V. Dobrovitski, L. 2 Magnetic resonance experiments ...

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Magnetic resonance experiments:

Standard experimental settings and theoretical concepts

Almost all modern approaches to dynamics and control of spins

and qubits are based on magnetic resonance-type settings.

𝐡𝑄

πœ”πΏ

Single spin or ensemble of spins in a strong magnetic field 𝐡𝑄

β€œQuantizing field” – determines

primary quantization axis(why β€œprimary”? Will see shortly)

Induces Larmor precession with the

frequency πœ”0

𝐻 = πœ”πΏ 𝑆𝑧 +𝐻′

Informally we say that 𝐻′ β‰ͺ πœ”πΏ , i.e. typical energies of 𝐻′ are much

smaller than πœ”πΏ. But it is 𝐻′ that is usually of most interest.

V. Dobrovitski, L. 2

How do we excite (β€œdrive”) spin dynamics?

xy

Rotating frame

S

Spin Oscillating field

co-rotating

(resonant)

counter-rotating

(negligible)

Pointer states | ۧ↑ and | ۧ↓ . How do we make spins move?

Oscillating field h along X, frequency πœ”πΏ – performs rotations.

Drives spins out of equilibrium state. How?

β„Žπ‘₯ 𝑑 = 2β„Ž cosπœ”πΏπ‘‘

𝐡𝑄

πœ”πΏ

Key concept: Rotating frame

πœ”πΏ πœ”πΏ πœ”πΏ

V. Dobrovitski, L. 2

Rabi oscillations and rotating frame

𝐻 = πœ”πΏ 𝑆𝑧 + β„Žπ‘₯ 𝑑 𝑆π‘₯ = πœ”πΏ 𝑆𝑧 + 2β„Ž 𝑆π‘₯ cos(πœ”π‘‘ + 𝛼)

We are interested only in dynamics at frequencies close to πœ”πΏ

Driving at the frequency πœ” close to πœ”πΏ : πœ” βˆ’ πœ”πΏ β‰ͺ πœ”πΏ , β„Ž β‰ͺ πœ”πΏ

Rotating frame transformation: π‘Š = exp(βˆ’π‘–πœ”π‘‘ 𝑆𝑧)Rotation with frequency πœ” (not πœ”πΏ!) around the Z-axis

π‘ˆ 𝑑 = π‘Š βˆ™ π‘ˆπ‘…(𝑑) , π‘ˆπ‘… 𝑑 – ev.op. in the rotating frame

𝑖 αˆΆπ‘ˆ = 𝐻 π‘ˆ 𝑑 β‡’ 𝑖 αˆΆπ‘ˆπ‘… = π‘Šβ€ π»π‘Š βˆ’πœ” 𝑆𝑧 π‘ˆπ‘… =

= πœ”πΏ βˆ’ πœ” 𝑆𝑧 + 2β„Ž cos(πœ”π‘‘ + 𝛼) eπ‘–πœ”π‘‘π‘†π‘§ 𝑆π‘₯ eβˆ’π‘–πœ”π‘‘π‘†π‘§ π‘ˆπ‘… =

= πœ”πΏ βˆ’ πœ” 𝑆𝑧 + β„Ž 𝑆π‘₯ cos 𝛼 + 𝑆𝑦 sin 𝛼 + {nonsec. terms} π‘ˆπ‘…

Secular Hamiltonian : 𝐻𝑅 = πœ”πΏ βˆ’ πœ” 𝑆𝑧 + β„Ž 𝑆π‘₯ cos 𝛼 + 𝑆𝑦 sin 𝛼

V. Dobrovitski, L. 2

Rabi oscillations and rotating frame

Isidor Rabi [Rah-bee], Nobel prize 1944

Weak β„Ž β‰ͺ πœ”πΏ time-dependent driving became strong β„Ž~|πœ”πΏ βˆ’πœ”|and time-independent

Ο‰L

β„Žπ‘₯(𝑑)

πœ”πΏ βˆ’ πœ”

h

Driven spins rotate around 𝑛 , 𝑆𝑧 oscillates: Rabi oscillations.

Labframe:

Rotatingframe:

𝑛lab𝑛

Rotating frame: we transform 𝐻 β†’ 𝐻𝑅 , density matrix 𝜌 β†’ πœŒπ‘… , …

But not the observables!

Different from interaction representation, rotating-wave approx., etc.

