Powder X-ray Diffraction (PXRD): Patterns for the bulk powders were collected with a Panalytical Empyrean Diffractometer system equipped with a PIXcel3D detector using CuKα radiation using samples loaded in glass capillaries (Charles Supper, Inc.) and sealed with vacuum grease. See Figures . Single Crystal X-Ray Crystallography (SCXRD): Suitable crystals were mounted on a thin glass fiber using perfluoropolyether oil, which was frozen in situ by a nitrogen gas cryostream flow. Data collection was performed on a Rigaku Super Nova diffractometer equipped with an AtlasS2 CCD, and Oxford 700 low-temperature attachment, using CuKα (λ = 1.54184). Using Olex2, structures were solved with the SHELX structure solution program using Direct Methods and refined with the SHELXL refinement package using least squares minimization. See additional details in ESI, Figures S1-S9 and ESI Section 3. Fourier Transform Infrared (FTIR): Spectra were obtained with an Agilent Cary-630 spectrometer, with an attenuated total reflectance module containing a diamond crystal. See additional info in ESI, Figures . Elemental Microanalyses: Elemental microanalyses were performed by Galbraith Laboratories, Inc. (Knoxville, TN). Photoluminescence (PL) Spectroscopy: Photoluminescence spectra were collected using an Edinburgh Instruments FLS1000 fluorimeter equipped with a 450 W Xenon arc lamp for steady-state measurements and a 375 nm picosecond pulsed light emitting diode for time-resolved measurements. Single-grating Czerny-Turner excitation and emission monochromators were used along with a cooled PMT-900 photomultiplier detector that covers a range of 185-900 nm. Absorption spectra were collected between 300-540 nm monitoring the emission at a wavelength of 550 nm. The calculated degree of CT is also reported for S0 and S1 with the associated oscillator strength for S1 excited states.