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phases of mitochondrial membrane potential fluctuations induced by tetramethylrhodamine methyl ester photoactivation Angela M.. Falchi, Raffaella Isola, Andrea Diana, Martina Putzolu and

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phases of mitochondrial membrane potential fluctuations induced by tetramethylrhodamine methyl ester

photoactivation

Angela M Falchi, Raffaella Isola, Andrea Diana, Martina Putzolu and Giacomo Diaz

Department of Cytomorphology, University of Cagliari, Monserrato, Italy

Fluctuations of the mitochondrial membrane potential

(MMPFs) have been investigated in mitochondria

of intact cells [1–7] and in isolated mitochondria

[2,8,9] stained with tetramethylrhodamine derivatives

(TMRM, TMRE and related compounds, hereafter

indicated as TMRM) It has been postulated that

mitochondrial depolarization is due to singlet oxygen

generated by the photoactivation of TMRM [10]

Depo-larization is followed by the efflux of the fluorescent

probe, which stops the production of singlet oxygen

This allows the mitochondrial potential to be recovered,

followed by a new influx of TMRM from the

cytosol Thus, the continuous illumination of

TMRM-stained mitochondria triggers cyclic depolarization and

repolarization phases, at least as long as mitochondria are able to counterbalance the oxidative and dissipative effects A hypothetical model of MMPFs induced by TMRM photoactivation is shown in Fig 1

If the role of TMRM is evident, on the other hand, the mechanism directly responsible for the mitochond-rial depolarization is not clear The existence of a link between NAD(P)H, reactive oxygen species (ROS) and the permeability transition pore (PTP) has been dem-onstrated in numerous studies However, the complex-ity of the interactions between ROS, NAD(P)H, PTP and mitochondrial potential does not allow the majority of phenomena to be represented by a simple cause–effect relationship For example, ROS cause

Keywords

fluorescent probes; mitochondria;

photoactivation; potential fluctuations;

tetramethylrhodamine methyl ester (TMRM)

Correspondence

G Diaz, Department of Cytomorphology,

University of Cagliari, I-40492 Monserrato,

Italy

Fax: +39 70 6754003

Tel: +39 70 6754081

E-mail: gdiaz@unica.it

(Received 5 October 2004, revised 21

January 2005, accepted 26 January 2005)

doi:10.1111/j.1742-4658.2005.04586.x

Depolarization and repolarization phases (D and R phases, respectively) of mitochondrial potential fluctuations induced by photoactivation of the fluorescent probe tetramethylrhodamine methyl ester (TMRM) were ana-lyzed separately and investigated using specific inhibitors and substrates The frequency of R phases was significantly inhibited by oligomycin and aurovertin (mitochondrial ATP synthase inhibitors), rotenone (mitochond-rial complex I inhibitor) and iodoacetic acid (inhibitor of the glycolytic enzyme glyceraldehyde-3-phosphate dehydrogenase) Succinic acid (mito-chondrial complex II substrate, given in the permeable form of dimethyl ester) abolished the rotenone-induced inhibition of R phases Taken together, these findings indicate that the activity of both respiratory chain and ATP synthase were required for the recovery of the mitochondrial potential The frequency of D phases prevailed over that of R phases in all experimental conditions, resulting in a progressive depolarization of mito-chondria accompanied by NAD(P)H oxidation and Ca2+influx D phases were not blocked by cyclosporin A (inhibitor of the permeability transition pore) or o-phenyl-EGTA (a Ca2+chelator), suggesting that the permeabil-ity transition pore was not involved in mitochondrial potential fluctuations

Abbreviations

CsA, cyclosporin A; DCDHF, 6-carboxy-2¢,7¢-dichlorodihydrofluorescein diacetate diacetomethyl ester; D phase, depolarization phase; IAA, iodoacetic acid; MMPF, mitochondrial membrane potential fluctuation; NP-EGTA, o-nitrophenyl EGTA; PTP, permeability transition pore; R phase, repolarization phase; ROS, reactive oxygen species; SAD, succinic acid dimethyl ester; TMRM, tetramethylrhodamine methyl ester.

