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Khadga J. Karki

Publications and source records attributed to Khadga J. Karki.

5 recordsLinked to original sources

Decoding phase and time-dependent interferograms of high-order harmonics

Interferometric measurements of high-harmonics induced by multiple laser fields in an emerging field of research that promises optimized yield of harmonics, and time and space-resolved nonlinear spectroscopy. Most of the measurements have been done by controlling the time-delay between the pulses. Here, we show that by changing one additional parameter, i.e. the phase-difference between the fields, together with the time-delay, one can, on the one hand, enhance the harmonic yield and, on the other hand, obtain in-depth information about the physical mechanisms that control the electron trajectories contributing to the high-harmonic generation. The two-dimensional interferograms obtained from such investigations can be used to find the values of time-delay and phase between the laser fields that maximize the yield of a particular harmonic. Results show that maximum yields of certain harmonics can be orders of magnitude larger than when using a single field or two fields with zero time-delay and phase difference. Our high-harmonics two-dimensional interferograms-based method paves the way for a simpler analysis of the attosecond electron dynamics in complex molecules and solids.

physics.optics↗

Unexpectedly large delocalization of the initial excitation in photosynthetic light harvesting

Electronic 2D spectroscopy allows nontrivial quantum effects in chemistry and biology to be explored in unprecedented detail. Here, we apply recently developed fluorescence detected coherent 2D spectroscopy to study the light harvesting antenna 2 (LH2) of photosynthetic purple bacteria. The method utilizes the destructive interference between two signal components thereby uncovering cross peaks which are not visible in conventional photon-echo based 2D and transient absorption measurements. Analyses of signal generating quantum pathways leads to the conclusion that, contrary to the currently prevailing physical picture, the two weakly-coupled pigment rings of LH2 share the initial electronic excitation leading to quantum mechanical correlation between the two clearly separate bands. These results are general and have consequences for the interpretation of excited states not only in photosynthesis but in all light absorbing systems. The initial delocalization could be the key for enhancing the light harvesting efficiency via biased motion towards the energy funnel.

physics.chem-ph↗

Optimization Schemes for Efficient Multiple Exciton Generation and Extraction in Colloidal Quantum Dots

Multiple exciton generation is a process in which more than one electron hole pair is generated per absorbed photon. It allows us to increase the efficiency of solar energy harvesting. Experimental studies have shown the multiple exciton generation yield of 1.2 in isolated colloidal quantum dots. However real photoelectric devices require the extraction of electron hole pairs to electric contacts. We provide a systematic study of the corresponding quantum coherent processes including extraction and injection and show that a proper design of extraction and injection rates enhances the yield significantly up to values around 1.6.

cond-mat.mes-hall↗

High Precision Measurements Using High Frequency Signals

Generalized lock-in amplifiers use digital cavities with Q-factors as high as 5X10^8. In this letter, we show that generalized lock-in amplifiers can be used to analyze microwave (giga-hertz) signals with a precision of few tens of hertz. We propose that the physical changes in the medium of propagation can be measured precisely by the ultra-high precision measurement of the signal. We provide evidence to our proposition by verifying the Newton's law of cooling by measuring the effect of change in temperature on the phase and amplitude of the signals propagating through two calibrated cables. The technique could be used to precisely measure different physical properties of the propagation medium, for example length, resistance, etc. Real time implementation of the technique can open up new methodologies of in-situ virtual metrology in material design.

physics.ins-det↗

Multiple exciton generation in nano-crystals revisited: Consistent calculation of the yield based on pump-probe spectroscopy

Multiple exciton generation (MEG) is a process in which more than one exciton is generated upon the absorption of a high energy photon, typically higher than two times the band gap, in semiconductor nanocrystals. It can be observed experimentally using time resolved spectroscopy such as the transient absorption measurements. Quantification of the MEG yield is usu- ally done by assuming that the bi-exciton signal is twice the signal from a single exciton. Herein we show that this assumption is not always justified and may lead to significant errors in the estimated MEG yields. We develop a methodology to determine proper scaling factors to the signals from the transient absorption experiments. Using the methodology we find modest MEG yields in lead chalcogenide nanocrystals including the nanorods.

physics.chem-ph↗