1) Inconvenient: time dependence of 𝑆π‘₯,𝑦 , mutual dependence,…

2) Rotating-frame observables are what is actually detected in standard

resonance experiments (I/Q channels)

See e.g. C. P. Slichter, β€œPrinciples of Magnetic Resonance”

V. Dobrovitski, L. 2

Spin driving: qualitative picture

Ideal:𝐻 = πœ”0

αˆ˜π‘†π‘§

| ۧ↑

| Ϋ§β†“πœ”

πœ”0

𝑃 πœ” = 𝛿(πœ” βˆ’ πœ”0)Single

sharp line

Noise:𝐻 = πœ” αˆ˜π‘†π‘§

| ۧ↑

| Ϋ§β†“πœ”

πœ”0

𝑃 πœ”

πœ”

β„Ž

Spins resonant

with driving

Broadened line,

determined by

𝑃 𝛽

Strong

driving:

πœ”

β„Ž

Weak

driving:

Spins resonant

with driving

V. Dobrovitski, L. 2

Rabi oscillations: strong driving

πœ”πΏ βˆ’ πœ”

h

Rotating frame:

𝑛 𝐻 = 𝐡 𝑆𝑧 + β„Ž 𝑆π‘₯ with 𝐡 = πœ”πΏ βˆ’ πœ”

How do we take noise into account ?

Weak non-resonant fields (πœ”β€², 𝐡′) : |πœ”0 βˆ’πœ”β€²| ≫ 𝐡′

If directed along X- and Y-axes: non-secular, neglect

V. Dobrovitski, L. 2

Therefore, only static noise along Z-axis matters: 𝐡 = 𝐡0 + 𝛽

πœ”πΏ = πœ”0 + 𝛽 , e.g. 𝑃 𝛽 =1

2πœ‹π‘2exp βˆ’

𝛽2

2𝑏2

Consider quasi-static noise: inhomogeneous broadening

This is precisely what we studied in the previous lecture

Rabi oscillations: strong driving

Strong off-resonant driving: β„Ž, 𝐡0 ≫ 𝑏

Initial state decays towards equilibrium (pointer) states

Pointer states – already analyzed earlier in detail

Decay of all components has Gaussian form, decay time 𝑇2βˆ—:

𝑇2βˆ— = π‘βˆ’1 for 𝐡0 ≫ β„Ž

𝑇2βˆ— = π‘βˆ’1 βˆ™ β„Ž/𝐡0 for 𝐡0 β‰ͺ β„Ž

V. Dobrovitski, L. 2

πœ”πΏ βˆ’ πœ”

h

Rotating frame: 𝑛

𝐻 = 𝐡 𝑆𝑧 + β„Ž 𝑆π‘₯ ,

𝐡 = πœ”πΏ βˆ’ πœ”

𝑃 𝛽

Any questions? Hint: 𝑇2βˆ— = π‘βˆ’1 β„Ž/𝐡0 for 𝐡0 β‰ͺ β„Ž. What about 𝐡0 = 0?

Rabi oscillations, strong driving

For 𝐡0 = 0 :

First order in 𝛽 is gone, but there is second:

Ξ© = Ξ©0 + 𝐡0 βˆ™ ΀𝛽 Ξ©0 + Ξ€β„Ž2 2Ξ©0 βˆ™ ΀𝛽 Ξ©02 +β‹―

Ξ© = 𝐡2 + β„Ž2 ≑ 𝛽2 + β„Ž2 β‰ˆ β„Ž + ΀𝛽2 2β„Ž

πœ‘ β‰ˆ β„Žπ‘‘ + ΀𝑑 𝛽2 2β„Ž

ࢱ𝑃 𝛽 𝑑𝛽 e𝑖𝑑𝛽2/(2β„Ž) = 1

2πœ‹π‘2ΰΆ±e𝑖

𝑑𝛽2

2β„Ž eβˆ’

𝛽2

2𝑏2 𝑑𝛽 = 1 βˆ’ 𝑖 𝑏2𝑑2β„Ž

βˆ’1/2=

= π‘Ÿ(𝑑) βˆ™ eπ‘–πœ‡(𝑑) , with π‘Ÿ = 1 + 𝑏2𝑑

2β„Ž

2 βˆ’1/4

and πœ‡ = 1

2tanβˆ’1

𝑏2𝑑

2β„Ž

Strong resonant driving: 𝐡0 = 0 , β„Ž ≫ 𝑏

Resonant: πœ” = πœ”0 , i.e. exactly at resonance with the line center

Spectroscopic language: driving saturates the line

The integral which determines the form of decay:

V. Dobrovitski, L. 2

Initial decay at 𝑑 β‰ͺ β„Ž/𝑏2 :

quadratic, π‘Ÿ 𝑑 β‰ˆ 1 βˆ’ 𝐴𝑑2 , with linearly changing phase πœ‡(𝑑), i.e.

