We present a new imaging method for pump-probe microscopy that explores non-collinear excitation. This method (crossed-beam pump-probe microscopy, or CBPM) can significantly improve the axial resolution when imaging through low-NA lenses, providing an alternative way for depth resolved, large field-of-view imaging. We performed a proof-of-concept demonstration, characterized CBPM's resolution using different imaging lenses, and measured an enhanced axial resolution for certain types of low-NA lenses.
Pump-probe microscopy is an emerging nonlinear imaging technique based on high repetition rate lasers and fast intensity modulation. Here we present new methods for pump-probe microscopy that keep the beam intensity constant and instead modulate the inter-pulse time delay, the relative polarization, or the pulse length. These techniques can improve image quality for samples that have poor heat dissipation or long-lived radiative states, and can selectively address nonlinear interactions in the sample. We experimentally demonstrate this approach and point out the advantages over conventional in…
A pump-probe dark-field X-ray microscopy (DFXM) experiment was carried out at the Advanced Photon Source (APS) with nanosecond drive laser pulses and hybrid mode X-ray probe pulses. We observe a thermal decay due to laser-induced heat diffusion in a Germanium single crystal which matches the theoretical prediction. The single pulse DFXM imaging in combination with the laser-pump X-ray probe method could reveal thermal strain formation and propagation of the acoustic wave "on-the-fly" generated by a laser-induced lattice deformation. This will open a new avenue of materials research on laser-in…
Pump-probe microscopy of melanin in tumors has been proposed to improve diagnosis of malignant melanoma, based on the hypothesis that aggressive cancers disaggregate melanin structure. However, measured signals of melanin are complex superpositions of multiple nonlinear processes, which makes interpretation challenging. Polarization control during measurement and data fitting is used to decompose signals of melanin into their underlying molecular mechanisms. We then identify the molecular mechanisms that are most susceptible to melanin disaggregation and derive false-coloring schemes to highli…
In this paper we describe the technical implementation of pump-probe cathodoluminescence microscopy (PP-CL), a novel technique for studying ultrafast dynamics in materials using combined excitation of electron and laser pulses. The PP-CL setup is based on a commercial scanning electron microscope combined with a femtosecond laser. Here we discuss the design, technical details, and characterization of the PP-CL setup. The luminescence emitted by the sample (either photoluminescence, cathodoluminescence or a combination of both) can be analyzed in terms of spectrum, temporal statistics, and freq…
Photoinduced carrier dynamics of nanostructures play a crucial role in developing novel functionalities in advanced materials. Optical pump-probe scanning tunneling microscopy (OPP-STM) represents distinctive capabilities of real-space imaging of such carrier dynamics with nanoscale spatial resolution. However, combining the advanced technology of ultrafast pulsed lasers with STM for stable time-resolved measurements has remained challenging. The recent OPP-STM system, whose laser-pulse timing is electrically controlled by external triggers, has significantly simplified this combination but li…
We present a simple method and its experimental implementation to completely determine the characteristics of the pump-and-probe pulse and the Stokes pulse in a coherent anti-Stokes Raman scattering microscope at sample level without additional autocorrelators. Our approach exploits the delay line, ubiquitous in such microscopes, to perform a convolution of the pump-and-probe and Stokes pulses as a function of their relative delay and it is based on the detection of the photons emitted from an appropriate non-linear sample. The analysis of the non-resonant four-wave-mixing and sum-frequency-ge…
Spatiotemporal dynamics of excitons in isolated semiconducting single-walled carbon nanotubes are studied using transient absorption microscopy. Differential reflection and transmission of an 810-nm probe pulse after excitation by a 750-nm pump pulse are measured. We observe a bi-exponentially decaying signal with a fast time constant of 0.66 ps and a slower time constant of 2.8 ps. Both constants are independent of the pump fluence. By spatially and temporally resolving the differential reflection, we are able to observe a diffusion of excitons, and measure a diffusion coefficient of 200 cm2/…
Phase-contrast microscopy converts the optical phase introduced by transparent, unlabeled specimens into modulation in the intensity image. Modern phase imaging techniques are capable of quantifying phase shift at each point in the field of view, enabling non-destructive applications in materials and life sciences. However, these attractive features come with the lack of molecular information. To fulfill this gap, we developed a bond-selective transient phase (BSTP) microscope using infrared absorption to excite molecular vibration, resulting in an optical phase change detected through a custo…
We propose the use of the subwavelength localization via adiabatic passage technique for fluorescence microscopy with nanoscale resolution in the far field. This technique uses a Λ-type medium coherently coupled to two laser pulses: the pump, with a node in its spatial profile, and the Stokes. The population of the Λ system is adiabatically transferred from one ground state to the other except at the node position, yielding a narrow population peak. This coherent localization allows fluorescence imaging with nanometer lateral resolution. We derive an analytical expression to asses the resoluti…