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depolarization, but they are themselves produced by

the respiratory chain at a rate that varies with the

membrane potential [11,12]; NAD(P)H energizes the

mitochondrion, but NAD(P)H is also an essential

sub-strate of glutathione and a direct scavenger of singlet

oxygen [10]; PTP opening causes depolarization, but

PTP may also be activated by depolarization [13];

PTP-induced depolarization may be inhibited by

oxy-gen radical scavengers, catalase and glutathione

[2,4,5,14]

Likewise, it is not clear how the mitochondrial

potential is restored after the TMRM efflux

Elimin-ation of ROS, if present, and switching of PTP to the

close configuration, if previously made to open, are

essential but not sufficient conditions for recovery of

the mitochondrial potential Mitochondrial

repolariza-tion requires the active support of the respiratory

chain and⁄ or the energetic contribution of ATP

hydro-lysis The latter mechanism has been found to occur in

response to depolarization induced by protonophores

or Ca2+ overloading [15,16] Moreover, ATP

hydro-lysis is the sole mechanism capable of energizing

DNA-depleted, metabolically inert mitochondria [17,18],

as well as mitochondria of blood eosinophils, which have a functional role in apoptosis but not in respir-ation [19]

The aim of this work was to investigate the mecha-nisms underlying MMPFs induced by TMRM photo-activation, by testing the effects of specific inhibitors

on mitochondrial depolarization and repolarization phases, analyzed separately

Results

The effect of TMRM photoactivation on the mitoch-ondrial potential can be evaluated by comparing the average curves of mitochondrial depolarization under conditions of continuous and discontinuous illumin-ation (Fig 2A) However, MMPFs were visible only

on plotting data of single mitochondria, and some rep-resentative traces are shown in Figs 2B and 6 The exact identification of depolarization phases (D phases) and repolarization phases (R phases) of MMPFs was obtained by derivative analysis, as illustrated in Fig 2C–D and Fig 3 (details are given in Experimen-tal Procedures)

Generation of ROS by mitochondria exposed to TMRM illumination was detected by 6-carboxy-2¢,7¢-dichlorodihydrofluorescein diacetate diacetomethyl ester (DCDHF) (Fig 4) ROS were not observed in mitochondria exposed to light in the absence of TMRM, nor in mitochondria filled with TMRM but not exposed to light [20] The intensity of ROS, as detected by DCDHF, was roughly proportional to the TMRM fluorescence This confirmed the necessity of selecting a homogeneous baseline fluorescence intensity

in order to avoid experimental data being confounded

by the effect of the initial amount of TMRM accumu-lated in mitochondria [21]

In all experimental groups, the frequency of D phases prevailed over that of R phases, resulting in a net depolarization at the end of the illumination per-iod In untreated cells, the ratio between D and R phases was about 3 : 1 The frequency of R phases was significantly reduced by rotenone, oligomycin, auro-vertin, and iodoacetic acid (IAA) (Fig 5A) The effect

of azide (P¼ 0.07) was not significant but close to the critical threshold R phases were almost completely abolished by the combination of aurovertin plus olygo-mycin, and rotenone plus olygomycin The effect of rotenone was removed by combination with succinic acid dimethyl ester (SAD) These findings suggest that the activity of both respiratory chain and ATP syn-thase is required to activate the R phase On the other hand, the frequency of D phases was substantially stable The frequency of D phases was not affected by

Fig 1 Schematic model of MMPFs induced by TMRM

tion under continuous illumination conditions TMRM

photoactiva-tion results in the generaphotoactiva-tion of singlet oxygen and NAD(P)H

oxidation Possible intermediary effectors of depolarization

(super-oxide, Ca 2+ , permeability transition pore, inner membrane anionic

channels, etc.) are indicated by the ‘?’ symbol Depolarization is

fol-lowed by the efflux of TMRM, which interrupts the generation of

singlet oxygen and allows the mitochondrial potential to be

recov-ered by the respiratory chain Repolarized mitochondria accumulate

new TMRM which starts a new cycle.