Rabi frequency is renormalized by ΀𝑏2 (2β„Ž).Looks like regular Gaussian, but…

Long-time decay at 𝑑 ≫ β„Ž/𝑏2 :

extremely slow power-law decay, π‘Ÿ(𝑑) ∝ π‘‘βˆ’1/2 with πœ‡ β‰ˆ πœ‹/4

where

πœ— = β„Žπ‘‘ + πœ‡(𝑑)

αˆ˜π‘†π‘₯ 𝑑 = αˆ˜π‘†π‘₯ (constant in time),

αˆ˜π‘†π‘§ 𝑑 = π‘Ÿ 𝑑 αˆ˜π‘†π‘§ cos πœ— + αˆ˜π‘†π‘¦ sin πœ—

αˆ˜π‘†π‘¦ 𝑑 = π‘Ÿ 𝑑 αˆ˜π‘†π‘¦ cos πœ— βˆ’ αˆ˜π‘†π‘§ sin πœ—

All operators are understood as averaged over the noise, the symbol … 𝛽 omitted

Rabi oscillations, strong resonant driving

Leading order in 𝑏/β„Ž β‰ͺ 1 : decaying rotation around X-axis

Explicit

results:

V. Dobrovitski, L. 2

Rabi oscillations, strong resonant driving

Leading order in 𝑏/β„Ž β‰ͺ 1 : quantization axis 𝑛 along X-axis

Note 1: this is in the rotating frame! In the lab frame the quantization

axis is precessing around the Z-axis, and the pointer states have

explicit time dependence.

Recall the comments from the previous lecture: pointer states can

depend on time.

Note 2: we have quasi-equilibriuim (pointer) states along the

rotating-frame X axis: 12(| ۧ↑ Β± | ۧ↓ )

Same idea is used in quantum optics: the concept of β€œdressed states”.

Atomic states change under strong optical driving, become an equal-

weight superposition of | ۧ𝑔 and | ۧ𝑒 .

But the theory is more complex: quantum photons instead of classical

driving field, account of spontaneous decay, etc.

V. Dobrovitski, L. 2

Transition from resonant to non-resonant regime occurs when first

and second orders are similar: 𝐡0 βˆ™ ΀𝛽 Ξ©0 ~ Ξ€β„Ž2 2Ξ©0 βˆ™ ΀𝛽 Ξ©02

In this case 𝐡0 is small, and the transition occurs when 𝐡0~𝑏

Strong driving changes the oscillation frequency of 𝑆π‘₯,𝑦 :

from 𝐡0 to Ξ©0 = 𝐡02 + β„Ž2 β‰ˆ 𝐡0 + β„Ž2/(2𝐡0)

Similar phenomenon in quantum optics: ac Stark shift of atomic

levels under strong optical driving

The power-law decay π‘‘βˆ’1/2 has no well-defined lifetime(formally, Rabi rotations in this regime have infinitely long lifetime)

Jumping ahead: cw spectroscopy would show two lines, split by β„ŽThese lines are narrow: Fourier transform of π‘‘βˆ’1/2 is πœ”βˆ’1/2

(formally, infinitely narrow)

Similar phenomenon in quantum optics: Autler-Townes splitting

Rabi oscillations, strong driving: comments

V. Dobrovitski, L. 2

Rabi oscillations: weak driving

Strong driving, weak noise (β„Ž ≫ 𝑏) : driving saturates the line

Weak driving: the regime of continuous-wave (cw) spectroscopy

V. Dobrovitski, L. 2

πœ”

β„Ž

Spins resonant

with driving

Strong

driving:

πœ”

β„Ž

Weak

driving:

