To obtain a mechanistic understanding of the chemical processes, techniques that offer a frame-by-frame visualization of molecular structure during a reaction are of vital importance. Numerous efforts and advances have been made in order to acquire such vivid molecular “movies”, especially in the electronic excited state. Ultrafast molecular spectroscopy method...
We demonstrate the generation of broadband up-converted multicolor array (BUMA) in a thin BK7 glass slide using two noncollinear weak near-IR laser pulses with various crossing angles. The BUMA signal arises from cubic nonlinear χ⁽³⁾:χ⁽³⁾ processes via cascaded four-wave mixing of the two incident beams. Broad and continuous tunability of...
We demonstrate a versatile and efficient setup to perform femtosecond stimulated Raman spectroscopy (FSRS). Technical innovations are implemented to achieve the wavelength tunability for both the picosecond narrowband Raman pump pulse and femtosecond broadband Raman probe pulse. Using a simplified one-grating scheme in a home-built second harmonic bandwidth compressor followed...
We demonstrate the simultaneous generation of multicolor femtosecond laser pulses spanning the wavelength range from UV to near IR in a 0.1 mm Type I beta-barium borate crystal from 800 nm fundamental and weak IR super-continuum white light (SCWL) pulses. The multicolor broadband laser pulses observed are attributed to two...
Intracellular pH (pH(i)) imaging is of paramount importance for life sciences. In this work, we implement the ultrafast electronic and stimulated Raman spectroscopies to unravel the fluorescence mechanism of an excitation-ratiometric pH(i) indicator in basic aqueous solution. After photoexcitation of the pH(i) indicator HPTS, a hidden charge-transfer (CT) state following...
We demonstrate the versatile broadband wavelength tunability of frequency upconverted multicolor cascaded fourwave-mixing (CFWM) signals spanning the continuous wavelength range from UV to near IR in a thin type-I BBO crystal using 35 fs, 800 nm fundamental and chirped IR supercontinuum white light pulses. Two sets of spatially dispersed CFWM...
Femtosecond stimulated Raman spectroscopy (FSRS) is an emerging molecular structural dynamics technique for functional materials characterization typically in the visible to near-IR range. To expand its applications we have developed a versatile FSRS setup in the ultraviolet region. We use the combination of a narrowband, ~400 nm Raman pump from...
Biosensors have become an indispensable tool set in life sciences. Among them, fluorescent protein-based biosensors have great biocompatibility and tunable emission properties but their development is largely on trial and error. To facilitate a rational design, we implement tunable femtosecond stimulated Raman spectroscopy, aided by transient absorption and quantum calculations,...
Tracking vibrational motions during a photochemical or photophysical process has gained momentum, due to its sensitivity to the progression of reaction and change of environment. In this work, we implemented an advanced ultrafast vibrational technique, femtosecond-stimulated Raman spectroscopy (FSRS), to monitor the excited state structural evolution of an engineered green...
We strategically modified the GFP core via chemical synthesis to make redder and brighter biomimetic fluorophores. Based on quantum calculations, solvatochromism analysis, and femtosecond Raman, we unveiled the additive effect of tuning the electronic ground and excited states, respectively, to achieve a dramatic emission redshift with a "double-donor-one-acceptor" structure.