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o-nitrophenyl EGTA (NP-EGTA) and vitamin E,

whereas a significant increase was found with

cyclospo-rin A (CsA) (Fig 5B) The Ca2+-binding ability of

NP-EGTA was verified by the release of Ca2+ found

after NP-EGTA photolysis (data not shown) These

findings seem to exclude an involvement of the PTP in

the D phase Accurate analysis of images also excluded

the occurrence of mitochondrial swelling, a marker of

permeability transition

The duration of D and R phases was 1.05 and

0.77 s, respectively The rate of fluorescence changes

in D and R phases was 15 and 12 gray valuesÆs)1,

respectively (Fig 5C–D) Interestingly, the rate of R

phases was not significantly altered, even when the

fre-quency of R phases was extremely low

The sum of all D and R phase changes accounted

for 78.4% of the total fluorescence change found at

the end of the illumination period (Fig 2A, curve a)

This discrepancy was probably due to the presence of

small MMPFs, not distinguishable from noise, which

were eliminated by the filtering method The effect of

probe bleaching was negligible (Fig 2A, curve c)

MMPFs were simultaneously detected in all

sub-regions of single mitochondrial filaments (Fig 6) No

evidence of longitudinal propagation of MMPFs was

ever detected, despite the remarkable length of some

mitochondria However, it cannot be excluded that

propagation of MMPFs may actually occur at a speed

Fig 2 TMRM florescence measurements (A) Effect of continuous

(curve a) and discontinuous (curve b) illumination on the

mitochond-rial TMRM fluorescence, sampled at time intervals of 1 s

Discon-tinuous illumination consisted of light cycles of 20 ms, sufficient to

acquire the image, followed by dark periods of 980 ms Data

repre-sent averages of several cells, so that MMPFs are not visible.

Curve c shows the fluorescence decay of TMRM due to

photo-bleaching, under continuous illumination Photobleaching

measure-ments were made on dried stains of TMRM to avoid fluorescence

recovery after photobleaching For all measurements, baseline

ues of fluorescence intensity were in the same range of gray

val-ues (70–130) (B) Representative trace of TMRM fluorescence

intensity changes occurring in a single mitochondrion, exposed to

continuous illumination and sampled at the rate of one image every

60 ms Typical MMPFs are evident, but the separation of D and R

phases is imprecise (C) Derivative curve of the TMRM trace R

and D phases are readily identified by negative and positive peaks,

respectively (D) Derivative curve after removal of noise (small

peaks) and other irregular (asymmetric) fluctuations The features

of noise fluctuations were preliminarily analyzed from the

autofluo-rescence of plastic film, using the same optical settings and

meth-ods applied to mitochondria The max height and max width of

derivative peaks of noise fluctuations were set as cut-off values for

mitochondrial data The asymmetry of peaks was also considered

to exclude irregular fluctuations with nonlinear slopes Details are

given in Experimental Procedures.

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faster than 0.17 lmÆms)1, which is the detection limit

of our system, based on the ratio between the longest

mitochondria analyzed (10 lm) and the time interval

between consecutive images (60 ms)

In contrast with the simultaneous appearance of

fluorescence changes, the fluorescence intensity was not

uniformly distributed throughout all subregions of

single mitochondrial filaments This fact was initially

ascribed to the alternation of in-focus and out-of-focus

subregions due to the sinuosity of the mitochondrial

filament This hypothesis was tested by taking images

at different focus levels, with the expectation of

obser-ving a progressive shift of fluorescence maxima along

the filament Surprisingly, the longitudinal distribution

of fluorescence levels was not modified by focus

chan-ges, suggesting that longitudinal differences of

fluores-cence intensity were not optical artifacts, but reflected

intrinsic properties of mitochondria or of the

sur-rounding cytoplasmic environment

TMRM photoactivation resulted in a 34% decrease

in the mitochondrial NAD(P)H autofluorescence, in close agreement with other investigations [10,22] The NAD(P)H decrease after exposure of cells to illumin-ation, in the absence of TMRM, was only 4% This indicated that TMRM photoactivation was the pri-mary cause of NAD(P)H oxidation The correlation between TMRM and NAD(P)H changes was detected

at the level of single mitochondria (Fig 7) Unfortu-nately, the relatively long exposure required for NAD(P)H autofluorescence did not allow the occur-rence of NAD(P)H fluctuations in parallel with the acquisition of MMPFs to be verified