Spins resonant

with driving

Typical initial state: along Z-axis, with 𝑆π‘₯(0) = 𝑆𝑦(0) = 0

𝑆𝑧 𝑑 = 𝑆𝑧0 βˆ™ 1 βˆ’ 2 𝑛π‘₯

2 sin2 Ξ€πœ‘ 2

πœ‘ = Ω𝑑 , Ξ© = β„Ž2 + 𝐡2 , 𝑛π‘₯ = β„Ž/Ξ©

Driving at frequency πœ” : can use previous results

Rabi oscillations: weak driving

𝑆𝑧(𝑑) = 𝑆𝑧(0) βˆ™ 1 βˆ’ β„Ž2 𝑃 𝛽 𝑑𝛽 βˆ™ 2sin2

𝑑

2β„Ž2+𝛽2

β„Ž2+𝛽2

We focus on β€œperturbative long” times: β„Žπ‘‘ β‰ͺ 1, but 𝑏𝑑 ≫ 1

Consider general line shape 𝑃(𝛽) with characteristic width 𝑏

𝑃 𝛽 is assumed to vary smoothly with 𝛽, on a scale 𝛽~𝑏

In contrast, 2sin2

𝑑

2β„Ž2+𝛽2

β„Ž2+𝛽2at large 𝑑 (but small β„Žπ‘‘!) has a

sharp peak of small width (∝ π‘‘βˆ’1) and large height (∝ 𝑑) at 𝛽 = 0;

decays fast as |𝛽| grows.

V. Dobrovitski, L. 2

If you have a dΓ©jΓ  vu feeling – you are right.

This is just standard time-dependent perturbation theory,

derivation of the Fermi Golden Rule

If you want more mathematical clarity (optional).

Important: 𝑃(𝛽) is dimensional quantity, with dimensionality [rad/s]βˆ’1

Because 𝑃 𝛽 𝑑𝛽 = 1 , and 𝑑𝛽 = 𝛽 =rad

s

Thus, 𝑝 π‘₯ = 𝑏 βˆ™ 𝑃(𝑏π‘₯) and 𝑝 π‘₯ 𝑑π‘₯ = 𝑃 𝛽 𝑑𝛽

1) Set β„Žπ‘‘ = 0 for convenience: this just means that we are working in the leading

order w.r.t. the small parameter β„Žπ‘‘. We should study 𝐼 = 𝑃 𝛽sin2 𝛽𝑑/2

𝛽2𝑑𝛽.

2) 𝑃(𝛽) has a typical scale 𝑏: means that it depends on dimensionless quantity

π‘₯ = 𝛽/𝑏, and there are no other parameters in this function, large or small.

So we re-write 𝐼 = 𝑃 𝛽sin2 𝛽𝑑/2

𝛽2𝑑𝛽 = 𝑝 π‘₯

sin2 π‘₯βˆ™π‘π‘‘/2

(π‘₯βˆ™π‘)2𝑑π‘₯

3) Use large dimensionless parameter πœƒ = 𝑏𝑑, consider πœƒ β†’ ∞.

𝐼 = 𝑝 π‘₯sin2 π‘₯βˆ™π‘π‘‘/2

(π‘₯βˆ™π‘)2𝑑π‘₯ =

𝑑

π‘βˆ™ 𝑝 π‘₯

sin2 πœƒβˆ™π‘₯/2

πœƒβˆ™π‘₯2𝑑π‘₯ , and ΀𝑑 𝑏 is a parameter

(it is dimensional, so it is neither small nor large – just a quantity)

4) Can show: 𝑔 π‘₯ = 2sin2 πœƒβˆ™π‘₯/2

πœƒβˆ™π‘₯2=

1βˆ’cos πœƒπ‘₯

πœƒπ‘₯2β†’ πœ‹ βˆ™ 𝛿(π‘₯) when πœƒ β†’ ∞

Consider the integral 𝐼 at πœƒ β†’ ∞, extend it to complex plane, calculate the residue at π‘₯ = 0.

Get the answer 𝐼 = πœ‹ ΀𝑑 𝑏 βˆ™ 𝑝 0 = πœ‹π‘‘ βˆ™ 𝑃(0)

Note: condition 𝑏𝑑 ≫ 1 is the key here; β„Žπ‘‘ β‰ͺ 1 is not crucial, can set β„Žπ‘‘ = 0

V. Dobrovitski, L. 2

𝑆𝑧(𝑑) = 𝑆𝑧(0) βˆ™ [1 βˆ’ πœ‹ β„Ž2𝑑 𝑃(0)]

Weak driving and cw spectroscopy

So we obtain:

Physical meaning? Initially, the spin is along quantizing field

Start driving it, 𝑆𝑧 decreases: spin flipped, energy absorbed.

