ISSN 00063509, Biophysics, 2012, Vol. 57, No. 2, pp. 144–152. © Pleiades Publishing, Inc., 2012.
Original Russian Text © Ph.S. Orekhov, A.K. Shaytan, K.V. Shaitan, 2012, published in Biofizika, 2012, Vol. 57, No. 2, pp. 221–231.
144
INTRODUCTION
Bacteriorhodopsin is a small (24 kDa) integral
membrane protein occurring in ElazariVolcani 1957
halobacteria of species Halobacterium salinarum
(formerly Halobacterium halobium). In the light,
bacteriorhodopsin creates a transmembrane proton
gradient, which is utilized in ATP synthesis and
implementation of other energy needs of the bacte
rium. Thus, in the halobacterium one finds an alter
native photosynthetic apparatus [1, 2] basically dif
ferent from that in other organisms, however, owing
to the simplicity of its design, capable of functioning
under most extreme environmental conditions. Its
efficiency is markedly lower than that of chlorophyll
photosynthesis (where the efficiency constitutes
35%), but still reaches 15% [3].
The central functional element of bacteriorhodop
sin is the chromophore, retinal, which absorbs a light
quantum and triggers a cascade of photochemical and
thermal conversions eventually leading to transfer of a
proton from the cytoplasm onto the outer side of the
membrane. Retinal is a conjugated polyene attached
covalently, via a Schiff base, to amino acid residue
Lys216 situated in the middle part of the Gprotein
transmembrane helix. In the ground (dark) form, not
excited by light, retinal exists in a state of thermody
Editor’s Note: I certify that this text exactly reproduces all factual
statements and closely conveys the phrasing and style of the
original publication. A.G.
namic equilibrium of two conformers: alltrans and
13cis,15syn [4]. Upon absorbing light of certain
energy, the alltransretinal undergoes a process of
photoisomerization, the equilibrium shifts and the
prevalent conformer becomes the 13cis,15anti form
(see Fig. 1), the process of thermal relaxation of which
in aggregate with structural rearrangements in the sur
rounding apoprotein is coupled with proton transport.
A remarkable peculiarity of bacteriorhodopsin (as
well as other retinalcontaining proteins) remaining in
the focus of the most modern research is the phenom
enon of socalled spectral tuning. It is well known
from experiments [5] that free retinal in vacuum pos
sesses an absorption maximum corresponding to
610 nm, while retinal in the composition of bacterior
hodopsin comes to absorb at 568 nm [6]. In this way,
the protein surroundings cause a blue shift of the reti
nal absorption maximum, at that different proteins,
differing in amino acid composition but retaining the
common plan of structure of retinalcontaining pro
teins (and also mutant forms of one and the same pro
tein) are characterized by different magnitudes of the
spectral shift.
A study of the regularities of modulation of the
spectra of retinalcontaining proteins (in particular,
development of methods of computer prediction of
the magnitudes of the spectral shift characterizing the
mutant forms of these proteins) is necessary for solving
applied tasks of nanotechnology connected with con
struction on the basis of retinalcontaining proteins of
MOLECULAR BIOPHYSICS
Calculation of Spectral Shifts of the Mutants
of Bacteriorhodopsin by QM/MM Methods
Ph. S. Orekhov, A. K. Shaytan, and K. V. Shaitan
Biological Faculty, Moscow State University, Moscow, 119991 Russia
Email: k.v.shaitan@molsim.org
Received September 12, 2011
Abstract—Spectral shifts of adsorption maxima for a number of mutants of bacteriorhodopsin have been cal
culated using QM/MM hybrid methodology. Along with this calculation, an analysis of possible mechanisms
of spectral modulation has been performed. Also we have carried out a comparative analysis of modern quan
tum chemical methods in respect of the level of optical spectra predictability they allow. We have shown that
modern hybrid quantum chemical methods reach an acceptable level of preciseness when applied in the cal
culation of spectral shifts even if the absolute values of adsorption maxima predicted by these methods are
underestimated. A number of rules has been found linking the value of spectral shift with the structural rear
rangement in the apoprotein. The methods we were using as well as those rules we have found out both may
be useful for development of nanoelectronical devices based on mutant species of bacteriorhodopsin (mem
ory elements, optical triggers etc.).
Keywords: computer modeling, QM/MM, bacteriorhodopsin, retinal, spectral shift.
DOI: 10.1134/S0006350912020170