Experiments with TMRM and Calcium Green-1 showed a net accumulation of Ca2+into mitochondria

at the end of the period of TMRM illumination (Fig 8) The fluorescence change was not attributable

to Calcium Green-1 dequenching, consequent on the TMRM efflux, because (a) no quenching of Calcium Green-1 fluorescence was found in TMRM-filled mito-chondria before depolarization, and (b) no dequench-ing was found in TMRM-depleted mitochondria after depolarization induced by fluorocarbonyl cyanide phe-nylhydrazone

No transients of the mitochondrial potential were found after Ca2+ release induced by ATP stimula-tion of the IP3 pathway, despite a prominent increase in nuclear and cytoplasmic Ca2+ followed

by synchronous oscillations in both compartments

Ca2+ oscillations exhibited a constant duration of about 12.5 s, independent of their intensity which was gradually decreasing (see Supplementary mater-ial) In agreement with the inhibition of R phases induced by NP-EGTA, Ca2+ release resulted in a significant increase in the mitochondrial potential and NAD(P)H content, presumably because of the activation of Ca2+-dependent mitochondrial dehydro-genases [23–25]

Discussion

MMPFs induced by TMRM photoactivation have been extensively investigated to assess the functional continuity of the mitochondrial network [3–7,26,27] A less explored aspect of MMPFs concerns the mecha-nisms involved in the cyclic loss and recovery of the mitochondrial potential In fact, the double role of the fluorescent probe as inducer and detector of MMPFs represents a limitation of experimental studies, as any treatment influencing the baseline TMRM concentra-tion will also modify the generaconcentra-tion of MMPFs, thus making it difficult to distinguish effects of different nature This aspect has not been adequately considered

Fig 3 MMPF recognition Mitochondrial D and R phases (upper

panel) were numerically recognized by derivative analysis as

posit-ive and negatposit-ive peaks (lower panel) For each peak, the features

of height, width and symmetry were calculated The peak height

was calculated as the peak amplitude (segment a) The peak width

was calculated as the interval between the zero-derivative time

points t1 and t2 The peak symmetry was calculated as the lowest

of the reciprocal ratios between the t2-p and p-t1 segments

Cut-off values for peak height, width and symmetry were set to filter

noise and irregular fluctuations (see Experimental procedures) The

change in the original fluorescence intensity scale was obtained as

the difference between f1 and f2 values observed at the t1 and t2

time points, respectively.

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in previous studies which examined MMPFs in

differ-ent experimdiffer-ental conditions

The effect of singlet oxygen on PTP, and the

involvement of PTP in MMPFs induced by

photo-dynamic action are still questions open to debate

Contrasting data obtained by the same group of

inves-tigators have suggested that PTP may be activated or

inhibited by singlet oxygen, in accordance with the

nature and localization of the photosensitizer [28,29]

The issue is complicated by the fact that superoxide, a

proven PTP inducer, is generated at higher rates by

the respiratory chain under oxidative stress conditions,

and singlet oxygen may be a substrate for superoxide

production at the level of complex III of the

respir-atory chain or reacting with NAD(P)H [10]

Further-more, it is not clear whether PTP is actually involved

in MMPFs In some investigations, mitochondrial

depolarization induced by TMRM or TMRE

photo-activation was inhibited or decreased by CsA [30,31]

