Phase-sensitive second-harmonic microscopy reveals polarity of topologically centrosymmetric molecular crystals

Kluge, Sebastian; Budde, Felix; Dohnke, I.; Rechsteiner, Peter; Hulliger, Jürg

doi:10.1063/1.1492850

Cited by 25 publications

(32 citation statements)

References 11 publications

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“…This also results in the flexibility of tuning the wavelength of the SHG signal by changing the excitation wavelength accordingly. The coherent nature of the SHG signal is also a main advantage, providing a possibility to detect the second harmonic signal with interferometric optical techniques [10][11][12][13].…”

Section: Introductionmentioning

confidence: 99%

Three-dimensional harmonic holographic microcopy using nanoparticles as probes for cell imaging

et al. 2009

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Luminescent markers play a key role in imaging techniques for life science since they provide a contrast mechanism between signal and background. We describe a new type of marker using second harmonic generation (SHG) from noncentrosymmetric BaTiO 3 nanocrystals. These nanoparticles are attractive due to their stable, non-saturating and coherent signal with a femtosecond-scale response time and broad flexibility in the choice of excitation wavelength. We obtained monodispersed BaTiO 3 nanoparticles in colloidal suspensions by coating the particle surface with amine groups. We characterized the SHG efficiency of 90-nm BaTiO 3 particles experimentally and theoretically. Moreover, we use the coherent SHG signal from BaTiO 3 nanoparticles for three-dimensional (3D) imaging without scanning. We built a harmonic holographic (H 2 ) microscope which records digital holograms at the second harmonic frequency. For the first time, high-resolution 3D distributions of these SHG markers in mammalian cells are successfully captured and interpreted by the H 2 microscope.

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Section: Introductionmentioning

confidence: 99%

Three-dimensional harmonic holographic microcopy using nanoparticles as probes for cell imaging

et al. 2009

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“…Although we do yet not know the difference in energy that gives rise to P chloro-surface T P nitro-surface , it is reasonable to assume a small difference here. The effect of polarity formation is confirmed by a second harmonic generation (SHG) response seen in CNS crystals: [13] for the first time, a grown-in bipolar state was confirmed for P2 1 /c. In Figure 7A a fundamental-wavepolarised parallel b axis reveals the preseence of polarity in both the upper and lower b sectors.…”

Section: Markov-chain Model Of Polarity Formationmentioning

confidence: 64%

“…2 Channel-type inclusion crystals, [11] whereby guest and host molecules co-crystallise to form a supramolecular material with a centrosymmetric host structure. 3 Organic solid solutions H 1Àx G x (H: host, G: guest), [12] whereby, for example, A ± D guest molecules substitute sites in a centrosymmetric lattice built by molecules H. 4 Single component organic crystals, [8,13] whereby A ± D molecules undergo 1808 orientational disorder during growth, thereby transforming a centrosymmetric seed into a twinned crystal with polarity in the growth sectors. Given whatever a type of packing and symmetry in molecular crystals (examples 1 ± 4 above), we assume here a set of sites to which attachments can be described by probabilities P entering a kind of equation given above [Eq.…”

Section: Markov-chain Model Of Polarity Formationmentioning

confidence: 99%

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Markov-type Evolution of Materials into a Polar State

Hulliger

2002

Chem. Eur. J.

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“…2). Phase-Sensitive Second Harmonic (Generation) Microscopy (PS-SHM) [32,33] Molecular building blocks showing β ijk optical non-linearity by a polar group in the solid, give rise to sector-wise and polarization dependent frequency doubling. If by interference with a reference 2ω 0 beam, the second harmonic light generated in the crystal (thin layer for transmission, bulk for confocal) is intensified in one sector, whereas in its symmetry related sector destructive interference will take place and vice versa.…”

Section: Wwwcrt-journalorgmentioning

confidence: 99%

Dissymetrization of molecular crystals: a driving force for property formation

Hulliger¹,

Batagiannis

2008

Cryst. Res. Technol.

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Phenomena of dissymetrization of molecular crystals are reviewed which lead to sector wise polar properties. Orientational disorder of prolate-type dipolar molecules taking place at attachment sites can produce partial polar alignment of dipoles in corresponding growth sectors of molecular crystals nucleating into topologically centric packings. As a result bi-polar crystals are obtained. In case of native polar groups, Monte Carlo simulations predict a basic behaviour for pyroelectric molecular crystals: the dipoles belonging to sectors of either the plus or minus direction of the unique axis show a non-vanishing probability to be gradually reversed. Domain reversal may start upon a single orientational defect developing into complete sector reversal. Basic features of growth induced stochastic polarity formation are confirmed by scanning pyroelectric microscopy, phase sensitive second harmonic generation microscopy and x-ray scattering. Real systems comprise channel-type inclusion compounds, single component molecular crystals, solid solutions and long chain proteins in natural tissues. Neumann's principle gives thought to physical properties of bulk crystals [2], although building blocks undergo attachment to surfaces confined to 2D point groups. For growth induced properties, Neumann's principle may thus be restated as follows [3]: The symmetry elements of a physical property of a growth sector include all symmetry elements of the point group of the growth sector. Properties resulting explicitly from processes at the crystal-nutrient interface are those, which in principle should disappear if thermalization of the bulk structure far off the surface has reached the minimum of free energy. Growth processes leading to the dissymmetrization of crystals are known for a long time [4][5][6] and were mainly discussed for minerals [7]. For a review discussing also molecular crystals featuring optical anomalies [8]. Recently, we have reviewed the impact of surface symmetry on growth-induced properties emerging from corresponding families of faces of the 32 point groups. Explicitly, a symmetry analysis for a vector property, i.e. pyroelectricity was performed [3].Here, we shall understand dissymetrization as a constructive phenomenon for physical property formation. Vector property formation is particularly interesting in the case of molecular crystals, constituted by prolate shaped dipolar molecules. After an extensive experimental [9][10][11][12] and theoretical [3,[13][14][15][16][17][18][19][20][21][22][23] analysis starting in 1995, we are about to conclude that any dipolar molecule crystallizing into a crystal structure described on average by a non-polar point group undergoes (to some extent) sector-wise dissymetrization, leading to sectors showing polar properties. Growth-induced polarity formation leads to non-classical twinning, i.e. bi-polar states of molecular crystals.The basic phenomenon behind growth induced polarity formation is symmetry breaking at the crystalnutrient interface. The probabilities of att...

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Phase-sensitive second-harmonic microscopy reveals polarity of topologically centrosymmetric molecular crystals

Cited by 25 publications

References 11 publications

Three-dimensional harmonic holographic microcopy using nanoparticles as probes for cell imaging

Three-dimensional harmonic holographic microcopy using nanoparticles as probes for cell imaging

Markov-type Evolution of Materials into a Polar State

Dissymetrization of molecular crystals: a driving force for property formation

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