Absorbed power π‘Š ∝ ΀𝑑 𝑆𝑧 𝑑𝑑

Measuring absorption while continuously driving spins at

frequency πœ” directly measures the line shape 𝑃(πœ”)

𝑑 𝑆𝑧𝑑𝑑

= βˆ’πœ‹β„Ž2𝑃(0) or, in the lab frame:𝑑 𝑆𝑧𝑑𝑑

∝ 𝑃(πœ”)

πœ”

β„ŽContinuous-wave (cw) spectroscopy

𝑏

𝑃(πœ”)

This is for 𝑑 β‰ͺ 1/β„Ž . What happens later, when β„Žπ‘‘~1 ?

V. Dobrovitski, L. 2

Most basic characterization of noise and

relaxation.NMR, ESR, optics, IR,… – idea is the same

V. Dobrovitski, L. 2

Weak driving and cw spectroscopy

Energy absorbed – from where? From the cw driving field

𝐻 𝑑 = Ԧ𝑒π‘₯ βˆ™ 2β„Ž cos(πœ”π‘‘ + 𝛼)

Absorbed power, average per oscillation period: π‘Š = βˆ’π‘€ βˆ™ ΀𝑑𝐻 𝑑𝑑I.e., there must be non-zero components 𝑆π‘₯(𝑑) and 𝑆𝑦(𝑑)

More detailed theory is needed, will discuss later (Bloch-Redfield)

Our system : ensemble of non-interacting energy-conserving spins

Initially absorb energy as described, but this cannot go on forever

Equlibrium state is not well defined. Spins keep precessing,

unhindered perpetual rotation: energy flows back and forth.

There must be some process that β€œresets” 𝑆𝑧(𝑑)

It could be slow fluctuations of 𝛽, interaction between spins, coupling to

environment, … The same problem as in standard statistical physics: origins of

stochasticity, thermalization, etc.

Serious problems with the current treatment

V. Dobrovitski, L. 2

Phenomenological Bloch equations

Phenomenological approach: there must be some relaxation process

that continually resets the spins and steers them to equilibrium.

Postulate that such a process is linear and memoryless, so the

system’s relaxation towards equilibrium (without driving) :

𝑑𝑀𝑧

𝑑𝑑= βˆ’

1

𝑇1(π‘€π‘§βˆ’π‘€π‘§

0)𝑑𝑀π‘₯,𝑦

𝑑𝑑= βˆ’

1

𝑇2𝑀π‘₯,𝑦

Relaxation time 𝑇1 – rate of longitudinal relaxation

Relaxation of the energy of spins in the quantizing field along Z.

How fast is the energy brought to or taken away from spins.

𝑀𝑧0 – equilibrium magnetization along the quantizing field

Relaxation time 𝑇2β€² – transverse relaxation. Does not involve energy

exchange, purely internal spin relaxation (e.g. spin-spin coupling)

1

𝑇2=

1

2𝑇1+

1

𝑇2β€² i.e. 𝑇2 ≀ 2𝑇1 – to ensure correctness

V. Dobrovitski, L. 2

Phenomenological Bloch equations

Example:

two-level system

(e.g. spin 1/2)

| Ϋ§π‘Ž

| ۧ𝑏

Ξ“π‘π‘Ž Ξ“π‘Žπ‘π‘‘

𝑑𝑑

π‘π‘Žπ‘π‘

=βˆ’Ξ“π‘Žπ‘ Ξ“π‘Žπ‘Ξ“π‘Žπ‘ Ξ“π‘Žπ‘

π‘π‘Žπ‘π‘

Rate equation:

Gives Bloch equation for 𝑀𝑧. But may not work for more levels!

Depends on rates, things may get complicated.

