Visualizing Chemical Dynamics in an Ionic Liquid Microdroplet using Ultrafast 2D IR Microscopy

Abstract

The manuscript posted describes the first use of 2D IR microscopy to spatially resolve chemical dynamics in a complex chemical environment. Full details of the 2D IR microscopy experiments, sample preparation, data analysis, and modeling are provided. The results reveal how chemical dynamics evolve across a room temperature ionic liquid microdroplet. In addition, this work demonstrates the power of 2D IR microscopy to quantitative information hidden by other chemical imaging approaches.

Ultrafast Coherence Delocalization in Real Space Simulated by Polaritons

“…We next imaged the spatial coherent transport by an ultrafast hyperspectral IR imaging setup. [ 41–43 ] This instrument was done by adding a pump pulse to enable a 2D IR pulse sequence (Figure 1a) in the hyperspectral IR microscopy (Figure 1d). This setup allowed up to five‐dimension imaging (3D in frequency and 2D in space).…”

“…[ 19,40 ] The 2D IR spectra show a unidirectional coherence delocalization, imaged by a home‐built hyperspectral microscope. [ 41–43 ] Spatial dynamics show the coherence delocalize from high to low‐frequency cavities, but the reverse is unfavored, driven by non‐Hermitian Lindbladian dynamics of photon delocalization and dissipation. To further understand the coherence spatial transport, we attempt to generate coherence directly between two neighboring cavities, referred as inter‐cavity coherence.…”

Transient 2D IR spectroscopy from micro- to milliseconds

“…However, the number of publications, which report on 2D IR instruments based on such Yb laser/amplifiers, is still rather limited. [12][13][14][15][16][17][18][19][20] The motivation of these works is either higher sensitivity, 16,19 or collecting very many 2D IR spectra, e.g., in the context of 2D-IR microscopy 17 or high-throughput applications. 15,18 Here, another application of the high repetition rates of these lasers is introduced, transient 2D IR spectroscopy.…”

Application of 2D IR Bioimaging: Hyperspectral Images of Formalin-Fixed Pancreatic Tissues and Observation of Slow Protein Degradation

“…2D IR spectroscopy provides information about protein environments through 2D line shapes, utilizes vibrational lifetimes to discriminate against solvent exposed and disordered proteins, and enhances resolution through off-diagonal cross peaks. 44,49,50 2D IR microscopy can be implemented in a number of ways, including point-mapping 37,39,51 approaches, 38 but either way, 2D IR microscopy is a collection of 2D IR spectra that form a hyperspectral image. 2D IR microscopy is a new technique that has mostly been applied to model systems.…”

“…Raman or IR images can be generated at a single well-defined frequency or hyperspectral data sets generated by measuring multiple frequencies or in a Fourier transform mode. ,,− A more recent hyperspectral vibrational imaging technique is two-dimensional (2D) IR microscopy, which is based on ultrafast 2D IR spectroscopy. − 2D IR spectroscopy uses a series of femtosecond pulses to generate multidimensional IR spectra that correlate vibrational modes through the physics of their vibrational couplings. − 2D IR spectroscopy is different than the analytical 2D correlation spectroscopy, − which is a means of analyzing data sets. 2D IR spectroscopy provides information about protein environments through 2D line shapes, utilizes vibrational lifetimes to discriminate against solvent exposed and disordered proteins, and enhances resolution through off-diagonal cross peaks. ,, 2D IR microscopy can be implemented in a number of ways, including point-mapping ,, and widefield approaches, but either way, 2D IR microscopy is a collection of 2D IR spectra that form a hyperspectral image. 2D IR microscopy is a new technique that has mostly been applied to model systems. ,,, The only biological systems studied so far are mouse, porcine, and human lens tissues and mouse kidney sections (stained with an IR active probe). ,, …”