General Information

GENERAL:

Microspectrophotometric data provide essential information in the planning and in the interpretation of X-ray crystallographic experiments. This is particularly true for studies on redox proteins, where the oxidation state of redox centres may be altered by electrons liberated by X-rays during data collection (for more details see Berglund, G.I., Carlsson, G.H., Smith, A.T., Szoke, H., Henriksen, A. & Hajdu, J. (2002) The catalytic pathway of horseradish peroxidase at high resolution. Nature 417, 463-468. and the supplementary material with this paper. Those papers can be found in the bottom of the page).

(1) DETECTORS AND MONOCHROMATORS:

We buy the detectors, spectrograph and the software from a company in Belfast (Andor). We match the monos and the detectors and modify the input assembly to take single fibres.

CCD DETECTOR SYSTEM WITH USB2.0 INTERFACE AND SHAMROCK 163 MONOCHROMATOR

The read out speed of the CCD is very high, the quantum efficiency is also high, the dark current is low, and illumination with a low intensity light is sufficient. This is important if you have photosensitive material in the beam. The CCD detector we use is a DV401A-UV iDus. The CCD chip a Marconi 40-11 (1024x127 pixels). For more details on the range of CCD see http://www.andor.com, "Products--Scientific Cameras--iDus--DV401A-UV”. We interface the CCD detector as above with the Andor Shamrock 163, 163 mm focal length spectrograph with 400 lines/mm grating, fixed entrance slit (50 micron and a 100 micron slit, these are interchangeable). Spectral range is as above (1-0.5 nm), but the dynamic range, the DQE and the read out speed is much better with the CCD. One can do spectral measurements to about 3.5-4 O.D. using rapid averaging techniques for each spectrum. The important point is to have a system that allows simultaneous measurements in a 500 nm wide spectral band path that can be placed anywhere between about 230-850 nm. The work is usually done in the range of 300-800 nm.  

 

 

(2) LIGHT SOURCES

We have two different light sources: A very powerful and very little HALOGEN LAMP is supplied as standard with the instrument. This halogen lamp can be used for spectral measurements in the 350-800 nm range. We can also supply a Zeiss CLX 500 XENON LAMP in addition to the halogen lamp with an output between ~180 - ~1000 nm, but this is extra.

(1) THE HALOGEN LAMP that comes with the basic instrument is specifically designed to inject a single optical fibre. And it does that very effectively. The lamp has a tiny bulb with 5 W power only, yet the light output at the other end of the fibre is many times higher than the output when one uses, say, a 1000 W projectorlamp to inject the fibre. This is due to the source size and the divergence just like with synchrotrons and anodes. This lamp is used for spectral illumination AND also for producing light for the observation microscope during sample manipulation.  

(2) The Zeiss CLX 500 XENON LAMP works between ~190 - ~1100 nm (for some reason Zeiss claims a different regime on their web site). It is suitable for UV-VIS-NIR absorption measurements and also for fluorescence applications. It is one of the best and simplest xenon lamps on the market. The model is equipped with a slow electronic shutter, has a shutter cable (2 pins), and SMA single fiber connector. For specs see http://www.zeiss.de/de/home_e.nsf then click on search and enter clx 500 (note the SPACE between clx and 500).  

THE USEFUL SPECTRAL RANGE:

The mirror lenses focus the spectrum onto a single spot without significant chromatic aberration. They work well in the wavelength range of about 150 - 10,000 nm (far UV to far infrared) which is quite spectacular. But..., we use optical fibers to link the mirror lenses to the lamp and to the monochromator and detector. These fibers limit the accessible spectral range. For application in protein crystallography, we use very high grade quartz single fibres with excellent light transmission in the 230-800 nm regime (you can probably push this a bit further with averaging but you are counting single photons then). If one would like to do infrared measurements, one could use special IR fibres, monochromators and detectors. We don't supply these presently but we have done FTIR measurements on thin crystals with these mirror lenses.

SIZE OF THE MEASUREMENT SPOT

This depends on the diameter of the illuminating fibre. With a 50 micron fibre (the standard stuff), the spot size in 4DXSystems' microspectrophotometer is between 20-25 micron. The size of this spot can be increased or reduced (to about 10 micron) if necessary. One should always make sure that the measurement spot is smaller than the sample.

 

SPECTRAL CALIBRATION OF THE MONOCHROMATOR/DETECTOR UNIT

This is done with a holmium filter built in the halogen lamp that is supplied as standard with the instrument. When we do experiments, we always calibrate the wavelength after switching on the instrument. Safety first - there are hundreds of people who are obsessed with turning micrometer screws and there is one on the monochromator.

 

REFERENCE SPECTRA FOR SPECTROPHOTOMETRIC MEASUREMENTS:

We usually use air as a reference. You can also pick up a reference spectrum from the mother liquor near the crystal. Have a look at Wilmot, C.M., Sjogren, T., Carlsson, G.H., Berglund, G.I. & Hajdu, J. (2002). Defining redox state of X-ray crystal structures by single-crystal ultraviolet-visible microspectrophotometry. Methods in Enzymology, vol 353, "Redox Cell Biology and Genetics, part B", pp 301-318, Ed. C. K. Sen & L. Packer, Academic Press (USA).The most reliable measurements are difference measurements following the trigger of a reaction. It is important to keep the crystal in the same orientation throughout. In contrast to solution measurements, crystals are anisotropic (if they are not cubic), and their spectrum is different from different directions. This is not a bug, this is a FEATURE of optical measurements on crystalline samples. To get something similar to the solution spectrum, one needs to integrate over different angles. Absorption of plane-polarised light with the electric vector parallel to the principal optical directions of the crystal obeys the Lambert-Beer law.

SHAPE OF THE CRYSTALS:

Crystals with parallel faces offer reproducible measurements when the light beam falls normal to one of the crystal faces.  

NON-FLAT CRYSTALS:

Try a non-flat cuvette in spectrophotometry. The effect is exactly the same as with a non flat crystal in microspectrophotometry. If you change the orientation of the non-flat cuvette (you can call this a prism), the apparent spectrum will change. You can however make accurate difference measurements relative to a fixed orientation, e.g. as a function of time, temperature, pH, etc.

MEASUREMENTS ON CRYSTALS MOUNTED IN CAPILLARIES:

 A capillary filled with liquid is a cylindrical lens. In order to obtain good spectra from such samples, it is important to center the capillary carefully and have its optical axis perpendicular and intersecting with the optical axis of the microspectrophotometer. Relative difference measurements can however be performed accurately even if the sample and the capillary is in some random but unchanging orientation.

FLUORESCENCE CAPABILITY:

Two measurement modes on single crystals are possible:(i) Orthogonal 3 axis arrangement with the excitation source perpendicular to the emission probe and both axes perpendicular to the spindle axis of the goniometer in the microspectrophotometer. The observation microscope can either face the emission probe or the excitation probe in this system. (ii) Single probe excitation/emission measurement system utilising a 7-fibre bundle in a "hexagonal close packed" geometry. In this arrangement, photo-excitation and emission-measurements are done through the same mirror lens. Excitation light is delivered through the 6 hexagonaly arranged outer fibres under a slight defocus. Fluorescent light is picked up by the central single fibre from the middle of the excitation patch. Both systems have their advantages: The first of these is flexible and is practically noise free. The second unit can suffer from back scattering but it is extremely compact and can be used in very crowded experimental environments often encountered at synchrotrons.

Berglund, Nature

Berglund, Suppl. 1

Berglund, Suppl. 2

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