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At Eastern Slovenia's Mežica Mine you can explore the upper reaches of the mine by bike
and go kayaking along the lakes of spring water that have pooled half a mile (800m) below ground © Photo courtesy of Podzemlje Pece
On this day, he’s planned a trip to Koroška’s Mežica Mine
a former lead and zinc extraction facility buried deep within a 7,000ft (2,125m)-high outcropping called Mt Peca
I express polite interest – how exciting can a lead mine be
I had no idea I was about to embark on an adventure I’ll remember the rest of my life
I learn about the mine from one of the coordinators of the Geopark
From Roman times to the end of the last century
the mine was a bountiful source of lead ore and rare minerals
nearly 600 miles (1,000km) of excavation tunnels were burrowed into the mountain to a depth of nearly 3,300ft (1,000m)
Working conditions for the miners were so harrowing
the mine and surrounding areas were referred to as the ‘Valley of Death.’ My ears perk up at that last part
but my hosts assure me the mine is perfectly safe for a short-term visit
I’m still not certain what we’ll be doing in the mine
until I see Marko wheel over a couple of mountain bikes
along with helmets and miner-style headlamps
he tells us the plan for the morning is to explore the upper reaches of the mine by bike
Then in the afternoon we’ll descend to the lowest levels by train
and go kayaking along the lakes of spring water that have pooled half a mile (800m) below ground
A blast of cold air greets us as we push open the heavy metal doors to the mine and walk our bikes inside
Temps below ground hover around 50 degrees Fahrenheit (10 degrees Celsius) year-round
and we’re wearing spring jackets to stay warm
Our eyes need a couple of minutes to adapt to the blackness
Marko starts the ride off slowly to allow us to adjust to the path’s narrow
uneven terrain and occasionally low-hanging ceilings
But soon he picks up the pace and the exhilaration of cycling inside of a mountain kicks in
The surface is rock-strewn but flat; the length of the trail
is suited to a confident beginner or intermediate rider (and kids over the age of 10)
Advanced mountain bikers may want to try their luck the mine’s more challenging track
dubbed the “Black Hole,” etched ominously into the mine’s even-narrower crevices
Marko pauses to point out some of the mine’s features: giant caverns of natural beauty
rusting buckets of ore sitting for decades and which attest to the day-to-day difficulties of working a mine
Here and there he points to surviving veins of white
rust-brown wulfenite still embedded in the walls (an on-site museum highlights the many metals and minerals that have been found inside the mine)
After a little more than an hour of riding
we re-emerge smiling – if temporarily blinded – into the bright summer sunshine
and in my mind I picture a typical ride with comfortable seats and windows
Matej and I climb into a tiny box of a carriage
each no wider than the length of my arm and only a few feet long
were once used to carry as many as eight miners at a time as deep as 1.8 miles (3km) below the surface
It’s hard to imagine today – the carriage feels cramped with just the three of us inside
I have a deep appreciation for the educational aspect of our visit
was a daily reality for thousands of men who once worked these seams
and descend a further 600 steps to the chamber’s low-lying pools of fresh water
we pause momentarily in a heated dressing room to don chest-high waders that will protect us from the chilly (43°F / 6°C) water
we walk into the water and fetch our kayaks
we’re free to aim our boats wherever we want and to follow the narrow channels wherever they lead
the space feels unexpectedly airy and peaceful; the silence is broken only by our laughter and the sounds of paddles dipping into the clear water
the water throws back shades of green and blue
I feel a temporary urge to dive in (and then I remember the temperature)
It dawns on me I’ll likely never forget this moment
This story was crafted collaboratively between Slovenia Tourism and Lonely Planet. Both parties provided research and curated content to produce this story. We disclose when information isn’t ours.