A recently introduced two-channel confocal microscope with correlated detection promises up to 50% improvement in transverse spatial resolution [Simon, Sergienko, Optics Express {\bf 18}, 9765 (2010)] via the use of photon correlations. Here we achieve similar results in a different manner, introducing a triple-confocal correlated microscope which exploits the correlations present in optical parametric amplifiers. It is based on tight focusing of pump radiation onto a thin sample positioned in front of a nonlinear crystal, followed by coincidence detection of signal and idler photons, each foc…
Watching the motion of electrons on their natural nanometre length- and femtosecond time scales is a fundamental goal and an open challenge of contemporary ultrafast science. Optical techniques and electron microscopy currently mostly provide either ultrahigh temporal or spatial resolution, yet, microscopy techniques with combined space-time resolution need further development. Here we create an ultrafast electron source by plasmon nanofocusing on a sharp gold taper and implement this source in an ultrafast point-projection electron microscope. This source is used, in an optical pump - electro…
Raman spectroscopy is one of the key techniques in the study of vibrational modes and molecular structures. In Coherent Anti-Stokes Raman Scattering (CARS) spectroscopy, a molecular vibrational spectrum is resolved via the third-order nonlinear interaction of pump, Stokes and probe photons, typically using a complex experimental setup with multiple beams and laser sources. Although CARS has become a widespread technique for label-free chemical imaging and detection of contaminants, its multi-source, multi-beam experimental implementation is challenging. In this work we present a simple and eas…
We demonstrate an approach for background-free three-dimensional imaging of director fields in liquid crystals using stimulated Raman scattering microscopy. This imaging technique is implemented using a single femtosecond pulsed laser and a photonic crystal fiber, providing Stokes and pump frequencies needed to access Raman shifts of different chemical bonds of molecules and allowing for chemically selective and broadband imaging of both pristine liquid crystals and composite materials. Using examples of model three-dimensional structures of director fields, we show that the described techniqu…
The resonant buildup of light within optical microcavities elevates the radiation pressure which mediates coupling of optical modes to the mechanical modes of a microcavity. Above a certain threshold pump power, regenerative mechanical oscillation occurs causing oscillation of certain mechanical eigenmodes. Here, we present a methodology to spatially image the micro-mechanical resonances of a toroid microcavity using a scanning probe technique. The method relies on recording the induced frequency shift of the mechanical eigenmode when in contact with a scanning probe tip. The method is passive…
We report on a quasi-nondegenerate pump-probe technique that is based on spectral-filtration of femtosecond laser pulses by a pair of mutually-spectrally-disjunctive interference filters. This cost- and space-efficient approach can be used even in pump-probe microscopy where collinear propagation of pump and probe pulses is dictated by utilization of a microscopic objective. This technique solves the contradictory requirements on an efficient removal of pump photons from the probe beam, to achieve a good signal-to-noise ratio, simultaneously with a needed spectral proximity of the excitation a…
We propose and theoretically analyze a new vibrational spectroscopy, termed electron- and light-induced stimulated Raman (ELISR) scattering, that combines the high spatial resolution of electron microscopy with the molecular sensitivity of surface-enhanced Raman spectroscopy. With ELISR, electron-beam excitation of plasmonic nanoparticles is utilized as a spectrally-broadband but spatially-confined Stokes beam in the presence of a diffraction-limited pump laser. To characterize this technique, we develop a numerical model and conduct full-field electromagnetic simulations to investigate two di…
We report on a combined photoluminescence imaging and atomic force microscopy study of single, isolated self-assembled InAs quantum dots (density <0.01 um^(-2) capped by a 95 nm GaAs layer, and emitting around 950 nm. By combining optical and scanning probe characterization techniques, we determine the position of single quantum dots with respect to comparatively large (100 nm to 1000 nm in-plane dimension) topographic features. We find that quantum dots often appear (>25% of the time) in the vicinity of these features, but generally do not exhibit significant differences in their non-resonant…
Energy carrier evolution is crucial for material performance. Ultrafast microscopy has been widely applied to visualize the spatiotemporal evolution of energy carriers. However, direct imaging of small amounts of energy carriers on nanoscale remains difficult due to extremely weak transient signals. Here we present a method for ultrasensitive and high-throughput imaging of energy carrier evolution in space and time. This method combines femtosecond pump-probe techniques with interferometric scattering microscopy (iSCAT), named Femto-iSCAT. The interferometric principle and unique spatially-mod…