But the main idea holds: equilibrium requires equilibration mechanism

| ۧ↑

| Ϋ§β†“πœ”

𝑃 πœ” | ۧ↑

| ۧ↓

Many lines

of zero

width

Many lines

of width 𝑇1βˆ’1

Simple spectroscopy (FT or cw) gives 𝑃 πœ” but often does not

say much about individual lines:

In general, response to driving depends on 𝑏, β„Ž, 𝑇1, line shape,…

Gives rise to many useful effects (hole burning, spin echo,…)

A few notes on NMR/ESR experimental settings

Large quantizing field 𝐡0, much larger than any other relevant

energy scale. But still π‘”πœ‡π΅π΅0 β‰ͺβ‰ͺ π‘˜π‘‡, so the initial state is:

𝜌 β‰ˆ1

𝑍exp βˆ’

π‘”πœ‡π΅π΅0 𝑆𝑧

π‘˜π‘‡β‰ˆ

1

𝑍1 βˆ’ πœ–π‘†π‘§ , i.e. 𝜌relevant ∝ 𝑆𝑧

The signal from πœŒβ€² = 1 is zero: this part of density matrix contributes

only to noise.

Irrelevant for the signal, important for analyzing signal-to-noise ratio.

because the identity part of the density matrix is not affected much.

V. Dobrovitski, L. 2

Dynamics in relevant experiments mostly unitary: π‘ˆ 1 π‘ˆβ€  = π‘ˆπ‘ˆβ€  = 1More generally: dynamics in NMR experiments is mostly unital,

i.e. maps 1 β†’ 1

Also, other ways to initialize spins are used more and more often:

optical (e.g. NV centers), dynamic nuclear polarization (DNP), etc.

Often the first step in qubit characterization

0) Qubit is initialized along the Z-axis

1) Apply resonant Rabi driving for a short time, rotate spins from the

Z-axis to the Y-axis (so-called πœ‹/2 pulse).

2) Measure 𝑆π‘₯(𝑑) and 𝑆𝑦 𝑑 : often called free induction decay (FID) (historical reasons: design of traditional NMR experiments)

or free coherence decay, or Ramsey measurement (in modified version)

3) Analyze 𝑓(𝑑): find 𝑇2βˆ— , examine the form of decay, deduce which

noise dephases the qubit and what are its properties.

V. Dobrovitski, L. 2

FT spectroscopy: qubit characterization

Note: We do not have to rotate the spin all the way to Y-axis, it is

enough to just provide non-zero 𝑆π‘₯0 and/or 𝑆𝑦

0 .

The form of decay will be the same, only the overall amplitude of

the signal will scale up or down. Will be important later.

NMR/ESR and the rotating frame: comments

Rotating frame: potential danger from non-seqular terms.

Contribution decreases slowly, as |πœ” βˆ’ πœ”0|βˆ’2. If the spectral

density grows faster – can accumulate and /diverge. Be careful!

Relatively rare in NMR/ESR, but often happens in quantum optics.

NMR experiments: Ξ€πœ” βˆ’ πœ”0 πœ”0~10βˆ’3 βˆ’ 10βˆ’5, measured in

ppm (part per million = 10βˆ’6). Secular approximation in rotating

frame works very well.

But for other spins and qubits more care may be required.

V. Dobrovitski, L. 2

One can apply πœ‹/2 pulse along X- or Y-axis, just by

choosing the phase of driving. Will be important later.

Can use either cw spectroscopy, measuring 𝑃(πœ”), or FT

approach, measuring 𝑓(𝑑). Usually, the two are related via

Fourier transform. But depends on the system (e.g. unusually long

𝑇1 or 𝑇2, so that driving saturates the line)

Beyond rotating-frame secular approximation

Secular approximation is of utter importance: spin motion in a

general time-dependent field is not analytically solvable.

Even computers may be useless: for instance, motion of a spin under driving that is not

ideally periodic (e.g. with another harmonic of incommensurate frequency) can exhibit

deterministic chaos.

What lies beyond secular approximation? Two examples

1. Bloch-Siegert shift

Oscillating field

co-rotating

(resonant)

counter-rotating

(negligible)

πœ”xy

Rotating frameπœ”

Influence of the counter-

rotating component?

