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We present here the control and measurement of temperature rise using femtosecond optical tweezers at near infrared (NIR) region. Based on our theoretical development, we have designed our experimental techniques. The high temporal sensitivity of position autocorrelation and equipartition theorem is simultaneously applied to elucidate temperature control and high precision measurement around focal volume. Experimentally we have made the benign NIR wavelength to induce local heating by adding very low fluorescent dye molecule with low average power. Local temperature control in aqueous solution exciting within optically absorbing window of the low quantum yield molecules can be possible due to non-radiative relaxation via thermal emission. The stochastic nature of Brownian particle has enough information of its surroundings. We have mapped the nano-dimension beam waist environment by probing the fluctuation of trapped particle. We have observed up to 30K temperature rise from room temperature at sub micro molar concentration. The gradient of temperature is as sharp as the fluence of pulsed laser focused by high numerical aperture objective. Thus, pulsed laser radiation always allows finer surgical techniques involving minimal thermal injuries. Our new techniques with multiphoton absorbing non-fluorescent dye can further be used to selective phototherapeutic diagnosis of cancer cells due to peak power dependent nonlinear phenomenon (NLO).

We present the effects of wavelength dependent temperature rise in a femtosecond optical tweezers. Our experiments involve the femtosecond trapping laser tunable from 740-820 nm at low power 25 mW to cause heating in the trapped volume within a homogeneous solution of sub micro-molar concentration of IR dye. The 780 nm high repetition rate laser acts as a resonant excitation source which helps to create the local heating effortlessly within the trapping volume. We have used both position autocorrelation and equipartion theorem to evaluate temperature at different wavelength having different absorption coefficient. Fixing the pulse width in the temporal domain gives constant bandwidth at spatial domain, which makes our system behave as a tunable temperature rise device with high precision. This observation leads us to calculate temperature as well as viscosity within the vicinity of the trapping zone. A mutual energy transfer occurs between the trapped bead and solvents that leads to transfer the thermal energy of solvents into the kinetic energy of the trap bead and vice-versa. Thus hot solvated molecules resulting from resonant and near resonant excitation of trapping wavelength can continuously dissipate heat to the trapped bead which will be reflected on frequency spectrum of Brownian noise exhibited by the bead. Temperature rise near the trapping zone can significantly change the viscosity of the medium. We observe temperature rise profile according to its Gaussian shaped absorption spectrum with different wavelength.

We present cumulative perturbation effects of femtosecond laser pulses on an optical tweezer. Our experiments involve a dual wavelength high repetition rate femtosecond laser, one at the non-heating wavelength of 780 nm while the other at 1560 nm to cause heating in the trapped volume under low power (100-800 μW) conditions. The 1560 nm high repetition rate laser acts as a resonant excitation source for the vibrational combination band of the hydroxyl group (OH) of water, which helps create the local heating effortlessly within the trapping volume. With such an experimental system, we are the first to observe direct effect of temperature on the corner frequency deduced from power spectrum. We can, thus, control and measure temperature precisely at the optical trap. This observation has lead us to calculate viscosity as well as temperature in the vicinity of the trapping zone. These experimental results also support the well-known fact that the nature of Brownian motion is the response of the optically trapped bead from the temperature change of surroundings. Temperature rise near the trapping zone can significantly change the viscosity of the medium. However, we notice that though the temperature and viscosity are changing as per our corner frequency calculations, the trap stiffness remains the same throughout our experiments within the temperature range of about 20 K.

Importance of various measurement schemes in studying thermal lens (TL) signal for laser based TL experiments is explored. We show that two different measurement schemes can result in two contrasting outcomes. In one experiment, two measurement schemes show diverging results for TL signal measurements, which gives a convoluted result and in the other experiment, the two measurement schemes give a converging result.

Using femtosecond time resolved degenerate pump-probe mass spectrometry coupled with simple linearly chirped frequency modulated pulse, we elucidate that the dynamics of retro-Diels-Alder-like reaction of diclopentadiene (DCPD) to cyclopentadiene (CPD) in supersonic molecular beam occurs in ultrafast time scale. Negatively chirped pulse enhances the ion yield of CPD, as compared to positively chirped pulse. This indicates that by changing the frequency (chirp) of the laser pulse we can control the ion yield of a chemical reaction.

We present a clever design concept of using femtosecond laser pulses in microscopy by selective excitation or de-excitation of one fluorophore over the other overlapping one. Using either a simple pair of femtosecond pulses with variable delay or using a train of laser pulses at 20-50 Giga-Hertz excitation, we show controlled fluorescence excitation or suppression of one of the fluorophores with respect to the other through wave-packet interference, an effect that prevails even after the fluorophore coherence timescale. Such an approach can be used both under the single-photon excitation as well as in the multi-photon excitation conditions resulting in effective higher spatial resolution. Such high spatial resolution advantage with broadband-pulsed excitation is of immense benefit to multi-photon microscopy and can also be an effective detection scheme for trapped nanoparticles with near-infrared light. Such sub-diffraction limit trapping of nanoparticles is challenging and a two-photon fluorescence diagnostics allows a direct observation of a single nanoparticle in a femtosecond high-repetition rate laser trap, which promises new directions to spectroscopy at the single molecule level in solution. The gigantic peak power of femtosecond laser pulses at high repetition rate, even at low average powers, provide huge instantaneous gradient force that most effectively result in a stable optical trap for spatial control at sub-diffraction limit. Such studies have also enabled us to explore simultaneous control of internal and external degrees of freedom that require coupling of various control parameters to result in spatiotemporal control, which promises to be a versatile tool for the microscopic world.