In others [2,6,10], the involvement of PTP was

exclu-ded Our data indicate that, at least in HeLa cells,

CsA not only does not prevent, but rather increases,

the frequency of D phases In addition, mitochondrial

swelling, a classical marker of permeability transition,

was never observed during our experiments, even after mitochondria reached a condition of permanent depo-larization Recently, propagation of MMPFs induced

by photo-oxidation has been correlated with the acti-vation of inner membrane anion channels [22,31] All the above data were obtained in mitochondria of intact cells An apparent contrast in the behavior of intact cells and isolated mitochondria has been observed by Huser & Blatter [2] who found that depo-larization induced by TMRM photoactivation was pre-vented by CsA in isolated mitochondria but not in mitochondria of intact cells To explain this discrep-ancy, it was hypothesized that mitochondria of intact cells are less sensitive to CsA because of the abundance

of CsA-binding proteins in the cytoplasm On the other hand, depolarization due to calcium-induced cal-cium release was found by Ichas et al [32] to be lar-gely prevented by CsA in mitochondria of intact cells Taken together, these findings indicate that CsA is an effective inhibitor of PTP even in intact cells, but PTP activation in intact cells is more sensitive to calcium stimulation than photoactivation of fluorescent probes

A further difference between these experimental mod-els is the self-propagation of the depolarization that

Fig 4 Generation of ROS by TMRM illumination Cells were loaded with TMRM and the ROS-sensitive probe DCDHF, with or without pre-incubation with vitamin E TMRM images (left) were taken at time zero DCDHF images (right) were taken at the end of the period of TMRM excitation (13.8 s) On comparison of images, a close correspondence is revealed between ROS and mitochondrial traces However, rather than being confined to the mitochondrial matrix, ROS appear to be spread in the surrounding cytoplasm, thereby suggesting a mech-anism of ROS release ROS are also present in the nucleus, which is entirely surrounded by the mitochondrial network Note that the blurred appearance of DCDHF is not an effect of poor focus, and that DCDHF does not accumulate in mitochondria, but is rather uniformly distri-buted throughout the cell [20] ROS were inhibited by vitamin E Production of ROS was not elicited by illumination alone in the absence of TMRM, nor, vice versa, by the sole TMRM in the absence of illumination (data not shown) Bar is 10 lm.

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accompanies calcium-induced calcium release [32], whereas depolarization induced by photo-oxidation, at least in the majority of cell types investigated, affects only the irradiated region but does not propagate to adjacent mitochondria [26] Only in cardiomyocytes, which possess specialized intermitochondrial junctions [26], has a local laser irradiation been found to activate

a cell-wide, slow traveling wave of depolarization associated with ROS-induced ROS release [22,31] However, MMPFs of cardiomyocytes were not preven-ted by intracellular Ca2+ buffering with EGTA or 1,2-bis-(aminophenoxy)ethane-N,N,N¢,N¢-tetra-acetic acid (BAPTA), in line with our data on HeLa cells The increase in mitochondrial Ca2+ found in our experi-ments after the induction of MMPFs may be explained

by local exchanges between mitochondria and neigh-boring Ca2+ domains of the endoplasmic reticulum [33–36], which may be responsible for the specific behavior of mitochondria of intact cells, as compared with isolated mitochondria

The higher susceptibility of isolated mitochondria to PTP [37] may also be considered in relation to the level

of ROS, as isolated mitochondria are generally suppor-ted by succinate⁄ rotenone, and the rate of ROS gen-eration is much higher in mitochondria respiring using complex II substrates (plus rotenone) than complex I substrates [38] In addition, MMPFs of isolated mito-chondria supported by NAD(P)H-linked substrates (malate and glutamate) have been found to be insensit-ive to CsA and negatinsensit-ive to the calcein assay for PTP opening [9,39]

NAD(P)H is important not only as an energetic sub-strate but also as an antioxidant subsub-strate of glutathi-one and as a singlet oxygen scavenger [10] However, our data suggest that NAD(P)H has a primary role in respiration, rather than as antioxidant, as R phases, which are more closely correlated to the energetic util-ization of NAD(P)H, were strongly inhibited by rote-none, whereas D phases, which are more closely