Use the counter-rotating

coordinate frame, neglect

the co-rotating component

In this frame: quantizing field 𝐡𝑄 β†’ large positive offset equal to

the Larmor frequency πœ”πΏ

V. Dobrovitski, L. 2

Compare:

Co-rotating frame: 𝐡𝑄 β†’ negative offset πœ”πΏ β†’ 𝐻𝑧 = πœ”πΏ βˆ’πœ” 𝑆𝑧

Counter-rotating frame: 𝐡𝑄 β†’ positive offset πœ”πΏ β†’ 𝐻𝑧′ = πœ”πΏ + πœ” 𝑆𝑧

I.e. in the counter-rotating frame: 𝐻𝐢𝑅 = πœ”πΏ + πœ” 𝑆𝑧 + β„Žπ‘†π‘₯

This Hamiltonian corresponds to precession around β‰ˆ Z-axis

(corrections to the axis are nonsecular, neglect them)

with the frequency

Ω𝐢𝑅 β‰ˆ πœ”πΏ +πœ” + 12 βˆ™ Ξ€β„Ž2 πœ”πΏ +πœ” β‰ˆ πœ”πΏ + πœ” + Ξ€β„Ž2 (4πœ”)

Transform back to the co-rotating frame: this rotation corresponds to

a frequency shift βˆ†πœ” = Ξ€β„Ž2 (4πœ”)

V. Dobrovitski, L. 2

1. The shift is always positive (similar to the β€œeffect of inverted pendulum”)

2. Note the difference with ac Stark shift: Bloch-Siegert shift comes

from the counter-rotating field

2. Sub-harmonic resonances

Main spin resonance: πœ” β‰ˆ πœ”πΏ.

Moreover, spin is a nonlinear system, so there are also resonances at

πœ” β‰ˆ 2πœ”πΏ , 3πœ”πΏ , …

But there are also sub-harmonic resonances at πœ” β‰ˆ 1

3πœ”πΏ ,

1

5πœ”πΏ , …

I.e. spin is not only nonlinear, but also a parametric system

Beyond rotating-frame secular approximation

Suggested projects:

Project 2: sub-harmonic resonances (based on the textbook by A. Abragam,

β€œPrinciples of Nuclear Magnetism”)

Project 1: accurate analysis of the Bloch-Siegert shift(based on the paper of Bloch and Siegert, Phys. Rev. 57, 522 (1940), and on the textbook

by A. Abragam, β€œPrinciples of Nuclear Magnetism”)

Brief summary:

1). Rotating frame, secular approximation. Transformation to the

rotating frame is different from the rotating-wave approximation or

interaction representation.

2). Rotating frame, strong driving: Rabi oscillations.

Pointer states along the total effective field, rotating in the lab frame.

Dephasing time depending on the frequency detuning πœ”πΏ βˆ’πœ”.

3). Strong resonant driving: extremely narrow-line pointer states

along the X-axis, power-law decoherence ∝ π‘‘βˆ’1/2

4). Weak driving: cw spectroscopy, measurement of 𝑃(πœ”)

5). FT spectroscopy: use of pulsed Rabi driving. Measuring coherence

decay 𝑓(𝑑), related to 𝑃(πœ”) via Fourier transform.

6). Need a theory for relaxation. Bloch equations - phenomenological

7). Physics beyond rotating-frame secular theory

V. Dobrovitski, L. 2

V. Dobrovitski, S. 2

𝑑𝑀𝑧

𝑑𝑑= βˆ’

1

𝑇1(π‘€π‘§βˆ’π‘€π‘§

0)𝑑𝑀π‘₯,𝑦

𝑑𝑑= βˆ’

1

𝑇2𝑀π‘₯,𝑦

Bloch equations, weak driving: lineshape

𝑑𝑀𝑧

𝑑𝑑= βˆ’π‘€π‘¦β„Ž βˆ’

1

𝑇1(π‘€π‘§βˆ’π‘€π‘§

0)

With field: add the Landau-Lifshits term αˆΆπ‘€ = 𝑀 Γ— 𝐻

Let us use this phenomenology in the rotating frame:

driving β„Ž along the X-axis, detuning 𝐡 = (πœ”πΏ βˆ’ πœ”) along the Z-axis

𝑑𝑀π‘₯

𝑑𝑑= 𝑀𝑦𝐡 βˆ’

1

𝑇2𝑀π‘₯

𝑑𝑀𝑦

𝑑𝑑= βˆ’π‘€π‘₯𝐡 +π‘€π‘§β„Ž βˆ’

1

𝑇2𝑀𝑦

Qualitative consideration:

driving tilts quantization axis away from Z by small angle (of the order Ξ€β„Ž 𝐡 or β„Žπ‘‡1,2)

𝑀𝑧 βˆ’π‘€π‘§0 is of the second order in this small tilt (cosine of small angle), i.e. of the

order of ( Ξ€β„Ž 𝐡)2 or (β„Žπ‘‡1,2)2. If we look at linear terms in β„Ž, we can take 𝑀𝑧 = 𝑀𝑧

0.

