp (MI-150, Edmund Optics, Barrington, IL, USA),

a manual xy-stage (Merzhäuser, Wezlar, Germany),

a microscope objective holder equipped with a 60× water immersion objective (Olympus, Tokyo, Japan),

a CCD camera to observe the sample (Guppy, Allied Vision GmbH, Stadtroda Germany),

two edge filters (532 razor sharp edge and 532 basic edge filters, Semrock, Rochester, NY, USA), both used to guide the laser light onto the sample and to block out the laser light prior to the Raman spectrometer,

an optical fiber to guide the Raman scattered light into a Raman spectrometer (Shamrock 303i, Andor Technology, Belfast, UK) equipped with an air-cooled CCD camera (Andor Technology, Belfast, UK).

The final setup is shown in Figure 3.
Raman measurements were carried out with a Shamrock 303i spectrometer and an excitation wavelength of 532 nm (DPSS 532 laser) at an integration time of 120 s at a power of 0.6 mW. The slit into the spectrometer was set to 50 μm giving a spectral resolution of 6 cm⁻¹. The laser beam was, in this study, intentionally defocused to 20 μm to average the signal from a large intracellular region from the single PASMC.

The samples’ morphologies were examined using a transmission electron microscope (FEI TecnaiG2F30; 200 kV). Thermo Fisher Scientific’s ESCALAB 250Xi photoelectron spectrometer was used to perform X-ray photoelectron spectroscopy with Mo as the excitation source. A JASCO V-770 spectrophotometer was used to acquire UV-vis absorption spectra. Ocean Optics QE Pro spectrofluorometer was used to measure the PL spectra. An Edinburgh FS5 spectrophotometer was used to measure the PL lifetime and PLQY. The fundamental-frequency 800 nm femtosecond laser pulse was generated by the Coherent Legend regenerative amplifier (100 fs, 1 kHz) which is seeded by a Coherent Vitesse oscillator (100 fs, 80 MHz). An automated optical parametric amplifier (Light Conversion, TOPAS Prime) pumped by the fundamental-frequency 800 nm femtosecond laser pulse was used to obtain the 1150 and 1500 nm femtosecond lasers employed in multiphoton FL. The two-photon and three-photon FL signals were collected by a spectrometer (ANDOR, Shamrock 303i) coupled with CCD (ANDOR, Newton DU920P). An Ultrafast System HELIOS spectrometer in a nondegenerate pump-probe configuration was used to measure TA. The 400 nm pump laser was obtained by propagating the 800 nm fundamental-frequency femtosecond laser pulse through a 0.5 mm thick BBO single crystal.