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A Publisher Correction to this article was published on 02 May 2024
This article has been updated
we introduce a novel approach using correlative analysis techniques to unravel detailed insights into the environmental influences on crystal growth
Tabular and bipyramidal wulfenite samples from the Mežica mine in north-eastern Slovenia were analysed to combine the morphological aspects of crystal growth with the atomic-resolution reconstruction of the positions of lead (Pb) and molybdenum (Mo) atoms in the parent crystal lattice
These combined data also allow us to present the formation mechanism that enables the development of bipyramidal or tabular morphologies in wulfenite
The bipyramidal and tabular crystals are chemically pure wulfenite (PbMoO4)
as confirmed by various advanced diffraction and spectroscopy techniques
The differences in the morphologies can be attributed to compositional changes during precipitation from a meteoric solution and thus
we propose a growth mechanism consisting of three different phases of growth
This innovative approach emphasises the importance of understanding the origin of crystal habits
as can help to decipher how external influences can affect the crystal structure and its surface
leading to the dissolution of preferred surfaces and the selective release of Pb and Mo
we introduce wulfenite crystals with a wide range of crystal habits from the Mežica area (Republic of Slovenia)
Wulfenite crystals provide an excellent opportunity to study and understand the relationship between their crystal habits and the underlying crystal chemistry
These results confirm that the precipitation of the wulfenite crystals from Mežica occurred at ambient temperature and atmospheric pressure
which is consistent with the conditions of the wulfenites grown by Vesselinov in the laboratory
The presented study aims to define well-linked analytical information across multiple length-scale orders
from the millimetre-scale morphological aspects of crystal growth to the micrometre-scale chemical composition of the crystal
leading to an atomically resolved reconstruction of the positions of Pb and Mo atoms in the lattice of the parent crystal
We hypothesised that the combined data would allow us to formulate the mechanism leading to the development of bipyramidal or tabular crystal habits for wulfenite
using Vesselinov’s findings as a theoretical basis
This innovative approach and comprehensive methodology highlights the importance of understanding the origin of crystal habits and their relationship with environment
this knowledge can help to decipher how external influences can affect the crystal structure and its surface
leading to the dissolution/weathering of preferential surfaces and consequently to the selective release of Pb and Mo
This knowledge is therefore also particularly valuable for environmental scientists and various technical fields
Schematic representation of the two most common morphological varieties of wulfenite crystals
Ideal wulfenite crystal structure viewed along the (c) [100] and (d) [001] zone axes
Electron-backscatter diffraction (EBSD) analysis was performed using an SEM FSEM JEOL 7600F equipped with an EBSD detector
The obtained data were processed using the ICSD 2003 database for wulfenite as a reference
Atomically resolved high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) images were acquired via a probe Cs aberration correction transmission electron microscope (TEM) (JEM-ARM 200CF; JEOL
also equipped with a JEOL Centurio 100 mm2 EDXS detector
operates at 200 keV and provides a spatial resolution of 0.08 nm in STEM mode
EDXS elemental maps were produced in STEM mode (STEM-EDXS) to evaluate the elemental distribution with a high spatial resolution
The specimen preparation for the SEM/EDXS and TEM analyses involved cutting crystal samples along the principle crystallographic zone axes
which was determined using the EBSD technique
SEM/EDXS specimens were cut parallel to [001]
thin electron-transparent lamellae from both bipyramidal and tabular specimens of wulfenite were produced by using a focused ion beam scanning electron microscope (FIB-SEM; Helios NanoLab 600i dual beam system
The TEM electron transparent lamellae were cut parallel to the (100) atomic plane
On the left is a photo of a heap of tabular wulfenites from Mežica
On the right are the clusters and specimens used in this study
(a) Cluster of orange translucent bipyramidal crystals
(b) bipyramidal specimen taken from the cluster
(c) cluster of yellowish translucent tabular wulfenite crystals
and (d) tabular specimen taken from the cluster shown in panel c
The crystal structure constructed from the refinement data
(a) View from [001] zone axis; (b) view from [111] zone
(a) and (b) Low-magnification SEM backscattered electron images showing layers of inclusions in the two bipyramidal specimens
where the growth change from tabular to bipyramidal can be observed on both images; the zone axis is [100]
(c) Higher magnification SEM BSE image showing a cluster of inclusions
The image is a colour-coded phase map created from EDXS analysis data
focusing on the rare descloizite inclusion
The orange colour represents the wulfenite phase
(a) Bipyramidal and tabular (b) crystals of the wulfenite sample
The lattice planes are marked on the crystals
The FIB-cut [100]-oriented lamella is shown in the inset obtained from tabular crystal
and O obtained from the same area as the presented ADF image showing a homogeneous elemental distribution in the studied area
(d) Constructed atomic model of the MoPbO4 crystal (data from SCXRD analysis) projected along the a-axis
and 16f mark the Wyckoff positions of the corresponding Mo
unprocessed HAADF-STEM image at high magnification
projected along the a-axis ([100] zone axis)
The high-resolution HAADF-STEM image with the superimposed atomic model viewed along the [100] zone axis is displayed in the inset
The lattice spacing between the atomic planes along the c-axis is shown (3.15 Å)