Our goal: consider very weak driving, β„Ž β‰ͺ 𝐡, 𝑇1,2βˆ’1and find the equilibrium

values of the transverse components 𝑀π‘₯ and 𝑀𝑦

and assume 𝑇2 ~ 𝑇1

V. Dobrovitski, S. 2

Bloch equations, weak driving: lineshape

𝑑𝑀π‘₯

𝑑𝑑= 𝑀𝑦𝐡 βˆ’

1

𝑇2𝑀π‘₯

𝑑𝑀𝑦

𝑑𝑑= βˆ’π‘€π‘₯𝐡 +𝑀𝑧

0β„Ž βˆ’1

𝑇2𝑀𝑦

𝑀+ = 𝑀π‘₯ + 𝑖𝑀𝑦 : 𝑑𝑀+

𝑑𝑑= βˆ’π‘– 𝑀+𝐡 βˆ’

1

𝑇2𝑀+ + 𝑖 𝑀𝑧

0β„Ž = βˆ’π‘„π‘€+ + 𝑖 𝑀𝑧0β„Ž

𝑀+ 𝑑 = πΆπ‘’βˆ’π‘„π‘‘ +𝑖 𝑀𝑧

0β„Ž

𝑄So that in equilibrium, at 𝑑 β†’ ∞ , 𝑀+ = ΀𝑖 𝑀𝑧

0β„Ž 𝑄

𝑀π‘₯ ∞ = β„Ž 𝑀𝑧0𝑇2 βˆ™

(πœ”πΏ βˆ’ πœ”) 𝑇2

1 + (πœ”πΏ βˆ’ πœ”)2 𝑇22

𝑀𝑦 ∞ = β„Ž 𝑀𝑧0𝑇2 βˆ™

1

1 + (πœ”πΏ βˆ’ πœ”)2 𝑇22

𝐻 𝑑 = Ԧ𝑒π‘₯ βˆ™ 2β„Ž cosπœ”π‘‘Driving in the lab frame:

𝑀 𝑑 = Ԧ𝑒π‘₯ βˆ™ 𝑀π‘₯ cosπœ”π‘‘ + Ԧ𝑒𝑦 βˆ™ 𝑀𝑦 cosπœ”π‘‘Magnetization in the lab frame:

Power absorbed per period: π‘Š = βˆ’π‘€ βˆ™ ΀𝑑𝐻 𝑑𝑑 ∝ β„Ž βˆ™ 𝑀𝑦 ∞

V. Dobrovitski, S. 2

Bloch equations, weak driving: lineshape

Absorption line 𝑃(πœ”) ∝ πœ’β€²β€²(πœ”) ∝ 𝑀𝑦 ∞ Dispersion line πœ’β€²(πœ”) ∝ 𝑀π‘₯ ∞

πœ”

𝑃 πœ”

πœ”πΏ

πœ”

πœ”πΏπœ’β€²(πœ”)

(πœ”πΏ βˆ’ πœ”) 𝑇2

1 + (πœ”πΏ βˆ’ πœ”)2 𝑇22

1

1 + (πœ”πΏ βˆ’ πœ”)2 𝑇22

Lorentzian

𝑃 πœ” =1

1 + (πœ”πΏ βˆ’ πœ”)2 𝑇22

What is the corresponding 𝒇(𝒕)?

Free decay, no driving, initial state 𝑀π‘₯ 0 β‰  0, 𝑀𝑦 0 = 𝑀𝑧 0 = 0

𝑑𝑀π‘₯

𝑑𝑑= 𝑀𝑦𝐡 βˆ’

1

𝑇2𝑀π‘₯

𝑑𝑀𝑦

𝑑𝑑= βˆ’π‘€π‘₯𝐡 βˆ’

1

𝑇2𝑀𝑦 β‡’

𝑓 𝑑 = eβˆ’π‘‘/𝑇2 cos(πœ”πΏ βˆ’ πœ”)𝑑

𝑀π‘₯ 𝑑 = 𝑀π‘₯ 0 eβˆ’π‘‘/𝑇2 cos 𝐡𝑑

Note: this is no longer a static noise field along Z, but still 𝑓 𝑑𝐹𝑇

𝑃(πœ”)

Fourier Transform