Fig 5 Effects of treatments on MMPFs The four panels show the changes of R and D phase frequencies (number per mitochondrion per minute) and fluorescence change rates (intensity change per second) after treatment with 10 l M NP-EGTA, 50 l M (+)a-toco-pherol acetate (Vit E), 2 l M CsA, 5 l M rotenone plus 7.7 m M SAD (rot + SAD), 6 m M NaN 3 (azide), 50 l M IAA, 5 l M rotenone (rot),

5 l M rotenone plus 10 l M oligomycin (rot + oligo), 10 l M oligomy-cin (oligo), 30 l M aurovertin (auro) and 30 l M aurovertin plus 10 l M

oligomycin (auro + oligo) Bars represent the median and interquar-tile range (25th )75th centile) The asymmetry of interquartile ranges is due to the skewness of data distributions Significant (P < 0.05) deviations from controls, calculated by the Student– Newman–Keuls test for multiple comparisons, are indicated by asterisks.

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correlated to oxidative phenomena, were substantially

unchanged, in spite of the higher NAD(P)H

availabil-ity after complex I inhibition

DCDHF traces were significantly decreased by

vita-min E However, vitavita-min E failed to inhibit MMPFs

The discrepancy between ROS inhibition and

mito-chondrial depolarization may tentatively be explained

by the observation that vitamin E is able to reduce

ROS present in the cytosol surrounding mitochondria

rather than ROS present in the mitochondrial matrix

[20] Contrasting effects of vitamin E have also been

found in the inhibition of mitochondrial depolarization

of rat and rabbit cardiomyocytes [31] However, data

obtained with specific superoxide scavengers [22] and

spin traps [30] have provided consistent evidence that

ROS represent a key factor in triggering MMPFs

The average duration of MMPFs (1–2 s) was in

close agreement with data obtained in previous studies

using relatively fast acquisition methods [2,4,5,8,30,33]

MMPFs of apparently longer duration in literature

result from data acquired at lower sampling rates [6,9]

R phases were strongly reduced by IAA, rotenone and ATP synthase inhibitors Whereas the effect of IAA and rotenone seems to be obvious, that of ATP syn-thase inhibitors is open to different interpretations One is that ATP synthesis may sustain repolarization

by increasing respiration and⁄ or by regulating the H+ influx A possible alternative is that ATP hydrolysis contributes to respiration to reach a critical H+ threshold for the import from the cytosol of energetic substrates Further investigation of these issues is required

Experimental procedures

Cell treatments

HeLa cells (ATCC) were grown in Dulbecco’s modified Eagle’s medium with high glucose Cells were supravitally stained with 100 nm TMRM for 30 min; 18 lm DCDHF

Fig 6 Simultaneous vs independent

MMPFs Simultaneous MMPFs were found

in all subregions of continuous mitochondrial

filaments (A) On the other hand, adjacent

mitochondria exhibited completely

independ-ent MMPFs (B).

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for 60 min; 5 lm Calcium Green-1 AM for 120 min Cells

were treated with 10 lm oligomycin (inhibitor of ATP

thase) for 10 min; 30 lm aurovertin (inhibitor of ATP

syn-thase) for 30 min; 5 lm rotenone (inhibitor of complex I)

for 30 min; 6 mm NaN3 (inhibitor of complex IV and V)

for 30 min; 50 lm IAA (inhibitor of the glycolytic enzyme

glyceraldehyde-3-phosphate dehydrogenase) for 30 min;

7.7 mm SAD (substrate of complex II) for 10 min; 2 lm

CsA (inhibitor of the PTP) for 30 min; 50 lm

(+)a-toco-pherol acetate (vitamin E) for 60 min or overnight; 10 lm

NP-EGTA (a cell permeant probe that binds Ca2+ with

high affinity until photolysed by UV light) for 30 min;