Twinning or structure defects can be ruled out as a possible explanation for the differences in the external morphology of wulfenite
as they could not be detected by SCXRD or HAADF-STEM
We would also expect to be able to detect these agents in the atomic resolution HAADF-STEM images
particularly outside of the thin inclusion-rich layer mentioned earlier
these images show no defects or impurities
supporting our conclusion that surface coverage did not significantly affect crystal growth
the possible presence of impurities in our study does not seem to alter the crystal symmetries of the bipyramidal and tabular samples to the extent that they could be considered as different crystallographic phases
since both morphologies belong to space group I41/a
The changes in concentrations mark the beginning and end of each growth phase of the wulfenite crystals
3. In the third phase, the ratio of CPb/CMoO4 in the solutions is greater than 1, which promotes the growth of wulfenite, especially in the directions < 001 > , so that tetragonal pyramids {101} began to grow on the tabular base of the crystals, giving them bipyramidal morphology (Fig. 4: Growth of {001} inhibited
Some crystals retain their tabular morphology during the third phase
It should be noted that carbonate inclusions are also present in these crystals in the form of bands
suggesting that they precipitated from the same solutions as bipyramidal wulfenite but did not experience surface growth due to factors such as orientation or spatial limitations that did not allow growth in the < 001 > directions
This explains why some clusters show both morphologies
although the crystals are spatially very close to each other
separated by distances of at most a few millimetres
Wulfenite crystals from the Mežica Mine exhibit bipyramidal and tabular morphologies
The bipyramidal crystals consist of a tabular base and two tetragonal pyramids that grow on opposite sides of the base
These inclusions are often arranged in layers
These layers occur throughout the tabular crystals and in the tabular base of the bipyramidal crystals
The SCXRD analysis confirmed that both forms belong to the same space group
The analysis also confirmed the pure wulfenite compositions determined from the EDXS
which were further confirmed by the HAADF-STEM analysis
The differences in morphology can therefore be attributed to changes in composition (concentrations of Pb2+ and MoO42−) during precipitation from the meteoric solution rather than to differences in lattice geometry
defects such as twinning or surface capping by carbonates
We propose a growth mechanism that consists of three phases of growth:
the concentration ratio between CPb and CMoO4 in the solution is lower than 1
which favours the growth of tabular crystals
carbonates precipitated from the solutions and are present as inclusions in the wulfenite
Carbonate precipitation occurs incidental with the change in the concentrations of Pb2+ and MoO42− (CPb/CMoO4 ratio becomes greater than 1)
In the third phase the CPb/CMoO4 > 1 ratio favours the pyramidal growth of wulfenite crystals
As some of the tabular crystals remained protected from the new influx of solutions
The data are available in the Department of Geology
Faculty of Natural Sciences and Engineering
University of Ljubljana and in the Department for Nanostructured Materials
Jozef Stefan Institute (contact person Nastja Rogan Šmuc
A Correction to this paper has been published: https://doi.org/10.1038/s41598-024-60770-8
Uptake of elements from a biological point of view
Evolution of crystal structure of PbMoO4 between 5 and 300 K: A low temperature powder neutron diffraction study
A new structural model for Pb-deficient PbWO4
An explanation for the origin of hemihedrism in wulfenite: The single-crystal structures of I 4 1/a and I tungstenian wulfenites
Cleavage nature and surface appearances of wulfenite by first-principles calculations and experimental measurment
Theoretical analysis of changes in habit of growing crystals in response to variable growth rates of individual faces
A study on the kinetic conditions corresponding to the growth of crystals of different morphologies
On the symmetry of wulfenite (Pb[MoO4]) from Mežica (Slovenia)
Hemimorphic wulfenite crystals from Mežica
The wulfenite—stolzite series: Centric or acentric structures?
Analysis of solid solutions stability in scheelite-type molybdates and tungstates
Kinetically induced morphological changes in laboratory-grown wulfenite crystals
[Older versions (pre-1997) should refer to Siemens Analytical X-ray Instruments Inc
SHELXT–integrated space-group and crystal-structure determination
geokemične in mineraloške značilnosti rude in prikamenine svinčevo-cinkovih orudenj mežiškega rudišča
Characterization of “sandwich” wulfenite from the Ojuela mine
Mexico: Evidence of preferred secondary nucleation on selected wulfenite faces
Surface capping agents and their roles in shape-controlled systhesis of colloidal metal nanocrystals
Twinning and epitaxial growth of taaffeite-type modulated structures in BeO-doped MgAl2O4
The significance of wulfenite morphology as shown on crystals from Mezica
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This work was carried out with the financial support of the Slovenian Research and Innovation agency and as part of the ERC complementary scheme N1-0164 (Molybdenum geobiochemical cycle in rocks and sediments)
conducted analyses and interpreted the data; N.G
The authors declare no competing interests
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The original online version of this Article was revised: The original version of this Article contained errors in the Figure legends of Figures 1
The legends of these Figures were inadvertently switched
Full information regarding the corrections made can be found in the correction for this Article
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DOI: https://doi.org/10.1038/s41598-024-60043-4
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