American Pharmaceutical Review: A Russell Publishing Publication

Combining Raman Spectroscopy and Microscopy to Support Pharmaceutical Development

Gary McGeorge, Ph.D.
Bristol-Myers Squibb Company

Introduction


Spectroscopic imaging has seen a significant increase in attention as a result of two independent processes. Firstly, the introduction of faster spectroscopic imaging technology has resulted in very high quality systems that can generate data on a timeframe of minutes, not hours. Secondly, the FDA has an increased interest in process analytical technology (PAT) as a tool to augment and support drug product manufacturing. Consequently, fast, accurate spectroscopic imaging systems that can analyze materials in a non-destructive fashion can clearly offer a distinct advantage to the pharmaceutical manufacturer. In this paper, a brief discussion of the spectroscopic imaging technique is provided, followed by the analysis of a drug candidate that crystallized as a mixture of polymorphs. FTRaman spectra were collected to provide the benchmark spectra for analysis followed by a restricted wavelength spectroscopic image. Raman mapping of a whole intact tablet with a FT-Raman system will serve as an example where the concentration dependence across the surface of the tablet was established. Both of these examples will hopefully demonstrate the utility of Raman imaging (mapping) to obtain additional information that can ensure the quality of a drug substance or oral dosage form.


Instrumentation

Raman mapping and imaging technologies have developed significantly to the point that more commercial instruments are available on the market. These microscope-based tools allow for very high-resolution imaging. Hyperspectral imaging (also known as direct-imaging) is a technique whereby a monochromator that preserves the spatial integrity of the image is placed directly in the optical path of a microscope. These monochromators can be acousto-optically (AOTF) [1] or liquid crystal (LCTF) tunable filters. Tuning the monochromator through various wavelengths sequentially allows for selectivity of the appropriate spectral regions to be probed. These spectrometers typically use green (514 nm) through to red (765 nm) laser irradiation. The resultant monochromatically filtered photons are collected on high sensitivity CCD or CID camera that can further enhance the utility of such an imaging technology. The power density compared to high-resolution confocal mapping Raman microscopy is significantly lower since the laser is distributed over the whole field of view. As a result, the lower power density is less destructive to samples.

Mapping technology is more common at the moment for the collection of spectroscopic images. Mapping systems, on the other hand, require one to aperture down tightly on the sample and collection of an entire spectrum at discrete sample positions. Sequentially moving the sample under the microscope and piecing the points together creates the image of choice. The spectral resolution can be very high with this methodology, and it is limited mostly by the spectrograph used for dispersive systems. However, the spatial resolution is related to both the aperture used to confine the active region of interest and the spatial accuracy of the microscope stage movement. Small apertures reduce the signal, therefore requiring high sensitivity detectors and more discrete steps to generate the same final image size. As such, acquiring a Raman spectral image can take many hours. For hyperspectral imaging, assuming one knows the spectral regions of interest, only a handful of wavelengths (images) are required for a full analysis. For the analysis of a moderate Raman scatterer, (where 4 wavelengths might be collected) it may take just a few minutes to collect the data.

Many Raman spectrometers operate by the Fourier transform principal (FT) and use near infra-red excitation (1064 nm). By the very nature of these spectrometers, high-resolution images are not attainable, and correspondingly would appear to be the perfect candidate for a macro-imaging system. Macro systems would provide lower resolution of detail, but at an increased speed. This approach is very useful if one needs to map an entire tablet, but is unsure of what components (peaks) to look for. An excellent discussion of the instrumentation and applications of Raman microscopy is given by Turrell and Corset [2].


Drug Substance


Many of the regulatory requirements during drug substance manufacturing focus on the chemical identity, purity, impurity profile and residual solvents from the synthetic process. An increasing number of examples have demonstrated that, additional to the composition, one needs to understand the physical nature (polymorphic [3] and morphologic) of a drug entity. In fact, one main source of morphologic variety arises from the crystallization of a different polymorph [4]. The FDA’s perspective and patent protection issues are of considerable interest to the pharmaceutical manufacturer. The FDA expects that the crystallization process is in control and that the polymorph generated will provide predictable properties in-vivo. Likewise for patent rights, it is important to understand and characterize allknown polymorphs of a particular NCE (new chemical entity). This requires knowledge of what the polymorph is, preferably via a single crystal structure or by inference via a combination of physical characterization techniques involving spectroscopy, powder XRD and thermal analyses [5]. Polymorphism, by definition, is the ability of a material to adopt multiple, independent, packing arrangements, which generates a crystalline lattice. To demonstrate the importance of polymorphism, the ROY compound, investigated by Byrn et. al. [6], has six known polymorphs. Each of these polymorphs has different colors.

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