20 lm ATP (activator of purinergic receptors and the IP3 pathway) given at the time of acquisition of images Drug combinations (aurovertin and oligomycin, rotenone and olygomycin, rotenone and SAD) were used at concentra-tions applied for single treatments Drug vehicles were:

Me2SO for TMRM, Calcium Green-1, oligomycin and rote-none; chloroform for aurovertin; ethanol for CsA; water for azide, IAA, vitamin E, NP-EGTA and ATP Stock solutions were prepared to obtain a 1 : 1000 (0.1%) dilu-tion of vehicles in the medium TMRM, DCDHF, Calcium Green-1 and NP-EGTA were from Molecular Probes

A

B

Fig 7 Correlation between TMRM changes and NAD(P)H

oxida-tion (A) NAD(P)H and TMRM images captured at the start and end

of the illumination period Bar is 10 lm (B) NAD(P)H and TMRM

fluorescence of 15 mitochondrial regions of the same cell Each bar

represents the change between the initial (upper edge) and final

(lower edge) value Mitochondrial regions are conventionally

ordered according to the final TMRM fluorescence intensity.

Fig 8 Ca2+ accumulation in mitochondria after MMPFs Calcium Green-1 and TMRM images captured at the start and end of the illumination period Bar is 10 lm The plot shows the Calcium Green-1 fluorescence along a line (indicated in the image) crossing two mitochondrial filaments, before and after illumination The hori-zontal width of mitochondrial profiles shown in the plot indicates that Ca2+influx is not accompanied by matrix swelling.

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(Eugene, OR, USA) All other compounds were from

Sigma (St Louis, MO, USA)

Imaging

Cells were observed with a 100· ⁄ 1.0 water immersion

objective, using a Zeiss Axioskop microscope (Oberkoken,

Germany) with a HBO 50 W L)2 mercury lamp (Osram,

Berlin, Germany) attenuated with a 0.3% transmittance

neutral filter Fluorescence filters were 528–552 ex, 580 sp.,

590-LP em for TMRM; 460–500 ex, 505 sp., 510–560 em

for DCDHF; 435–485 ex, 500 sp., 515–555 em for Calcium

Green-1; 340–380 ex, 400 sp., 435–485 em for NAD(P)H

Images were acquired with a 12-bit cooled CCD camera

(Sensicam; PCO Computer Optics, Kelheim, Germany)

with a 1280· 1024 pixel chip and 2 · 2 pixel binning

Opti-cal settings provided a nominal over-resolution of 0.1 lmÆ

pixel)1 TMRM images were acquired every 60 ms, in series

of 230 images during 13.8 s of continuous illumination

(16.67 frames per s) The series was truncated at the 230th

image, as no MMPFs were observed after this time

TMRM images were preprocessed with a 3· 3 average

fil-ter to reduce random noise and unweighted time average

(n¼ 8) to reduce pixel replication noise Calcium Green-1

images were acquired with an exposure of 1 s Because of

the relatively long period (12.5 s) of Ca2+ oscillations

induced by ATP, in these experiments the acquisition of

images was prolonged to 1 min, at the rate of 1 frameÆs)1

Induction of MMPFs

Preliminary experiments showed that MMPFs depended on

the intensity and duration of illumination and fluorescence

intensity of mitochondria Illumination conditions were

eas-ily controlled, using the same optical settings in all

experi-ments On the other hand, the mitochondrial fluorescence

was more difficult to control, because of conspicuous

differ-ences in the amount of TMRM loaded by single cells [21]

Under a condition of continuous illumination required for

fast image acquisition, MMPFs were optimally detected in

mitochondria exhibiting a specific range of fluorescence

intensity, represented by the gray value range 70–130 No

MMPFs were found in mitochondria with a lower

fluores-cence (gray value < 70) On the other hand, mitochondria

with higher fluorescence (gray value > 130) displayed a

very fast depolarization In this case, the detection of

MMPFs was hindered by a massive release of TMRM in

the cytosol These data were obtained under a condition of

continuous illumination (20 ms exposure and 40 ms readout

for each image) Mitochondrial depolarization and MMPFs

were reduced when illumination was discontinuous, and

completely abolished when the 20 ms illumination of a

sin-gle image was followed by a dark period of 980 ms (one

frameÆper second) The effect of probe bleaching under

con-tinuous illumination was measured from the fluorescence

decay of TMRM stains obtained by spraying microdroplets

of 100 lm TMRM on a coverslip TMRM stains were dried

to avoid fluorescence recovery after photobleaching, and subsequently only those with a fluorescence intensity in the range of mitochondria (gray values 70–130) were selected for measurement The effect of continuous and discontinu-ous illumination and bleaching are shown in Fig 2A

Sampling

Morphological criteria for the selection of mitochondria were the (a) perfect focus, (b) homogeneous thickness (no swelling or stretching), (c) separation from each other (no crossing), (d) sufficient extension to allow the measurement

of three to five points along the filament, and (e) absence of movements The occurrence of movements in the x–y plane and in the z-axis was carefully checked comparing the pixel positions and focus drift of mitochondria through the stack

of images However, owing to the relatively short duration

of sessions and linear extension of mitochondrial filaments, the number of cases of exclusion was very small

Analysis of fluctuations

D and R phases were identified by numerical differentiation obtained, for each time point, as the difference between the three preceding and the three following time points:

FI0n¼ ðFIn3þ FIn2þ FIn1Þ  ðFInþ1þ FInþ2þ FInþ3Þ where FI is fluorescence intensity This operation trans-formed D and R phases into peaks of different sign (posit-ive and negat(posit-ive, respect(posit-ively), duration and intensity (Figs 2B,C and 3) The fluorescence change rate (ratio between fluorescence intensity change and duration) and frequency (number of events per mitochondrion per minute) were also calculated from the primary parameters The overall noise (inclusive of random and stationary noise, due

to current interference, instability of the arc lamp, occa-sional vibrations, etc.) was evaluated from the autofluores-cence of an inert plastic film, using the same optical settings (fluorescence filters, microscope magnification, iris opening, CCD gain, exposure, frame rate, etc.) and proce-dures (image processing, numerical methods) applied to cells The fluorescence intensity of the plastic film was made physically equivalent to the average fluorescence intensity

of TMRM by means of neutral density filters interposed between the lamp and the microscope The max height (¼ 3) and max width (¼ 9) of derivative peaks of the plas-tic material were set as cut-off values to remove all noise fluctuations from TMRM data However, it is possible that small MMPFs, not distinguishable from noise, may have been eliminated by the filtering method The symmetry of derivative peaks was also taken into account to remove irregular fluctuations characterized by nonlinear slopes Symmetry was calculated as the lowest of the reciprocal

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ratios between the t1-p and p-t2 segments (Fig 3)

Sym-metry was 1 for perfectly centered peaks and less than 1,

tending to zero, for increasingly irregular peaks, irrespective

of the tail direction The value of 0.333 was set as cut-off

for symmetry The relative frequency of rejections because

of height, width and symmetry was 78%, 16% and 6%,

respectively (Fig 2D) Data were processed with specific

routines developed for Microsoft Excel (Seattle, WA, USA)

and Statistica (StatSoft, Tulsa, OK, USA) Owing to the

considerable skewness of distributions, data were

summar-ized by the median and the 25th)75th centile (interquartile)

range Differences were tested by analysis of variance

followed by the Student–Newman–Keuls test for multiple

comparisons

Acknowledgements

We thank Professor Vincenzo Fiorentini (Physics

Department, University of Cagliari) for helpful

sugges-tions concerning numerical methods The research was

supported by grants from MIUR-FIRB

(RBAU01C-CAJ_003), Istituto Zooprofilattico Sperimentale della

Sardegna (IZS SA⁄ 001 ⁄ 2001) and Regione Autonoma

della Sardegna, Assessorato dell’Igiene e Sanita` e

dell’Assistenza Sociale

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